From 471a07b07567d6ad88597fbe8b4354798c681c65 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Thu, 24 Sep 2026 01:05:09 -0700 Subject: [PATCH 01/43] Fix pheasy anharmonic fitting and add fit options --- docs/user/codes/vasp.md | 18 +- pyproject.toml | 5 +- src/atomate2/common/flows/hiphive.py | 12 +- src/atomate2/common/flows/pheasy.py | 141 ++++-- src/atomate2/common/jobs/hiphive.py | 76 +-- src/atomate2/common/jobs/pheasy.py | 665 +++++++++++++++++---------- src/atomate2/common/jobs/phonons.py | 111 +++++ src/atomate2/vasp/flows/pheasy.py | 93 ++-- tests/common/jobs/test_pheasy.py | 304 ++++++++++++ tests/vasp/flows/test_pheasy.py | 65 +++ tutorials/pheasy_workflow.ipynb | 10 +- 11 files changed, 1131 insertions(+), 369 deletions(-) create mode 100644 tests/common/jobs/test_pheasy.py diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index edd4f46cc3..ee9e9ba3a7 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -345,12 +345,14 @@ phonon_flow = PhononMaker(min_length=15.0, store_force_constants=False).make( #### Pheasy Alternatively, users can accelerate the calculation of interatomic force constants using the machine-learning-based [Pheasy code](https://doi.org/10.48550/arXiv.2508.01020). -`Pheasy` can be installed with `pip install pheasy`. +The `pheasy` extra, `pip install "atomate2[pheasy]"`, installs the pheasy version this workflow needs, together with phonopy and ALM. +ALM is compiled from source. If that build fails, see the ALM instructions below. By design, these workflows have the same basic structure as the harmonic forcefield workflows and use [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) in part to compute the phonon spectrum. To use `Pheasy` in the previous example, we would replace the import string to `from atomate2.vasp.flows.pheasy import PhononMaker`. This workflow was used to build the Materials Project's Harmonic Phonon Database, described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1). -By default, this workflow does not compute anharmonic force constants, but can be extended to using the `cal_anhar_fcs` kwarg and the `ALAMODE` code. +By default, this workflow does not compute anharmonic force constants, but can be extended to using the `cal_anhar_fcs` kwarg. +ALM, from the ALAMODE package, counts the free force constants used to size the random displacement sets. To install ALAMODE, see their [installation guidelines](https://alamode.readthedocs.io/en/latest/install.html#). Linux and MacOS x86-64 users can try to install using conda forge: @@ -366,6 +368,7 @@ cd ALM/python python setup.py build pip install -e . ``` +The `pheasy` extra pins ALM to commit `f1d668f`. When building ALM by hand, check out that commit. NB: MacOS users will need to ensure that `gcc` and `g++` are used rather than `clang` - both can be installed with `homebrew`. Note also that `boost` and `eigen` can be installed via `homebrew`. For example, using `gcc-15` from `homebrew`, one might set: @@ -373,6 +376,17 @@ For example, using `gcc-15` from `homebrew`, one might set: export CC=gcc-15 ; CXX=g++-15 ; CXX_FLAGS=-DOPENMP ``` +With `cal_anhar_fcs=True`, the anharmonic force constants are fitted with LASSO to a second set of randomly displaced supercells. +The number of these supercells is set from the number of free force constants, so that the fit has 100 force equations per free force constant. +Unless `num_disp_anhar` is set, at least 20 supercells are used, and above 600 the job stops and asks for a shorter cutoff, a larger supercell or an explicit `num_disp_anhar`. An explicit `num_disp_anhar` is used as given. +`anhar_max_order` selects third-order force constants (3, the default) or third- and fourth-order force constants (4). +`anhar_fit_methods` selects how the second-order force constants are treated. +`"cocktail"` (the default) keeps them fixed to the harmonic fit, and `"one-shot"` fits them together with the higher orders and writes the results to a `one_shot` folder. +Both can be requested in one run. +If the cross-validated LASSO penalty lands on either end of the search, `10**anhar_alpha_min` or pheasy's `1e-2`, a warning is raised. +The harmonic and anharmonic LASSO fits are seeded, so that repeated runs give the same force constants. +The anharmonic force constants are written to files in the job folder and are not stored in the output document. + #### hiPhive The same force constants can instead be fitted with [hiPhive](https://hiphive.materialsmodeling.org/), which builds a cluster expansion of the force constant potential and fits it by regression. diff --git a/pyproject.toml b/pyproject.toml index db6701c909..75d5a4cbcc 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -52,8 +52,9 @@ mp = ["mp-api>=0.37.5"] # phonon.save -> phonopy.load round-trip used by the Grüneisen workflow # ("Force constants shape disagrees with crystal structure setting"). phonons = ["phonopy>=2.43,<5", "seekpath>=2.0.0"] -pheasy = ["hiphive==1.3.1", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@support-disp-force-matrix-input"] -alamode = ["alm @ git+https://github.com/ttadano/ALM.git@develop#subdirectory=python"] +# the pheasy fork adds the --disp_matrix_file and --force_matrix_file options +pheasy = ["atomate2[phonons,alamode]", "hiphive==1.3.1", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@e67a777ecfde5ab368d71167837b099df75cfd4c"] +alamode = ["alm @ git+https://github.com/ttadano/ALM.git@f1d668fdee66e7e7218a04c88daf19d0e14fce0c#subdirectory=python"] hiphive = ["hiphive==1.3.1", "trainstation>=1.0", "atomate2[phonons,alamode]"] lobster = ["ijson>=3.2.2", "lobsterpy>=0.6.0"] defects = [ diff --git a/src/atomate2/common/flows/hiphive.py b/src/atomate2/common/flows/hiphive.py index 7fb63172fb..37bbd9a543 100644 --- a/src/atomate2/common/flows/hiphive.py +++ b/src/atomate2/common/flows/hiphive.py @@ -1,4 +1,4 @@ -"""Flow for calculating (an)harmonic FCs and phonon renormalisation with hiPhive.""" +"""Flow for calculating harmonic FCs with hiPhive.""" from __future__ import annotations @@ -6,6 +6,8 @@ from dataclasses import dataclass, field from typing import TYPE_CHECKING, Literal +from pymatgen.util.due import Doi, due + from atomate2.common.flows.phonons import BasePhononMaker as PurePhonopyMaker from atomate2.common.jobs.hiphive import ( generate_frequencies_eigenvectors, @@ -28,6 +30,14 @@ SUPPORTED_CODES = frozenset(("vasp", "aims", "forcefields")) +@due.dcite( + Doi("10.1002/adts.201800184"), + description="hiPhive, force constant potentials by regression.", +) +@due.dcite( + Doi("10.1088/0953-8984/26/22/225402"), + description="ALM, used to count the free force constants.", +) @dataclass class BasePhononMaker(PurePhonopyMaker, ABC): """Maker to calculate harmonic phonons with the cluster-expansion code hiPhive. diff --git a/src/atomate2/common/flows/pheasy.py b/src/atomate2/common/flows/pheasy.py index 12ed008b71..158c90efab 100644 --- a/src/atomate2/common/flows/pheasy.py +++ b/src/atomate2/common/flows/pheasy.py @@ -1,4 +1,4 @@ -"""Flow for calculating (an)harmonic FCs and phonon renormalisation with pheasy.""" +"""Flow for calculating harmonic and anharmonic FCs with pheasy.""" from __future__ import annotations @@ -10,6 +10,7 @@ from atomate2.common.flows.phonons import BasePhononMaker as PurePhonopyMaker from atomate2.common.jobs.pheasy import ( + _check_anharmonic_settings, generate_frequencies_eigenvectors, generate_phonon_displacements, get_supercell_size, @@ -17,6 +18,7 @@ from atomate2.common.jobs.phonons import run_phonon_displacements if TYPE_CHECKING: + from collections.abc import Sequence from pathlib import Path from emmet.core.math import Matrix3D @@ -34,24 +36,34 @@ Doi("10.26434/chemrxiv.15004632/v1"), description="Materials Project's Harmonic Phonon Database.", ) +@due.dcite( + Doi("10.48550/arXiv.2508.01020"), + description="Pheasy code for (an)harmonic force constants.", +) +@due.dcite( + Doi("10.1088/0953-8984/26/22/225402"), + description="ALM, used to count the free force constants.", +) @dataclass class BasePhononMaker(PurePhonopyMaker, ABC): - """Maker to calculate harmonic phonons with LASSO-based ML code Pheasy. - - Calculate the zero-K harmonic phonons of a material and higher-order FCs. - Initially, a tight structural relaxation is performed to obtain a structure - without forces on the atoms. Subsequently, supercells with all atoms displaced - by a small amplitude (generally using 0.01 A) are generated and accurate forces - are computed for these structures for the second order force constants. With the - help of pheasy (LASSO technique), these forces are then converted into a dynamical - matrix. In this Workflow, we separate the harmonic phonon calculations and - anharmonic force constants calculations. To correct for polarization effects, a + """Maker to calculate harmonic phonons and anharmonic FCs with Pheasy. + + Calculate the zero-K harmonic phonons of a material and, optionally, its + anharmonic FCs. Initially, a tight structural relaxation is performed to obtain + a structure without forces on the atoms. Subsequently, displaced supercells + (generally using 0.01 A) are generated and accurate forces are computed for + them. If phonopy needs more than three finite displacements, all atoms are + displaced randomly and pheasy fits the second order force constants with LASSO. + Otherwise, the finite displacements are used with a least-squares fit. These + force constants are then converted into a dynamical matrix. In this Workflow, + we separate the harmonic phonon calculations and anharmonic force constants + calculations. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can be performed. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. For the anharmonic force constants, the supercells with all atoms displaced by a larger amplitude (generally using 0.08 A) are generated and accurate forces are computed for these structures. With the help of pheasy (LASSO technique), - the third- and fourth-order force constants are extracted at once. + the third-order (and optionally fourth-order) force constants are extracted. .. Note:: It is heavily recommended to symmetrize the structure before passing it to @@ -59,10 +71,8 @@ class BasePhononMaker(PurePhonopyMaker, ABC): displacement calculations will be required for pheasy phonon calculation. It is recommended to check the convergence parameters here and adjust them if necessary. The default might not be strict enough for your specific case. - Additionally, for high-throughoput calculations, it is recommended to calculate - the residual forces on the atoms in the supercell after the relaxation. Then the - forces on displaced supercells can deduct the residual forces to reduce the - error in the dynamical matrix. + The residual forces of the undisplaced supercell are always subtracted from + the forces of the displaced supercells. Parameters ---------- @@ -83,35 +93,62 @@ class BasePhononMaker(PurePhonopyMaker, ABC): number of displacements to be generated using a random-displacement approach for harmonic phonon calculations. The default value is 0 and the number of displacements is automatically determined by the number of atoms in the - supercell and its space group. + supercell and its space group. Not used when phonopy needs at most three + finite displacements. cal_anhar_fcs: bool - if set to True, anharmonic force constants(FCs) up to fourth-order FCs will - be calculated. The default value is False, and only harmonic phonons will - be calculated. + if set to True, anharmonic force constants(FCs) up to order + anhar_max_order will be calculated. The default value is False, and only + harmonic phonons will be calculated. displacement_anhar: float - displacement distance for anharmonic force constants(FCs) up to fourth-order - FCs, for most cases 0.08 A is a good choice, but it can be increased to 0.1 A. + displacement distance for the anharmonic force constants(FCs). The default + is 0.08 A. num_disp_anhar: int number of displacements to be generated using a random-displacement approach - for anharmonic phonon calculations. The default value is 0 and the number of - displacements is automatically determined by the number of atoms in the - supercell, cutoff distance for anharmonic FCs its space group. generally, - 50 large-distance displacements are enough for most cases. + for anharmonic phonon calculations. A non-zero value is used as given. The + default value is 0, and then the number is set so that the fit has 100 force + equations per free force constant, with at least 20 displaced supercells. + Above 600 the job stops. The free force constants are counted with ALM, which + uses its own symmetry search, for this supercell and fcs_cutoff_radius. The + second-order FCs are included when "one-shot" is requested. + anhar_max_order: int + highest order of the anharmonic FCs, 3 or 4. The default of 3 fits the + third-order FCs. 4 also fits fourth-order FCs. + anhar_fit_methods: Sequence[Literal["cocktail", "one-shot"]] + how the anharmonic FCs are fitted to the large-distance dataset. + "cocktail" keeps the second-order FCs fixed to the harmonic fit and fits + only the higher orders. "one-shot" fits the second- and higher-order FCs + together from the same dataset and writes them to the "one_shot" folder. + Both can be requested. The default is ("cocktail",). The cocktail FCs are + written to the job folder, and the one-shot FCs, including fc2.hdf5, to its + one_shot subfolder: FORCE_CONSTANTS_3RD and fc3.hdf5, plus + FORCE_CONSTANTS_4TH and fc4.hdf5 at fourth order. They are not stored in the + output document. The LASSO fits are seeded, so a run is reproducible. With + few displaced supercells, the one-shot result depends on that seed. + anhar_alpha_min: int + base-10 exponent of the smallest LASSO penalty tried by cross-validation + in the anharmonic fits. It must be an integer below -2. The default of -12 + is below pheasy's own default of -6. If the chosen penalty lands on either + end of the search, 10**anhar_alpha_min or pheasy's 1e-2, a warning is + raised. fcs_cutoff_radius: list - cutoff distance for anharmonic force constants(FCs) up to fourth-order FCs. - The default value is [-1, 12, 10], which means that the cutoff distance for - second-order FCs is the Wigner-Seitz cell boundary and the cutoff distance - for third-order FCs is 12 Borh, and the cutoff distance for fourth-order FCs - is 10 Bohr. Generally, the default value is good enough. + cutoff distance in Bohr for each FC order, starting at second order. The + default value is [-1, 12, 10]. The first entry is not used, since pheasy + fits the second-order FCs without a cutoff. The second and third entries + are the cutoffs for third- and fourth-order FCs. The cutoff of each fitted + order, up to anhar_max_order, must be positive. Longer cutoffs increase + the number of free FCs, and with it the number of displaced supercells. min_length: float minimum length of lattice constants will be used to create the supercell, - the default value is 14.0 A. In most cases, the default value is good - enough, but it can be increased for larger supercells. - prefer_90_degrees: bool - if set to True, supercell algorithm will first try to find a supercell - with 3 90 degree angles. + the default value is 8.0 A. It can be increased for larger supercells. + max_atoms: float | None + maximum number of atoms in the supercell. + force_90_degrees: bool + if set to True, only supercells with three 90 degree angles are allowed. + force_diagonal: bool + if set to True, only diagonal supercell matrices are allowed. The pheasy + commands take the diagonal of the supercell matrix. get_supercell_size_kwargs: dict - kwargs that will be passed to get_supercell_size to determine supercell size + not used by this workflow. use_symmetrized_structure: str allowed strings: "primitive", "conventional", None @@ -174,14 +211,12 @@ class BasePhononMaker(PurePhonopyMaker, ABC): cal_anhar_fcs: bool = False displacement_anhar: float = 0.08 num_disp_anhar: int = 0 + anhar_max_order: int = 3 + anhar_fit_methods: Sequence[Literal["cocktail", "one-shot"]] = ("cocktail",) + anhar_alpha_min: int = -12 fcs_cutoff_radius: list = field( default_factory=lambda: [-1, 12, 10] ) # units in Bohr - renorm_phonon: bool = False - renorm_temp: list = field(default_factory=lambda: [100, 700, 100]) - cal_ther_cond: bool = False - ther_cond_mesh: list = field(default_factory=lambda: [20, 20, 20]) - ther_cond_temp: list = field(default_factory=lambda: [100, 700, 100]) min_length: float | None = 8.0 max_atoms: float | None = 200 force_90_degrees: bool = True @@ -203,6 +238,17 @@ class BasePhononMaker(PurePhonopyMaker, ABC): store_force_constants: bool = True socket: bool = False + def __post_init__(self) -> None: + """Check the anharmonic settings before any calculation is run.""" + _check_anharmonic_settings( + self.anhar_max_order, + self.anhar_fit_methods, + self.cal_anhar_fcs, + self.fcs_cutoff_radius, + self.anhar_alpha_min, + self.num_disp_anhar, + ) + def get_displacements( self, structure: Structure, supercell_matrix: Matrix3D ) -> Job | Flow: @@ -232,6 +278,8 @@ def get_displacements( use_symmetrized_structure=self.use_symmetrized_structure, kpath_scheme=self.kpath_scheme, code=self.code, + anhar_max_order=self.anhar_max_order, + anhar_fit_methods=self.anhar_fit_methods, ) def run_displacements( @@ -309,11 +357,6 @@ def get_results( displacement=self.displacement, cal_anhar_fcs=self.cal_anhar_fcs, fcs_cutoff_radius=self.fcs_cutoff_radius, - renorm_phonon=self.renorm_phonon, - renorm_temp=self.renorm_temp, - cal_ther_cond=self.cal_ther_cond, - ther_cond_mesh=self.ther_cond_mesh, - ther_cond_temp=self.ther_cond_temp, sym_reduce=self.sym_reduce, symprec=self.symprec, use_symmetrized_structure=self.use_symmetrized_structure, @@ -332,6 +375,10 @@ def get_results( optimization_run_uuid=optimization_run_uuid, create_thermal_displacements=self.create_thermal_displacements, store_force_constants=self.store_force_constants, + num_displaced_supercells=self.num_displaced_supercells, + anhar_max_order=self.anhar_max_order, + anhar_fit_methods=self.anhar_fit_methods, + anhar_alpha_min=self.anhar_alpha_min, **self.generate_frequencies_eigenvectors_kwargs, ) diff --git a/src/atomate2/common/jobs/hiphive.py b/src/atomate2/common/jobs/hiphive.py index da27fb44c3..f1b073707e 100644 --- a/src/atomate2/common/jobs/hiphive.py +++ b/src/atomate2/common/jobs/hiphive.py @@ -38,6 +38,8 @@ from atomate2.common.jobs.phonons import ( _generate_phonon_object, _get_kpath, + _get_num_harmonic_supercells, + _get_num_irreducible_fcs, _run_band_structure_and_plot, _run_total_dos_and_plot, ) @@ -48,20 +50,14 @@ logger = logging.getLogger(__name__) -try: - from alm import ALM -except ImportError: - ALM = None - -# Safety margin below hiPhive's maximum allowed cutoff, in Angstrom. -# Configurations per suggested displacement set. ALM sizes num_disp_sc so the -# equation count reaches its own free-parameter tally, and this scales from -# there. pheasy uses 1.8. hiPhive's cluster space has a different, smaller -# parameter count, and the ratio between the two varies by a factor of three -# across materials, so 1.8 leaves a low-symmetry cell with too little data for -# a LASSO fit and the modes come out soft. +# Configurations per suggested displacement set. The minimum set is sized from +# ALM's free-parameter tally so the equation count reaches it (see +# _get_num_harmonic_supercells), and this scales from there. pheasy uses the +# same 1.8. hiPhive's own cluster space has a smaller parameter count than +# ALM's tally, and the ratio between the two differs between materials. _N_CONFIG_MULTIPLIER = 1.8 +# Safety margin below hiPhive's maximum allowed cutoff, in Angstrom. _CUTOFF_MARGIN = 0.1 # hiPhive refuses a cutoff that clears a neighbour shell by less than its @@ -290,11 +286,12 @@ def generate_phonon_displacements( random_seed: int | None = 103, verbose: bool = False, ) -> list[Structure]: - """Generate small-distance perturbed structures with phonopy based on two ways. + """Generate the displaced supercells with phonopy. - 1. finite-displacment method (one displaced atom) when the displacement number - is less than 3. 2. random-displacement method (all-displaced atoms) when the - displacement number is more than 3. + The finite-displacement method (one displaced atom) is used when phonopy + needs at most three displacements, and the random-displacement method (all + atoms displaced) otherwise. The undisplaced supercell is added last, for + the residual forces. Parameters ---------- @@ -322,11 +319,6 @@ def generate_phonon_displacements( Whether to log warnings. """ - # TODO: remove ALMODE dependence for 2nd order force constants - if not ALM: - raise ImportError( - "Error importing ALM. Please ensure the 'alm' library is installed." - ) phonon = _generate_phonon_object( structure, supercell_matrix, @@ -353,46 +345,28 @@ def generate_phonon_displacements( # of the matrix can not always guarantee accurate results, you # may need to displace more random configurations. Use at least one or # two more configurations based on the suggested number of displacements. - supercell_ph = phonon.supercell - lattice = supercell_ph.cell - positions = supercell_ph.scaled_positions - numbers = supercell_ph.numbers - natom = len(numbers) - - # get the number of free parameters of 2ND FCs from ALM, labeled as n_fp - with ALM(lattice, positions, numbers) as alm: - alm.define(1) - alm.suggest() - n_fp = alm._get_number_of_irred_fc_elements(1) # noqa: SLF001 - - # get the number of displaced supercells based on the number of free parameters - num_disp_sc = int(np.ceil(n_fp / (3.0 * natom))) + num_har = _get_num_harmonic_supercells( + phonon, num_displaced_supercells, multiplier=_N_CONFIG_MULTIPLIER + ) if verbose: + (n_fp,) = _get_num_irreducible_fcs(phonon.supercell, 2) logger.info( - f"There are {n_fp} free parameters for the second-order " - "force constants (FCs)." - f"There are {3 * natom * num_disp_sc} equations used to " - "obtain the second-order FCs." - "CAUTION: you may need to increase the number of " - "displacements in some cases." - "If the number of atoms in the supercell are less than 100 and " + f"There are {n_fp} free parameters for the second-order force " + f"constants (FCs), and {num_har} displaced supercells are used to " + "fit them. CAUTION: you may need to increase the number of " + "displacements in some cases. " + "If the number of atoms in the supercell is less than 100 and " "all lattice constants are less than 10 Å, the user is advised " "to use 1-2 more randomly-displaced configurations." ) - # get the number of displaced supercells from phonopy to compared with the number - # of 3, if the number of displaced supercells is less than 3, we will use the finite - # displacement method to generate the supercells. Otherwise, we will use the random - # displacement method to generate the supercells. + # if phonopy needs more than three finite displacements, we use the random + # displacement method instead if len(phonon.displacements) > 3: phonon.generate_displacements( distance=displacement, - number_of_snapshots=( - num_displaced_supercells - if num_displaced_supercells != 0 - else int(np.ceil(num_disp_sc * _N_CONFIG_MULTIPLIER)) + 1 - ), + number_of_snapshots=num_har, random_seed=random_seed, ) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 29c80cfb58..eb2648b817 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -3,8 +3,12 @@ from __future__ import annotations import logging +import numbers +import re import shlex +import shutil import subprocess +import warnings from pathlib import Path from typing import TYPE_CHECKING @@ -18,7 +22,7 @@ from hiphive.utilities import extract_parameters from jobflow import job from packaging.version import parse as parse_version -from phonopy.file_IO import parse_FORCE_CONSTANTS, write_force_constants_to_hdf5 +from phonopy.file_IO import parse_FORCE_CONSTANTS from phonopy.interface.vasp import write_vasp from phonopy.structure.symmetry import symmetrize_borns_and_epsilon from pymatgen.core import Structure @@ -31,25 +35,23 @@ ) from atomate2.common.jobs.phonons import ( + ANGSTROM_TO_BOHR, _generate_phonon_object, _get_kpath, + _get_num_harmonic_supercells, + _get_num_irreducible_fcs, _run_band_structure_and_plot, _run_total_dos_and_plot, ) if TYPE_CHECKING: + from collections.abc import Sequence + from emmet.core.math import Matrix3D + from phonopy.structure.atoms import PhonopyAtoms logger = logging.getLogger(__name__) -try: - from alm import ALM -except ImportError: - ALM = None - -# CODATA 2018: 1 Angstrom = 1 / 0.529177210903 Bohr -ANGSTROM_TO_BOHR = 1.8897261246257702 - _DEFAULT_FILE_PATHS = { "force_displacements": "dataset_forces.npy", "displacements": "dataset_disps.npy", @@ -65,8 +67,283 @@ "harmonic_force_matrix": "force_matrix.npy", "anharmonic_force_matrix": "force_matrix_anhar.npy", "website": "phonon_website.json", + "one_shot_dir": "one_shot", + "anharmonic_fit_log": "pheasy_anharmonic_fit.log", } +# The anharmonic training set is sized so that the fit has this many force +# equations per free force constant. The floor keeps the set from becoming +# very small. Above the ceiling the job stops instead of requesting more +# displaced supercells. +_EQUATIONS_PER_FREE_FC = 100 +_MIN_NUM_DISP_ANHAR = 20 +_MAX_NUM_DISP_ANHAR = 600 + +_ANHARMONIC_FIT_METHODS = ("cocktail", "one-shot") + +# many-body terms kept in the anharmonic fit for each maximum order, as passed +# to pheasy with --nbody and to ALM when counting the free force constants +_NBODY = {3: [2, 3], 4: [2, 3, 3]} + + +def _get_num_anharmonic_supercells( + supercell: PhonopyAtoms, + num_disp_anhar: int, + anhar_max_order: int, + fcs_cutoff_radius: Sequence[float], + anhar_fit_methods: Sequence[str], +) -> int: + """ + Get the number of randomly displaced supercells for the anharmonic fit. + + A non-zero num_disp_anhar is returned as given. Otherwise, each supercell + gives 3 * natom force equations, and the number of supercells is set so + that there are _EQUATIONS_PER_FREE_FC equations per free force constant, + with at least _MIN_NUM_DISP_ANHAR supercells. Above _MAX_NUM_DISP_ANHAR a + ValueError is raised. The free force constants are those of third (and + fourth) order, plus those of second order when the one-shot fit is + requested, since it fits all orders together. Second-order force constants + are counted without a cutoff, as pheasy fits them. ALM counts the + irreducible force constants before the acoustic sum rules are applied, with + its own symmetry search, so the count is expected to be at least the number + pheasy fits. + + Parameters + ---------- + supercell: PhonopyAtoms + Supercell used for the force constant fit. + num_disp_anhar: int + Number of displaced supercells requested by the user, 0 for automatic. + anhar_max_order: int + Highest force constant order in the anharmonic fit, 3 or 4. + fcs_cutoff_radius: Sequence[float] + Cutoff radius in Bohr for each order, starting at second order. + anhar_fit_methods: Sequence[str] + Anharmonic fit methods that will use this dataset. + + Returns + ------- + int + Number of anharmonic displaced supercells. + """ + if num_disp_anhar != 0: + return num_disp_anhar + # pheasy fits the second-order force constants without a cutoff + cutoffs = [-1, *fcs_cutoff_radius[1:]] + n_irred = _get_num_irreducible_fcs( + supercell, anhar_max_order, cutoffs, nbody=_NBODY[anhar_max_order] + ) + n_free = sum(n_irred[1:]) + if "one-shot" in anhar_fit_methods: + n_free += n_irred[0] + natom = len(supercell.numbers) + num = int(np.ceil(_EQUATIONS_PER_FREE_FC * n_free / (3.0 * natom))) + num = max(num, _MIN_NUM_DISP_ANHAR) + if num > _MAX_NUM_DISP_ANHAR: + raise ValueError( + f"{num} displaced supercells are needed for {n_free} free force " + f"constants, more than the limit of {_MAX_NUM_DISP_ANHAR}. Reduce " + "fcs_cutoff_radius, use a larger supercell, or set num_disp_anhar " + "to accept the cost." + ) + return num + + +def _check_anharmonic_settings( + anhar_max_order: int, + anhar_fit_methods: Sequence[str], + cal_anhar_fcs: bool = True, + fcs_cutoff_radius: Sequence[float] | None = None, + anhar_alpha_min: int | None = None, + num_disp_anhar: int = 0, +) -> None: + """ + Check the settings of the anharmonic force constant fit. + + Parameters + ---------- + anhar_max_order: int + Highest force constant order in the anharmonic fit. + anhar_fit_methods: Sequence[str] + Anharmonic fit methods. + cal_anhar_fcs: bool + Whether the anharmonic force constants are calculated. + fcs_cutoff_radius: Sequence[float] | None + Cutoff radius in Bohr for each order, starting at second order. + anhar_alpha_min: int | None + Base-10 exponent of the smallest LASSO penalty. pheasy only accepts an + integer, below its largest penalty of 1e-2. + num_disp_anhar: int + Number of anharmonic displaced supercells requested by the user. + """ + if anhar_max_order not in (3, 4): + raise ValueError(f"anhar_max_order must be 3 or 4, not {anhar_max_order}.") + unknown = set(anhar_fit_methods) - set(_ANHARMONIC_FIT_METHODS) + if ( + unknown + or len(anhar_fit_methods) == 0 + or len(set(anhar_fit_methods)) != len(anhar_fit_methods) + ): + raise ValueError( + f"anhar_fit_methods must be a non-empty subset of " + f"{_ANHARMONIC_FIT_METHODS} without repeats, not {list(anhar_fit_methods)}." + ) + if ( + isinstance(num_disp_anhar, bool) + or not isinstance(num_disp_anhar, numbers.Integral) + or num_disp_anhar < 0 + ): + raise ValueError( + f"num_disp_anhar must be a non-negative integer, not {num_disp_anhar!r}." + ) + if cal_anhar_fcs and fcs_cutoff_radius is not None: + # one cutoff per order from 3 to anhar_max_order, after the fc2 entry + anhar_radii = list(fcs_cutoff_radius[1 : anhar_max_order - 1]) + # pheasy reads a negative cutoff as a neighbour shell, ALM as no cutoff + if len(anhar_radii) != anhar_max_order - 2 or min(anhar_radii) <= 0: + raise ValueError( + f"fcs_cutoff_radius needs a positive cutoff in Bohr for each order " + f"from 3 to {anhar_max_order}, not {list(fcs_cutoff_radius)}." + ) + if anhar_alpha_min is not None and ( + isinstance(anhar_alpha_min, bool) + or not isinstance(anhar_alpha_min, numbers.Integral) + or anhar_alpha_min >= -2 + ): + raise ValueError( + f"anhar_alpha_min must be an integer below -2, not {anhar_alpha_min!r}." + ) + + +def _check_lasso_alpha(log_file: Path, alpha_min: int) -> None: + """ + Warn if the cross-validated LASSO penalty is on either bound of the search. + + On the lower bound, the search wanted an even weaker penalty than it was + allowed to try, so the fitted force constants depend on that bound. On the + upper bound, the penalty is the strongest one tried. Raises an error if + pheasy wrote no log or no penalty. + + Parameters + ---------- + log_file: Path + Log file written by pheasy during the fit. + alpha_min: int + Base-10 exponent of the smallest penalty in the search. + """ + if not log_file.exists(): + raise FileNotFoundError( + f"pheasy exited without writing {log_file}, so the result of the " + "anharmonic fit is unknown." + ) + match = re.search(r"alpha_opt:\s*([-+0-9.eE]+)", log_file.read_text()) + if match is None: + raise RuntimeError(f"No LASSO alpha found in {log_file}, the fit failed.") + alpha_opt = float(match.group(1)) + match_max = re.search(r"alpha_max:\s*1e([-+0-9]+)", log_file.read_text()) + if match_max is not None and alpha_opt >= 10.0 ** int(match_max.group(1)) * ( + 1 - 1e-6 + ): + warnings.warn( + f"The LASSO penalty chosen by cross-validation ({alpha_opt:e}) is on " + f"the upper bound in {log_file}. The fitted force constants may be " + "heavily penalized. Check them.", + stacklevel=2, + ) + if alpha_opt <= 10.0**alpha_min * (1 + 1e-6): + warnings.warn( + f"The LASSO penalty chosen by cross-validation ({alpha_opt:e}) is on " + f"the lower bound 1e{alpha_min} in {log_file}. The anharmonic force " + "constants depend on this bound and may be wrong. Lower " + "anhar_alpha_min and refit.", + stacklevel=2, + ) + + +def _run_anharmonic_fit( + method: str, + supercell_matrix: np.ndarray, + symprec: float, + anhar_max_order: int, + fcs_cutoff_radius: Sequence[float], + num_anhar: int, + anhar_alpha_min: int, + work_dir: Path, + random_seed: int | None = 103, +) -> None: + """ + Fit the anharmonic force constants with pheasy using LASSO. + + Both methods use the same randomly displaced supercells. + + - "cocktail" keeps the second-order force constants fixed to the harmonic + fit (FORCE_CONSTANTS in work_dir) and fits only the higher orders. + - "one-shot" fits the second- and higher-order force constants together. + + pheasy writes FORCE_CONSTANTS_3RD and fc3.hdf5 to work_dir, and + FORCE_CONSTANTS_4TH and fc4.hdf5 for fourth order. The one-shot fit also + writes its second-order force constants, fc2.hdf5. + + Parameters + ---------- + method: str + "cocktail" or "one-shot". + supercell_matrix: np.ndarray + Diagonal supercell matrix. + symprec: float + Symmetry precision, the same one used for the displacements. + anhar_max_order: int + Highest force constant order, 3 or 4. + fcs_cutoff_radius: Sequence[float] + Cutoff radius in Bohr for each order, starting at second order. + num_anhar: int + Number of anharmonic displaced supercells. + anhar_alpha_min: int + Base-10 exponent of the smallest LASSO penalty in the search. + work_dir: Path + Folder holding POSCAR and the anharmonic displacement and force + matrices. + random_seed: int | None + Seed for the random coordinate descent in pheasy's LASSO fit. Without + it, the cross-validated penalty and the fitted force constants change + from run to run on the same forces. + """ + dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) + base = f"pheasy --dim {dim} -w {anhar_max_order} --symprec {float(symprec)}" + cutoffs = f"--c3 {float(fcs_cutoff_radius[1] / ANGSTROM_TO_BOHR)}" + if anhar_max_order == 4: + cutoffs += f" --c4 {float(fcs_cutoff_radius[2] / ANGSTROM_TO_BOHR)}" + nbody = "--nbody " + " ".join(str(n) for n in _NBODY[anhar_max_order]) + fix_fc2 = "--fix_fc2 --fc2_fmt PHONOPY " if method == "cocktail" else "" + log_file = _DEFAULT_FILE_PATHS["anharmonic_fit_log"] + seed = f"--seed {int(random_seed)} " if random_seed is not None else "" + + commands = [ + # clusters and orbits + f"{base} -s {nbody} {cutoffs}", + # null space + f"{base} -c", + # sensing matrix from the displacement matrix + ( + f"{base} -d --ndata {int(num_anhar)} --disp_file " + f"--disp_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_displacements']}" + ), + # LASSO fit. OLS, pheasy's default, gives dense force constants. + # --std and --rasr are not passed to the anharmonic fit. + ( + f"{base} -f {fix_fc2}-l LASSO --alpha_min {anhar_alpha_min} {seed}" + f"--ndata {int(num_anhar)} --hdf5 " + f"--force_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_force_matrix']} " + f"-o {log_file}" + ), + ] + # pheasy appends to its log, so remove the log of an earlier fit + (work_dir / log_file).unlink(missing_ok=True) + for cmd in commands: + subprocess.run(shlex.split(cmd), cwd=work_dir, check=True) + + _check_lasso_alpha(work_dir / log_file, anhar_alpha_min) + @job def get_supercell_size( @@ -77,7 +354,7 @@ def get_supercell_size( force_diagonal: bool, ) -> list[list[float]]: """ - Determine supercell size with given min_length and max_length. + Determine the supercell matrix with pymatgen's CubicSupercellTransformation. Parameters ---------- @@ -85,14 +362,12 @@ def get_supercell_size( Input structure that will be used to determine supercell min_length: float minimum length of cell in Angstrom - max_length: float - maximum length of cell in Angstrom - prefer_90_degrees: bool - if True, the algorithm will try to find a cell with 90 degree angles first - allow_orthorhombic: bool - if True, orthorhombic supercells are allowed - **kwargs: - Additional parameters that can be set. + max_atoms: int + maximum number of atoms in the supercell + force_90_degrees: bool + if True, only supercells with three 90 degree angles are allowed + force_diagonal: bool + if True, only diagonal supercell matrices are allowed """ transformation = CubicSupercellTransformation( min_length=min_length, @@ -115,21 +390,25 @@ def generate_phonon_displacements( cal_anhar_fcs: bool, displacement_anhar: float, num_disp_anhar: int, - fcs_cutoff_radius: list[int], + fcs_cutoff_radius: list[float], sym_reduce: bool, symprec: float, use_symmetrized_structure: str | None, kpath_scheme: str, code: str, + anhar_max_order: int = 3, + anhar_fit_methods: Sequence[str] = ("cocktail",), random_seed: int | None = 103, verbose: bool = False, ) -> list[Structure]: - """Generate small-distance perturbed structures with phonopy based on two ways. + """Generate the displaced supercells with phonopy. - (we will directly use the pheasy to generate the supercell in the near future) - 1. finite-displacment method (one displaced atom) when the displacement number - is less than 3. 2. random-displacement method (all-displaced atoms) when the - displacement number is more than 3. + The small-distance set for the harmonic force constants uses the + finite-displacement method (one displaced atom) when phonopy needs at most + three displacements, and the random-displacement method (all atoms + displaced) otherwise. With cal_anhar_fcs, a large-distance set of randomly + displaced supercells is added for the anharmonic force constants. The + undisplaced supercell is added last, for the residual forces. Parameters ---------- @@ -138,13 +417,20 @@ def generate_phonon_displacements( supercell_matrix: np.array array to describe supercell matrix displacement: float - displacement in Angstrom (default: 0.01) + displacement in Angstrom num_displaced_supercells: int - number of displaced supercells defined by users + number of harmonic random displacements, 0 for automatic. Not used when + phonopy needs at most three finite displacements. cal_anhar_fcs: bool - TODO : docstr + if True, also generate the large-distance displacements used for the + anharmonic force constants displacement_anhar: float - TODO : docstr + displacement in Angstrom for the anharmonic force constants + num_disp_anhar: int + number of anharmonic displaced supercells, 0 to set it from the number + of free force constants + fcs_cutoff_radius: list[float] + cutoff radius in Bohr for each force constant order, from second order sym_reduce: bool if True, symmetry will be used to generate displacements symprec: float @@ -155,17 +441,17 @@ def generate_phonon_displacements( scheme to generate kpath code: str code to perform the computations + anhar_max_order: int + highest anharmonic force constant order, 3 or 4 + anhar_fit_methods: Sequence[str] + anharmonic fit methods, used to size the anharmonic dataset random_seed : int | None = 103 - Random seed to use in generating randomly-displaced structures. + Random seed for the harmonic random displacements. The anharmonic set + uses random_seed + 1. verbose : bool = False - Whether to log warnings. + Whether to log warnings and the numbers of displaced supercells. """ - # TODO: remove ALMODE dependence for 2nd order force constants - if not ALM: - raise ImportError( - "Error importing ALM. Please ensure the 'alm' library is installed." - ) phonon = _generate_phonon_object( structure, supercell_matrix, @@ -178,91 +464,58 @@ def generate_phonon_displacements( verbose=verbose, ) - # 1. the ALM module is used to determine the number of free parameters - # (irreducible force constants) corresponding to the second order - # force constants (FCs) given a supercell. - # 2. Based on the number of free parameters, we can determine how many - # displaced supercells we need to use to extract the second order force - # constants. Generally, the number of free parameters should be less than - # 3 * natom(supercell) * num_displaced_supercells. However, the full rank - # of the matrix can not always guarantee accurate results, you - # may need to displace more random configurations. Use at least one or - # two more configurations based on the suggested number of displacements. supercell_ph = phonon.supercell - lattice = supercell_ph.cell - positions = supercell_ph.scaled_positions - numbers = supercell_ph.numbers - natom = len(numbers) - - # get the number of free parameters of 2ND FCs from ALM, labeled as n_fp - with ALM(lattice, positions, numbers) as alm: - alm.define(1) - alm.suggest() - n_fp = alm._get_number_of_irred_fc_elements(1) # noqa: SLF001 - - # get the number of displaced supercells based on the number of free parameters - num_disp_sc = int(np.ceil(n_fp / (3.0 * natom))) + num_har = _get_num_harmonic_supercells(phonon, num_displaced_supercells) if verbose: + (n_fp,) = _get_num_irreducible_fcs(supercell_ph, 2) logger.info( - f"There are {n_fp} free parameters for the second-order " - "force constants (FCs)." - f"There are {3 * natom * num_disp_sc} equations used to " - "obtain the second-order FCs." - "CAUTION: you may need to increase the number of " - "displacements in some cases." - "If the number of atoms in the supercell are less than 100 and " - "all lattice constants are less than 10 Å, the user is advised " - "to use 1-2 more randomly-displaced configurations." + f"There are {n_fp} free parameters for the second-order force " + f"constants (FCs), and {num_har} displaced supercells are used to " + "fit them. CAUTION: you may need to increase the number " + "of displacements in some cases. If the number of atoms in the " + "supercell is less than 100 and all lattice constants are less than " + "10 Å, the user is advised to use 1-2 more randomly-displaced " + "configurations." ) - # get the number of displaced supercells from phonopy to compared with the number - # of 3, if the number of displaced supercells is less than 3, we will use the finite - # displacement method to generate the supercells. Otherwise, we will use the random - # displacement method to generate the supercells. + # if phonopy needs more than three finite displacements, we use the random + # displacement method instead if len(phonon.displacements) > 3: phonon.generate_displacements( distance=displacement, - number_of_snapshots=( - num_displaced_supercells - if num_displaced_supercells != 0 - else int(np.ceil(num_disp_sc * 1.8)) + 1 - ), + number_of_snapshots=num_har, random_seed=random_seed, ) supercells = phonon.supercells_with_displacements displacements = [get_pmg_structure(cell) for cell in supercells] - # Here, the ALAMODE code is used to determine the number of - # third and fourth-order FCs are needed for the supercell if cal_anhar_fcs: - # Due to the cutoff radius of the force constants use the unit of Bohr in ALM, - # we need to convert the cutoff radius from Angstrom to Bohr. - with ALM(lattice * ANGSTROM_TO_BOHR, positions, numbers) as alm: - # Define the force constants up to fourth order with a list of - # cutoff radius - alm.define(3, fcs_cutoff_radius) - # Perform symmetry analysis and suggest irreducible force constants. - alm.suggest() - # Get the number of irreducible elements for both 3RD- and 4TH-order - # force constants - n_rd_anh = alm._get_number_of_irred_fc_elements( # noqa: SLF001 - 2 - ) + alm._get_number_of_irred_fc_elements(3) # noqa: SLF001 - # we can determine how many displaced supercells we need to use to extract - # the 3rd and 4th order force constants, and we can add a scaling factor - # to reduce the number of displaced supercells due to we use the lasso - # technique. - num_d_anh = int(np.ceil(n_rd_anh / (3.0 * natom))) - num_dis_cells_anhar = num_disp_anhar if num_disp_anhar != 0 else num_d_anh - - num_dis_cells_anhar = 20 - # generate the supercells for anharmonic force constants + _check_anharmonic_settings( + anhar_max_order, + anhar_fit_methods, + fcs_cutoff_radius=fcs_cutoff_radius, + num_disp_anhar=num_disp_anhar, + ) + num_dis_cells_anhar = _get_num_anharmonic_supercells( + supercell_ph, + num_disp_anhar, + anhar_max_order, + fcs_cutoff_radius, + anhar_fit_methods, + ) + if verbose: + logger.info( + f"{num_dis_cells_anhar} displaced supercells are used for the " + "anharmonic force constants." + ) + # generate the supercells for anharmonic force constants. A different + # seed keeps them from repeating the directions of a random harmonic set. phonon.generate_displacements( distance=displacement_anhar, number_of_snapshots=num_dis_cells_anhar, - random_seed=random_seed, + random_seed=None if random_seed is None else random_seed + 1, ) supercells = phonon.supercells_with_displacements displacements += [get_pmg_structure(cell) for cell in supercells] @@ -282,11 +535,7 @@ def generate_frequencies_eigenvectors( supercell_matrix: np.array, displacement: float, cal_anhar_fcs: bool, - fcs_cutoff_radius: list[int], - renorm_phonon: bool, - cal_ther_cond: bool, - ther_cond_mesh: list[int], - ther_cond_temp: list[int], + fcs_cutoff_radius: list[float], sym_reduce: bool, symprec: float, use_symmetrized_structure: str | None, @@ -296,10 +545,20 @@ def generate_frequencies_eigenvectors( total_dft_energy: float, epsilon_static: Matrix3D = None, born: Matrix3D = None, + num_displaced_supercells: int = 0, + anhar_max_order: int = 3, + anhar_fit_methods: Sequence[str] = ("cocktail",), + anhar_alpha_min: int = -12, + random_seed: int | None = 103, **kwargs, ) -> PhononBSDOSDoc: """ - Analyze the phonon runs and summarize the results. + Fit the force constants with pheasy and summarize the phonon results. + + The harmonic force constants give the band structure, density of states + and thermodynamic properties in the output document. With cal_anhar_fcs, + the anharmonic force constants are also fitted and written to files in + the job folder. They are not stored in the output document. Parameters ---------- @@ -309,6 +568,10 @@ def generate_frequencies_eigenvectors( array to describe supercell displacement: float displacement in Angstrom used for supercell computation + cal_anhar_fcs: bool + if True, the anharmonic force constants are fitted as well + fcs_cutoff_radius: list[float] + cutoff radius in Bohr for each force constant order, from second order sym_reduce: bool if True, symmetry will be used in phonopy symprec: float @@ -327,11 +590,30 @@ def generate_frequencies_eigenvectors( The high-frequency dielectric constant born: Matrix3D Born charges - verbose : bool = False - Whether to log error messages. + num_displaced_supercells: int + number of harmonic random displacements requested by the user, + 0 for automatic. Must match the value used to generate them. + anhar_max_order: int + highest anharmonic force constant order, 3 or 4 + anhar_fit_methods: Sequence[str] + "cocktail" (fixed second-order FCs), "one-shot" (all orders fitted + together, written to the one_shot folder), or both + anhar_alpha_min: int + base-10 exponent of the smallest LASSO penalty in the anharmonic fits + random_seed : int | None = 103 + Seed for the harmonic and anharmonic LASSO fits, so that they are + reproducible. kwargs: dict - Additional parameters that are passed to PhononBSDOSDoc.from_forces_born + Further options read by this job, such as npoints_band, filename_bs, + filename_dos, kpoint_density_dos and store_force_constants. """ + _check_anharmonic_settings( + anhar_max_order, + anhar_fit_methods, + cal_anhar_fcs, + fcs_cutoff_radius, + anhar_alpha_min, + ) phonon = _generate_phonon_object( structure, supercell_matrix, @@ -405,34 +687,7 @@ def generate_frequencies_eigenvectors( # separate the dataset into harmonic and anharmonic parts num_har = dataset_disps_array_use.shape[0] if cal_anhar_fcs: - if not ALM: - raise ImportError( - "Error importing ALM. Please ensure the 'alm' library is installed." - ) - - supercell_ph = phonon.supercell - lattice = supercell_ph.cell - positions = supercell_ph.scaled_positions - numbers = supercell_ph.numbers - natom = len(numbers) - - # get the number of free parameters of 2ND FCs from ALM, labeled as n_fp - with ALM(lattice, positions, numbers) as alm: - alm.define(1) - alm.suggest() - n_fp = alm._get_number_of_irred_fc_elements(1) # noqa: SLF001 - - # get the number of displaced supercells based on the - # number of free parameters - num = int(np.ceil(n_fp / (3.0 * natom))) - - # get the number of displaced supercells from phonopy to compared - # with the number of 3, if the number of displaced supercells is - # less than 3, we will use the finite displacement method to generate - # the supercells. Otherwise, we will use the random displacement - # method to generate the supercells. - num_disp_f = len(phonon.displacements) - num_har = int(np.ceil(num * 1.8)) if num_disp_f > 3 else num_disp_f + num_har = _get_num_harmonic_supercells(phonon, num_displaced_supercells) np.save( _DEFAULT_FILE_PATHS["harmonic_displacements"], @@ -475,11 +730,8 @@ def generate_frequencies_eigenvectors( prim = ase_read("POSCAR") supercell = ase_read("SPOSCAR") - # Create the clusters and orbitals for second order force constants - # For the variables: --w, --nbody, they are used to specify the order of the - # force constants. in the near future, we will add the option to specify the - # order of the force constants. And these two variables can be defined by the - # users. + # Create the clusters and orbitals for second order force constants. + # The harmonic fit is always second order (-w 2, --nbody 2). pheasy_cmd_1 = ( f"pheasy --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " @@ -523,6 +775,7 @@ def generate_frequencies_eigenvectors( f"-w 2 --symprec {float(symprec)} " f"-l LASSO --std --rasr BHH --ndata {int(num_har)} " f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" + + (f" --seed {int(random_seed)}" if random_seed is not None else "") ) else: @@ -543,12 +796,14 @@ def generate_frequencies_eigenvectors( subprocess.call(shlex.split(pheasy_cmd_3)) subprocess.call(shlex.split(pheasy_cmd_4)) - # When this code is run on Github tests, it is failing because it is - # not able to find the FORCE_CONSTANTS file. This is because the file is - # somehow getting generated in some temp directory. Can you fix the bug? fc_file = Path(_DEFAULT_FILE_PATHS["force_constants"]) + if cal_anhar_fcs and not fc_file.exists(): + raise RuntimeError( + "The harmonic pheasy fit did not write FORCE_CONSTANTS, so the " + "anharmonic force constants cannot be fitted." + ) - if cal_anhar_fcs and fc_file.exists(): + if cal_anhar_fcs: np.save( _DEFAULT_FILE_PATHS["anharmonic_displacements"], dataset_disps_array_use[num_har:, :, :], @@ -559,85 +814,31 @@ def generate_frequencies_eigenvectors( ) num_anhar = dataset_forces_array_disp.shape[0] - num_har - # We next begin to generate the anharmonic force constants up to fourth - # order using the LASSO method - pheasy_cmd_5 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -s -w 4 --symprec " - f"{float(symprec)} " - f"--nbody 2 3 3 --c3 {float(fcs_cutoff_radius[1] / ANGSTROM_TO_BOHR)} " - f"--c4 {float(fcs_cutoff_radius[2] / ANGSTROM_TO_BOHR)}" - ) - - pheasy_cmd_6 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -c --symprec " - f"{float(symprec)} -w 4" - ) - pheasy_cmd_7 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -w 4 -d --symprec " - f"{float(symprec)} " - f"--ndata {int(num_anhar)} --disp_file " - f"--disp_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_displacements']}" - ) - pheasy_cmd_8 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -f -w 4 --fix_fc2 " - f"--symprec {float(symprec)} " - f"--ndata {int(num_anhar)} " - f"--force_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_force_matrix']}" - ) - - subprocess.call(shlex.split(pheasy_cmd_5)) - subprocess.call(shlex.split(pheasy_cmd_6)) - subprocess.call(shlex.split(pheasy_cmd_7)) - subprocess.call(shlex.split(pheasy_cmd_8)) - - # begin to renormzlize the phonon energies - if renorm_phonon: - pheasy_cmd_9 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -f -w 4 --fix_fc2 " - f"--hdf5 --symprec {float(symprec)} " - f"--ndata {int(num_anhar)}" - ) - - subprocess.call(shlex.split(pheasy_cmd_9)) - - # write the born charges and dielectric constant to the pheasy format - - # begin to convert the force constants to the phonopy and phono3py format - # for the further lattice thermal conductivity calculations - if cal_ther_cond and fc_file.exists(): - # convert the 2ND order force constants to the phonopy format - fc_phonopy_text = parse_FORCE_CONSTANTS(filename=fc_file) - write_force_constants_to_hdf5(fc_phonopy_text, filename="fc2.hdf5") - - # convert the 3RD order force constants to the phonopy format - - prim_hiphive = ase_read("POSCAR") - supercell_hiphive = ase_read("SPOSCAR") - fcs = HiPhiveForceConstants.read_shengBTE( - supercell_hiphive, "FORCE_CONSTANTS_3RD", prim_hiphive - ) - fcs.write_to_phono3py("fc3.hdf5") - - phono3py_cmd = ( - f"phono3py --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} {int(supercell_matrix[2][2])} " - f"--fc2 --fc3 --br --isotope --wigner " - f"--mesh {ther_cond_mesh[0]} {ther_cond_mesh[1]} {ther_cond_mesh[2]} " - f"--tmin {ther_cond_temp[0]} --tmax {ther_cond_temp[1]} " - f"--tstep {ther_cond_temp[2]}" - ) - - subprocess.call(shlex.split(phono3py_cmd)) + # The cocktail fit runs here, next to the harmonic FORCE_CONSTANTS it + # keeps fixed. The one-shot fit runs in its own folder, because both + # fits write FORCE_CONSTANTS_3RD and fc3.hdf5. + for method in anhar_fit_methods: + work_dir = Path.cwd() + if method == "one-shot": + work_dir = Path(_DEFAULT_FILE_PATHS["one_shot_dir"]).resolve() + work_dir.mkdir(exist_ok=True) + for filename in ( + "POSCAR", + _DEFAULT_FILE_PATHS["anharmonic_displacements"], + _DEFAULT_FILE_PATHS["anharmonic_force_matrix"], + ): + shutil.copy(filename, work_dir / filename) + _run_anharmonic_fit( + method=method, + supercell_matrix=supercell_matrix, + symprec=symprec, + anhar_max_order=anhar_max_order, + fcs_cutoff_radius=fcs_cutoff_radius, + num_anhar=num_anhar, + anhar_alpha_min=anhar_alpha_min, + work_dir=work_dir, + random_seed=random_seed, + ) if fc_file.exists(): # Read the force constants from the output file of pheasy code @@ -678,10 +879,8 @@ def generate_frequencies_eigenvectors( # If imaginary modes are present, we first use the hiphive code to enforce # some symmetry constraints to eliminate the imaginary modes (generally work # for small imaginary modes near Gamma point). If the imaginary modes are - # still present, we will use the pheasy code to generate the force constants - # using a shorter cutoff (10 A) to eliminate the imaginary modes, also we - # just want to remove the imaginary modes near Gamma point. In the future, - # we will only use the pheasy code to do the job. + # still present, a pheasy refit with a shorter cutoff (10 A) follows, but + # its result is currently not used (see the NOTE below). if imaginary_modes: # Define a cluster space using the largest cutoff you can @@ -727,7 +926,11 @@ def generate_frequencies_eigenvectors( ) # Using a shorter cutoff (10 A) to generate the force constants to - # eliminate the imaginary modes near Gamma point in pheasy code + # eliminate the imaginary modes near Gamma point in pheasy code. + # NOTE: the force constants are read back below from + # FORCE_CONSTANTS_short_cutoff, the file the hiPhive step above wrote, so + # the result of this pheasy refit is not used. If the refit succeeds, it + # overwrites FORCE_CONSTANTS in the job folder. if imaginary_modes: pheasy_cmd_11 = ( f"pheasy --dim {int(supercell_matrix[0][0])} " diff --git a/src/atomate2/common/jobs/phonons.py b/src/atomate2/common/jobs/phonons.py index d013269ba7..a148f047d0 100644 --- a/src/atomate2/common/jobs/phonons.py +++ b/src/atomate2/common/jobs/phonons.py @@ -44,7 +44,10 @@ from atomate2.vasp.jobs.base import BaseVaspMaker if TYPE_CHECKING: + from collections.abc import Sequence + from emmet.core.math import Matrix3D + from phonopy.structure.atoms import PhonopyAtoms from atomate2.aims.jobs.base import BaseAimsMaker from atomate2.ase.jobs import AseRelaxMaker @@ -52,6 +55,114 @@ logger = logging.getLogger(__name__) +# CODATA 2018: 1 Angstrom = 1 / 0.529177210903 Bohr +ANGSTROM_TO_BOHR = 1.8897261246257702 + + +def _get_num_irreducible_fcs( + supercell: PhonopyAtoms, + max_order: int, + fcs_cutoff_radius: Sequence[float] | None = None, + nbody: Sequence[int] | None = None, +) -> list[int]: + """ + Count the symmetry-irreducible force constants of each order with ALM. + + Used by the pheasy and hiPhive workflows to size their displacement sets. + + Parameters + ---------- + supercell: PhonopyAtoms + Supercell used for the force constant fit. + max_order: int + Highest force constant order to count, 2, 3 or 4. + fcs_cutoff_radius: Sequence[float] | None + Cutoff radius in Bohr for each order, starting at second order. + Only needed when max_order is larger than 2. + nbody: Sequence[int] | None + Largest number of atoms in a cluster for each order, starting at second + order, as in ALM's define. None keeps all clusters. + + Returns + ------- + list[int] + Number of irreducible force constants for each order, starting at + second order. + """ + try: + from alm import ALM + except ImportError as exc: + raise ImportError( + "Error importing ALM. Please ensure the 'alm' library is installed." + ) from exc + + positions = supercell.scaled_positions + numbers = supercell.numbers + + if max_order == 2: + # TODO: remove ALMODE dependence for 2nd order force constants + # the harmonic count uses no cutoff, so the lattice stays in Angstrom + with ALM(supercell.cell, positions, numbers) as alm: + alm.define(1) + alm.suggest() + return [alm._get_number_of_irred_fc_elements(1)] # noqa: SLF001 + + # ALM expects the lattice in Bohr when cutoff radii in Bohr are given, and + # one cutoff per order and per pair of elements + n_elements = len(set(numbers)) + cutoff_radii = [ + np.full((n_elements, n_elements), radius) + for radius in fcs_cutoff_radius[: max_order - 1] + ] + with ALM(supercell.cell * ANGSTROM_TO_BOHR, positions, numbers) as alm: + alm.define(max_order - 1, cutoff_radii=cutoff_radii, nbody=nbody) + alm.suggest() + return [ + alm._get_number_of_irred_fc_elements(order) # noqa: SLF001 + for order in range(1, max_order) + ] + + +def _get_num_harmonic_supercells( + phonon: Phonopy, num_displaced_supercells: int, multiplier: float = 1.8 +) -> int: + """ + Get the number of displaced supercells used for the harmonic force constants. + + Used by the pheasy and hiPhive workflows. In pheasy, both the displacement + generation and the fit call this function, so the dataset is always split + into its harmonic and anharmonic parts at the same place. + + If phonopy needs three or fewer finite displacements, these are used as + they are. Otherwise random displacements are used. Their number is either + given by the user or set from the number of free second-order force + constants, n_fp. The minimum is ceil(n_fp / (3 * natom)). Because the full + rank of the matrix does not guarantee an accurate fit, multiplier times + this minimum plus one configuration is used. + + Parameters + ---------- + phonon: Phonopy + Phonopy object holding the finite displacements. + num_displaced_supercells: int + Number of random displacements requested by the user, 0 for automatic. + multiplier: float + Number of configurations per minimum configuration set. + + Returns + ------- + int + Number of harmonic displaced supercells. + """ + if len(phonon.displacements) <= 3: + return len(phonon.displacements) + if num_displaced_supercells != 0: + return num_displaced_supercells + (n_fp,) = _get_num_irreducible_fcs(phonon.supercell, 2) + natom = len(phonon.supercell.numbers) + num_disp_sc = int(np.ceil(n_fp / (3.0 * natom))) + return int(np.ceil(num_disp_sc * multiplier)) + 1 + def _get_kpath( structure: Structure, kpath_scheme: str, symprec: float, **kpath_kwargs diff --git a/src/atomate2/vasp/flows/pheasy.py b/src/atomate2/vasp/flows/pheasy.py index fca5039a00..14a4368c4a 100644 --- a/src/atomate2/vasp/flows/pheasy.py +++ b/src/atomate2/vasp/flows/pheasy.py @@ -18,22 +18,24 @@ @dataclass class PhononMaker(BasePhononMaker): - """Maker to calculate harmonic phonons with LASSO-based ML code Pheasy. + """Maker to calculate harmonic phonons and anharmonic FCs with Pheasy. - Calculate the zero-K harmonic phonons of a material and higher-order FCs. - Initially, a tight structural relaxation is performed to obtain a structure - without forces on the atoms. Subsequently, supercells with all atoms displaced - by a small amplitude (generally using 0.01 A) are generated and accurate forces - are computed for these structures for the second order force constants. With the - help of pheasy (LASSO technique), these forces are then converted into a dynamical - matrix. In this Workflow, we separate the harmonic phonon calculations and - anharmonic force constants calculations. To correct for polarization effects, a + Calculate the zero-K harmonic phonons of a material and, optionally, its + anharmonic FCs. Initially, a tight structural relaxation is performed to obtain + a structure without forces on the atoms. Subsequently, displaced supercells + (generally using 0.01 A) are generated and accurate forces are computed for + them. If phonopy needs more than three finite displacements, all atoms are + displaced randomly and pheasy fits the second order force constants with LASSO. + Otherwise, the finite displacements are used with a least-squares fit. These + force constants are then converted into a dynamical matrix. In this Workflow, + we separate the harmonic phonon calculations and anharmonic force constants + calculations. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can be performed. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. For the anharmonic force constants, the supercells with all atoms displaced by a larger amplitude (generally using 0.08 A) are generated and accurate forces are computed for these structures. With the help of pheasy (LASSO technique), - the third- and fourth-order force constants are extracted at once. + the third-order (and optionally fourth-order) force constants are extracted. .. Note:: It is heavily recommended to symmetrize the structure before passing it to @@ -62,35 +64,66 @@ class PhononMaker(BasePhononMaker): number of displacements to be generated using a random-displacement approach for harmonic phonon calculations. The default value is 0 and the number of displacements is automatically determined by the number of atoms in the - supercell and its space group. + supercell and its space group. Not used when phonopy needs at most three + finite displacements. cal_anhar_fcs: bool - if set to True, anharmonic force constants(FCs) up to fourth-order FCs will - be calculated. The default value is False, and only harmonic phonons will - be calculated. + if set to True, anharmonic force constants(FCs) up to order + anhar_max_order will be calculated. The default value is False, and only + harmonic phonons will be calculated. displacement_anhar: float - displacement distance for anharmonic force constants(FCs) up to fourth-order - FCs, for most cases 0.08 A is a good choice, but it can be increased to 0.1 A. + displacement distance for the anharmonic force constants(FCs). The default + is 0.08 A. num_disp_anhar: int number of displacements to be generated using a random-displacement approach - for anharmonic phonon calculations. The default value is 0 and the number of - displacements is automatically determined by the number of atoms in the - supercell, cutoff distance for anharmonic FCs its space group. generally, - 50 large-distance displacements are enough for most cases. + for anharmonic phonon calculations. A non-zero value is used as given. The + default value is 0, and then the number is set so that the fit has 100 force + equations per free force constant, with at least 20 displaced supercells. + Above 600 the job stops. The free force constants are counted with ALM, which + uses its own symmetry search, for this supercell and fcs_cutoff_radius. The + second-order FCs are included when "one-shot" is requested. + anhar_max_order: int + highest order of the anharmonic FCs, 3 or 4. The default of 3 fits the + third-order FCs. 4 also fits fourth-order FCs. + anhar_fit_methods: Sequence[Literal["cocktail", "one-shot"]] + how the anharmonic FCs are fitted to the large-distance dataset. + "cocktail" keeps the second-order FCs fixed to the harmonic fit and fits + only the higher orders. "one-shot" fits the second- and higher-order FCs + together from the same dataset and writes them to the "one_shot" folder. + Both can be requested. The default is ("cocktail",). The cocktail FCs are + written to the job folder, and the one-shot FCs, including fc2.hdf5, to its + one_shot subfolder: FORCE_CONSTANTS_3RD and fc3.hdf5, plus + FORCE_CONSTANTS_4TH and fc4.hdf5 at fourth order. They are not stored in the + output document. The LASSO fits are seeded, so a run is reproducible. With + few displaced supercells, the one-shot result depends on that seed. + anhar_alpha_min: int + base-10 exponent of the smallest LASSO penalty tried by cross-validation + in the anharmonic fits. It must be an integer below -2. The default of -12 + is below pheasy's own default of -6. If the chosen penalty lands on either + end of the search, 10**anhar_alpha_min or pheasy's 1e-2, a warning is + raised. fcs_cutoff_radius: list - cutoff distance for anharmonic force constants(FCs) up to fourth-order FCs. - The default value is [-1, 12, 10], which means that the cutoff distance for - second-order FCs is the Wigner-Seitz cell boundary and the cutoff distance - for third-order FCs is 12 Borh, and the cutoff distance for fourth-order FCs - is 10 Bohr. Generally, the default value is good enough. + cutoff distance in Bohr for each FC order, starting at second order. The + default value is [-1, 12, 10]. The first entry is not used, since pheasy + fits the second-order FCs without a cutoff. The second and third entries + are the cutoffs for third- and fourth-order FCs. The cutoff of each fitted + order, up to anhar_max_order, must be positive. Longer cutoffs increase + the number of free FCs, and with it the number of displaced supercells. min_length: float minimum length of lattice constants will be used to create the supercell, - the default value is 14.0 A. In most cases, the default value is good - enough, but it can be increased for larger supercells. + the default value is 8.0 A. It can be increased for larger supercells. + max_atoms: float | None + maximum number of atoms in the supercell. + force_90_degrees: bool + if set to True, only supercells with three 90 degree angles are allowed. + force_diagonal: bool + if set to True, only diagonal supercell matrices are allowed. The pheasy + commands take the diagonal of the supercell matrix. prefer_90_degrees: bool - if set to True, supercell algorithm will first try to find a supercell - with 3 90 degree angles. + not used by this workflow, which uses force_90_degrees instead. + allow_orthorhombic: bool + not used by this workflow. get_supercell_size_kwargs: dict - kwargs that will be passed to get_supercell_size to determine supercell size + not used by this workflow. use_symmetrized_structure: str allowed strings: "primitive", "conventional", None diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py new file mode 100644 index 0000000000..3bf0bb7067 --- /dev/null +++ b/tests/common/jobs/test_pheasy.py @@ -0,0 +1,304 @@ +"""Tests for the anharmonic force constant fit of the pheasy workflow. + +Forces come from ASE's EMT potential, so the jobs run end to end without any +DFT reference data. +""" + +import warnings +from pathlib import Path + +import h5py +import numpy as np +import pytest +from ase.build import bulk +from ase.calculators.emt import EMT +from jobflow import run_locally +from phonopy.file_IO import parse_FORCE_CONSTANTS +from pymatgen.core import Lattice, Structure +from pymatgen.io.ase import AseAtomsAdaptor + +import atomate2.common.jobs.pheasy as pheasy_jobs +from atomate2.common.jobs.pheasy import ( + _check_lasso_alpha, + _get_num_anharmonic_supercells, + generate_frequencies_eigenvectors, + generate_phonon_displacements, +) +from atomate2.common.jobs.phonons import ( + _generate_phonon_object, + _get_num_irreducible_fcs, +) + +# fcs_cutoff_radius in Bohr. 8 Bohr (4.2 A) covers the first two neighbour +# shells of fcc Cu (2.55 and 3.61 A) and stays inside the 10.8 A supercell. +FCS_CUTOFF_RADIUS = [-1, 8, 8] + +COMMON_KWARGS = { + "supercell_matrix": [[3, 0, 0], [0, 3, 0], [0, 0, 3]], + "displacement": 0.01, + "sym_reduce": True, + "symprec": 1e-3, + "use_symmetrized_structure": None, + "kpath_scheme": "seekpath", + "code": "vasp", +} + +FIT_KWARGS = { + "total_dft_energy": None, + "static_run_job_dir": None, + "static_run_uuid": None, + "born_run_job_dir": None, + "born_run_uuid": None, + "optimization_run_job_dir": None, + "optimization_run_uuid": None, +} + + +def _emt_displacement_data(structures: list[Structure]) -> dict: + forces = [] + for structure in structures: + atoms = AseAtomsAdaptor.get_atoms(structure) + atoms.calc = EMT() + forces.append(atoms.get_forces().tolist()) + return { + "forces": forces, + "displaced_structures": structures, + "dirs": [None] * len(structures), + "uuids": [None] * len(structures), + } + + +def _max_abs_fc(filename: Path, key: str) -> float: + with h5py.File(filename) as f: + return float(np.abs(f[key][:]).max()) + + +def _cu_structure() -> Structure: + return AseAtomsAdaptor.get_structure(bulk("Cu", "fcc", a=3.61, cubic=True)) + + +@pytest.mark.parametrize("num_displaced_supercells", [0, 3]) +def test_harmonic_and_anharmonic_split(tmp_dir, num_displaced_supercells): + """The fit job must split the forces where the displacement job did. + + Before this was fixed, the fit job used one harmonic supercell fewer than + the displacement job made, and it ignored num_displaced_supercells. + """ + # a distorted Cu cell needs more than three finite displacements, so the + # random-displacement path is used for the harmonic force constants + structure = Structure( + Lattice.orthorhombic(3.6, 3.7, 3.8), + ["Cu"] * 4, + [[0, 0, 0], [0.5, 0.5, 0.02], [0.5, 0.03, 0.5], [0.01, 0.5, 0.5]], + ) + kwargs = {**COMMON_KWARGS, "supercell_matrix": [[2, 0, 0], [0, 2, 0], [0, 0, 2]]} + assert len(_generate_phonon_object(structure, **kwargs).displacements) > 3 + anhar_kwargs = { + "cal_anhar_fcs": True, + "fcs_cutoff_radius": [-1, 6, 6], + "num_displaced_supercells": num_displaced_supercells, + } + + job = generate_phonon_displacements( + structure=structure, + displacement_anhar=0.03, + num_disp_anhar=20, + **anhar_kwargs, + **kwargs, + ) + responses = run_locally(job, create_folders=True, ensure_success=True) + displacements = responses[job.uuid][1].output + # the harmonic set, 20 anharmonic supercells, then the undisplaced supercell + num_har = len(displacements) - 20 - 1 + assert num_har == (num_displaced_supercells or 14) + + job = generate_frequencies_eigenvectors( + structure=structure, + displacement_data=_emt_displacement_data(displacements), + **anhar_kwargs, + **FIT_KWARGS, + **kwargs, + ) + run_locally(job, create_folders=True, ensure_success=True) + + (fit_dir,) = (path.parent for path in Path.cwd().glob("job_*/disp_matrix.npy")) + harmonic = np.load(fit_dir / "disp_matrix.npy") + anharmonic = np.load(fit_dir / "disp_matrix_anhar.npy") + assert harmonic.shape[0] == num_har + assert anharmonic.shape[0] == 20 + + # the anharmonic set is drawn with its own seed, so its directions differ + # from those of the random harmonic set + assert not np.allclose(harmonic[0] / 0.01, anharmonic[0] / 0.03) + + +def test_get_num_anharmonic_supercells(monkeypatch): + phonon = _generate_phonon_object(_cu_structure(), **COMMON_KWARGS) + kwargs = { + "supercell": phonon.supercell, + "anhar_max_order": 3, + "fcs_cutoff_radius": [-1, 12, 10], + "anhar_fit_methods": ["one-shot"], + } + + # a value set by the user is used as it is + assert _get_num_anharmonic_supercells(num_disp_anhar=7, **kwargs) == 7 + + # sized from the free force constants, above the floor of 20 + assert _get_num_irreducible_fcs(phonon.supercell, 3, [-1, 12]) == [25, 324] + assert _get_num_anharmonic_supercells(num_disp_anhar=0, **kwargs) == 108 + + # the first cutoff is not used, since pheasy fits fc2 without a cutoff + fc2_cutoff = {**kwargs, "fcs_cutoff_radius": [5, 12, 10]} + assert _get_num_anharmonic_supercells(num_disp_anhar=0, **fc2_cutoff) == 108 + + # fourth order, with the three-body limit this workflow passes to pheasy + order_4 = {**kwargs, "anhar_max_order": 4, "anhar_fit_methods": ["cocktail"]} + assert _get_num_anharmonic_supercells(num_disp_anhar=0, **order_4) == 224 + + # a binary compound, L1_2 Cu3Au, needs one cutoff per pair of elements + cu3au = Structure( + Lattice.cubic(3.75), + ["Au", "Cu", "Cu", "Cu"], + [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], + ) + binary = { + **kwargs, + "supercell": _generate_phonon_object(cu3au, **COMMON_KWARGS).supercell, + } + assert _get_num_anharmonic_supercells(num_disp_anhar=0, **binary) == 337 + + # above the ceiling the job stops + monkeypatch.setattr(pheasy_jobs, "_MAX_NUM_DISP_ANHAR", 30) + with pytest.raises(ValueError, match="more than the limit of 30"): + _get_num_anharmonic_supercells(num_disp_anhar=0, **kwargs) + + +def test_check_lasso_alpha(tmp_dir): + log_file = Path("pheasy_anharmonic_fit.log") + + log_file.write_text("- alpha_min: 1e-12\n- alpha_opt: 2.947052e-09\n") + with warnings.catch_warnings(): + warnings.simplefilter("error") + _check_lasso_alpha(log_file, alpha_min=-12) + + log_file.write_text("- alpha_min: 1e-12\n- alpha_opt: 1.000000e-12\n") + with pytest.warns(UserWarning, match="on the lower bound"): + _check_lasso_alpha(log_file, alpha_min=-12) + + log_file.write_text("- alpha_max: 1e-2\n- alpha_opt: 1.000000e-02\n") + with pytest.warns(UserWarning, match="on the upper bound"): + _check_lasso_alpha(log_file, alpha_min=-12) + + log_file.write_text("Fitting force constants via the ordinary least-square.\n") + with pytest.raises(RuntimeError, match="No LASSO alpha"): + _check_lasso_alpha(log_file, alpha_min=-12) + + log_file.unlink() + with pytest.raises(FileNotFoundError, match="exited without writing"): + _check_lasso_alpha(log_file, alpha_min=-12) + + +def test_anharmonic_fit_cocktail_and_one_shot(tmp_dir): + structure = _cu_structure() + anhar_kwargs = { + "cal_anhar_fcs": True, + "fcs_cutoff_radius": FCS_CUTOFF_RADIUS, + "anhar_fit_methods": ["cocktail", "one-shot"], + } + + job = generate_phonon_displacements( + structure=structure, + num_displaced_supercells=0, + displacement_anhar=0.03, + num_disp_anhar=0, + **anhar_kwargs, + **COMMON_KWARGS, + ) + responses = run_locally(job, create_folders=True, ensure_success=True) + displacements = responses[job.uuid][1].output + # one finite displacement for fcc Cu, the anharmonic set at its floor of + # 20, then the undisplaced supercell + assert len(displacements) == 1 + 20 + 1 + + job = generate_frequencies_eigenvectors( + structure=structure, + displacement_data=_emt_displacement_data(displacements), + **anhar_kwargs, + **FIT_KWARGS, + **COMMON_KWARGS, + ) + # a LASSO penalty on either bound of the search fails the test + with warnings.catch_warnings(): + warnings.filterwarnings("error", message="The LASSO penalty") + run_locally(job, create_folders=True, ensure_success=True) + + (fit_dir,) = (path.parent for path in Path.cwd().glob("job_*/fc3.hdf5")) + one_shot_dir = fit_dir / "one_shot" + + # both fits used LASSO + for folder in (fit_dir, one_shot_dir): + log = (folder / "pheasy_anharmonic_fit.log").read_text() + assert "coordinate descent LASSO" in log + + # the one-shot fc2 agrees with the harmonic fc2, which it does not overwrite + harmonic_fc2 = np.abs(parse_FORCE_CONSTANTS(fit_dir / "FORCE_CONSTANTS")).max() + assert _max_abs_fc(one_shot_dir / "fc2.hdf5", "fc2") == pytest.approx( + harmonic_fc2, rel=0.05 + ) + + # third-order force constants in eV/A^3. With 20 supercells, the one-shot + # value changed by about 10 percent with the LASSO seed in local runs, + # while the cocktail value did not, so only the cocktail value is pinned. + cocktail_fc3 = _max_abs_fc(fit_dir / "fc3.hdf5", "fc3") + assert cocktail_fc3 == pytest.approx(4.551, rel=0.02) + assert _max_abs_fc(one_shot_dir / "fc3.hdf5", "fc3") == pytest.approx( + cocktail_fc3, rel=0.15 + ) + + +def test_anharmonic_fit_fourth_order(tmp_dir): + """The fourth-order fit runs and writes fc4.""" + structure = _cu_structure() + anhar_kwargs = { + "cal_anhar_fcs": True, + "fcs_cutoff_radius": FCS_CUTOFF_RADIUS, + "anhar_max_order": 4, + "anhar_fit_methods": ["cocktail"], + } + + job = generate_phonon_displacements( + structure=structure, + num_displaced_supercells=0, + # the workflow default. At 0.03 A, cross-validation chose the lowest + # penalty, 1e-12. + displacement_anhar=0.08, + num_disp_anhar=20, + **anhar_kwargs, + **COMMON_KWARGS, + ) + responses = run_locally(job, create_folders=True, ensure_success=True) + displacements = responses[job.uuid][1].output + + job = generate_frequencies_eigenvectors( + structure=structure, + displacement_data=_emt_displacement_data(displacements), + **anhar_kwargs, + **FIT_KWARGS, + **COMMON_KWARGS, + ) + # a LASSO penalty on either bound of the search fails the test + with warnings.catch_warnings(): + warnings.filterwarnings("error", message="The LASSO penalty") + run_locally(job, create_folders=True, ensure_success=True) + + (fit_dir,) = (path.parent for path in Path.cwd().glob("job_*/fc4.hdf5")) + assert (fit_dir / "FORCE_CONSTANTS_4TH").exists() + assert ( + "coordinate descent LASSO" + in (fit_dir / "pheasy_anharmonic_fit.log").read_text() + ) + + # force constants in eV/A^3 and eV/A^4 + assert _max_abs_fc(fit_dir / "fc3.hdf5", "fc3") == pytest.approx(4.601, rel=0.02) + assert _max_abs_fc(fit_dir / "fc4.hdf5", "fc4") == pytest.approx(48.92, rel=0.05) diff --git a/tests/vasp/flows/test_pheasy.py b/tests/vasp/flows/test_pheasy.py index 81effe8249..d057def21f 100644 --- a/tests/vasp/flows/test_pheasy.py +++ b/tests/vasp/flows/test_pheasy.py @@ -154,3 +154,68 @@ def test_pheasy_wf_vasp(mock_vasp, clean_dir, si_structure: Structure, test_dir) assert thermo_props["heat_capacity"][1] == pytest.approx(20.0, abs=2.5) # the high-T limit must approach (but not exceed) Dulong-Petit (3R per atom) assert 23.0 < thermo_props["heat_capacity"][2] < 3 * 8.3145 + + +@pytest.mark.parametrize( + ("settings", "match"), + [ + ({"cal_anhar_fcs": True, "anhar_max_order": 5}, "anhar_max_order"), + ({"cal_anhar_fcs": True, "anhar_fit_methods": ["joint"]}, "anhar_fit_methods"), + ({"cal_anhar_fcs": True, "anhar_fit_methods": []}, "anhar_fit_methods"), + ({"cal_anhar_fcs": True, "fcs_cutoff_radius": [-1, -2, 10]}, "positive"), + ({"anhar_alpha_min": -12.0}, "integer below -2"), + ({"cal_anhar_fcs": True, "num_disp_anhar": -1}, "non-negative integer"), + ( + {"cal_anhar_fcs": True, "anhar_fit_methods": ["cocktail", "cocktail"]}, + "without repeats", + ), + ({"anhar_alpha_min": -1}, "integer below -2"), + ( + { + "cal_anhar_fcs": True, + "anhar_max_order": 4, + "fcs_cutoff_radius": [-1, 12], + }, + "positive", + ), + ], +) +def test_pheasy_anharmonic_settings_are_checked(settings, match): + with pytest.raises(ValueError, match=match): + PhononMaker(**settings) + + +def test_pheasy_maker_passes_anharmonic_settings(si_structure: Structure): + """Both pheasy jobs must get the same settings, or the dataset is split wrong.""" + # every value differs from its default, so a dropped keyword is caught + settings = { + "cal_anhar_fcs": True, + "num_displaced_supercells": 5, + "num_disp_anhar": 30, + "displacement_anhar": 0.05, + "anhar_max_order": 4, + "anhar_fit_methods": ["cocktail", "one-shot"], + "anhar_alpha_min": -10, + "fcs_cutoff_radius": [-1, 11, 9], + "displacement": 0.02, + "symprec": 1e-4, + "sym_reduce": False, + } + flow = PhononMaker(**settings).make(structure=si_structure) + jobs = {job.name: job for job in flow.jobs} + displacements = jobs["generate_phonon_displacements"].function_kwargs + fit = jobs["generate_frequencies_eigenvectors"].function_kwargs + for key in ( + "cal_anhar_fcs", + "num_displaced_supercells", + "anhar_max_order", + "anhar_fit_methods", + "fcs_cutoff_radius", + "displacement", + "symprec", + "sym_reduce", + ): + assert displacements[key] == fit[key] == settings[key] + assert displacements["num_disp_anhar"] == 30 + assert displacements["displacement_anhar"] == 0.05 + assert fit["anhar_alpha_min"] == -10 diff --git a/tutorials/pheasy_workflow.ipynb b/tutorials/pheasy_workflow.ipynb index 1a27755a5b..6f6742b043 100644 --- a/tutorials/pheasy_workflow.ipynb +++ b/tutorials/pheasy_workflow.ipynb @@ -46,7 +46,7 @@ "\n", "The workflow has the same basic structure as the phonopy-based phonon workflow and uses [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) to post-process the force constants into band structures, densities of states, and thermodynamic properties.\n", "\n", - "To run this tutorial, the `pheasy` extra must be installed: `pip install 'atomate2[phonons,pheasy]'`. Anharmonic force-constant extraction (`cal_anhar_fcs=True`) additionally requires the `alamode` extra — see the atomate2 VASP documentation for installation hints." + "To run this tutorial, the `pheasy` extra must be installed: `pip install 'atomate2[pheasy]'`. It includes phonopy and ALM. ALM is compiled from source. See the atomate2 VASP documentation if that build fails." ] }, { @@ -83,7 +83,7 @@ "cell_type": "markdown", "metadata": {}, "source": [ - "Then we use the pheasy `PhononMaker` to generate a `Flow`. The maker mirrors the phonopy-based `PhononMaker`; the most important additional switches are `cal_anhar_fcs` (extract anharmonic force constants up to fourth order and renormalize the phonon energies) and `fcs_cutoff_radius` (cutoff radii for the second-, third- and fourth-order force constants). Here we only extract harmonic force constants for silicon. As always, a tight structural relaxation is performed first — make sure it is converged very accurately for production runs." + "Then we use the pheasy `PhononMaker` to generate a `Flow`. The maker mirrors the phonopy-based `PhononMaker`; the most important additional switches are `cal_anhar_fcs` (extract anharmonic force constants, third order by default, set by `anhar_max_order`) and `fcs_cutoff_radius` (cutoff radii in Bohr for the third- and fourth-order force constants, the first entry is not used). Here we only extract harmonic force constants for silicon. As always, a tight structural relaxation is performed first — make sure it is converged very accurately for production runs." ] }, { @@ -117,7 +117,7 @@ "cell_type": "markdown", "metadata": {}, "source": [ - "The flow relaxes the bulk structure, generates a set of randomly displaced supercells, computes their forces with VASP, and then fits the force constants with pheasy. We can visualize the flow first." + "The flow relaxes the bulk structure, generates the displaced supercells (a single finite displacement for silicon), computes their forces with VASP, and then fits the force constants with pheasy. We can visualize the flow first." ] }, { @@ -209,9 +209,9 @@ "cell_type": "markdown", "metadata": {}, "source": [ - "## Anharmonic force constants and phonon renormalization\n", + "## Anharmonic force constants\n", "\n", - "To go beyond the harmonic approximation, set `cal_anhar_fcs=True`. Pheasy will then extract third- and fourth-order force constants with LASSO regression (the cutoff radii are controlled by `fcs_cutoff_radius`). With `renorm_phonon=True`, the phonon energies are additionally renormalized at the temperatures given by `renorm_temp`. The lattice thermal conductivity can additionally be computed with `cal_ther_cond=True` (requires phono3py). Both options need more displaced supercells than the harmonic run shown here — pheasy will tell you how many it generated.\n", + "To go beyond the harmonic approximation, set `cal_anhar_fcs=True`. Pheasy will then extract third-order force constants with LASSO regression, and fourth-order ones too with `anhar_max_order=4` (the cutoff radii are controlled by `fcs_cutoff_radius`). The number of anharmonic displaced supercells is set from the number of free force constants, with at least 20. Above 600 the job stops unless `num_disp_anhar` is set.\n", "\n", "The same workflow is also available for forcefields via `from atomate2.forcefields.flows.pheasy import PhononMaker`, which is a cheap way to try it out without DFT." ] From db70c81c014bb7fd9b25808ffad1931c45bf1918 Mon Sep 17 00:00:00 2001 From: Jiongzhi ZHENG Date: Tue, 29 Sep 2026 20:17:01 +0800 Subject: [PATCH 02/43] Update pheasy.py --- src/atomate2/common/jobs/pheasy.py | 3 ++- 1 file changed, 2 insertions(+), 1 deletion(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index eb2648b817..1bedf0183a 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -1,4 +1,5 @@ -"""Jobs for running phonon calculations with phonopy and pheasy.""" +"""Jobs for running phonon，Higher-order FCs calculations with phonopy and pheasy. +and lattice thermal conductivity calculations using SHENGBTE and FOURPHONON.""" from __future__ import annotations From e0e191b9b16ab55a485db7a3ee78faf9a8e6f351 Mon Sep 17 00:00:00 2001 From: Jiongzhi ZHENG Date: Tue, 29 Sep 2026 20:24:40 +0800 Subject: [PATCH 03/43] Update pheasy.py --- src/atomate2/common/jobs/pheasy.py | 6 ++++++ 1 file changed, 6 insertions(+) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 1bedf0183a..3bca46db70 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -840,6 +840,12 @@ def generate_frequencies_eigenvectors( work_dir=work_dir, random_seed=random_seed, ) + + # End of anharmonic fit section + # and begin to calculate the anharmonic phonon priopoerties + # (e.g., phonon lifetimes, linewidths, etc.) using SHENGBTE and FOURPHONON. + # maybe we also need to do the phonon renormalization here. + # TODO: Implement the calculation of anharmonic phonon properties and phonon renormalization here. if fc_file.exists(): # Read the force constants from the output file of pheasy code From 537609c4f15ae035a49cc8807bb65a85e5ce6729 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 29 Sep 2026 22:27:02 -0700 Subject: [PATCH 04/43] Fix lint in pheasy job comments --- src/atomate2/common/jobs/pheasy.py | 18 +++++++++++------- 1 file changed, 11 insertions(+), 7 deletions(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 3bca46db70..578ab1e492 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -1,5 +1,8 @@ -"""Jobs for running phonon，Higher-order FCs calculations with phonopy and pheasy. -and lattice thermal conductivity calculations using SHENGBTE and FOURPHONON.""" +"""Jobs for running phonon and higher-order FC calculations with phonopy and pheasy. + +Lattice thermal conductivity calculations using ShengBTE and FourPhonon are +planned. +""" from __future__ import annotations @@ -840,12 +843,13 @@ def generate_frequencies_eigenvectors( work_dir=work_dir, random_seed=random_seed, ) - + # End of anharmonic fit section - # and begin to calculate the anharmonic phonon priopoerties - # (e.g., phonon lifetimes, linewidths, etc.) using SHENGBTE and FOURPHONON. - # maybe we also need to do the phonon renormalization here. - # TODO: Implement the calculation of anharmonic phonon properties and phonon renormalization here. + # and begin to calculate the anharmonic phonon properties + # (e.g., phonon lifetimes, linewidths, etc.) using ShengBTE and FourPhonon. + # maybe we also need to do the phonon renormalization here. + # TODO: Implement the calculation of anharmonic phonon properties and + # phonon renormalization here. if fc_file.exists(): # Read the force constants from the output file of pheasy code From ac4d511342ba8e2e7cbd10619c50c341f1e2821b Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Wed, 30 Sep 2026 09:09:03 -0700 Subject: [PATCH 05/43] Run the pheasy short-cutoff refit in its own folder with the matrix files --- docs/user/codes/vasp.md | 2 ++ src/atomate2/common/jobs/pheasy.py | 40 +++++++++++++++++++----------- tests/common/jobs/test_pheasy.py | 40 ++++++++++++++++++++++++++++++ 3 files changed, 67 insertions(+), 15 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index ee9e9ba3a7..7edc691cfc 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -350,6 +350,8 @@ ALM is compiled from source. If that build fails, see the ALM instructions below By design, these workflows have the same basic structure as the harmonic forcefield workflows and use [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) in part to compute the phonon spectrum. To use `Pheasy` in the previous example, we would replace the import string to `from atomate2.vasp.flows.pheasy import PhononMaker`. This workflow was used to build the Materials Project's Harmonic Phonon Database, described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1). +The pheasy fits can fail for a cell that is not in a standard setting, for example the primitive cell of MgO (mp-1265) as the Materials Project serves it. +For such a structure, set `use_symmetrized_structure="primitive"`, as was done for the database. By default, this workflow does not compute anharmonic force constants, but can be extended to using the `cal_anhar_fcs` kwarg. ALM, from the ALAMODE package, counts the free force constants used to size the random displacement sets. diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 578ab1e492..da3aaac57e 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -72,6 +72,7 @@ "anharmonic_force_matrix": "force_matrix_anhar.npy", "website": "phonon_website.json", "one_shot_dir": "one_shot", + "refit_dir": "short_cutoff_refit", "anharmonic_fit_log": "pheasy_anharmonic_fit.log", } @@ -890,8 +891,7 @@ def generate_frequencies_eigenvectors( # If imaginary modes are present, we first use the hiphive code to enforce # some symmetry constraints to eliminate the imaginary modes (generally work # for small imaginary modes near Gamma point). If the imaginary modes are - # still present, a pheasy refit with a shorter cutoff (10 A) follows, but - # its result is currently not used (see the NOTE below). + # still present, a pheasy refit with a shorter cutoff (10 A) follows. if imaginary_modes: # Define a cluster space using the largest cutoff you can @@ -937,12 +937,19 @@ def generate_frequencies_eigenvectors( ) # Using a shorter cutoff (10 A) to generate the force constants to - # eliminate the imaginary modes near Gamma point in pheasy code. - # NOTE: the force constants are read back below from - # FORCE_CONSTANTS_short_cutoff, the file the hiPhive step above wrote, so - # the result of this pheasy refit is not used. If the refit succeeds, it - # overwrites FORCE_CONSTANTS in the job folder. + # eliminate the imaginary modes near Gamma point in pheasy code. The refit + # runs in its own folder, so FORCE_CONSTANTS of the harmonic fit, which the + # cocktail fit kept fixed, stays unchanged. if imaginary_modes: + refit_dir = Path(_DEFAULT_FILE_PATHS["refit_dir"]).resolve() + refit_dir.mkdir(exist_ok=True) + for filename in ( + "POSCAR", + _DEFAULT_FILE_PATHS["harmonic_displacements"], + _DEFAULT_FILE_PATHS["harmonic_force_matrix"], + ): + shutil.copy(filename, refit_dir / filename) + pheasy_cmd_11 = ( f"pheasy --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " @@ -963,7 +970,8 @@ def generate_frequencies_eigenvectors( f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -w 2 -d --symprec " f"{float(symprec)} --c2 10.0 " - f"--ndata {int(num_har)} --disp_file" + f"--ndata {int(num_har)} --disp_file " + f"--disp_matrix_file {_DEFAULT_FILE_PATHS['harmonic_displacements']}" ) phonon.generate_displacements(distance=displacement) @@ -974,7 +982,8 @@ def generate_frequencies_eigenvectors( f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --c2 10.0 " f"--full_ifc -w 2 --symprec {float(symprec)} " - f"-l LASSO --std --rasr BHH --ndata {int(num_har)}" + f"-l LASSO --std --rasr BHH --ndata {int(num_har)} " + f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" ) else: @@ -983,15 +992,16 @@ def generate_frequencies_eigenvectors( f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --full_ifc " f"--c2 10.0 -w 2 --symprec {float(symprec)} " - f"--rasr BHH --ndata {int(num_har)}" + f"--rasr BHH --ndata {int(num_har)} " + f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" ) - subprocess.call(shlex.split(pheasy_cmd_11)) - subprocess.call(shlex.split(pheasy_cmd_12)) - subprocess.call(shlex.split(pheasy_cmd_13)) - subprocess.call(shlex.split(pheasy_cmd_14)) + for cmd in (pheasy_cmd_11, pheasy_cmd_12, pheasy_cmd_13, pheasy_cmd_14): + subprocess.run(shlex.split(cmd), cwd=refit_dir, check=True) - force_constants = parse_FORCE_CONSTANTS(filename=new_fc_file) + force_constants = parse_FORCE_CONSTANTS( + filename=refit_dir / _DEFAULT_FILE_PATHS["force_constants"] + ) phonon.force_constants = force_constants phonon.symmetrize_force_constants() diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index 3bf0bb7067..16d749e82b 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -27,6 +27,7 @@ from atomate2.common.jobs.phonons import ( _generate_phonon_object, _get_num_irreducible_fcs, + _run_band_structure_and_plot, ) # fcs_cutoff_radius in Bohr. 8 Bohr (4.2 A) covers the first two neighbour @@ -132,6 +133,45 @@ def test_harmonic_and_anharmonic_split(tmp_dir, num_displaced_supercells): assert not np.allclose(harmonic[0] / 0.01, anharmonic[0] / 0.03) +def test_imaginary_mode_refit(tmp_dir, monkeypatch): + """The short-cutoff refit reads the matrix files and runs in its own folder.""" + + def _report_imaginary_modes(*args, **kwargs): + bs_symm_line, _ = _run_band_structure_and_plot(*args, **kwargs) + return bs_symm_line, True + + monkeypatch.setattr( + pheasy_jobs, "_run_band_structure_and_plot", _report_imaginary_modes + ) + structure = _cu_structure() + kwargs = { + **COMMON_KWARGS, + "supercell_matrix": [[2, 0, 0], [0, 2, 0], [0, 0, 2]], + "cal_anhar_fcs": False, + "fcs_cutoff_radius": FCS_CUTOFF_RADIUS, + } + + job = generate_phonon_displacements( + structure=structure, + num_displaced_supercells=0, + displacement_anhar=0.03, + num_disp_anhar=0, + **kwargs, + ) + responses = run_locally(job, create_folders=True, ensure_success=True) + job = generate_frequencies_eigenvectors( + structure=structure, + displacement_data=_emt_displacement_data(responses[job.uuid][1].output), + **FIT_KWARGS, + **kwargs, + ) + run_locally(job, create_folders=True, ensure_success=True) + + (fit_dir,) = (path.parent for path in Path.cwd().glob("job_*/disp_matrix.npy")) + refit = fit_dir / "short_cutoff_refit" / "FORCE_CONSTANTS" + assert parse_FORCE_CONSTANTS(str(refit)).shape == (32, 32, 3, 3) + + def test_get_num_anharmonic_supercells(monkeypatch): phonon = _generate_phonon_object(_cu_structure(), **COMMON_KWARGS) kwargs = { From c48688747fef88974fe9bc706066e2486e0d2d50 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Wed, 30 Sep 2026 15:46:12 -0700 Subject: [PATCH 06/43] Make pheasy read the supercell of the force data --- pyproject.toml | 3 +- src/atomate2/common/jobs/pheasy.py | 32 +++++++++++++-------- tests/common/jobs/test_pheasy.py | 46 ++++++++++++++++++++++++++++++ 3 files changed, 68 insertions(+), 13 deletions(-) diff --git a/pyproject.toml b/pyproject.toml index affab73559..7d9110d588 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -53,7 +53,8 @@ mp = ["mp-api>=0.37.5"] # ("Force constants shape disagrees with crystal structure setting"). phonons = ["phonopy>=2.43,<5", "seekpath>=2.0.0"] # the pheasy fork adds the --disp_matrix_file and --force_matrix_file options -pheasy = ["atomate2[phonons,alamode]", "hiphive==1.5", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@e67a777ecfde5ab368d71167837b099df75cfd4c"] +# and fixes the --scell option +pheasy = ["atomate2[phonons,alamode]", "hiphive==1.5", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@1728f16642d5f2763f27695cd29ffada0f755d7f"] alamode = ["alm @ git+https://github.com/ttadano/ALM.git@f1d668fdee66e7e7218a04c88daf19d0e14fce0c#subdirectory=python"] hiphive = ["hiphive==1.5", "trainstation>=1.0", "atomate2[phonons,alamode]"] lobster = ["ijson>=3.2.2", "lobsterpy>=0.6.0"] diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index da3aaac57e..f882e3580e 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -314,7 +314,10 @@ def _run_anharmonic_fit( from run to run on the same forces. """ dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) - base = f"pheasy --dim {dim} -w {anhar_max_order} --symprec {float(symprec)}" + base = ( + f"pheasy --scell SPOSCAR --dim {dim} -w {anhar_max_order} " + f"--symprec {float(symprec)}" + ) cutoffs = f"--c3 {float(fcs_cutoff_radius[1] / ANGSTROM_TO_BOHR)}" if anhar_max_order == 4: cutoffs += f" --c4 {float(fcs_cutoff_radius[2] / ANGSTROM_TO_BOHR)}" @@ -631,7 +634,10 @@ def generate_frequencies_eigenvectors( verbose=False, ) - # Write the POSCAR and SPOSCAR files for the input of pheasy code + # Write the POSCAR and SPOSCAR files for the input of pheasy code. pheasy + # reads SPOSCAR (--scell SPOSCAR), so its atoms are in the order of the + # displacement and force matrices. The supercell pheasy builds itself from + # POSCAR can put an atom on a cell face one lattice vector away. supercell = phonon._supercell # noqa: SLF001 write_vasp("POSCAR", get_phonopy_structure(structure)) write_vasp("SPOSCAR", supercell) @@ -738,7 +744,7 @@ def generate_frequencies_eigenvectors( # Create the clusters and orbitals for second order force constants. # The harmonic fit is always second order (-w 2, --nbody 2). pheasy_cmd_1 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} " f"-s -w 2 --symprec {float(symprec)} --nbody 2" @@ -747,7 +753,7 @@ def generate_frequencies_eigenvectors( # Create the null space to further reduce the free parameters for # specific force constants and make them physically correct. pheasy_cmd_2 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -c --symprec " f"{float(symprec)} -w 2" @@ -756,7 +762,7 @@ def generate_frequencies_eigenvectors( # Generate the Compressive Sensing matrix,i.e., displacement matrix # for the input of machine leaning method.i.e., LASSO, pheasy_cmd_3 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -w 2 -d " f"--symprec {float(symprec)} " @@ -774,7 +780,7 @@ def generate_frequencies_eigenvectors( # constraint, i.e., tag: --rasr BHH, is enforced during the # fitting process. pheasy_cmd_4 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --full_ifc " f"-w 2 --symprec {float(symprec)} " @@ -786,7 +792,7 @@ def generate_frequencies_eigenvectors( else: # Calculate the force constants using the least-squred method pheasy_cmd_4 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --full_ifc " f"-w 2 --symprec {float(symprec)} " @@ -829,6 +835,7 @@ def generate_frequencies_eigenvectors( work_dir.mkdir(exist_ok=True) for filename in ( "POSCAR", + "SPOSCAR", _DEFAULT_FILE_PATHS["anharmonic_displacements"], _DEFAULT_FILE_PATHS["anharmonic_force_matrix"], ): @@ -945,13 +952,14 @@ def generate_frequencies_eigenvectors( refit_dir.mkdir(exist_ok=True) for filename in ( "POSCAR", + "SPOSCAR", _DEFAULT_FILE_PATHS["harmonic_displacements"], _DEFAULT_FILE_PATHS["harmonic_force_matrix"], ): shutil.copy(filename, refit_dir / filename) pheasy_cmd_11 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -s -w 2 --c2 " f"10.0 --symprec {float(symprec)} " @@ -959,14 +967,14 @@ def generate_frequencies_eigenvectors( ) pheasy_cmd_12 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -c --symprec " f"{float(symprec)} --c2 10.0 -w 2" ) pheasy_cmd_13 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -w 2 -d --symprec " f"{float(symprec)} --c2 10.0 " @@ -978,7 +986,7 @@ def generate_frequencies_eigenvectors( if len(phonon.displacements) > 3: pheasy_cmd_14 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --c2 10.0 " f"--full_ifc -w 2 --symprec {float(symprec)} " @@ -988,7 +996,7 @@ def generate_frequencies_eigenvectors( else: pheasy_cmd_14 = ( - f"pheasy --dim {int(supercell_matrix[0][0])} " + f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --full_ifc " f"--c2 10.0 -w 2 --symprec {float(symprec)} " diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index 16d749e82b..6bb45d0b0f 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -172,6 +172,52 @@ def _report_imaginary_modes(*args, **kwargs): assert parse_FORCE_CONSTANTS(str(refit)).shape == (32, 32, 3, 3) +def test_atom_on_cell_face(tmp_dir): + """An atom on a cell face must not spoil the harmonic fit. + + pheasy used to build its own supercell from POSCAR. Reading POSCAR can move + an atom on a cell face by one lattice vector, and the atoms of that supercell + then no longer matched the order of the force data. + """ + # Cu on the diamond sites of an fcc primitive cell, with the second atom + # just below x = 1 instead of at x = 0, as in a relaxed Si cell. For this + # lattice, reading POSCAR moves that atom by one lattice vector. + structure = Structure( + Lattice([[0, 2.725, 2.725], [2.725, 0, 2.725], [2.725, 2.725, 0]]), + ["Cu", "Cu"], + [[0.25, 0.25, 0.25], [1 - 1e-16, 0, 0]], + ) + kwargs = { + **COMMON_KWARGS, + "supercell_matrix": [[4, 0, 0], [0, 4, 0], [0, 0, 4]], + "cal_anhar_fcs": False, + "fcs_cutoff_radius": FCS_CUTOFF_RADIUS, + } + + job = generate_phonon_displacements( + structure=structure, + num_displaced_supercells=0, + displacement_anhar=0.03, + num_disp_anhar=0, + **kwargs, + ) + responses = run_locally(job, create_folders=True, ensure_success=True) + job = generate_frequencies_eigenvectors( + structure=structure, + displacement_data=_emt_displacement_data(responses[job.uuid][1].output), + **FIT_KWARGS, + **kwargs, + ) + run_locally(job, create_folders=True, ensure_success=True) + + (fit_dir,) = (path.parent for path in Path.cwd().glob("job_*/disp_matrix.npy")) + fc = parse_FORCE_CONSTANTS(str(fit_dir / "FORCE_CONSTANTS")) + disps = np.load(fit_dir / "disp_matrix.npy") + forces = np.load(fit_dir / "force_matrix.npy") + residual = forces + np.einsum("ijab,njb->nia", fc, disps) + assert np.linalg.norm(residual) < 0.05 * np.linalg.norm(forces) + + def test_get_num_anharmonic_supercells(monkeypatch): phonon = _generate_phonon_object(_cu_structure(), **COMMON_KWARGS) kwargs = { From 6782ea69c5cd4f416f93735a6ed71c7f9c8955b2 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Thu, 24 Sep 2026 14:55:14 -0700 Subject: [PATCH 07/43] Add finite-temperature phonon workflow from MD snapshots and pheasy --- docs/user/codes/vasp.md | 48 ++ src/atomate2/ase/md.py | 12 +- .../flows/finite_temperature_phonons.py | 437 ++++++++++ .../common/jobs/finite_temperature_phonons.py | 765 ++++++++++++++++++ src/atomate2/common/jobs/pheasy.py | 168 ++-- .../schemas/finite_temperature_phonons.py | 234 ++++++ .../flows/finite_temperature_phonons.py | 415 ++++++++++ .../vasp/flows/finite_temperature_phonons.py | 225 ++++++ src/atomate2/vasp/sets/core.py | 37 + tests/ase/test_md.py | 23 + .../jobs/test_finite_temperature_phonons.py | 663 +++++++++++++++ tests/common/jobs/test_pheasy.py | 45 +- .../flows/test_finite_temperature_phonons.py | 248 ++++++ tests/vasp/test_sets.py | 22 + 14 files changed, 3270 insertions(+), 72 deletions(-) create mode 100644 src/atomate2/common/flows/finite_temperature_phonons.py create mode 100644 src/atomate2/common/jobs/finite_temperature_phonons.py create mode 100644 src/atomate2/common/schemas/finite_temperature_phonons.py create mode 100644 src/atomate2/forcefields/flows/finite_temperature_phonons.py create mode 100644 src/atomate2/vasp/flows/finite_temperature_phonons.py create mode 100644 tests/common/jobs/test_finite_temperature_phonons.py create mode 100644 tests/vasp/flows/test_finite_temperature_phonons.py diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 7edc691cfc..1e4dcfac0d 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -402,6 +402,54 @@ The notebook `tutorials/hiphive_workflow.ipynb` reproduces it. Results on low-symmetry cells should be checked against the phonopy workflow before being trusted. The cluster space grows faster there than the number of displacements the workflow generates, and the fit can return spurious soft modes. +#### Finite-temperature phonons + +`FiniteTemperaturePhononMaker` fits effective harmonic force constants at a finite temperature, as in the temperature-dependent effective potential ([TDEP](https://doi.org/10.1103/PhysRevB.84.180301)) method. +They include the anharmonic effects at that temperature, at the volume of the relaxed structure. +Thermal expansion is not included. +The structure is relaxed first. +An NVT MD run then samples the displacements at the temperature. +By default, it runs for 8 ps at 300 K with a time step of 1 fs and a Nosé-Hoover thermostat. +The first 1 ps is left out, and 50 snapshots are picked evenly spread over the rest. +Static calculations give the forces on the snapshots and on the undisplaced supercell. +The displacements are measured from the relaxed positions. +Pheasy then fits the second-order force constants to them with LASSO. +As in the pheasy phonon workflow, a `DielectricMaker` computes the Born charges and the dielectric tensor for the non-analytical correction. +It needs the `pheasy` extra, like the pheasy phonon workflow above. + +```python +from atomate2.vasp.flows.finite_temperature_phonons import ( + FiniteTemperaturePhononMaker, +) + +flow = FiniteTemperaturePhononMaker(temperature=300).make(structure) +``` + +The MD uses looser settings than the statics, for example ENCUT = 500 eV instead of 600 eV. +Only the forces of the statics enter the fit. +The relaxation, the MD and the statics use the same functional, +U, smearing and k-point settings. +The MD and the statics start from the magnetic moments of the relaxed structure, if it has any. +Both set ISPIN from the relaxation directory with `auto_ispin`. +`md_runs` splits the MD into consecutive jobs, for example to stay within the walltime of a queue. +Each job continues from the positions and velocities of the previous one. +The thermostat variables start again from zero in each job. + +The trajectory is also checked before the fit. +The check looks for melting and for a move away from the reference structure. +It also looks at the drift of the potential energy late in the run. +The result is stored in `trajectory_health` of the output `FiniteTemperaturePhononDoc`, and a warning is raised when the check fails. +Imaginary modes are counted at the q-points commensurate with the supercell. +They are reported and not removed. + +The MD and the statics can also come from different codes. +Three more makers are in `atomate2.forcefields.flows.finite_temperature_phonons`. +`VaspMDMLFFStaticFiniteTemperaturePhononMaker` runs the MD with VASP and the statics with a force field. +`MLFFMDVaspStaticFiniteTemperaturePhononMaker` runs the MD with a force field and the statics with VASP. +`ForceFieldFiniteTemperaturePhononMaker` uses a force field for all steps. +Each has a `from_force_field_name` method to choose the force field. +They need the package of the force field, for example `mace-torch` for MACE. +All of them use the same fit. + ### Grüneisen parameter workflow Calculates mode-dependent Grüneisen parameters with the help of [Phonopy](https://doi.org/10.7566/JPSJ.92.012001). diff --git a/src/atomate2/ase/md.py b/src/atomate2/ase/md.py index 4a52c29e2d..d7a574b9cf 100644 --- a/src/atomate2/ase/md.py +++ b/src/atomate2/ase/md.py @@ -62,6 +62,7 @@ class DynamicsPresets(Enum): nvt_berendsen = "ase.md.nvtberendsen.NVTBerendsen" nvt_langevin = "ase.md.langevin.Langevin" nvt_nose_hoover = "ase.md.npt.NPT" + nvt_nose_hoover_chain = "ase.md.nose_hoover_chain.NoseHooverChainNVT" npt_berendsen = "ase.md.nptberendsen.NPTBerendsen" npt_nose_hoover = "ase.md.npt.NPT" # noqa: PIE796 npt_nose_hoover_chain = "ase.md.nose_hoover_chain.MTKNPT" @@ -403,13 +404,22 @@ def run_ase( md_runner.attach(md_observer, interval=self.traj_interval) + can_set_temperature = hasattr(md_runner, "_temperature_K") or hasattr( + md_runner, "set_temperature" + ) + if not can_set_temperature and np.ptp(self.t_schedule) > 0: + raise ValueError( + f"{type(md_runner).__name__} cannot follow a temperature schedule." + ) + def _callback(dyn: MolecularDynamics = md_runner) -> None: if self.ensemble == MDEnsemble.nve: return if hasattr(dyn, "_temperature_K"): dyn._temperature_K = self.t_schedule[dyn.nsteps] # noqa: SLF001 - else: + elif hasattr(dyn, "set_temperature"): dyn.set_temperature(temperature_K=self.t_schedule[dyn.nsteps]) + # NoseHooverChainNVT has neither and keeps its initial temperature if self.ensemble == MDEnsemble.nvt: return diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py new file mode 100644 index 0000000000..332332409a --- /dev/null +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -0,0 +1,437 @@ +"""Flow for effective harmonic phonons at a finite temperature.""" + +from __future__ import annotations + +import numbers +from abc import ABC, abstractmethod +from dataclasses import dataclass +from enum import Enum +from typing import TYPE_CHECKING, Literal + +import numpy as np +from jobflow import Flow, Maker, OutputReference +from pymatgen.util.due import Doi, due + +from atomate2 import SETTINGS +from atomate2.common.jobs.finite_temperature_phonons import ( + fit_finite_temperature_phonons, + get_md_restart_structure, + get_md_supercell, + select_md_snapshots, +) +from atomate2.common.jobs.pheasy import get_supercell_size +from atomate2.common.jobs.phonons import run_phonon_displacements + +if TYPE_CHECKING: + from pathlib import Path + + from emmet.core.math import Matrix3D + from jobflow import Job + from pymatgen.core import Structure + +SUPPORTED_CODES = frozenset(("vasp", "forcefields")) +_THERMOSTATS = ("nose-hoover", "langevin") +_ROTATIONAL_SUM_RULES = ("BH", "H", "BHH") + + +def _get_force_field(maker: Maker, code: str) -> tuple[str | None, dict | None]: + """Get the calculator name and keyword arguments of a force field maker.""" + if code != "forcefields": + return None, None + name = maker.calculator_meta + return str(name.value if isinstance(name, Enum) else name), dict( + maker.calculator_kwargs + ) + + +@due.dcite( + Doi("10.48550/arXiv.2508.01020"), + description="Pheasy code for (an)harmonic force constants.", +) +@due.dcite( + Doi("10.1103/PhysRevB.84.180301"), + description="Effective harmonic force constants fitted to MD, as in TDEP.", +) +@dataclass +class BaseFiniteTemperaturePhononMaker(Maker, ABC): + """ + Maker for effective harmonic phonons at a finite temperature. + + The structure is relaxed first. An NVT MD run at the temperature then starts + from the undisplaced supercell. The frames of the first equilibration_time + are left out, and n_snapshots snapshots are picked evenly spread over the + rest of the trajectory. The phonon displacement maker computes the forces on + these snapshots and on the undisplaced supercell. The displacements of the + snapshots are measured from the relaxed positions. pheasy fits one set of + second-order force constants to the displacements and forces with LASSO, as + in the temperature-dependent effective potential method. These force + constants contain the anharmonic effects at the temperature and at the + volume of the relaxed structure. Thermal expansion is not included. They + give the phonon band structure and density of states. Imaginary modes are + reported, not removed. + + The MD maker and the phonon displacement maker are independent. Either can + be a VASP or a force field maker, so the forces can come from a different + level of theory than the trajectory. The residual forces of the undisplaced + supercell always come from the phonon displacement maker. + + The trajectory is also checked. The check looks for melting and for a move + away from the reference structure. It also looks at the drift of the + potential energy late in the run. The result is stored in the output + document. A warning is raised if the check fails, but the fit is still done. + + .. Note:: + The atoms of the relaxed structure are sorted by electronegativity + before the supercell is built, as the VASP input sets do. The atoms are + then in the same order in every calculation. The magnetic moments of the + relaxed structure, if any, are carried over to the supercell, the + snapshots and every MD job. phonopy and pheasy find the symmetry + without the magnetic moments, as in the atomate2 phonon workflows. The + band structure uses the seekpath k-path. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + temperature: float + MD temperature in K. + md_time: float + Length of the MD trajectory in ps. + md_time_step: float + MD time step in fs. + equilibration_time: float + Time at the start of the trajectory that is left out, in ps. + n_snapshots: int + Number of MD snapshots in the fit. + thermostat: Literal["nose-hoover", "langevin"] + Thermostat of the NVT MD. + md_runs: int + Number of consecutive MD jobs that make up the trajectory. Each job + continues from the positions and velocities of the previous one. The + thermostat variables start again from zero in each job. + min_length: float + Each lattice vector of the diagonal supercell is at least min_length + long, in Angstrom. + symprec: float + Symmetry precision for phonopy and pheasy. + rotational_sum_rule: Literal["BH", "H", "BHH"] | None + Rotational sum rule passed to pheasy with --rasr. None imposes none. + alpha_min: int + Base-10 exponent of the smallest LASSO penalty in the cross-validation, + passed to pheasy with --alpha_min. The default of -6 is pheasy's own + default. A warning is raised if the chosen penalty is on either bound of + the search. + random_seed: int | None + Seed of the LASSO fit, and of the initial velocities of a force field + MD. + tol_imaginary_modes: float + Frequencies below -tol_imaginary_modes in THz are imaginary. + store_force_constants: bool + Whether to store the force constants in the output document. + code: str + Code of the phonon displacement calculations, 'vasp' or 'forcefields'. + md_code: str + Code of the MD, 'vasp' or 'forcefields'. + socket: bool + If True, the phonon displacement calculations run as a single batched + calculation. This is not supported by VASP. + bulk_relax_maker: Maker | None + Maker for the relaxation of the unit cell. None skips the relaxation. + born_maker: Maker | None + VASP maker for the Born effective charges and the dielectric tensor, + used for the non-analytical correction. None skips it. + md_maker: Maker + Maker for the MD. The flow sets its temperature, time step, number of + steps and thermostat. + phonon_displacement_maker: Maker + Maker for the static calculations on the snapshots and the undisplaced + supercell. + """ + + name: str = "finite temperature phonon" + temperature: float = 300.0 + md_time: float = 8.0 + md_time_step: float = 1.0 + equilibration_time: float = 1.0 + n_snapshots: int = 50 + thermostat: Literal["nose-hoover", "langevin"] = "nose-hoover" + md_runs: int = 1 + min_length: float = 12.0 + symprec: float = SETTINGS.PHONON_SYMPREC + rotational_sum_rule: Literal["BH", "H", "BHH"] | None = "BHH" + alpha_min: int = -6 + random_seed: int | None = 103 + tol_imaginary_modes: float = 0.1 + store_force_constants: bool = True + code: str | None = None + md_code: str | None = None + socket: bool = False + bulk_relax_maker: Maker | None = None + born_maker: Maker | None = None + md_maker: Maker | None = None + phonon_displacement_maker: Maker | None = None + + def __post_init__(self) -> None: + """Check the settings before any calculation is run.""" + if self.md_maker is None or self.phonon_displacement_maker is None: + raise ValueError("md_maker and phonon_displacement_maker must be set.") + for key in ("code", "md_code"): + if getattr(self, key) not in SUPPORTED_CODES: + raise ValueError( + f"{key} must be one of {sorted(SUPPORTED_CODES)}, not " + f"{getattr(self, key)!r}." + ) + if self.thermostat not in _THERMOSTATS: + raise ValueError( + f"thermostat must be one of {_THERMOSTATS}, not {self.thermostat!r}." + ) + if self.rotational_sum_rule not in (*_ROTATIONAL_SUM_RULES, None): + raise ValueError( + f"rotational_sum_rule must be one of {_ROTATIONAL_SUM_RULES} or " + f"None, not {self.rotational_sum_rule!r}." + ) + for key in ("md_runs", "n_snapshots"): + value = getattr(self, key) + if ( + isinstance(value, bool) + or not isinstance(value, numbers.Integral) + or value < 1 + ): + raise ValueError(f"{key} must be a positive integer, not {value!r}.") + if ( + isinstance(self.alpha_min, bool) + or not isinstance(self.alpha_min, numbers.Integral) + or self.alpha_min >= -2 + ): + raise ValueError( + f"alpha_min must be an integer below -2, not {self.alpha_min!r}." + ) + if min(self.temperature, self.md_time, self.md_time_step) <= 0: + raise ValueError("temperature, md_time and md_time_step must be positive.") + n_steps = round(self.md_time * 1000 / self.md_time_step) + n_equil = round(self.equilibration_time * 1000 / self.md_time_step) + if self.equilibration_time < 0 or n_steps - n_equil < self.n_snapshots: + raise ValueError( + f"The MD has {n_steps} steps. After leaving out equilibration_time, " + f"fewer than the {self.n_snapshots} snapshots are left." + ) + if self.md_runs > n_steps: + raise ValueError( + f"md_runs ({self.md_runs}) is larger than the {n_steps} MD steps." + ) + + def get_md_steps(self) -> list[int]: + """Get the number of MD steps of each MD job.""" + n_steps = round(self.md_time * 1000 / self.md_time_step) + base, extra = divmod(n_steps, self.md_runs) + return [base + (idx < extra) for idx in range(self.md_runs)] + + def make( + self, + structure: Structure, + prev_dir: str | Path | None = None, + supercell_matrix: Matrix3D | None = None, + born: list[Matrix3D] | None = None, + epsilon_static: Matrix3D | None = None, + ) -> Flow: + """ + Make a flow to calculate effective harmonic phonons at a temperature. + + Parameters + ---------- + structure: Structure + The unit cell. + prev_dir: str | Path | None + A previous calculation directory. It is passed to the relaxation. + The born job, the MD jobs and the phonon displacement calculations + get the relaxation directory, or this directory if there is no + relaxation. + supercell_matrix: Matrix3D | None + Diagonal supercell matrix. If None, it is chosen from min_length. + born: list[Matrix3D] | None + Born effective charges of the relaxed structure with its atoms + sorted by electronegativity. If given with epsilon_static, the + born_maker is not run. + epsilon_static: Matrix3D | None + High-frequency dielectric tensor. + + Returns + ------- + Flow + """ + if supercell_matrix is not None and not isinstance( + supercell_matrix, OutputReference + ): + matrix = np.array(supercell_matrix) + if not np.allclose(matrix, np.diag(np.diag(matrix))): + raise ValueError("pheasy needs a diagonal supercell matrix.") + + jobs: list[Job | Flow] = [] + optimization_run_job_dir = optimization_run_uuid = None + born_run_job_dir = born_run_uuid = None + + if self.bulk_relax_maker is not None: + relax = self.bulk_relax_maker.make(structure, prev_dir=prev_dir) + jobs.append(relax) + structure = relax.output.structure + prev_dir = relax.output.dir_name + optimization_run_job_dir = relax.output.dir_name + optimization_run_uuid = relax.output.uuid + + if supercell_matrix is None: + # pheasy needs a diagonal supercell matrix. With force_diagonal, + # the size only depends on min_length. + supercell_job = get_supercell_size( + structure, + self.min_length, + None, + force_90_degrees=True, + force_diagonal=True, + ) + jobs.append(supercell_job) + supercell_matrix = supercell_job.output + + if self.born_maker is not None and (born is None or epsilon_static is None): + born_job = self.born_maker.make(structure, prev_dir=prev_dir) + jobs.append(born_job) + born = born_job.output.calcs_reversed[0].output.outcar["born"] + epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static + born_run_job_dir = born_job.output.dir_name + born_run_uuid = born_job.output.uuid + + reference_job = get_md_supercell( + structure, supercell_matrix, self.symprec, self.code + ) + jobs.append(reference_job) + reference = reference_job.output + + all_md_jobs, md_jobs = self.make_md(reference, prev_dir) + jobs.extend(all_md_jobs) + md_dirs = [md_job.output.dir_name for md_job in md_jobs] + + snapshot_job = select_md_snapshots( + md_dirs, + self.md_code, + reference, + self.temperature, + self.md_time_step, + self.equilibration_time, + self.n_snapshots, + ) + jobs.append(snapshot_job) + + displacement_calcs = run_phonon_displacements( + displacements=snapshot_job.output["structures"], + structure=structure, + supercell_matrix=supercell_matrix, + phonon_maker=self.phonon_displacement_maker, + socket=self.socket, + prev_dir_argname=self.prev_calc_dir_argname, + prev_dir=prev_dir, + store_displaced_structures=True, + ) + jobs.append(displacement_calcs) + + force_field_name, force_field_kwargs = _get_force_field( + self.phonon_displacement_maker, self.code + ) + md_force_field_name, md_force_field_kwargs = _get_force_field( + self.md_maker, self.md_code + ) + fit_job = fit_finite_temperature_phonons( + structure=structure, + supercell_matrix=supercell_matrix, + snapshot_data=snapshot_job.output, + displacement_data=displacement_calcs.output, + temperature=self.temperature, + thermostat=self.thermostat, + md_time_step=self.md_time_step, + equilibration_time=self.equilibration_time, + code=self.code, + md_code=self.md_code, + symprec=self.symprec, + force_field_name=force_field_name, + force_field_kwargs=force_field_kwargs, + md_force_field_name=md_force_field_name, + md_force_field_kwargs=md_force_field_kwargs, + md_uuids=[md_job.uuid for md_job in md_jobs], + md_dirs=md_dirs, + optimization_run_uuid=optimization_run_uuid, + optimization_run_job_dir=optimization_run_job_dir, + born_run_uuid=born_run_uuid, + born_run_job_dir=born_run_job_dir, + rotational_sum_rule=self.rotational_sum_rule, + alpha_min=self.alpha_min, + random_seed=self.random_seed, + tol_imaginary_modes=self.tol_imaginary_modes, + born=born, + epsilon_static=epsilon_static, + store_force_constants=self.store_force_constants, + ) + jobs.append(fit_job) + return Flow(jobs, fit_job.output, name=self.name) + + def make_md( + self, + reference: Structure | OutputReference, + prev_dir: str | Path | None, + ) -> tuple[list[Job | Flow], list[Job]]: + """ + Make the MD jobs, starting from the undisplaced supercell. + + The first MD job starts from the undisplaced supercell. Each later one + continues from the final positions and velocities of the previous one. + + Parameters + ---------- + reference: Structure | OutputReference + The undisplaced supercell. + prev_dir: str | Path | None + A previous calculation directory, passed to each MD job. + + Returns + ------- + tuple[list[Job | Flow], list[Job]] + All jobs to add to the flow, and the MD jobs in the order of the + trajectory. + """ + jobs: list[Job | Flow] = [] + md_jobs: list[Job] = [] + structure = reference + md_steps = self.get_md_steps() + for idx, n_steps in enumerate(md_steps, start=1): + md_job = self.get_md_maker(n_steps).make(structure, prev_dir=prev_dir) + if len(md_steps) > 1: + md_job.append_name(f" {idx}/{len(md_steps)}") + jobs.append(md_job) + md_jobs.append(md_job) + if idx < len(md_steps): + restart = get_md_restart_structure( + md_job.output.dir_name, self.md_code, reference + ) + jobs.append(restart) + structure = restart.output + return jobs, md_jobs + + @property + @abstractmethod + def prev_calc_dir_argname(self) -> str | None: + """Name of the argument that passes prev_dir to the phonon displacement maker. + + As this differs between codes, it is implemented by the inheriting class. + """ + + @abstractmethod + def get_md_maker(self, n_steps: int) -> Maker: + """ + Get the maker of one MD job, with the settings of this flow. + + Parameters + ---------- + n_steps: int + Number of MD steps of the job. + + Returns + ------- + Maker + """ diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py new file mode 100644 index 0000000000..7999e1add0 --- /dev/null +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -0,0 +1,765 @@ +"""Jobs for effective harmonic phonons from MD snapshots and pheasy.""" + +from __future__ import annotations + +import logging +import warnings +from pathlib import Path +from typing import TYPE_CHECKING + +import numpy as np +from ase.io import read as ase_read +from ase.units import kB +from jobflow import job +from monty.io import zopen +from monty.os.path import zpath +from phonopy.file_IO import parse_FORCE_CONSTANTS +from phonopy.harmonic.dynmat_to_fc import get_commensurate_points +from phonopy.interface.vasp import write_vasp +from phonopy.structure.symmetry import symmetrize_borns_and_epsilon +from pymatgen.core import Structure +from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure +from pymatgen.io.vasp import Incar, Kpoints, Poscar, Xdatcar +from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine +from pymatgen.phonon.dos import PhononDos + +from atomate2.common.jobs.pheasy import ( + _DEFAULT_FILE_PATHS, + _check_lasso_alpha, + _run_harmonic_fit, +) +from atomate2.common.jobs.phonons import ( + _generate_phonon_object, + _get_kpath, + _run_band_structure_and_plot, + _run_total_dos_and_plot, +) +from atomate2.common.schemas.finite_temperature_phonons import ( + FiniteTemperaturePhononDoc, + TrajectoryHealth, +) +from atomate2.common.schemas.phonons import ( + ForceConstants, + PhononJobDirs, + PhononUUIDs, + get_factor, +) +from atomate2.utils.path import strip_hostname + +if TYPE_CHECKING: + from collections.abc import Sequence + + from emmet.core.math import Matrix3D + from phonopy import Phonopy + +logger = logging.getLogger(__name__) + +# file of the force field MD trajectory, written in the ASE format +ASE_TRAJECTORY_FILE = "md_trajectory.traj" +_KPATH_SCHEME = "seekpath" + +# Thresholds of the trajectory check. The MD starts from the reference structure, +# so a large displacement in the first frames means the atom order does not match. +_START_LIMIT = 0.5 # Angstrom +_RMS_LIMIT = 1.0 # Angstrom +_LINDEMANN_LIMIT = 0.12 +_SHIFT_RATIO_LIMIT = 1.5 +_DRIFT_SIGMA = 3.0 +_N_START_FRAMES = 10 + + +def _get_phonopy( + structure: Structure, supercell_matrix: Matrix3D, symprec: float, code: str +) -> Phonopy: + """Get the phonopy object of the sorted structure and the supercell.""" + return _generate_phonon_object( + structure.get_sorted_structure(), + supercell_matrix, + displacement=0.01, + sym_reduce=True, + symprec=symprec, + use_symmetrized_structure=None, + kpath_scheme=_KPATH_SCHEME, + code=code, + ) + + +def _get_site_properties(reference: Structure) -> dict: + """Get the magnetic moments of the reference, the only site property kept.""" + if "magmom" in reference.site_properties: + return {"magmom": reference.site_properties["magmom"]} + return {} + + +@job +def get_md_supercell( + structure: Structure, supercell_matrix: Matrix3D, symprec: float, code: str +) -> Structure: + """ + Build the supercell used as the reference structure of the MD and the fit. + + The atoms of the structure are sorted by electronegativity, as the VASP + input sets do. The supercell is then the one phonopy builds, so that its + atoms are in the order of the force constant fit. Each atom of the + supercell gets the magnetic moment of its atom in the unit cell, if the + structure has magnetic moments. + + Parameters + ---------- + structure: Structure + Relaxed unit cell. + supercell_matrix: Matrix3D + Supercell matrix. + symprec: float + Symmetry precision for phonopy. + code: str + Code of the phonon displacement calculations. + + Returns + ------- + Structure + The undisplaced supercell. + """ + structure = structure.get_sorted_structure() + supercell = _get_phonopy(structure, supercell_matrix, symprec, code).supercell + site_properties = {} + if "magmom" in structure.site_properties: + unit_index = [supercell.u2u_map[idx] for idx in supercell.s2u_map] + magmoms = structure.site_properties["magmom"] + site_properties["magmom"] = [magmoms[idx] for idx in unit_index] + return Structure( + supercell.cell, + supercell.symbols, + supercell.scaled_positions, + site_properties=site_properties, + ) + + +@job +def get_md_restart_structure( + md_dir: str, md_code: str, reference: Structure +) -> Structure: + """ + Get the final positions and velocities of an MD run. + + For VASP, they are read from CONTCAR, with the velocities in Angstrom/fs. + For force fields, they are read from the last frame of the ASE trajectory + file, with the velocities in ASE units. In both cases, the velocities are a + site property that the next MD run starts from. The thermostat variables + are not carried over, so they start again from zero in the next run. The + magnetic moments of the reference, if any, are added as a site property. + + Parameters + ---------- + md_dir: str + Directory of the MD run. + md_code: str + Code of the MD, "vasp" or "forcefields". + reference: Structure + The undisplaced supercell the MD started from. + + Returns + ------- + Structure + The final structure, with a "velocities" site property. + """ + directory = Path(strip_hostname(md_dir)) + if md_code == "vasp": + structure = Poscar.from_file(zpath(str(directory / "CONTCAR"))).structure + elif md_code == "forcefields": + atoms = ase_read(directory / ASE_TRAJECTORY_FILE, index=-1) + structure = Structure( + atoms.cell[:], + atoms.get_chemical_symbols(), + atoms.get_positions(), + coords_are_cartesian=True, + site_properties={"velocities": atoms.get_velocities().tolist()}, + ) + else: + raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") + for key, values in _get_site_properties(reference).items(): + structure.add_site_property(key, values) + return structure + + +def _read_vasp_md(directory: Path) -> tuple[np.ndarray, np.ndarray, list[str], float]: + """Read the frames, energies and time step of a VASP MD run.""" + incar = Incar.from_file(zpath(str(directory / "INCAR"))) + xdatcar = Xdatcar(zpath(str(directory / "XDATCAR"))) + frac_coords = np.array([frame.frac_coords for frame in xdatcar.structures]) + species = [str(site.specie) for site in xdatcar.structures[0]] + + # the free energy F of each ionic step + with zopen(zpath(str(directory / "OSZICAR")), mode="rt") as file: + energies = [ + float(line.split(" F= ")[1].split()[0]) + for line in file + if " T= " in line and " F= " in line + ] + if len(energies) != len(frac_coords): + raise ValueError( + f"{directory} has {len(frac_coords)} frames in XDATCAR but " + f"{len(energies)} MD steps in OSZICAR. XDATCAR must have a frame at " + "every step, with NBLOCK = 1." + ) + return frac_coords, np.array(energies), species, float(incar["POTIM"]) + + +def _read_ase_md( + directory: Path, time_step: float, skip_first: bool +) -> tuple[np.ndarray, np.ndarray, list[str], float]: + """Read the frames and energies of a force field MD run.""" + frames = ase_read(directory / ASE_TRAJECTORY_FILE, index=":") + if skip_first: + # the starting structure is the last frame of the previous MD run + frames = frames[1:] + frac_coords = np.array([atoms.get_scaled_positions() for atoms in frames]) + energies = np.array([atoms.get_potential_energy() for atoms in frames]) + return frac_coords, energies, frames[0].get_chemical_symbols(), time_step + + +def _get_displacements(frac_coords: np.ndarray, reference: Structure) -> np.ndarray: + """Cartesian displacements from the reference with the minimum image.""" + diff = frac_coords - reference.frac_coords + diff -= np.round(diff) + return diff @ reference.lattice.matrix + + +def _remove_center_of_mass(disps: np.ndarray, reference: Structure) -> np.ndarray: + """Remove the displacement of the center of mass from each frame.""" + masses = np.array([site.specie.atomic_mass for site in reference]) + center = np.einsum("i,fia->fa", masses, disps) / masses.sum() + return disps - center[:, None, :] + + +def _assess_trajectory( + frac_coords: np.ndarray, + energies: np.ndarray, + reference: Structure, + temperature: float, +) -> TrajectoryHealth: + """ + Check whether the MD trajectory stayed at the reference structure. + + The displacement of the center of mass of each frame is removed from its + displacements. The checks are applied in this order. + + - A root mean square displacement above 0.5 Angstrom in the first 10 + frames means the atoms are not in the order of the reference. + - A root mean square vibration u_vib above 0.12 of the nearest-neighbor + distance means the structure melted. + - A total displacement u_ref above 1.5 times u_vib means the mean + positions moved away from the reference. + - A change of the mean potential energy from the second to the last + quarter of the frames above 3 times the standard deviation of the + energy in the last fifth means the structure transformed (falling energy) + or is disordering (rising energy). + - A root mean square displacement above 1 Angstrom in the last fifth of the + frames points at diffusion or very soft motion. + + The energy drift is measured late in the trajectory, because a run that + starts from the reference must gain 3/2 k_B T of potential energy to reach + equipartition. + + Parameters + ---------- + frac_coords: np.ndarray + Fractional coordinates of each frame, with shape (n_frames, n_atoms, 3). + energies: np.ndarray + Potential energy of each frame in eV. + reference: Structure + The undisplaced supercell. + temperature: float + MD temperature in K. + + Returns + ------- + TrajectoryHealth + """ + n_frames, n_atoms = frac_coords.shape[:2] + disps = _remove_center_of_mass( + np.array([_get_displacements(frame, reference) for frame in frac_coords]), + reference, + ) + rms = np.sqrt(np.mean(np.sum(disps**2, axis=2), axis=1)) + rms_start = float(rms[:_N_START_FRAMES].mean()) + rms_end = float(rms[-max(1, n_frames // 5) :].mean()) + + # split the displacement in the second half into a static and a vibrational + # part, u_ref**2 = u_shift**2 + u_vib**2 + tail = disps[n_frames // 2 :] + msd_ref = float(np.mean(np.sum(tail**2, axis=2))) + msd_shift = float(np.mean(np.sum(tail.mean(axis=0) ** 2, axis=1))) + u_ref = np.sqrt(msd_ref) + u_shift = np.sqrt(msd_shift) + u_vib = np.sqrt(max(msd_ref - msd_shift, 0.0)) + + distances = reference.distance_matrix.copy() + np.fill_diagonal(distances, np.inf) + d_nn = float(distances.min(axis=1).mean()) + lindemann_ratio = u_vib / d_nn + shift_ratio = u_ref / max(u_vib, 1e-9) + + energy = energies / n_atoms + quarter = len(energy) // 4 + drift = ( + float(energy[3 * quarter :].mean() - energy[quarter : 2 * quarter].mean()) + if quarter >= 5 + else None + ) + fluctuation = float(energy[-max(1, len(energy) // 5) :].std()) + big_drift = drift is not None and abs(drift) > _DRIFT_SIGMA * max(fluctuation, 1e-9) + + if rms_start > _START_LIMIT: + verdict = "reference_mismatch" + elif lindemann_ratio > _LINDEMANN_LIMIT: + verdict = "melted" + elif shift_ratio > _SHIFT_RATIO_LIMIT: + verdict = "transformed" if big_drift and drift < 0 else "shifted_or_diffusing" + elif big_drift: + verdict = "transformed" if drift < 0 else "disordering" + elif rms_end > _RMS_LIMIT: + verdict = "diffusing_or_soft" + else: + verdict = "stable" + + return TrajectoryHealth( + verdict=verdict, + is_stable=verdict == "stable", + n_frames=n_frames, + rms_displacement_start=rms_start, + rms_displacement_end=rms_end, + u_ref=u_ref, + u_shift=u_shift, + u_vib=u_vib, + nearest_neighbor_distance=d_nn, + lindemann_ratio=lindemann_ratio, + shift_ratio=shift_ratio, + energy_drift=drift, + energy_fluctuation=fluctuation, + equipartition_rise=1.5 * kB * temperature, + ) + + +@job(data=["structures"]) +def select_md_snapshots( + md_dirs: Sequence[str], + md_code: str, + reference: Structure, + temperature: float, + md_time_step: float, + equilibration_time: float, + n_snapshots: int, +) -> dict: + """ + Pick snapshots from the MD trajectory and check the trajectory. + + The trajectories of all MD runs are joined in order, with a frame at every + time step. The time of a frame is its index in the joined trajectory times + the time step, so the first frame is at time zero. The frames of the first + equilibration_time are left out, and n_snapshots frames are picked evenly + spread over the rest. For VASP, XDATCAR, OSZICAR and the POTIM of INCAR are + read from each run directory. For force fields, the ASE trajectory file is + read. The run directories must be readable from where this job runs. + + Parameters + ---------- + md_dirs: Sequence[str] + Directories of the MD runs, in order. + md_code: str + Code of the MD, "vasp" or "forcefields". + reference: Structure + The undisplaced supercell the MD started from. + temperature: float + MD temperature in K. + md_time_step: float + MD time step in fs. Only used for force field trajectories. + equilibration_time: float + Time at the start of the trajectory that is left out, in ps. + n_snapshots: int + Number of snapshots. + + Returns + ------- + dict + The structures for the phonon displacement calculations, the + snapshots followed by the undisplaced supercell. The MD time of each + snapshot in ps. The number of frames times the time step in ps. The + root mean square displacement of the snapshots in Angstrom, with the + displacement of the center of mass removed. The trajectory check. + """ + directories = [Path(strip_hostname(md_dir)) for md_dir in md_dirs] + if len(set(directories)) != len(directories): + raise ValueError( + f"Each MD run must have its own directory, but the directories are " + f"{md_dirs}." + ) + frac_coords, energies, time_steps = [], [], set() + for idx, directory in enumerate(directories): + if md_code == "vasp": + coords, energy, species, time_step = _read_vasp_md(directory) + elif md_code == "forcefields": + coords, energy, species, time_step = _read_ase_md( + directory, md_time_step, skip_first=idx > 0 + ) + else: + raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") + if species != [str(site.specie) for site in reference]: + raise ValueError( + f"The atoms of the MD in {directory} are not in the order of the " + "reference supercell." + ) + frac_coords.append(coords) + energies.append(energy) + time_steps.add(time_step) + if len(time_steps) != 1: + raise ValueError(f"The MD runs have different time steps: {time_steps} fs.") + time_step = time_steps.pop() + all_coords = np.concatenate(frac_coords) + all_energies = np.concatenate(energies) + n_frames = len(all_coords) + + n_equil = round(equilibration_time * 1000 / time_step) + n_left = n_frames - n_equil + if n_left < n_snapshots: + raise ValueError( + f"The trajectory has {n_frames} frames of {time_step} fs. After " + f"leaving out {equilibration_time} ps, {max(n_left, 0)} frames are " + f"left, fewer than the {n_snapshots} snapshots." + ) + stride = n_left // n_snapshots + indices = list(range(n_equil, n_frames, stride))[:n_snapshots] + + site_properties = _get_site_properties(reference) + snapshots = [ + Structure( + reference.lattice, + reference.species, + all_coords[idx], + site_properties=site_properties, + ) + for idx in indices + ] + disps = _remove_center_of_mass( + np.array([_get_displacements(all_coords[idx], reference) for idx in indices]), + reference, + ) + health = _assess_trajectory(all_coords, all_energies, reference, temperature) + if not health.is_stable: + warnings.warn( + f"The MD trajectory did not stay at the reference structure (verdict: " + f"{health.verdict}). The fitted force constants may not describe it.", + stacklevel=2, + ) + return { + "structures": [*snapshots, reference], + "snapshot_times": [idx * time_step / 1000 for idx in indices], + "md_time": n_frames * time_step / 1000, + "rms_displacement": float(np.sqrt(np.mean(np.sum(disps**2, axis=2)))), + "trajectory_health": health.model_dump(), + } + + +def _get_rms_displacement(phonon: Phonopy, temperature: float, tol: float) -> float: + """ + Get the classical root mean square displacement from the force constants. + + The modes are those of the supercell at the Gamma point. A mode with a + frequency above tol in THz adds k_B T divided by its eigenvalue of the + dynamical matrix, times the sum over the atoms and Cartesian components of + its squared eigenvector component divided by the atomic mass. The sum over + the modes is divided by the number of atoms. The modes at or below tol are + left out. They include the three acoustic modes at the Gamma point, which + move the center of mass. + """ + masses = np.repeat(np.array(phonon.supercell.masses), 3) + n_dof = len(masses) + force_constants = phonon.force_constants.transpose(0, 2, 1, 3).reshape(n_dof, n_dof) + inv_sqrt_mass = 1 / np.sqrt(masses) + dynmat = force_constants * np.outer(inv_sqrt_mass, inv_sqrt_mass) + eigvals, eigvecs = np.linalg.eigh((dynmat + dynmat.T) / 2) + frequencies = np.sign(eigvals) * np.sqrt(np.abs(eigvals)) * get_factor("vasp") + keep = frequencies > tol + weights = np.sum(eigvecs[:, keep] ** 2 / masses[:, None], axis=0) + msd = kB * temperature * np.sum(weights / eigvals[keep]) + return float(np.sqrt(msd / len(phonon.supercell.masses))) + + +@job( + output_schema=FiniteTemperaturePhononDoc, + data=[PhononDos, PhononBandStructureSymmLine, ForceConstants], +) +def fit_finite_temperature_phonons( + structure: Structure, + supercell_matrix: Matrix3D, + snapshot_data: dict, + displacement_data: dict, + temperature: float, + thermostat: str, + md_time_step: float, + equilibration_time: float, + code: str, + md_code: str, + symprec: float, + force_field_name: str | None = None, + force_field_kwargs: dict | None = None, + md_force_field_name: str | None = None, + md_force_field_kwargs: dict | None = None, + md_uuids: list[str] | None = None, + md_dirs: list[str] | None = None, + optimization_run_uuid: str | None = None, + optimization_run_job_dir: str | None = None, + born_run_uuid: str | None = None, + born_run_job_dir: str | None = None, + rotational_sum_rule: str | None = "BHH", + alpha_min: int = -6, + random_seed: int | None = 103, + tol_imaginary_modes: float = 0.1, + born: list[Matrix3D] | None = None, + epsilon_static: Matrix3D | None = None, + store_force_constants: bool = True, + npoints_band: int = 101, + kpoint_density_dos: int = 7_000, +) -> FiniteTemperaturePhononDoc: + """ + Fit effective second-order force constants to MD snapshots with pheasy. + + The forces on the undisplaced supercell, the last phonon displacement + calculation, are subtracted from the forces on the snapshots. pheasy then + fits the second-order force constants with LASSO, with standardized data + and without a cutoff. phonopy imposes translational and permutation + symmetry on them. They give the phonon band structure along the seekpath + k-path and the density of states. Imaginary modes are reported, not + removed. + + Parameters + ---------- + structure: Structure + Relaxed unit cell. This job sorts its atoms by electronegativity. + supercell_matrix: Matrix3D + Diagonal supercell matrix. + snapshot_data: dict + Output of :obj:`select_md_snapshots`. + displacement_data: dict + Output of the phonon displacement calculations on the snapshots and on + the undisplaced supercell, which comes last. + temperature: float + MD temperature in K. + thermostat: str + Thermostat of the MD. + md_time_step: float + MD time step in fs. + equilibration_time: float + Time at the start of the trajectory that was left out, in ps. + code: str + Code of the phonon displacement calculations. + md_code: str + Code of the MD. + symprec: float + Symmetry precision for phonopy and pheasy. + force_field_name: str | None + Force field of the phonon displacement calculations, if any. + force_field_kwargs: dict | None + Keyword arguments of the force field calculator of the phonon + displacement calculations. + md_force_field_name: str | None + Force field of the MD, if any. + md_force_field_kwargs: dict | None + Keyword arguments of the force field calculator of the MD. + md_uuids: list[str] | None + UUIDs of the MD jobs. + md_dirs: list[str] | None + Directories of the MD jobs. + optimization_run_uuid: str | None + UUID of the relaxation. + optimization_run_job_dir: str | None + Directory of the relaxation. + born_run_uuid: str | None + UUID of the Born charge calculation. + born_run_job_dir: str | None + Directory of the Born charge calculation. + rotational_sum_rule: str | None + Rotational sum rule passed to pheasy with --rasr, or None for none. + alpha_min: int + Base-10 exponent of the smallest LASSO penalty in the cross-validation. + random_seed: int | None + Seed of the LASSO fit in pheasy. + tol_imaginary_modes: float + Frequencies below -tol_imaginary_modes in THz are imaginary. + born: list[Matrix3D] | None + Born effective charges of the sorted unit cell, for the non-analytical + correction of the dynamical matrix. + epsilon_static: Matrix3D | None + High-frequency dielectric tensor, needed together with born. + store_force_constants: bool + Whether to store the force constants in the output document. + npoints_band: int + Number of q-points per band structure segment. + kpoint_density_dos: int + Number of q-points per reciprocal atom of the density of states mesh. + + Returns + ------- + FiniteTemperaturePhononDoc + """ + supercell_matrix = np.array(supercell_matrix) + if not np.allclose(supercell_matrix, np.diag(np.diag(supercell_matrix))): + raise ValueError("pheasy needs a diagonal supercell matrix.") + + structure = structure.get_sorted_structure() + if born is not None and len(born) != len(structure): + raise ValueError("The number of Born charges is not the number of atoms.") + phonon = _get_phonopy(structure, supercell_matrix, symprec, code) + supercell = get_pmg_structure(phonon.supercell) + + forces = np.array(displacement_data["forces"]) + structures = displacement_data["displaced_structures"] + if len(structures) != len(snapshot_data["snapshot_times"]) + 1: + raise ValueError( + "The phonon displacement calculations must be the snapshots followed " + "by the undisplaced supercell." + ) + if not np.allclose(structures[-1].frac_coords, supercell.frac_coords, atol=1e-6): + raise ValueError( + "The last phonon displacement calculation is not the undisplaced supercell." + ) + residual_forces = forces[-1] + fit_forces = forces[:-1] - residual_forces + disps = np.array( + [_get_displacements(s.frac_coords, supercell) for s in structures[:-1]] + ) + n_data = len(disps) + + write_vasp("POSCAR", get_phonopy_structure(structure)) + write_vasp("SPOSCAR", phonon.supercell) + np.save(_DEFAULT_FILE_PATHS["harmonic_displacements"], disps) + np.save(_DEFAULT_FILE_PATHS["harmonic_force_matrix"], fit_forces) + + # Remove the files of an earlier fit. pheasy appends to its log, and a failed + # fit would leave the old force constants behind. + log_file = Path(_DEFAULT_FILE_PATHS["harmonic_fit_log"]) + log_file.unlink(missing_ok=True) + fc_file = Path(_DEFAULT_FILE_PATHS["force_constants"]) + fc_file.unlink(missing_ok=True) + _run_harmonic_fit( + supercell_matrix, + symprec, + n_data, + rotational_sum_rule=rotational_sum_rule, + alpha_min=alpha_min, + random_seed=random_seed, + log_file=str(log_file), + ) + + if not fc_file.exists(): + raise RuntimeError(f"pheasy did not write {fc_file}.") + lasso_alpha = _check_lasso_alpha(log_file, alpha_min, alpha_min_name="alpha_min") + phonon.force_constants = parse_FORCE_CONSTANTS(filename=str(fc_file)) + phonon.symmetrize_force_constants() + + # the fitted forces are F = -Phi u + predicted = -np.einsum("ijab,mjb->mia", phonon.force_constants, disps) + force_rmse = float(np.sqrt(np.mean((fit_forces - predicted) ** 2))) + + borns = epsilon = None + if born is not None and epsilon_static is not None: + borns, epsilon = symmetrize_borns_and_epsilon( + ucell=phonon.unitcell, + borns=np.array(born), + epsilon=np.array(epsilon_static), + symprec=symprec, + primitive_matrix=phonon.primitive_matrix, + supercell_matrix=phonon.supercell_matrix, + ) + if not np.all(np.isclose(borns, 0.0)): + phonon.nac_params = { + "born": borns, + "dielectric": epsilon, + "factor": 14.399652, + } + + # frequencies at the q-points commensurate with the supercell + matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix + phonon.run_qpoints(get_commensurate_points(np.rint(matrix).astype(int))) + frequencies = phonon.qpoints.frequencies + + kpath_dict, kpath_concrete = _get_kpath( + structure=get_pmg_structure(phonon.primitive), + kpath_scheme=_KPATH_SCHEME, + symprec=symprec, + ) + bs_symm_line, has_imaginary_modes = _run_band_structure_and_plot( + phonon, + kpath_dict, + kpath_concrete, + _DEFAULT_FILE_PATHS["band_structure"], + has_nac=phonon.nac_params is not None, + npoints_band=npoints_band, + filename_bs=_DEFAULT_FILE_PATHS["band_structure_plot"], + tol_imaginary_modes=tol_imaginary_modes, + ) + kpoint = Kpoints.automatic_density( + structure=get_pmg_structure(phonon.primitive), + kppa=kpoint_density_dos, + force_gamma=True, + ) + dos = _run_total_dos_and_plot( + phonon, + kpoint, + _DEFAULT_FILE_PATHS["dos"], + filename_dos=_DEFAULT_FILE_PATHS["dos_plot"], + ) + phonon.save(_DEFAULT_FILE_PATHS["phonopy"]) + + return FiniteTemperaturePhononDoc.from_structure( + meta_structure=structure, + structure=structure, + temperature=temperature, + code=code, + md_code=md_code, + force_field_name=force_field_name, + force_field_kwargs=force_field_kwargs, + md_force_field_name=md_force_field_name, + md_force_field_kwargs=md_force_field_kwargs, + thermostat=thermostat, + md_time_step=md_time_step, + md_time=snapshot_data["md_time"], + equilibration_time=equilibration_time, + n_snapshots=n_data, + snapshot_times=snapshot_data["snapshot_times"], + supercell_matrix=phonon.supercell_matrix.tolist(), + primitive_matrix=phonon.primitive_matrix.tolist(), + rotational_sum_rule=rotational_sum_rule, + lasso_alpha=lasso_alpha, + force_rmse=force_rmse, + max_residual_force=float(np.abs(residual_forces).max()), + rms_displacement=snapshot_data["rms_displacement"], + rms_displacement_from_force_constants=_get_rms_displacement( + phonon, temperature, tol_imaginary_modes + ), + trajectory_health=snapshot_data["trajectory_health"], + tol_imaginary_modes=tol_imaginary_modes, + has_imaginary_modes=has_imaginary_modes, + n_imaginary_modes=int(np.sum(frequencies < -tol_imaginary_modes)), + min_frequency=float(frequencies.min()), + phonon_bandstructure=bs_symm_line, + phonon_dos=dos, + force_constants=ForceConstants(phonon.force_constants.tolist()) + if store_force_constants + else None, + born=borns.tolist() if borns is not None else None, + epsilon_static=epsilon.tolist() if epsilon is not None else None, + md_uuids=md_uuids, + md_dirs=md_dirs, + uuids=PhononUUIDs( + optimization_run_uuid=optimization_run_uuid, + displacements_uuids=displacement_data["uuids"], + born_run_uuid=born_run_uuid, + ), + jobdirs=PhononJobDirs( + displacements_job_dirs=displacement_data["dirs"], + born_run_job_dir=born_run_job_dir, + optimization_run_job_dir=optimization_run_job_dir, + taskdoc_run_job_dir=str(Path.cwd()), + ), + ) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index f882e3580e..c9f588f78a 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -74,6 +74,7 @@ "one_shot_dir": "one_shot", "refit_dir": "short_cutoff_refit", "anharmonic_fit_log": "pheasy_anharmonic_fit.log", + "harmonic_fit_log": "pheasy_harmonic_fit.log", } # The anharmonic training set is sized so that the fit has this many force @@ -220,7 +221,9 @@ def _check_anharmonic_settings( ) -def _check_lasso_alpha(log_file: Path, alpha_min: int) -> None: +def _check_lasso_alpha( + log_file: Path, alpha_min: int, alpha_min_name: str = "anhar_alpha_min" +) -> float: """ Warn if the cross-validated LASSO penalty is on either bound of the search. @@ -235,11 +238,18 @@ def _check_lasso_alpha(log_file: Path, alpha_min: int) -> None: Log file written by pheasy during the fit. alpha_min: int Base-10 exponent of the smallest penalty in the search. + alpha_min_name: str + Name of the setting that gives alpha_min, used in the warning. + + Returns + ------- + float + The penalty chosen by cross-validation. """ if not log_file.exists(): raise FileNotFoundError( f"pheasy exited without writing {log_file}, so the result of the " - "anharmonic fit is unknown." + "fit is unknown." ) match = re.search(r"alpha_opt:\s*([-+0-9.eE]+)", log_file.read_text()) if match is None: @@ -258,11 +268,85 @@ def _check_lasso_alpha(log_file: Path, alpha_min: int) -> None: if alpha_opt <= 10.0**alpha_min * (1 + 1e-6): warnings.warn( f"The LASSO penalty chosen by cross-validation ({alpha_opt:e}) is on " - f"the lower bound 1e{alpha_min} in {log_file}. The anharmonic force " - "constants depend on this bound and may be wrong. Lower " - "anhar_alpha_min and refit.", + f"the lower bound 1e{alpha_min} in {log_file}. The force constants " + f"depend on this bound and may be wrong. Lower {alpha_min_name} and " + "refit.", stacklevel=2, ) + return alpha_opt + + +def _run_harmonic_fit( + supercell_matrix: np.ndarray, + symprec: float, + num_har: int, + use_lasso: bool = True, + rotational_sum_rule: str | None = "BHH", + alpha_min: int | None = None, + random_seed: int | None = 103, + log_file: str | None = None, +) -> None: + """ + Fit the second-order force constants with pheasy in the current folder. + + pheasy reads POSCAR, SPOSCAR and the harmonic displacement and force + matrices, and writes FORCE_CONSTANTS. The caller removes the files of an + earlier fit and checks the result, since the pheasy phonon workflow and + the finite-temperature workflow check different things. + + Parameters + ---------- + supercell_matrix: np.ndarray + Diagonal supercell matrix. + symprec: float + Symmetry precision. + num_har: int + Number of displaced supercells in the fit. + use_lasso: bool + If True, fit with LASSO on standardized data. If False, fit with + pheasy's default least squares. + rotational_sum_rule: str | None + Rotational sum rule passed to pheasy with --rasr, or None for none. + alpha_min: int | None + Base-10 exponent of the smallest LASSO penalty in the search. None + keeps pheasy's default. Ignored without LASSO. + random_seed: int | None + Seed for the LASSO fit. Ignored without LASSO. + log_file: str | None + Log file of the fit. None keeps pheasy's default. + """ + dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) + base = f"pheasy --scell SPOSCAR --dim {dim} -w 2 --symprec {float(symprec)}" + fit = f"{base} -f --full_ifc" + if use_lasso: + fit += " -l LASSO --std" + if alpha_min is not None: + fit += f" --alpha_min {int(alpha_min)}" + if random_seed is not None: + fit += f" --seed {int(random_seed)}" + if rotational_sum_rule is not None: + fit += f" --rasr {rotational_sum_rule}" + fit += ( + f" --ndata {int(num_har)} " + f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" + ) + if log_file is not None: + fit += f" -o {log_file}" + + commands = [ + # clusters and orbits of the second-order force constants + f"{base} -s --nbody 2", + # null space + f"{base} -c", + # sensing matrix from the displacement matrix + ( + f"{base} -d --ndata {int(num_har)} --disp_file " + f"--disp_matrix_file {_DEFAULT_FILE_PATHS['harmonic_displacements']}" + ), + fit, + ] + for cmd in commands: + subprocess.run(shlex.split(cmd), check=True) def _run_anharmonic_fit( @@ -741,71 +825,17 @@ def generate_frequencies_eigenvectors( prim = ase_read("POSCAR") supercell = ase_read("SPOSCAR") - # Create the clusters and orbitals for second order force constants. - # The harmonic fit is always second order (-w 2, --nbody 2). - pheasy_cmd_1 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} " - f"-s -w 2 --symprec {float(symprec)} --nbody 2" - ) - - # Create the null space to further reduce the free parameters for - # specific force constants and make them physically correct. - pheasy_cmd_2 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -c --symprec " - f"{float(symprec)} -w 2" - ) - - # Generate the Compressive Sensing matrix,i.e., displacement matrix - # for the input of machine leaning method.i.e., LASSO, - pheasy_cmd_3 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -w 2 -d " - f"--symprec {float(symprec)} " - f"--ndata {int(num_har)} --disp_file " - f"--disp_matrix_file {_DEFAULT_FILE_PATHS['harmonic_displacements']}" - ) - - # Here we set a criteria to determine which method to use to generate the - # force constants. If the number of displacements is larger than 3, we - # will use the LASSO method to generate the force constants. Otherwise, - # we will use the least-squred method to generate the force constants. - if len(phonon.displacements) > 3: - # Calculate the force constants using the LASSO method due to the - # random-displacement method Obviously, the rotaional invariance - # constraint, i.e., tag: --rasr BHH, is enforced during the - # fitting process. - pheasy_cmd_4 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -f --full_ifc " - f"-w 2 --symprec {float(symprec)} " - f"-l LASSO --std --rasr BHH --ndata {int(num_har)} " - f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" - + (f" --seed {int(random_seed)}" if random_seed is not None else "") - ) - - else: - # Calculate the force constants using the least-squred method - pheasy_cmd_4 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " - f"{int(supercell_matrix[1][1])} " - f"{int(supercell_matrix[2][2])} -f --full_ifc " - f"-w 2 --symprec {float(symprec)} " - f"--rasr BHH --ndata {int(num_har)} " - f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" - ) - + # With more than 3 displacements, the random-displacement data are fitted + # with LASSO. Otherwise, least squares is used. The rotational sum rule + # BHH is enforced in both. logger.info("Start running pheasy in cluster") - - subprocess.call(shlex.split(pheasy_cmd_1)) - subprocess.call(shlex.split(pheasy_cmd_2)) - subprocess.call(shlex.split(pheasy_cmd_3)) - subprocess.call(shlex.split(pheasy_cmd_4)) + _run_harmonic_fit( + supercell_matrix, + symprec, + num_har, + use_lasso=len(phonon.displacements) > 3, + random_seed=random_seed, + ) fc_file = Path(_DEFAULT_FILE_PATHS["force_constants"]) if cal_anhar_fcs and not fc_file.exists(): diff --git a/src/atomate2/common/schemas/finite_temperature_phonons.py b/src/atomate2/common/schemas/finite_temperature_phonons.py new file mode 100644 index 0000000000..eae1e3f6c6 --- /dev/null +++ b/src/atomate2/common/schemas/finite_temperature_phonons.py @@ -0,0 +1,234 @@ +"""Schemas for the finite-temperature phonon workflow.""" + +from typing import Literal + +from emmet.core.math import Matrix3D +from emmet.core.structure import StructureMetadata +from pydantic import BaseModel, Field +from pymatgen.core import Structure +from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine +from pymatgen.phonon.dos import PhononDos + +from atomate2.common.schemas.phonons import ForceConstants, PhononJobDirs, PhononUUIDs + + +class TrajectoryHealth(BaseModel): + """Check whether the MD trajectory stayed at the reference structure. + + A second-order fit describes small vibrations around the reference + structure. If the atoms melt, move to another structure or diffuse, the + fitted force constants may not describe small vibrations around the + reference. The fit error does not show this, so it is measured on the + trajectory. The displacement of the center of mass of each frame is + removed from its displacements. + """ + + verdict: ( + Literal[ + "stable", + "melted", + "transformed", + "shifted_or_diffusing", + "disordering", + "diffusing_or_soft", + "reference_mismatch", + ] + | None + ) = Field( + None, + description="Result of the check. 'reference_mismatch' means the atoms of " + "the MD are not in the order of the reference. Every other verdict except " + "'stable' means the trajectory left the reference structure.", + ) + is_stable: bool | None = Field(None, description="True if the verdict is 'stable'.") + n_frames: int | None = Field(None, description="Number of MD frames analysed.") + rms_displacement_start: float | None = Field( + None, + description="Root mean square displacement from the reference structure in " + "the first 10 frames, in Angstrom. The MD starts from the reference, so a " + "large value points at a mismatch in atom order.", + ) + rms_displacement_end: float | None = Field( + None, + description="Root mean square displacement from the reference structure in " + "the last fifth of the frames, in Angstrom.", + ) + u_ref: float | None = Field( + None, + description="Root mean square displacement from the reference structure in " + "the second half of the frames, in Angstrom.", + ) + u_shift: float | None = Field( + None, + description="Root mean square displacement of the mean atomic positions from " + "the reference structure in the second half of the frames, in Angstrom.", + ) + u_vib: float | None = Field( + None, + description="Root mean square vibration around the mean atomic positions in " + "the second half of the frames, in Angstrom. u_ref**2 = u_shift**2 + " + "u_vib**2.", + ) + nearest_neighbor_distance: float | None = Field( + None, + description="Nearest-neighbor distance of each atom in the reference " + "structure, averaged over the atoms, in Angstrom.", + ) + lindemann_ratio: float | None = Field( + None, description="u_vib divided by the nearest-neighbor distance." + ) + shift_ratio: float | None = Field(None, description="u_ref divided by u_vib.") + energy_drift: float | None = Field( + None, + description="Mean potential energy in the last quarter of the frames minus " + "that in the second quarter, in eV/atom. None for fewer than 20 frames.", + ) + energy_fluctuation: float | None = Field( + None, + description="Standard deviation of the potential energy in the last fifth of " + "the frames, in eV/atom.", + ) + equipartition_rise: float | None = Field( + None, + description="Potential energy per atom that a harmonic MD run gains when " + "it starts from the reference structure, 3/2 k_B T, in eV/atom.", + ) + + +class FiniteTemperaturePhononDoc(StructureMetadata): + """Effective harmonic phonons at a finite temperature.""" + + structure: Structure | None = Field( + None, + description="Relaxed unit cell, with its atoms sorted by electronegativity.", + ) + temperature: float | None = Field(None, description="MD temperature in K.") + code: str | None = Field( + None, + description="Code of the phonon displacement calculations that give the " + "forces, 'vasp' or 'forcefields'.", + ) + md_code: str | None = Field( + None, description="Code of the MD, 'vasp' or 'forcefields'." + ) + force_field_name: str | None = Field( + None, + description="Force field of the phonon displacement calculations, if a " + "force field was used.", + ) + force_field_kwargs: dict | None = Field( + None, + description="Keyword arguments of the force field calculator of the phonon " + "displacement calculations.", + ) + md_force_field_name: str | None = Field( + None, description="Force field of the MD, if a force field was used." + ) + md_force_field_kwargs: dict | None = Field( + None, description="Keyword arguments of the force field calculator of the MD." + ) + thermostat: str | None = Field(None, description="Thermostat of the NVT MD.") + md_time_step: float | None = Field(None, description="MD time step in fs.") + md_time: float | None = Field( + None, + description="Number of MD frames read from disk times the time step, in ps.", + ) + equilibration_time: float | None = Field( + None, description="Time at the start of the trajectory left out, in ps." + ) + n_snapshots: int | None = Field( + None, description="Number of MD snapshots in the force constant fit." + ) + snapshot_times: list[float] | None = Field( + None, + description="MD time of each snapshot in ps, with the first frame of the " + "trajectory at time zero.", + ) + supercell_matrix: Matrix3D | None = Field( + None, description="Supercell matrix of the MD and the statics." + ) + primitive_matrix: Matrix3D | None = Field( + None, description="Primitive matrix used by phonopy." + ) + rotational_sum_rule: str | None = Field( + None, description="Rotational sum rule passed to pheasy with --rasr." + ) + lasso_alpha: float | None = Field( + None, description="LASSO penalty chosen by cross-validation in pheasy." + ) + force_rmse: float | None = Field( + None, + description="Root mean square error of the symmetrized force constants on " + "the snapshot forces used in the fit, in eV/Angstrom.", + ) + max_residual_force: float | None = Field( + None, + description="Largest force component on the undisplaced supercell, in " + "eV/Angstrom. The residual forces of this supercell are subtracted from the " + "snapshot forces before the fit.", + ) + rms_displacement: float | None = Field( + None, + description="Root mean square displacement of the snapshots from the " + "reference structure, with the displacement of the center of mass of each " + "snapshot removed, in Angstrom.", + ) + rms_displacement_from_force_constants: float | None = Field( + None, + description="Classical root mean square displacement at the temperature from " + "the fitted force constants, in Angstrom. It sums the modes of the " + "supercell at the Gamma point with a frequency above tol_imaginary_modes.", + ) + trajectory_health: TrajectoryHealth | None = Field( + None, description="Check of the MD trajectory." + ) + tol_imaginary_modes: float | None = Field( + None, description="Frequencies below -tol_imaginary_modes in THz are imaginary." + ) + has_imaginary_modes: bool | None = Field( + None, description="True if the band structure has imaginary modes." + ) + n_imaginary_modes: int | None = Field( + None, + description="Number of imaginary modes at the q-points commensurate with the " + "supercell.", + ) + min_frequency: float | None = Field( + None, + description="Lowest frequency at the q-points commensurate with the " + "supercell, in THz. Imaginary frequencies are negative.", + ) + phonon_bandstructure: PhononBandStructureSymmLine | None = Field( + None, description="Phonon band structure of the effective force constants." + ) + phonon_dos: PhononDos | None = Field( + None, description="Phonon density of states of the effective force constants." + ) + force_constants: ForceConstants | None = Field( + None, + description="Effective second-order force constants of the supercell in " + "eV/Angstrom^2.", + ) + born: list[Matrix3D] | None = Field( + None, + description="Symmetrized Born effective charges. They are used for the " + "non-analytical correction unless they are all zero.", + ) + epsilon_static: Matrix3D | None = Field( + None, + description="Symmetrized high-frequency dielectric tensor, used for the " + "non-analytical correction together with born.", + ) + md_uuids: list[str] | None = Field(None, description="UUIDs of the MD jobs.") + md_dirs: list[str] | None = Field(None, description="Directories of the MD jobs.") + uuids: PhononUUIDs | None = Field( + None, + description="UUIDs of the relaxation, the phonon displacement calculations " + "and the Born charge calculation. The undisplaced supercell is the last " + "phonon displacement calculation.", + ) + jobdirs: PhononJobDirs | None = Field( + None, + description="Directories of the relaxation, the phonon displacement " + "calculations, the Born charge calculation and the fit.", + ) diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py new file mode 100644 index 0000000000..354c7494c8 --- /dev/null +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -0,0 +1,415 @@ +"""Define the force field makers for finite-temperature phonons.""" + +from __future__ import annotations + +import math +from dataclasses import dataclass, field, replace +from typing import TYPE_CHECKING + +from ase import units + +from atomate2.ase.md import MDEnsemble +from atomate2.common.flows.finite_temperature_phonons import ( + BaseFiniteTemperaturePhononMaker, +) +from atomate2.common.jobs.finite_temperature_phonons import ASE_TRAJECTORY_FILE +from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.md import ForceFieldMDMaker +from atomate2.vasp.flows.finite_temperature_phonons import FiniteTemperaturePhononMaker + +if TYPE_CHECKING: + from jobflow import Maker + from typing_extensions import Self + + from atomate2.forcefields import MLFF + +_DEFAULT_FORCE_FIELD = "MACE-MP-0" + +# VASP sets the Nose mass for SMASS = 0 so that the temperature oscillates with a +# period of about 40 time steps. With ASE's thermostat mass Q = 3 N k_B T tdamp**2, the +# linearised Nose-Hoover period is close to pi * sqrt(2) * tdamp. +_NOSE_HOOVER_TDAMP_STEPS = 40 / (math.pi * math.sqrt(2)) + + +def _get_md_maker( + force_field_name: str | MLFF | dict, calculator_kwargs: dict | None = None +) -> ForceFieldMDMaker: + """Get the force field MD maker, whose settings the flow sets.""" + return ForceFieldMDMaker( + force_field_name=force_field_name, + calculator_kwargs=calculator_kwargs or {}, + store_trajectory="no", + ionic_step_data=("energy",), + ) + + +def _get_force_field_md_maker( + maker: BaseFiniteTemperaturePhononMaker, n_steps: int +) -> ForceFieldMDMaker: + """ + Get the force field MD maker of one MD job of a finite-temperature flow. + + See :obj:`ForceFieldFiniteTemperaturePhononMaker` for the MD settings. + + Parameters + ---------- + maker: .BaseFiniteTemperaturePhononMaker + The finite-temperature phonon maker. + n_steps: int + Number of MD steps of the job. + + Returns + ------- + ForceFieldMDMaker + """ + md_maker = maker.md_maker + if not isinstance(md_maker, ForceFieldMDMaker): + raise TypeError( + f"The MD maker must be a ForceFieldMDMaker, not {type(md_maker).__name__}." + ) + if md_maker.dynamics is not None or md_maker.ase_md_kwargs: + raise ValueError( + "The flow sets the thermostat. The MD maker must not set dynamics or " + "ase_md_kwargs." + ) + if maker.thermostat == "nose-hoover": + dynamics = "nose-hoover-chain" + md_kwargs = { + "tdamp": _NOSE_HOOVER_TDAMP_STEPS * maker.md_time_step * units.fs, + "tchain": 1, + } + else: + # AseMDMaker sets its default friction of 10 ps^-1 + dynamics = "langevin" + md_kwargs = {} + return replace( + md_maker, + ensemble=MDEnsemble.nvt, + temperature=maker.temperature, + n_steps=n_steps, + time_step=maker.md_time_step, + dynamics=dynamics, + ase_md_kwargs=md_kwargs, + traj_file=ASE_TRAJECTORY_FILE, + traj_file_fmt="ase", + traj_interval=1, + mb_velocity_seed=maker.random_seed, + zero_linear_momentum=True, + ) + + +@dataclass +class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): + """ + Maker for effective harmonic phonons at a finite temperature with a force field. + + The relaxation, the MD and the phonon displacement calculations all use one + force field, MACE-MP-0 by default. Use :obj:`from_force_field_name` to use + another one. The MD writes an ASE trajectory file with a frame at every + time step. The snapshots are read from this file, and the trajectory is not + stored in the output document of the MD job. The Nose-Hoover thermostat is + ASE's NoseHooverChainNVT with one thermostat variable, like MDALGO = 2 in + VASP. Its time constant gives a period of about 40 time steps, like SMASS = + 0 in VASP. The Langevin thermostat has the default friction of + :obj:`.AseMDMaker`, 10 ps^-1. The initial velocities of the first MD job + follow the Maxwell-Boltzmann distribution, seeded with random_seed, with + zero total momentum. + + See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + bulk_relax_maker: .ForceFieldRelaxMaker | None + Maker for the relaxation of the unit cell. It keeps the symmetry of + the structure. None skips the relaxation. + born_maker: .Maker | None + Maker for the Born effective charges and the dielectric tensor. It is + None by default, as in the force field pheasy phonon workflow. + md_maker: .ForceFieldMDMaker + Maker for the MD. It must not set dynamics or ase_md_kwargs, since the + flow sets the thermostat. + phonon_displacement_maker: .ForceFieldStaticMaker + Maker for the static calculations on the snapshots and the undisplaced + supercell. + code: str + Code of the phonon displacement calculations. + md_code: str + Code of the MD. + """ + + name: str = "force field finite temperature phonon" + bulk_relax_maker: ForceFieldRelaxMaker | None = field( + default_factory=lambda: ForceFieldRelaxMaker( + force_field_name=_DEFAULT_FORCE_FIELD, + relax_kwargs={"fmax": 1e-5}, + fix_symmetry=True, + ) + ) + md_maker: ForceFieldMDMaker = field( + default_factory=lambda: _get_md_maker(_DEFAULT_FORCE_FIELD) + ) + phonon_displacement_maker: ForceFieldStaticMaker = field( + default_factory=lambda: ForceFieldStaticMaker( + force_field_name=_DEFAULT_FORCE_FIELD + ) + ) + code: str = "forcefields" + md_code: str = "forcefields" + + @property + def prev_calc_dir_argname(self) -> None: + """Name of the argument that passes prev_dir to the phonon displacement maker. + + Force field makers take no previous directory. + """ + return + + def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: + """ + Get the force field MD maker of one MD job. + + Parameters + ---------- + n_steps: int + Number of MD steps of the job. + + Returns + ------- + ForceFieldMDMaker + """ + return _get_force_field_md_maker(self, n_steps) + + @classmethod + def from_force_field_name( + cls, + force_field_name: str | MLFF | dict, + calculator_kwargs: dict | None = None, + relax_initial_structure: bool = True, + **kwargs, + ) -> Self: + """ + Create a finite-temperature phonon flow from a force field name. + + The relaxation, the MD and the phonon displacement calculations use the + force field, and born_maker is None. These makers replace any given in + kwargs. + + Parameters + ---------- + force_field_name : str or .MLFF or dict + The name of the force field. + calculator_kwargs : dict | None + The keyword arguments to pass to the calculator. + relax_initial_structure: bool = True + Whether to relax the initial structure. + **kwargs + Additional kwargs to pass to ForceFieldFiniteTemperaturePhononMaker. + + Returns + ------- + ForceFieldFiniteTemperaturePhononMaker + """ + calculator_kwargs = calculator_kwargs or {} + phonon_displacement_maker = ForceFieldStaticMaker( + force_field_name=force_field_name, + calculator_kwargs=calculator_kwargs, + ) + kwargs.update( + bulk_relax_maker=( + ForceFieldRelaxMaker( + force_field_name=force_field_name, + calculator_kwargs=calculator_kwargs, + relax_kwargs={"fmax": 1e-5}, + fix_symmetry=True, + ) + if relax_initial_structure + else None + ), + md_maker=_get_md_maker(force_field_name, calculator_kwargs), + phonon_displacement_maker=phonon_displacement_maker, + born_maker=None, + ) + return cls( + name=( + f"{phonon_displacement_maker.mlff.name} Finite Temperature Phonon Maker" + ), + **kwargs, + ) + + +@dataclass +class VaspMDMLFFStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker): + """ + Maker for finite-temperature phonons from VASP MD and force field statics. + + The relaxation and the MD are those of + :obj:`.FiniteTemperaturePhononMaker`. The forces on the snapshots and on + the undisplaced supercell come from a force field, MACE-MP-0 by default. + Use :obj:`from_force_field_name` to use another one. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + bulk_relax_maker: .Maker | None + Maker for the relaxation of the unit cell. None skips the relaxation. + born_maker: .Maker | None + Maker for the Born effective charges and the dielectric tensor. It is + None by default, as in the force field pheasy phonon workflow, since + the force constants come from the force field. + md_maker: .MDMaker + Maker for the MD, see :obj:`.FiniteTemperaturePhononMaker`. + phonon_displacement_maker: .ForceFieldStaticMaker + Maker for the static calculations on the snapshots and the undisplaced + supercell. + code: str + Code of the phonon displacement calculations. + """ + + name: str = "vasp md mlff static finite temperature phonon" + born_maker: Maker | None = None + phonon_displacement_maker: Maker = field( + default_factory=lambda: ForceFieldStaticMaker( + force_field_name=_DEFAULT_FORCE_FIELD + ) + ) + code: str = "forcefields" + + @property + def prev_calc_dir_argname(self) -> None: + """Name of the argument that passes prev_dir to the phonon displacement maker. + + Force field makers take no previous directory. + """ + return + + @classmethod + def from_force_field_name( + cls, + force_field_name: str | MLFF | dict, + calculator_kwargs: dict | None = None, + **kwargs, + ) -> Self: + """ + Create a finite-temperature phonon flow whose statics use a force field. + + The phonon displacement calculations use the force field, and born_maker + is None. These makers replace any given in kwargs. + + Parameters + ---------- + force_field_name : str or .MLFF or dict + The name of the force field. + calculator_kwargs : dict | None + The keyword arguments to pass to the calculator. + **kwargs + Additional kwargs to pass to + VaspMDMLFFStaticFiniteTemperaturePhononMaker. + + Returns + ------- + VaspMDMLFFStaticFiniteTemperaturePhononMaker + """ + phonon_displacement_maker = ForceFieldStaticMaker( + force_field_name=force_field_name, + calculator_kwargs=calculator_kwargs or {}, + ) + kwargs.update( + phonon_displacement_maker=phonon_displacement_maker, born_maker=None + ) + return cls( + name=( + f"VASP MD {phonon_displacement_maker.mlff.name} Static Finite " + "Temperature Phonon Maker" + ), + **kwargs, + ) + + +@dataclass +class MLFFMDVaspStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker): + """ + Maker for finite-temperature phonons from force field MD and VASP statics. + + The relaxation, the Born charges and the phonon displacement calculations + are those of :obj:`.FiniteTemperaturePhononMaker`. The MD uses a force + field, MACE-MP-0 by default, and starts from the supercell of the + VASP-relaxed structure. Use :obj:`from_force_field_name` to use another + force field. The MD settings are those of + :obj:`ForceFieldFiniteTemperaturePhononMaker`. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + bulk_relax_maker: .Maker | None + Maker for the relaxation of the unit cell. None skips the relaxation. + born_maker: .BaseVaspMaker | None + Maker for the Born effective charges and the dielectric tensor, used + for the non-analytical correction. It is a DielectricMaker by default, + as in the VASP pheasy phonon workflow. None skips it. + md_maker: .ForceFieldMDMaker + Maker for the MD. It must not set dynamics or ase_md_kwargs, since the + flow sets the thermostat. + phonon_displacement_maker: .BaseVaspMaker + Maker for the static calculations on the snapshots and the undisplaced + supercell. + md_code: str + Code of the MD. + """ + + name: str = "mlff md vasp static finite temperature phonon" + md_maker: Maker = field(default_factory=lambda: _get_md_maker(_DEFAULT_FORCE_FIELD)) + md_code: str = "forcefields" + + def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: + """ + Get the force field MD maker of one MD job. + + Parameters + ---------- + n_steps: int + Number of MD steps of the job. + + Returns + ------- + ForceFieldMDMaker + """ + return _get_force_field_md_maker(self, n_steps) + + @classmethod + def from_force_field_name( + cls, + force_field_name: str | MLFF | dict, + calculator_kwargs: dict | None = None, + **kwargs, + ) -> Self: + """ + Create a finite-temperature phonon flow whose MD uses a force field. + + The MD maker built for the force field replaces any given in kwargs. + + Parameters + ---------- + force_field_name : str or .MLFF or dict + The name of the force field. + calculator_kwargs : dict | None + The keyword arguments to pass to the calculator. + **kwargs + Additional kwargs to pass to + MLFFMDVaspStaticFiniteTemperaturePhononMaker. + + Returns + ------- + MLFFMDVaspStaticFiniteTemperaturePhononMaker + """ + md_maker = _get_md_maker(force_field_name, calculator_kwargs) + kwargs.update(md_maker=md_maker) + return cls( + name=( + f"{md_maker.mlff.name} MD VASP Static Finite Temperature Phonon Maker" + ), + **kwargs, + ) diff --git a/src/atomate2/vasp/flows/finite_temperature_phonons.py b/src/atomate2/vasp/flows/finite_temperature_phonons.py new file mode 100644 index 0000000000..a82e3335ba --- /dev/null +++ b/src/atomate2/vasp/flows/finite_temperature_phonons.py @@ -0,0 +1,225 @@ +"""Define the VASP maker for finite-temperature phonons.""" + +from __future__ import annotations + +from dataclasses import dataclass, field, fields, replace +from typing import TYPE_CHECKING + +from atomate2.common.flows.finite_temperature_phonons import ( + BaseFiniteTemperaturePhononMaker, +) +from atomate2.vasp.flows.core import DoubleRelaxMaker +from atomate2.vasp.jobs.core import DielectricMaker, TightRelaxMaker +from atomate2.vasp.jobs.md import MDMaker +from atomate2.vasp.jobs.phonons import PhononDisplacementMaker +from atomate2.vasp.sets.core import ( + LangevinMDSetGenerator, + MDSetGenerator, + StaticSetGenerator, + TightRelaxSetGenerator, +) + +if TYPE_CHECKING: + from jobflow import Maker + + from atomate2.vasp.jobs.base import BaseVaspMaker + +# The relaxation, the MD and the phonon displacement calculations use the same +# smearing and k-point density. +_ELECTRONIC_INCAR = {"ISMEAR": 0, "SIGMA": 0.05} +_KPOINTS = {"reciprocal_density": 100} + +# The MD only samples the displacements. The forces of the fit come from the +# phonon displacement calculations, which use tighter settings. +_MD_INCAR = { + "ENCUT": 500, + "EDIFF": 1e-5, + "PREC": "Normal", + "ALGO": "Normal", + "LREAL": "Auto", + "NBLOCK": 1, + "LWAVE": False, + "LCHARG": False, + **_ELECTRONIC_INCAR, +} +_STATIC_INCAR = { + "IBRION": 2, + "ISIF": 3, + "NSW": 0, + "ENCUT": 600, + "ENAUG": 1360, + "EDIFF": 1e-7, + "PREC": "Accurate", + "ALGO": "Normal", + "LASPH": True, + "NELM": 200, + "LREAL": False, + "LAECHG": False, + "LCHARG": False, + "LWAVE": False, + **_ELECTRONIC_INCAR, +} +_RELAX_INCAR = { + key: _STATIC_INCAR[key] for key in ("ENCUT", "ENAUG", "PREC", "LASPH") +} | _ELECTRONIC_INCAR + +# INCAR tags of the MD that the flow sets +_MD_FLOW_TAGS = ( + "IBRION", + "ISIF", + "LANGEVIN_GAMMA", + "MDALGO", + "NSW", + "POTIM", + "SMASS", + "TEBEG", + "TEEND", +) + + +def _get_relax_maker() -> DoubleRelaxMaker: + """Get a tight relaxation with the basis set and smearing of the statics.""" + return DoubleRelaxMaker.from_relax_maker( + TightRelaxMaker( + input_set_generator=TightRelaxSetGenerator( + user_incar_settings=dict(_RELAX_INCAR), + user_kpoints_settings=dict(_KPOINTS), + ) + ) + ) + + +def _get_md_maker() -> MDMaker: + """Get the MD maker, whose temperature, steps and thermostat the flow sets.""" + return MDMaker( + input_set_generator=MDSetGenerator( + user_incar_settings=dict(_MD_INCAR), + user_kpoints_settings=dict(_KPOINTS), + ) + ) + + +def _get_phonon_displacement_maker() -> PhononDisplacementMaker: + """Get the static maker for the forces on the snapshots.""" + return PhononDisplacementMaker( + input_set_generator=StaticSetGenerator( + user_incar_settings=dict(_STATIC_INCAR), + user_kpoints_settings=dict(_KPOINTS), + auto_ispin=True, + ) + ) + + +@dataclass +class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): + """ + Maker for effective harmonic phonons at a finite temperature with VASP. + + The relaxation, the MD and the phonon displacement calculations use VASP. + The functional, the spin settings and +U follow the atomate2 VASP defaults. + All three use ISMEAR = 0 with SIGMA = 0.05 and the same reciprocal_density + setting of 100. The relaxation is a double tight relaxation with ENCUT = + 600 eV, ENAUG = 1360 eV and PREC = Accurate, as in the phonon displacement + calculations. These also use EDIFF = 1e-7. The MD uses ENCUT = 500 eV, + EDIFF = 1e-5 and PREC = Normal, and writes every step to XDATCAR with + NBLOCK = 1. The Nose-Hoover thermostat uses MDALGO = 2 and SMASS = 0. The + Langevin thermostat uses MDALGO = 3 with LANGEVIN_GAMMA = 10 ps^-1 for each + species. VASP draws the initial velocities of the first MD job. The MD and + the phonon displacement calculations start from the magnetic moments of the + relaxed structure, if it has any. They all get the same prev_dir, the + relaxation directory by default. auto_ispin of the MD and of the phonon + displacement calculations sets ISPIN from it. + + See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + bulk_relax_maker: .Maker | None + Maker for the relaxation of the unit cell. None skips the relaxation. + born_maker: .BaseVaspMaker | None + Maker for the Born effective charges and the dielectric tensor, used + for the non-analytical correction. It is a DielectricMaker by default, + as in the VASP pheasy phonon workflow. None skips it. + md_maker: .MDMaker + Maker for the MD, with an :obj:`.MDSetGenerator`. Its + user_incar_settings must not contain IBRION, ISIF, LANGEVIN_GAMMA, + MDALGO, NSW, POTIM, SMASS, TEBEG or TEEND, since the flow sets them. + NBLOCK must be 1 if it is set. + phonon_displacement_maker: .BaseVaspMaker + Maker for the static calculations on the snapshots and the undisplaced + supercell. + code: str + Code of the phonon displacement calculations. + md_code: str + Code of the MD. + """ + + bulk_relax_maker: Maker | None = field(default_factory=_get_relax_maker) + born_maker: BaseVaspMaker | None = field(default_factory=DielectricMaker) + md_maker: Maker = field(default_factory=_get_md_maker) + phonon_displacement_maker: Maker = field( + default_factory=_get_phonon_displacement_maker + ) + code: str = "vasp" + md_code: str = "vasp" + + @property + def prev_calc_dir_argname(self) -> str | None: + """Name of the argument that passes prev_dir to the phonon displacement maker. + + Returns + ------- + str + """ + return "prev_dir" + + def get_md_maker(self, n_steps: int) -> MDMaker: + """ + Get the VASP MD maker of one MD job. + + Parameters + ---------- + n_steps: int + Number of MD steps of the job. + + Returns + ------- + MDMaker + """ + md_maker = self.md_maker + if not isinstance(md_maker, MDMaker) or not isinstance( + md_maker.input_set_generator, MDSetGenerator + ): + raise TypeError( + "The MD maker must be a VASP MDMaker with an MDSetGenerator." + ) + generator = md_maker.input_set_generator + user_incar = generator.user_incar_settings + if tags := sorted(set(_MD_FLOW_TAGS) & set(user_incar)): + raise ValueError(f"The flow sets {tags}. Remove them from the MD maker.") + if int(user_incar.get("NBLOCK", 1)) != 1: + raise ValueError( + "The MD must write every step to XDATCAR, so NBLOCK must be 1." + ) + if isinstance(generator, LangevinMDSetGenerator): + if self.thermostat != "langevin": + raise ValueError( + "The MD maker has a Langevin thermostat. Set thermostat to " + "'langevin'." + ) + elif self.thermostat == "langevin": + init_fields = [f.name for f in fields(generator) if f.init] + generator = LangevinMDSetGenerator( + **{name: getattr(generator, name) for name in init_fields} + ) + generator = replace( + generator, + ensemble="nvt", + start_temp=self.temperature, + end_temp=self.temperature, + nsteps=n_steps, + time_step=self.md_time_step, + ) + return replace(md_maker, input_set_generator=generator) diff --git a/src/atomate2/vasp/sets/core.py b/src/atomate2/vasp/sets/core.py index a56e943e10..19a50ba702 100644 --- a/src/atomate2/vasp/sets/core.py +++ b/src/atomate2/vasp/sets/core.py @@ -10,6 +10,7 @@ import numpy as np from pymatgen.core.periodic_table import Element +from pymatgen.io.vasp import Poscar try: from pymatgen.io.vasp.sets import LobsterSet # type: ignore[attr-defined] @@ -723,6 +724,42 @@ def _get_ensemble_defaults(structure: Structure, ensemble: str) -> dict[str, Any raise ValueError(f"Expect {ensemble=} to be one of {supported}") from err +@dataclass +class LangevinMDSetGenerator(MDSetGenerator): + """ + Class to generate VASP input sets for NVT MD with a Langevin thermostat. + + Parameters + ---------- + langevin_gamma + Friction coefficient in ps^-1, the same for each species. The VASP + ``LANGEVIN_GAMMA`` parameter. + **kwargs + Other keyword arguments that will be passed to :obj:`MDSetGenerator`. + """ + + langevin_gamma: float = 10.0 + + @property + def incar_updates(self) -> dict: + """Get updates to the INCAR for a Langevin NVT MD job. + + Returns + ------- + dict + A dictionary of updates to apply. + """ + if self.ensemble.lower() != "nvt": + raise ValueError(f"Expect ensemble='nvt', not {self.ensemble!r}.") + updates = super().incar_updates + # the Nose mass is only used by the Nose-Hoover thermostat + updates.pop("SMASS", None) + # one value for each species block of the POSCAR + n_species = len(Poscar(self.structure).site_symbols) + updates.update(MDALGO=3, LANGEVIN_GAMMA=[self.langevin_gamma] * n_species) + return updates + + @dataclass class LobsterTightStaticSetGenerator(LobsterSet): """ diff --git a/tests/ase/test_md.py b/tests/ase/test_md.py index f764908555..77178680a8 100644 --- a/tests/ase/test_md.py +++ b/tests/ase/test_md.py @@ -74,6 +74,29 @@ def test_npt_init_kwargs(si_structure, clean_dir, caplog): assert "The `NPT` module in ASE is no longer recommended" in caplog.text +def test_nvt_nose_hoover_chain(si_structure, clean_dir): + """NoseHooverChainNVT runs at a constant temperature only.""" + maker = LennardJonesMDMaker( + ensemble="nvt", + dynamics="nose-hoover-chain", + temperature=300, + n_steps=5, + ase_md_kwargs={"tdamp": 10, "tchain": 1}, + ) + result = maker.run_ase(si_structure) + assert len(result.trajectory) == 6 + + maker = LennardJonesMDMaker( + ensemble="nvt", + dynamics="nose-hoover-chain", + temperature=[300, 600], + n_steps=5, + ase_md_kwargs={"tdamp": 10}, + ) + with pytest.raises(ValueError, match="cannot follow a temperature schedule"): + maker.run_ase(si_structure) + + @pytest.mark.parametrize("calculator_name", list(name_to_maker)) def test_ase_nvt_maker(calculator_name, lj_fcc_ne_pars, fcc_ne_structure, clean_dir): # Langevin thermostat no longer works with single atom structures in ase>3.24.x diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py new file mode 100644 index 0000000000..699bbf4a7f --- /dev/null +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -0,0 +1,663 @@ +"""Tests of the finite-temperature phonon workflow. + +The end-to-end test runs the force field workflow with ASE's EMT potential, so +it needs no reference data. It lives here and not under tests/forcefields, +because pheasy is only installed in the test-non-ase CI job. +""" + +import gzip +from pathlib import Path + +import numpy as np +import pytest +from ase import units +from ase.build import bulk +from ase.calculators import emt +from ase.calculators.singlepoint import SinglePointCalculator +from ase.io import write as ase_write +from jobflow import run_locally +from phonopy import Phonopy +from phonopy.harmonic.dynmat_to_fc import get_commensurate_points +from pymatgen.core import Lattice, Structure +from pymatgen.io.ase import AseAtomsAdaptor +from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure + +from atomate2.common.jobs.finite_temperature_phonons import ( + ASE_TRAJECTORY_FILE, + _assess_trajectory, + _get_rms_displacement, + _remove_center_of_mass, + fit_finite_temperature_phonons, + get_md_restart_structure, + get_md_supercell, + select_md_snapshots, +) +from atomate2.forcefields.flows.finite_temperature_phonons import ( + ForceFieldFiniteTemperaturePhononMaker, + _get_force_field_md_maker, +) +from atomate2.forcefields.jobs import ForceFieldStaticMaker +from atomate2.forcefields.md import ForceFieldMDMaker + +EMT_CALCULATOR = {"@module": "ase.calculators.emt", "@callable": "EMT"} +TEMPERATURE = 300.0 +TEST_DIR = Path(__file__).resolve().parents[2] / "test_data" + + +@pytest.fixture +def cu_supercell(): + """A 2x2x2 supercell of the cubic cell of fcc Cu, 32 atoms.""" + atoms = bulk("Cu", "fcc", a=3.61, cubic=True) * (2, 2, 2) + return AseAtomsAdaptor.get_structure(atoms) + + +def _frames(reference, n_frames, sigma, rng, shift=None): + """Fractional coordinates of frames with Gaussian displacements in Angstrom.""" + disps = rng.normal(0, sigma, size=(n_frames, len(reference), 3)) + if shift is not None: + disps += shift + cart = reference.cart_coords + disps + return np.array([reference.lattice.get_fractional_coords(c) for c in cart]) + + +def _trajectory(reference, rng, sigma=0.05, shift=None, energies=None): + """A trajectory of 400 frames that starts at the reference, and its energies.""" + frac = _frames(reference, 400, sigma, rng) + frac[:10] = _frames(reference, 10, 0.01, rng) + if shift is not None: + frac[200:] = _frames(reference, 200, sigma, rng, shift=shift) + if energies is None: + energies = rng.normal(0, 1e-3, 400) * len(reference) + return frac, energies + + +def _verdict(reference, frac, energies): + return _assess_trajectory(frac, energies, reference, TEMPERATURE).verdict + + +def test_assess_trajectory(cu_supercell): + rng = np.random.default_rng(1) + n_atoms = len(cu_supercell) + + frac, energies = _trajectory(cu_supercell, rng) + health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + assert health.verdict == "stable" + assert health.is_stable + assert health.n_frames == 400 + # u_vib is sqrt(3) sigma for Gaussian displacements + assert health.u_vib == pytest.approx(np.sqrt(3) * 0.05, rel=0.05) + assert health.u_ref**2 == pytest.approx(health.u_shift**2 + health.u_vib**2) + assert health.nearest_neighbor_distance == pytest.approx(3.61 / np.sqrt(2)) + assert health.equipartition_rise == pytest.approx(1.5 * units.kB * TEMPERATURE) + + # a translation of the whole cell is not a displacement + moved = frac + np.array([0.1, 0.05, 0]) + health_moved = _assess_trajectory(moved, energies, cu_supercell, TEMPERATURE) + assert health_moved.verdict == "stable" + assert health_moved.u_ref == pytest.approx(health.u_ref) + + # a vibration of 0.2 A per direction is above the Lindemann limit + frac, energies = _trajectory(cu_supercell, rng, sigma=0.2) + assert _verdict(cu_supercell, frac, energies) == "melted" + + # the mean positions move in the second half, with a flat energy + shift = rng.normal(0, 0.4, size=(n_atoms, 3)) + frac, energies = _trajectory(cu_supercell, rng, shift=shift) + health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + assert health.verdict == "shifted_or_diffusing" + assert health.shift_ratio > 1.5 + + # the same move with a falling energy is a transformation + falling = np.concatenate([np.zeros(200), np.linspace(0, -0.1, 200)]) * n_atoms + frac, energies = _trajectory(cu_supercell, rng, shift=shift, energies=falling) + assert _verdict(cu_supercell, frac, energies) == "transformed" + + # a falling energy without a move is a transformation too + frac, energies = _trajectory(cu_supercell, rng, energies=falling) + assert _verdict(cu_supercell, frac, energies) == "transformed" + + # a rising energy at the reference is disordering + rising = np.linspace(0, 0.1, 400) * n_atoms + frac, energies = _trajectory(cu_supercell, rng, energies=rising) + health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + assert health.verdict == "disordering" + assert health.energy_drift == pytest.approx(0.05, rel=0.05) + + # a large move at the very end, in a structure with long bonds, stays below + # the other limits + sparse = Structure(Lattice.cubic(8.0), ["Cu"], [[0, 0, 0]]) * (3, 3, 3) + frac, energies = _trajectory(sparse, rng) + move = rng.choice([-2.2, 2.2], size=(len(sparse), 3)) / np.sqrt(3) + frac[360:] = _frames(sparse, 40, 0.05, rng, shift=move) + health = _assess_trajectory(frac, energies, sparse, TEMPERATURE) + assert health.verdict == "diffusing_or_soft" + assert health.rms_displacement_end > 1.0 + + # large displacements in the first frames mean the atom order is wrong + frac, energies = _trajectory(cu_supercell, rng) + frac[:10] = frac[:10][:, rng.permutation(n_atoms)] + assert _verdict(cu_supercell, frac, energies) == "reference_mismatch" + + # too few frames to compare the quarters + health = _assess_trajectory(frac[:15], energies[:15], cu_supercell, TEMPERATURE) + assert health.energy_drift is None + + +def _write_vasp_md(directory, reference, frac, energies, gz=False): + """Write the INCAR, XDATCAR and OSZICAR of a VASP MD run with POTIM = 2.""" + directory.mkdir() + lat = reference.lattice.matrix + lines = ["Cu", "1.0", *[" ".join(f"{x:.10f}" for x in row) for row in lat]] + lines += ["Cu", str(len(reference))] + oszicar = [] + for idx, (coords, energy) in enumerate(zip(frac, energies, strict=True), 1): + lines.append(f"Direct configuration= {idx:5d}") + lines += [" ".join(f"{x:.10f}" for x in row) for row in coords] + oszicar += [ + "DAV: 1 -0.1E+02 -0.1E+02 -0.1E+02 100 0.1E+00", + ( + f"{idx:6d} T= 300. E= -.1E+02 F= {energy:.8E} " + f"E0= {energy:.8E} EK= 0.1E+00 SP= 0.0E+00 SK= 0.0E+00" + ), + ] + files = { + "INCAR": "IBRION = 0\nPOTIM = 2.0\n", + "XDATCAR": "\n".join(lines) + "\n", + "OSZICAR": "\n".join(oszicar) + "\n", + } + for name, text in files.items(): + if gz: + with gzip.open(directory / f"{name}.gz", "wt") as file: + file.write(text) + else: + (directory / name).write_text(text) + + +def test_select_md_snapshots_vasp(cu_supercell): + rng = np.random.default_rng(2) + frac = _frames(cu_supercell, 300, 0.05, rng) + energies = rng.normal(-100, 0.01, 300) + # two runs with POTIM = 2 fs, the second one gzipped + _write_vasp_md(Path("md1"), cu_supercell, frac[:150], energies[:150]) + _write_vasp_md(Path("md2"), cu_supercell, frac[150:], energies[150:], gz=True) + md_dirs = ["host:" + str(Path("md1").resolve()), str(Path("md2").resolve())] + + # 0.1 ps is 50 frames of 2 fs, so 250 frames are left for 10 snapshots + output = select_md_snapshots.original( + md_dirs, "vasp", cu_supercell, TEMPERATURE, 1.0, 0.1, 10 + ) + structures = output["structures"] + assert len(structures) == 11 + assert structures[-1] == cu_supercell + indices = range(50, 300, 25) + for structure, idx in zip(structures[:-1], indices, strict=True): + diff = structure.frac_coords - frac[idx] + assert np.allclose(diff - np.round(diff), 0, atol=1e-8) + assert output["snapshot_times"] == pytest.approx([idx * 0.002 for idx in indices]) + assert output["md_time"] == pytest.approx(0.6) + assert output["rms_displacement"] == pytest.approx(np.sqrt(3) * 0.05, rel=0.1) + assert output["trajectory_health"]["n_frames"] == 300 + + with pytest.raises(ValueError, match="fewer than the 300 snapshots"): + select_md_snapshots.original( + md_dirs[:1], "vasp", cu_supercell, 300, 1, 0.1, 300 + ) + + # atoms of another species at the same positions + other = cu_supercell.copy() + other.replace_species({"Cu": "Ag"}) + with pytest.raises(ValueError, match="not in the order of the reference"): + select_md_snapshots.original(md_dirs[:1], "vasp", other, 300, 1, 0.1, 10) + + # the same run twice, once with a host name + with pytest.raises(ValueError, match="its own directory"): + select_md_snapshots.original( + [md_dirs[0], str(Path("md1").resolve())], + "vasp", + cu_supercell, + 300, + 1, + 0.1, + 10, + ) + + Path("md4").mkdir() + for name in ("INCAR", "XDATCAR"): + (Path("md4") / name).write_text((Path("md1") / name).read_text()) + (Path("md4") / "OSZICAR").write_text("") + with pytest.raises(ValueError, match=r"0 MD steps in OSZICAR\..*NBLOCK = 1"): + select_md_snapshots.original( + [str(Path("md4").resolve())], "vasp", cu_supercell, 300, 1, 0.1, 10 + ) + + +def _write_ase_md(directory, reference, frac, energies): + frames = [] + for coords, energy in zip(frac, energies, strict=True): + atoms = AseAtomsAdaptor.get_atoms(reference) + atoms.set_scaled_positions(coords) + atoms.calc = SinglePointCalculator(atoms, energy=energy) + frames.append(atoms) + directory.mkdir() + ase_write(directory / ASE_TRAJECTORY_FILE, frames) + + +def test_select_md_snapshots_forcefields(cu_supercell): + rng = np.random.default_rng(3) + frac = _frames(cu_supercell, 151, 0.05, rng) + energies = rng.normal(0, 0.01, 151) + # the second run starts from the last frame of the first one + _write_ase_md(Path("md1"), cu_supercell, frac[:101], energies[:101]) + _write_ase_md(Path("md2"), cu_supercell, frac[100:], energies[100:]) + + output = select_md_snapshots.original( + [str(Path(name).resolve()) for name in ("md1", "md2")], + "forcefields", + cu_supercell, + 300, + 2.0, + 0.02, + 14, + ) + assert output["trajectory_health"]["n_frames"] == 151 + # 10 frames of 2 fs are left out, and 141 frames are left for 14 snapshots + indices = range(10, 150, 10) + assert output["snapshot_times"] == pytest.approx([idx * 0.002 for idx in indices]) + for structure, idx in zip(output["structures"][:-1], indices, strict=True): + diff = structure.frac_coords - frac[idx] + assert np.allclose(diff - np.round(diff), 0, atol=1e-8) + + # the snapshots keep the magnetic moments of the reference + magmoms = [1.0] * len(cu_supercell) + magnetic = cu_supercell.copy(site_properties={"magmom": magmoms}) + output = select_md_snapshots.original( + [str(Path("md1").resolve())], "forcefields", magnetic, 300, 2.0, 0.02, 14 + ) + for structure in output["structures"]: + assert structure.site_properties == {"magmom": magmoms} + + # a trajectory that leaves the reference gives a warning + melted = _frames(cu_supercell, 101, 0.3, rng) + melted[:10] = cu_supercell.frac_coords + _write_ase_md(Path("md3"), cu_supercell, melted, energies[:101]) + with pytest.warns(UserWarning, match="verdict: melted"): + output = select_md_snapshots.original( + [str(Path("md3").resolve())], + "forcefields", + cu_supercell, + 300, + 2.0, + 0.02, + 14, + ) + assert output["trajectory_health"]["verdict"] == "melted" + + +def test_get_md_supercell(): + """The supercell has the atom order of phonopy and the magnetic moments.""" + structure = Structure( + Lattice.cubic(4.17), + ["O", "Ni", "O", "Ni"], + [[0.5, 0, 0], [0, 0, 0], [0, 0.5, 0], [0.5, 0.5, 0]], + site_properties={"magmom": [0.0, 2.0, 0.0, -2.0]}, + ) + matrix = np.diag([2, 2, 1]) + supercell = get_md_supercell.original(structure, matrix, 1e-3, "vasp") + assert len(supercell) == 16 + assert [str(site.specie) for site in supercell] == ["Ni"] * 8 + ["O"] * 8 + # each atom of the sorted unit cell has four images in a row + assert supercell.site_properties["magmom"] == [2.0] * 4 + [-2.0] * 4 + [0.0] * 8 + + supercell = get_md_supercell.original( + structure.copy().remove_site_property("magmom"), + np.diag([2, 2, 1]), + 1e-3, + "vasp", + ) + assert supercell.site_properties == {} + + +def test_get_md_restart_structure(cu_supercell): + rng = np.random.default_rng(4) + velocities = rng.normal(0, 0.01, size=(len(cu_supercell), 3)) + reference = cu_supercell.copy(site_properties={"magmom": [1.0] * 32}) + + # a CONTCAR of a VASP MD, with the predictor-corrector block after the + # velocities + md_dir = TEST_DIR / "vasp/Si_multi_md/molecular_dynamics_1/outputs" + si_reference = Structure( + np.eye(3) * 3.87, ["Si", "Si"], [[0, 0, 0], [0.25, 0.25, 0.25]] + ) + restart = get_md_restart_structure.original(str(md_dir), "vasp", si_reference) + assert restart.site_properties["velocities"][0] == pytest.approx( + [0.40252568e-03, -0.31480439e-02, -0.16045943e-02] + ) + assert "magmom" not in restart.site_properties + + Path("vasp").mkdir() + structure = cu_supercell.copy(site_properties={"velocities": velocities}) + structure.to(filename="vasp/CONTCAR", fmt="poscar") + restart = get_md_restart_structure.original( + str(Path("vasp").resolve()), "vasp", reference + ) + assert np.allclose(restart.site_properties["velocities"], velocities, atol=1e-8) + assert restart.site_properties["magmom"] == [1.0] * 32 + + Path("ase").mkdir() + atoms = AseAtomsAdaptor.get_atoms(cu_supercell) + atoms.set_velocities(velocities) + ase_write(Path("ase") / ASE_TRAJECTORY_FILE, [atoms.copy(), atoms]) + restart = get_md_restart_structure.original( + str(Path("ase").resolve()), "forcefields", reference + ) + assert np.allclose(restart.site_properties["velocities"], velocities) + assert np.allclose(restart.cart_coords, cu_supercell.cart_coords) + assert restart.site_properties["magmom"] == [1.0] * 32 + + with pytest.raises(ValueError, match="MD code must be"): + get_md_restart_structure.original("ase", "lammps", reference) + + +def test_get_rms_displacement(): + """An Einstein crystal has = 3 k_B T / k per atom.""" + structure = AseAtomsAdaptor.get_structure(bulk("Cu", "fcc", a=3.61, cubic=True)) + phonon = Phonopy(get_phonopy_structure(structure), np.diag([2, 2, 2])) + n_atoms = len(phonon.supercell) + spring = 2.0 # eV/A^2 + force_constants = np.zeros((n_atoms, n_atoms, 3, 3)) + force_constants[np.arange(n_atoms), np.arange(n_atoms)] = spring * np.eye(3) + phonon.force_constants = force_constants + rms = _get_rms_displacement(phonon, TEMPERATURE, 0.1) + assert rms == pytest.approx(np.sqrt(3 * units.kB * TEMPERATURE / spring)) + + +def test_rms_displacement_matches_mode_sampling(): + """Canonical mode sampling of Cu3Au gives the rms of the force constants. + + Each sample gets a random translation. Removing the displacement of the + center of mass takes it out again. The unweighted mean of the displacements + is not zero for two species, so it would not. + """ + structure = Structure( + Lattice.cubic(3.75), + ["Cu", "Cu", "Cu", "Au"], + [[0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0], [0, 0, 0]], + ) + phonon = _emt_phonon(structure, np.diag([2, 2, 2])) + masses = np.repeat(phonon.supercell.masses, 3) + n_atoms = len(phonon.supercell) + dynmat = phonon.force_constants.transpose(0, 2, 1, 3).reshape( + 3 * n_atoms, 3 * n_atoms + ) / np.sqrt(np.outer(masses, masses)) + eigvals, eigvecs = np.linalg.eigh((dynmat + dynmat.T) / 2) + keep = eigvals > 1e-6 + + rng = np.random.default_rng(6) + n_samples = 4000 + amplitudes = rng.normal(size=(n_samples, keep.sum())) * np.sqrt( + units.kB * TEMPERATURE / eigvals[keep] + ) + disps = (amplitudes @ eigvecs[:, keep].T / np.sqrt(masses)).reshape( + n_samples, n_atoms, 3 + ) + disps += rng.normal(0, 0.1, size=(n_samples, 1, 3)) + + reference = get_pmg_structure(phonon.supercell) + removed = _remove_center_of_mass(disps, reference) + rms = np.sqrt(np.mean(np.sum(removed**2, axis=2))) + assert rms == pytest.approx( + _get_rms_displacement(phonon, TEMPERATURE, 0.1), rel=0.02 + ) + unweighted = disps - disps.mean(axis=1, keepdims=True) + assert not np.allclose(unweighted, removed, atol=1e-3) + + +@pytest.mark.parametrize( + ("kwargs", "match"), + [ + ({"thermostat": "berendsen"}, "thermostat must be one of"), + ({"rotational_sum_rule": "X"}, "rotational_sum_rule must be one of"), + ({"md_runs": 0}, "md_runs must be a positive integer"), + ({"n_snapshots": 2.5}, "n_snapshots must be a positive integer"), + ({"alpha_min": -2}, "alpha_min must be an integer below -2"), + ({"alpha_min": -6.0}, "alpha_min must be an integer below -2"), + ({"md_time_step": 0}, "must be positive"), + ({"equilibration_time": 8.0}, "fewer than the 50 snapshots"), + ({"equilibration_time": -1.0}, "fewer than the 50 snapshots"), + ( + {"md_time": 0.01, "equilibration_time": 0, "n_snapshots": 5, "md_runs": 20}, + "larger than the 10", + ), + ({"md_maker": None}, "md_maker and phonon_displacement_maker must be set"), + ({"code": "aims"}, "code must be one of"), + ({"md_code": None}, "md_code must be one of"), + ], +) +def test_maker_checks(kwargs, match): + with pytest.raises(ValueError, match=match): + ForceFieldFiniteTemperaturePhononMaker(**kwargs) + + +def test_force_field_md_maker(cu_supercell): + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT_CALCULATOR, + md_time=1.0, + md_time_step=2.0, + equilibration_time=0.5, + md_runs=3, + random_seed=5, + ) + assert maker.get_md_steps() == [167, 167, 166] + md_maker = maker.get_md_maker(167) + assert md_maker.n_steps == 167 + assert md_maker.time_step == 2.0 + assert md_maker.temperature == TEMPERATURE + assert md_maker.mb_velocity_seed == 5 + assert md_maker.dynamics == "nose-hoover-chain" + assert md_maker.ase_md_kwargs["tchain"] == 1 + # a thermostat period of 40 steps, 80 fs + period = np.pi * np.sqrt(2) * md_maker.ase_md_kwargs["tdamp"] / units.fs + assert period == pytest.approx(80.0) + # the maker of the flow is not changed + assert maker.md_maker.n_steps == 1000 + assert maker.md_maker.dynamics is None + # the force field relaxation keeps the symmetry + assert maker.bulk_relax_maker.fix_symmetry + assert ForceFieldFiniteTemperaturePhononMaker().bulk_relax_maker.fix_symmetry + + # the MD jobs have a number only when there are several + flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) + md_names = [job.name for job in flow.jobs if "MD" in job.name] + assert md_names == ["ASE MD 1/3", "ASE MD 2/3", "ASE MD 3/3"] + maker = ForceFieldFiniteTemperaturePhononMaker(md_time=2.0) + flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) + assert [job.name for job in flow.jobs if "MD" in job.name] == ["ASE MD"] + + langevin = ForceFieldFiniteTemperaturePhononMaker( + thermostat="langevin" + ).get_md_maker(10) + # AseMDMaker sets its default friction when the job runs + assert langevin.dynamics == "langevin" + assert langevin.ase_md_kwargs == {} + + maker = ForceFieldFiniteTemperaturePhononMaker( + md_maker=ForceFieldMDMaker(ase_md_kwargs={"tdamp": 10}) + ) + with pytest.raises(ValueError, match="must not set dynamics or ase_md_kwargs"): + maker.get_md_maker(10) + with pytest.raises(TypeError, match="must be a ForceFieldMDMaker"): + _get_force_field_md_maker( + ForceFieldFiniteTemperaturePhononMaker(md_maker=ForceFieldStaticMaker()), 10 + ) + + +def _commensurate_frequencies(phonon): + matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix + phonon.run_qpoints(get_commensurate_points(np.rint(matrix).astype(int))) + return np.sort(phonon.qpoints.frequencies.ravel()) + + +def _emt_phonon(structure, supercell_matrix): + """0 K phonopy object of EMT, with its force constants.""" + phonon = Phonopy( + get_phonopy_structure(structure), supercell_matrix, primitive_matrix="auto" + ) + phonon.generate_displacements(distance=0.01) + forces = [] + for cell in phonon.supercells_with_displacements: + atoms = AseAtomsAdaptor.get_atoms(get_pmg_structure(cell)) + atoms.calc = emt.EMT() + forces.append(atoms.get_forces()) + phonon.forces = forces + phonon.produce_force_constants() + return phonon + + +def test_fit_recovers_harmonic_force_constants(): + """Forces from known force constants give them back, with the NAC applied.""" + structure = Structure( + Lattice.cubic(3.75), + ["Cu", "Cu", "Cu", "Au"], + [[0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0], [0, 0, 0]], + ) + supercell_matrix = np.diag([2, 2, 2]).tolist() + phonon = _emt_phonon(structure, supercell_matrix) + supercell = get_pmg_structure(phonon.supercell) + disps = np.random.default_rng(0).normal(0, 0.03, (20, len(supercell), 3)) + forces = -np.einsum("ijab,mjb->mia", phonon.force_constants, disps) + snapshots = [ + Structure( + supercell.lattice, + supercell.species, + supercell.cart_coords + disp, + coords_are_cartesian=True, + ) + for disp in disps + ] + displacement_data = { + "forces": [*forces, np.zeros((len(supercell), 3))], + "displaced_structures": [*snapshots, supercell], + "uuids": ["uuid"] * 21, + "dirs": ["dir"] * 21, + } + snapshot_data = { + "snapshot_times": [0.0] * 20, + "md_time": 1.0, + "rms_displacement": 0.05, + "trajectory_health": {}, + } + born = [np.eye(3).tolist()] * 3 + [(-3 * np.eye(3)).tolist()] + fit_kwargs = { + "structure": structure, + "supercell_matrix": supercell_matrix, + "snapshot_data": snapshot_data, + "displacement_data": displacement_data, + "temperature": TEMPERATURE, + "thermostat": "nose-hoover", + "md_time_step": 1.0, + "equilibration_time": 0.5, + "code": "forcefields", + "md_code": "forcefields", + "symprec": 1e-3, + "rotational_sum_rule": None, + "epsilon_static": (10 * np.eye(3)).tolist(), + "npoints_band": 11, + } + doc = fit_finite_temperature_phonons.original(born=born, **fit_kwargs) + assert doc.force_rmse < 0.01 * np.sqrt(np.mean(forces**2)) + force_constants = np.array(doc.force_constants.force_constants) + assert np.abs(force_constants - phonon.force_constants).max() < 0.05 + assert np.array(doc.born).shape == (4, 3, 3) + assert doc.phonon_bandstructure.has_nac + assert not doc.has_imaginary_modes + assert doc.uuids.displacements_uuids == ["uuid"] * 21 + assert doc.jobdirs.displacements_job_dirs == ["dir"] * 21 + + # the Born charges are checked before pheasy runs + fc_time = Path("FORCE_CONSTANTS").stat().st_mtime_ns + with pytest.raises(ValueError, match="number of Born charges"): + fit_finite_temperature_phonons.original(born=born[:3], **fit_kwargs) + assert Path("FORCE_CONSTANTS").stat().st_mtime_ns == fc_time + + with pytest.raises(ValueError, match="diagonal supercell matrix"): + fit_finite_temperature_phonons.original( + **{**fit_kwargs, "supercell_matrix": [[1, 1, 0], [0, 1, 0], [0, 0, 1]]} + ) + with pytest.raises(ValueError, match="snapshots followed by the undisplaced"): + fit_finite_temperature_phonons.original( + **{**fit_kwargs, "snapshot_data": {"snapshot_times": [0.0] * 19}} + ) + shuffled = { + **displacement_data, + "displaced_structures": [supercell, *snapshots], + } + with pytest.raises(ValueError, match="not the undisplaced supercell"): + fit_finite_temperature_phonons.original( + **{**fit_kwargs, "displacement_data": shuffled} + ) + + +def test_finite_temperature_phonon_maker_emt(clean_dir): + """Run the whole force field workflow with EMT on L1_2 Cu3Au at 300 K.""" + # Au first, so that sorting the atoms by electronegativity reorders them + structure = Structure( + Lattice.cubic(3.75), + ["Au", "Cu", "Cu", "Cu"], + [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], + ) + # a 2x2x2 supercell of the cubic cell, 32 atoms, and 2 ps of MD at 2 fs in + # two MD jobs + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT_CALCULATOR, + min_length=7.0, + md_time=2.0, + md_time_step=2.0, + md_runs=2, + equilibration_time=0.5, + n_snapshots=12, + ) + flow = maker.make(structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + doc = responses[flow.output.uuid][1].output + + assert [str(site.specie) for site in doc.structure] == ["Cu", "Cu", "Cu", "Au"] + assert doc.temperature == TEMPERATURE + assert doc.thermostat == "nose-hoover" + assert doc.md_code == doc.code == "forcefields" + assert doc.md_force_field_name == doc.force_field_name == "ase.calculators.emt.EMT" + assert doc.force_field_kwargs == {} + # 1000 steps and the starting structure + assert doc.md_time == pytest.approx(2.002) + assert doc.n_snapshots == 12 + assert len(doc.snapshot_times) == 12 + assert min(doc.snapshot_times) == pytest.approx(0.5) + assert len(doc.md_uuids) == len(doc.md_dirs) == 2 + assert len(doc.uuids.displacements_uuids) == 13 + assert doc.uuids.optimization_run_uuid is not None + assert doc.uuids.born_run_uuid is None + assert doc.supercell_matrix == ((2, 0, 0), (0, 2, 0), (0, 0, 2)) + assert doc.trajectory_health.verdict == "stable" + assert doc.max_residual_force < 1e-8 + assert 0 < doc.force_rmse < 0.2 + assert doc.lasso_alpha > 0 + # Cu3Au is stable at 300 K + assert not doc.has_imaginary_modes + assert doc.n_imaginary_modes == 0 + assert doc.min_frequency > -0.1 + # the snapshot amplitude agrees with the one of the fitted force constants + assert doc.rms_displacement == pytest.approx( + doc.rms_displacement_from_force_constants, rel=0.25 + ) + force_constants = np.array(doc.force_constants.force_constants) + assert force_constants.shape == (32, 32, 3, 3) + fit_dir = Path(doc.jobdirs.taskdoc_run_job_dir) + for name in ("FORCE_CONSTANTS", "phonopy.yaml", "pheasy_harmonic_fit.log"): + assert (fit_dir / name).exists() + + # at a fixed volume, the frequencies stay close to the 0 K ones of EMT + phonon = _emt_phonon(doc.structure, np.array(doc.supercell_matrix)) + freqs_0k = _commensurate_frequencies(phonon) + phonon.force_constants = force_constants + freqs = _commensurate_frequencies(phonon) + top = len(freqs) // 3 + assert freqs[-top:].mean() == pytest.approx(freqs_0k[-top:].mean(), rel=0.15) diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index 6bb45d0b0f..4a5cecb565 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -21,6 +21,7 @@ from atomate2.common.jobs.pheasy import ( _check_lasso_alpha, _get_num_anharmonic_supercells, + _run_harmonic_fit, generate_frequencies_eigenvectors, generate_phonon_displacements, ) @@ -260,17 +261,57 @@ def test_get_num_anharmonic_supercells(monkeypatch): _get_num_anharmonic_supercells(num_disp_anhar=0, **kwargs) +def test_run_harmonic_fit(monkeypatch): + """The fit flags of the pheasy workflow and the finite-temperature fit.""" + calls = [] + + def fake_run(args, check): + calls.append((args, check)) + + monkeypatch.setattr(pheasy_jobs.subprocess, "run", fake_run) + matrix = np.diag([2, 3, 4]) + + _run_harmonic_fit(matrix, 1e-3, 5) + assert [args[:4] for args, _ in calls] == [["pheasy", "--dim", "2", "3"]] * 4 + assert all(check for _, check in calls) + assert [args[9] for args, _ in calls] == ["-s", "-c", "-d", "-f"] + fit = " ".join(calls[-1][0]) + assert "-l LASSO --std --seed 103 --rasr BHH --ndata 5" in fit + assert "--alpha_min" not in fit + assert " -o " not in fit + + calls.clear() + _run_harmonic_fit(matrix, 1e-3, 3, use_lasso=False) + fit = " ".join(calls[-1][0]) + assert "-f --full_ifc --rasr BHH --ndata 3" in fit + for flag in ("-l", "--std", "--seed"): + assert flag not in calls[-1][0] + + calls.clear() + _run_harmonic_fit( + matrix, 1e-3, 5, rotational_sum_rule=None, alpha_min=-8, log_file="x.log" + ) + fit = " ".join(calls[-1][0]) + assert "--alpha_min -8 --seed 103 --ndata 5" in fit + assert fit.endswith("-o x.log") + assert "--rasr" not in fit + + def test_check_lasso_alpha(tmp_dir): log_file = Path("pheasy_anharmonic_fit.log") log_file.write_text("- alpha_min: 1e-12\n- alpha_opt: 2.947052e-09\n") with warnings.catch_warnings(): warnings.simplefilter("error") - _check_lasso_alpha(log_file, alpha_min=-12) + assert _check_lasso_alpha(log_file, alpha_min=-12) == pytest.approx( + 2.947052e-09 + ) log_file.write_text("- alpha_min: 1e-12\n- alpha_opt: 1.000000e-12\n") - with pytest.warns(UserWarning, match="on the lower bound"): + with pytest.warns(UserWarning, match="on the lower bound.*anhar_alpha_min"): _check_lasso_alpha(log_file, alpha_min=-12) + with pytest.warns(UserWarning, match="Lower alpha_min and refit"): + _check_lasso_alpha(log_file, alpha_min=-12, alpha_min_name="alpha_min") log_file.write_text("- alpha_max: 1e-2\n- alpha_opt: 1.000000e-02\n") with pytest.warns(UserWarning, match="on the upper bound"): diff --git a/tests/vasp/flows/test_finite_temperature_phonons.py b/tests/vasp/flows/test_finite_temperature_phonons.py new file mode 100644 index 0000000000..b29e691af6 --- /dev/null +++ b/tests/vasp/flows/test_finite_temperature_phonons.py @@ -0,0 +1,248 @@ +import pytest +from jobflow import Flow, OutputReference +from pymatgen.core import Lattice, Structure + +from atomate2.forcefields.flows.finite_temperature_phonons import ( + MLFFMDVaspStaticFiniteTemperaturePhononMaker, + VaspMDMLFFStaticFiniteTemperaturePhononMaker, +) +from atomate2.forcefields.jobs import ForceFieldStaticMaker +from atomate2.forcefields.md import ForceFieldMDMaker +from atomate2.vasp.flows.finite_temperature_phonons import FiniteTemperaturePhononMaker +from atomate2.vasp.jobs.core import StaticMaker +from atomate2.vasp.jobs.md import MDMaker +from atomate2.vasp.sets.core import LangevinMDSetGenerator, MDSetGenerator + + +@pytest.fixture +def nio_supercell(): + """A 3x3x3 supercell of rock-salt NiO, which gets +U in VASP.""" + structure = Structure( + Lattice.cubic(4.17), ["Ni", "O"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ) + return structure * (3, 3, 3) + + +@pytest.mark.parametrize( + ("maker_cls", "md_code", "code"), + [ + (FiniteTemperaturePhononMaker, "vasp", "vasp"), + (VaspMDMLFFStaticFiniteTemperaturePhononMaker, "vasp", "forcefields"), + (MLFFMDVaspStaticFiniteTemperaturePhononMaker, "forcefields", "vasp"), + ], +) +def test_vasp_flows(si_structure, maker_cls, md_code, code): + maker = maker_cls(md_runs=2) + assert (maker.md_code, maker.code) == (md_code, code) + flow = maker.make(si_structure) + names = [job.name for job in flow.jobs] + # the Born charges are computed when the statics use VASP, as in the + # pheasy phonon workflows + born_names = ["dielectric"] if code == "vasp" else [] + md_names = ["molecular dynamics" if md_code == "vasp" else "ASE MD"] * 2 + assert names == [ + "double relax", + "get_supercell_size", + *born_names, + "get_md_supercell", + f"{md_names[0]} 1/2", + "get_md_restart_structure", + f"{md_names[1]} 2/2", + "select_md_snapshots", + "run_phonon_displacements", + "fit_finite_temperature_phonons", + ] + relax = flow.jobs[0] + reference, md_1, restart, md_2, snapshots, statics, fit = flow.jobs[-7:] + assert isinstance(relax, Flow) + + # a diagonal supercell + supercell = flow.jobs[1] + assert supercell.function_args[1:] == (12.0, None) + assert supercell.function_kwargs["force_diagonal"] + + # the first MD starts from the undisplaced supercell, the second from the + # end of the first, and both get the relaxation directory + assert md_1.function_args[0].uuid == reference.uuid + assert md_2.function_args[0].uuid == restart.uuid + assert restart.function_args == (md_1.output.dir_name, md_code, reference.output) + for md_job in (md_1, md_2): + assert md_job.function_kwargs["prev_dir"].uuid == relax.output.uuid + assert maker.get_md_steps() == [4000, 4000] + + args = snapshots.function_args + assert [ref.uuid for ref in args[0]] == [md_1.uuid, md_2.uuid] + assert args[1:] == (md_code, reference.output, 300.0, 1.0, 1.0, 50) + + # the statics get the snapshots followed by the undisplaced supercell, and + # only VASP statics get the relaxation directory + static_kwargs = statics.function_kwargs + assert static_kwargs["displacements"].uuid == snapshots.uuid + assert static_kwargs["prev_dir"].uuid == relax.output.uuid + assert static_kwargs["prev_dir_argname"] == ("prev_dir" if code == "vasp" else None) + assert static_kwargs["phonon_maker"] == maker.phonon_displacement_maker + + fit_kwargs = fit.function_kwargs + assert fit_kwargs["md_code"] == md_code + assert fit_kwargs["code"] == code + assert fit_kwargs["md_uuids"] == [md_1.uuid, md_2.uuid] + assert fit_kwargs["displacement_data"].uuid == statics.uuid + assert fit_kwargs["optimization_run_uuid"] == relax.output.uuid + assert fit_kwargs["rotational_sum_rule"] == "BHH" + assert fit_kwargs["alpha_min"] == -6 + if code == "forcefields": + assert fit_kwargs["force_field_name"] == "MACE-MP-0" + assert fit_kwargs["force_field_kwargs"] == {"model": "medium"} + assert fit_kwargs["md_force_field_name"] is None + else: + assert fit_kwargs["force_field_name"] is None + if md_code == "forcefields": + assert fit_kwargs["md_force_field_name"] == "MACE-MP-0" + if code == "vasp": + born = flow.jobs[2] + assert fit_kwargs["born"].uuid == born.uuid + assert fit_kwargs["epsilon_static"].uuid == born.uuid + assert fit_kwargs["born_run_uuid"] == born.uuid + assert born.function_kwargs["prev_dir"].uuid == relax.output.uuid + else: + assert fit_kwargs["born"] is None + assert fit_kwargs["born_run_uuid"] is None + assert fit.output.uuid == flow.output.uuid + + +def test_flow_from_output_reference(): + """The structure can be the output of an earlier job.""" + structure = OutputReference("1234", attributes=(("a", "structure"),)) + flow = FiniteTemperaturePhononMaker().make(structure) + assert flow.jobs[0].name == "double relax" + assert [job.name for job in flow.jobs][4] == "molecular dynamics" + + +def test_non_diagonal_supercell_matrix(si_structure): + with pytest.raises(ValueError, match="diagonal supercell matrix"): + FiniteTemperaturePhononMaker().make( + si_structure, supercell_matrix=[[1, 1, 0], [0, 1, 0], [0, 0, 1]] + ) + + +def test_relax_md_and_static_settings_match(nio_supercell, test_dir): + """The relaxation, the MD and the statics must see the same Hamiltonian.""" + maker = FiniteTemperaturePhononMaker(md_time=4.0, md_time_step=0.5) + md_generator = maker.get_md_maker(maker.get_md_steps()[0]).input_set_generator + static_generator = maker.phonon_displacement_maker.input_set_generator + relax_generator = maker.bulk_relax_maker.relax_maker1.input_set_generator + # alternating magnetic moments on Ni, as carried over from a relaxation + magmoms = [2.0, -2.0] * 13 + [2.0] + [0.0] * 27 + magnetic = nio_supercell.copy(site_properties={"magmom": magmoms}) + sets = { + "md": md_generator.get_input_set(magnetic, potcar_spec=True), + "static": static_generator.get_input_set(magnetic, potcar_spec=True), + "relax": relax_generator.get_input_set(magnetic, potcar_spec=True), + } + for key in ("GGA", "ISPIN", "MAGMOM", "LDAU", "LDAUU", "LDAUL", "ISMEAR", "SIGMA"): + values = {name: input_set.incar.get(key) for name, input_set in sets.items()} + assert values["md"] == values["static"] == values["relax"], key + assert sets["md"].incar["GGA"] == "Ps" + assert sets["md"].incar["LDAUU"] == [6.2, 0] + assert sets["md"].incar["MAGMOM"] == magmoms + assert sets["md"].kpoints.kpts == sets["static"].kpoints.kpts + assert sets["relax"].kpoints.kpts == sets["static"].kpoints.kpts + for key in ("ENCUT", "ENAUG", "PREC"): + assert sets["relax"].incar[key] == sets["static"].incar[key], key + + # 4 ps at 0.5 fs, every step written to XDATCAR + md_incar, static_incar = sets["md"].incar, sets["static"].incar + assert md_incar["NSW"] == 8000 + assert md_incar["POTIM"] == 0.5 + assert md_incar["NBLOCK"] == 1 + assert md_incar["TEBEG"] == md_incar["TEEND"] == 300 + assert (md_incar["IBRION"], md_incar["ISIF"]) == (0, 2) + assert (md_incar["MDALGO"], md_incar["SMASS"]) == (2, 0) + assert md_incar["ENCUT"] == 500 + assert static_incar["ENCUT"] == 600 + assert static_incar["EDIFF"] == 1e-7 + assert static_incar["NSW"] == 0 + + # the same holds after a previous calculation sets the spin + si = Structure.from_file(test_dir / "structures" / "Si.cif") * (3, 3, 3) + prev_dir = test_dir / "vasp" / "Si_pheasy" / "tight_relax_2" / "outputs" + prev_sets = { + name: generator.get_input_set(si, prev_dir=prev_dir, potcar_spec=True) + for name, generator in ( + ("md", md_generator), + ("static", static_generator), + ("relax", relax_generator), + ) + } + for key in ("ISPIN", "MAGMOM", "ISMEAR", "SIGMA"): + assert prev_sets["md"].incar.get(key) == prev_sets["static"].incar.get(key) + assert prev_sets["md"].kpoints.kpts == prev_sets["static"].kpoints.kpts + assert prev_sets["relax"].kpoints.kpts == prev_sets["static"].kpoints.kpts + + +def test_langevin_thermostat(nio_supercell): + maker = FiniteTemperaturePhononMaker(thermostat="langevin", temperature=600) + md_maker = maker.get_md_maker(100) + assert isinstance(md_maker.input_set_generator, LangevinMDSetGenerator) + incar = md_maker.input_set_generator.get_input_set( + nio_supercell, potcar_spec=True + ).incar + assert incar["MDALGO"] == 3 + assert incar["LANGEVIN_GAMMA"] == [10.0, 10.0] + assert incar["TEBEG"] == incar["TEEND"] == 600 + assert incar["ENCUT"] == 500 + # the maker of the flow is not changed + assert type(maker.md_maker.input_set_generator) is MDSetGenerator + + # a Langevin MD maker needs the Langevin thermostat + maker = FiniteTemperaturePhononMaker(md_maker=md_maker) + with pytest.raises(ValueError, match="Set thermostat to 'langevin'"): + maker.get_md_maker(100) + maker = FiniteTemperaturePhononMaker(md_maker=md_maker, thermostat="langevin") + assert maker.get_md_maker(100).input_set_generator.nsteps == 100 + + +def test_md_maker_checks(): + maker = FiniteTemperaturePhononMaker( + md_maker=MDMaker( + input_set_generator=MDSetGenerator(user_incar_settings={"POTIM": 2}) + ) + ) + with pytest.raises(ValueError, match=r"The flow sets \['POTIM'\]"): + maker.get_md_maker(10) + + maker = FiniteTemperaturePhononMaker( + md_maker=MDMaker( + input_set_generator=MDSetGenerator(user_incar_settings={"NBLOCK": 10}) + ) + ) + with pytest.raises(ValueError, match="NBLOCK must be 1"): + maker.get_md_maker(10) + + with pytest.raises(TypeError, match="VASP MDMaker with an MDSetGenerator"): + FiniteTemperaturePhononMaker(md_maker=StaticMaker()).get_md_maker(10) + + +def test_from_force_field_name(): + maker = VaspMDMLFFStaticFiniteTemperaturePhononMaker.from_force_field_name( + "MACE-MP-0", + calculator_kwargs={"model": "medium-omat-0"}, + temperature=500.0, + phonon_displacement_maker=StaticMaker(), + ) + assert maker.name == ("VASP MD MACE_MP_0 Static Finite Temperature Phonon Maker") + assert maker.temperature == 500.0 + assert isinstance(maker.md_maker, MDMaker) + # the maker built for the force field replaces the one given + displacement_maker = maker.phonon_displacement_maker + assert isinstance(displacement_maker, ForceFieldStaticMaker) + assert displacement_maker.calculator_kwargs["model"] == "medium-omat-0" + assert maker.born_maker is None + + maker = MLFFMDVaspStaticFiniteTemperaturePhononMaker.from_force_field_name( + "MACE-MP-0" + ) + assert maker.name == "MACE_MP_0 MD VASP Static Finite Temperature Phonon Maker" + assert isinstance(maker.md_maker, ForceFieldMDMaker) + assert (maker.md_code, maker.code) == ("forcefields", "vasp") + assert type(maker.born_maker).__name__ == "DielectricMaker" diff --git a/tests/vasp/test_sets.py b/tests/vasp/test_sets.py index 483ee027c6..bce3610021 100644 --- a/tests/vasp/test_sets.py +++ b/tests/vasp/test_sets.py @@ -9,6 +9,7 @@ HSERelaxSetGenerator, HSEStaticSetGenerator, HSETightRelaxSetGenerator, + LangevinMDSetGenerator, LobsterTightStaticSetGenerator, MDSetGenerator, NonSCFSetGenerator, @@ -337,3 +338,24 @@ def test_md_set_generator_sorts_structure(): n_types_in_poscar = len(vasp_input["POSCAR"].natoms) n_langevin_gamma = len(vasp_input["INCAR"]["LANGEVIN_GAMMA"]) assert n_types_in_poscar == n_langevin_gamma + + +def test_langevin_md_set_generator(): + """LANGEVIN_GAMMA has one value for each species block of the POSCAR.""" + structure = Structure( + lattice=Lattice.cubic(10), + species=["Al", "Cl", "Al", "Cl", "O", "Li"], + coords=[[0.1 * i, 0.1 * i, 0.1 * i] for i in range(6)], + ) + input_gen = LangevinMDSetGenerator(start_temp=600, end_temp=600, langevin_gamma=5) + vasp_input = input_gen.get_input_set(structure, potcar_spec=True) + incar = vasp_input["INCAR"] + assert incar["MDALGO"] == 3 + assert incar["LANGEVIN_GAMMA"] == [5] * len(vasp_input["POSCAR"].natoms) + assert incar["TEBEG"] == incar["TEEND"] == 600 + assert "SMASS" not in incar + + with pytest.raises(ValueError, match="Expect ensemble='nvt'"): + LangevinMDSetGenerator(ensemble="npt").get_input_set( + structure, potcar_spec=True + ) From caa65ef0cb568e5e0bac700944b01bf2e281c870 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Wed, 30 Sep 2026 09:52:29 -0700 Subject: [PATCH 08/43] Allow force field jobs without torch installed --- src/atomate2/forcefields/utils.py | 7 ++++++- 1 file changed, 6 insertions(+), 1 deletion(-) diff --git a/src/atomate2/forcefields/utils.py b/src/atomate2/forcefields/utils.py index d6388d845a..2cd486e43e 100644 --- a/src/atomate2/forcefields/utils.py +++ b/src/atomate2/forcefields/utils.py @@ -496,7 +496,12 @@ def revert_default_dtype() -> Generator[None]: Originally added for use with MACE(Relax|Static)Maker. https://github.com/ACEsuit/mace/issues/328 """ - import torch + try: + import torch + except ImportError: + # force fields that do not use torch, such as EMT, have no dtype to revert + yield + return orig = torch.get_default_dtype() yield From 50d1eec372f1a57d4ca2a8e7b67f9d39e77a8f6f Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Wed, 30 Sep 2026 16:17:08 -0700 Subject: [PATCH 09/43] Update the harmonic fit test for the --scell option --- tests/common/jobs/test_pheasy.py | 6 ++++-- 1 file changed, 4 insertions(+), 2 deletions(-) diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index 4a5cecb565..0dc02c8a66 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -272,9 +272,11 @@ def fake_run(args, check): matrix = np.diag([2, 3, 4]) _run_harmonic_fit(matrix, 1e-3, 5) - assert [args[:4] for args, _ in calls] == [["pheasy", "--dim", "2", "3"]] * 4 + assert [args[:6] for args, _ in calls] == [ + ["pheasy", "--scell", "SPOSCAR", "--dim", "2", "3"] + ] * 4 assert all(check for _, check in calls) - assert [args[9] for args, _ in calls] == ["-s", "-c", "-d", "-f"] + assert [args[11] for args, _ in calls] == ["-s", "-c", "-d", "-f"] fit = " ".join(calls[-1][0]) assert "-l LASSO --std --seed 103 --rasr BHH --ndata 5" in fit assert "--alpha_min" not in fit From 5420d29a2a6dcc7bf311974a72883c25f43fae12 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Thu, 1 Oct 2026 06:14:22 -0700 Subject: [PATCH 10/43] Pin pheasy to the commit with the faster sensing matrix --- pyproject.toml | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pyproject.toml b/pyproject.toml index 7d9110d588..8cfc833508 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -54,7 +54,7 @@ mp = ["mp-api>=0.37.5"] phonons = ["phonopy>=2.43,<5", "seekpath>=2.0.0"] # the pheasy fork adds the --disp_matrix_file and --force_matrix_file options # and fixes the --scell option -pheasy = ["atomate2[phonons,alamode]", "hiphive==1.5", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@1728f16642d5f2763f27695cd29ffada0f755d7f"] +pheasy = ["atomate2[phonons,alamode]", "hiphive==1.5", "numpy<=2.2", "pheasy @ git+https://gitlab.com/hpsahasrabuddhe/pheasy.git@9f24162a4ed0f0ab8911d382fd2617944aade55d"] alamode = ["alm @ git+https://github.com/ttadano/ALM.git@f1d668fdee66e7e7218a04c88daf19d0e14fce0c#subdirectory=python"] hiphive = ["hiphive==1.5", "trainstation>=1.0", "atomate2[phonons,alamode]"] lobster = ["ijson>=3.2.2", "lobsterpy>=0.6.0"] From f7d7c5281bacd56e3cbdcaa5a4f0a1631fb5ef63 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Thu, 1 Oct 2026 15:09:13 -0700 Subject: [PATCH 11/43] Converge the anharmonic LASSO fit with --tol 1e-8 --- src/atomate2/common/jobs/pheasy.py | 6 ++++-- tests/common/jobs/test_pheasy.py | 4 ++++ 2 files changed, 8 insertions(+), 2 deletions(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index c9f588f78a..e55be1c781 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -421,10 +421,12 @@ def _run_anharmonic_fit( f"--disp_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_displacements']}" ), # LASSO fit. OLS, pheasy's default, gives dense force constants. - # --std and --rasr are not passed to the anharmonic fit. + # --std and --rasr are not passed to the anharmonic fit. With pheasy's + # default --tol of 1e-4 the fits at small penalties do not converge, and + # the penalty chosen by cross-validation can change between machines. ( f"{base} -f {fix_fc2}-l LASSO --alpha_min {anhar_alpha_min} {seed}" - f"--ndata {int(num_anhar)} --hdf5 " + f"--tol 1e-8 --ndata {int(num_anhar)} --hdf5 " f"--force_matrix_file {_DEFAULT_FILE_PATHS['anharmonic_force_matrix']} " f"-o {log_file}" ), diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index 0dc02c8a66..e91fad382e 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -350,9 +350,13 @@ def test_anharmonic_fit_cocktail_and_one_shot(tmp_dir): # 20, then the undisplaced supercell assert len(displacements) == 1 + 20 + 1 + # the converged cocktail fit picks a penalty of about 1e-12, the default + # lower bound, so the bound is lowered to keep the penalty inside the + # search. In local runs the force constants did not change with the bound. job = generate_frequencies_eigenvectors( structure=structure, displacement_data=_emt_displacement_data(displacements), + anhar_alpha_min=-14, **anhar_kwargs, **FIT_KWARGS, **COMMON_KWARGS, From e7a677cdf79489705319fa83bd7161d3cc97cb94 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Fri, 2 Oct 2026 07:29:02 -0700 Subject: [PATCH 12/43] Link the phonon database and pass get_supercell_size_kwargs to the pheasy supercell job --- docs/user/codes/vasp.md | 2 +- src/atomate2/common/flows/pheasy.py | 11 ++++++++--- src/atomate2/common/jobs/pheasy.py | 8 ++++++-- src/atomate2/vasp/flows/pheasy.py | 2 +- tests/common/jobs/test_pheasy.py | 23 +++++++++++++++++++++++ tutorials/pheasy_workflow.ipynb | 2 +- 6 files changed, 40 insertions(+), 8 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 1e4dcfac0d..b8eddcb9c4 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -349,7 +349,7 @@ The `pheasy` extra, `pip install "atomate2[pheasy]"`, installs the pheasy versio ALM is compiled from source. If that build fails, see the ALM instructions below. By design, these workflows have the same basic structure as the harmonic forcefield workflows and use [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) in part to compute the phonon spectrum. To use `Pheasy` in the previous example, we would replace the import string to `from atomate2.vasp.flows.pheasy import PhononMaker`. -This workflow was used to build the Materials Project's Harmonic Phonon Database, described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1). +This workflow was used to build the [Materials Project's Harmonic Phonon Database](https://next-gen.materialsproject.org/materials?has_props=phonon), described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1). The pheasy fits can fail for a cell that is not in a standard setting, for example the primitive cell of MgO (mp-1265) as the Materials Project serves it. For such a structure, set `use_symmetrized_structure="primitive"`, as was done for the database. diff --git a/src/atomate2/common/flows/pheasy.py b/src/atomate2/common/flows/pheasy.py index 158c90efab..8e3d5f64a9 100644 --- a/src/atomate2/common/flows/pheasy.py +++ b/src/atomate2/common/flows/pheasy.py @@ -6,7 +6,7 @@ from dataclasses import dataclass, field from typing import TYPE_CHECKING, Literal -from pymatgen.util.due import Doi, due +from pymatgen.util.due import Doi, Url, due from atomate2.common.flows.phonons import BasePhononMaker as PurePhonopyMaker from atomate2.common.jobs.pheasy import ( @@ -33,9 +33,13 @@ @due.dcite( - Doi("10.26434/chemrxiv.15004632/v1"), + Url("https://next-gen.materialsproject.org/materials?has_props=phonon"), description="Materials Project's Harmonic Phonon Database.", ) +@due.dcite( + Doi("10.26434/chemrxiv.15004632/v1"), + description="Preprint on the Materials Project's Harmonic Phonon Database.", +) @due.dcite( Doi("10.48550/arXiv.2508.01020"), description="Pheasy code for (an)harmonic force constants.", @@ -148,7 +152,7 @@ class BasePhononMaker(PurePhonopyMaker, ABC): if set to True, only diagonal supercell matrices are allowed. The pheasy commands take the diagonal of the supercell matrix. get_supercell_size_kwargs: dict - not used by this workflow. + kwargs that will be passed to get_supercell_size to determine supercell size use_symmetrized_structure: str allowed strings: "primitive", "conventional", None @@ -400,6 +404,7 @@ def get_supercell_matrix(self, structure: Structure) -> Job | Flow: self.max_atoms, self.force_90_degrees, self.force_diagonal, + **self.get_supercell_size_kwargs, ) @property diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index e55be1c781..580567bb2b 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -446,6 +446,7 @@ def get_supercell_size( max_atoms: int, force_90_degrees: bool, force_diagonal: bool, + **kwargs, ) -> list[list[float]]: """ Determine the supercell matrix with pymatgen's CubicSupercellTransformation. @@ -462,14 +463,17 @@ def get_supercell_size( if True, only supercells with three 90 degree angles are allowed force_diagonal: bool if True, only diagonal supercell matrices are allowed + **kwargs: + Additional parameters passed to CubicSupercellTransformation. They + override the defaults angle_tolerance=1e-2 and allow_orthorhombic=False. """ + kwargs = {"angle_tolerance": 1e-2, "allow_orthorhombic": False} | kwargs transformation = CubicSupercellTransformation( min_length=min_length, max_atoms=max_atoms, force_90_degrees=force_90_degrees, force_diagonal=force_diagonal, - angle_tolerance=1e-2, - allow_orthorhombic=False, + **kwargs, ) transformation.apply_transformation(structure=structure) return transformation.transformation_matrix.transpose().tolist() diff --git a/src/atomate2/vasp/flows/pheasy.py b/src/atomate2/vasp/flows/pheasy.py index 14a4368c4a..d934c538dd 100644 --- a/src/atomate2/vasp/flows/pheasy.py +++ b/src/atomate2/vasp/flows/pheasy.py @@ -123,7 +123,7 @@ class PhononMaker(BasePhononMaker): allow_orthorhombic: bool not used by this workflow. get_supercell_size_kwargs: dict - not used by this workflow. + kwargs that will be passed to get_supercell_size to determine supercell size use_symmetrized_structure: str allowed strings: "primitive", "conventional", None diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index e91fad382e..f9ae158bd8 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -30,6 +30,7 @@ _get_num_irreducible_fcs, _run_band_structure_and_plot, ) +from atomate2.forcefields.flows.pheasy import PhononMaker # fcs_cutoff_radius in Bohr. 8 Bohr (4.2 A) covers the first two neighbour # shells of fcc Cu (2.55 and 3.61 A) and stays inside the 10.8 A supercell. @@ -299,6 +300,28 @@ def fake_run(args, check): assert "--rasr" not in fit +def test_get_supercell_size_kwargs(monkeypatch): + received = {} + transformation = pheasy_jobs.CubicSupercellTransformation + + def record_kwargs(**kwargs): + received.update(kwargs) + return transformation(**kwargs) + + monkeypatch.setattr(pheasy_jobs, "CubicSupercellTransformation", record_kwargs) + + # the maker passes get_supercell_size_kwargs on to the job + maker = PhononMaker(get_supercell_size_kwargs={"angle_tolerance": 0.1}) + job = maker.get_supercell_matrix(_cu_structure()) + assert job.function_kwargs == {"angle_tolerance": 0.1} + + # the job passes them to CubicSupercellTransformation. The other default + # is kept. + job.function(*job.function_args, **job.function_kwargs) + assert received["angle_tolerance"] == 0.1 + assert received["allow_orthorhombic"] is False + + def test_check_lasso_alpha(tmp_dir): log_file = Path("pheasy_anharmonic_fit.log") diff --git a/tutorials/pheasy_workflow.ipynb b/tutorials/pheasy_workflow.ipynb index 6f6742b043..91f318cd21 100644 --- a/tutorials/pheasy_workflow.ipynb +++ b/tutorials/pheasy_workflow.ipynb @@ -42,7 +42,7 @@ "\n", "The [Pheasy code](https://doi.org/10.48550/arXiv.2508.01020) extracts (an)harmonic interatomic force constants from a set of displaced supercell calculations using machine-learning (LASSO) regression. Compared to the finite-displacement approach in the standard phonon workflow, far fewer (randomly displaced) supercells are needed, which substantially reduces the number of DFT calculations.\n", "\n", - "This workflow was used to build the Materials Project's Harmonic Phonon Database, described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1).\n", + "This workflow was used to build the [Materials Project's Harmonic Phonon Database](https://next-gen.materialsproject.org/materials?has_props=phonon), described in [this preprint](https://chemrxiv.org/doi/full/10.26434/chemrxiv.15004632/v1).\n", "\n", "The workflow has the same basic structure as the phonopy-based phonon workflow and uses [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) to post-process the force constants into band structures, densities of states, and thermodynamic properties.\n", "\n", From d8db2f17e55cd0295de6d79a1dfae5067c434b3b Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Fri, 2 Oct 2026 08:41:34 -0700 Subject: [PATCH 13/43] Note in the docs that the anharmonic pheasy workflow is less tested --- docs/user/codes/vasp.md | 6 ++++++ 1 file changed, 6 insertions(+) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index b8eddcb9c4..a1944938b9 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -354,6 +354,12 @@ The pheasy fits can fail for a cell that is not in a standard setting, for examp For such a structure, set `use_symmetrized_structure="primitive"`, as was done for the database. By default, this workflow does not compute anharmonic force constants, but can be extended to using the `cal_anhar_fcs` kwarg. + +```{warning} +The anharmonic part of this workflow has not been tested as widely as the harmonic part. +It might still change in future versions. +``` + ALM, from the ALAMODE package, counts the free force constants used to size the random displacement sets. To install ALAMODE, see their [installation guidelines](https://alamode.readthedocs.io/en/latest/install.html#). From 660506fed80afb4ed81e2b8cba3464b26e9826b8 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sat, 3 Oct 2026 12:50:29 -0700 Subject: [PATCH 14/43] Converge the harmonic LASSO fit with --tol 1e-8 pheasy's default --tol of 1e-4 leaves the fit unconverged. Refits of the same data then give different force constants on different machines. --- src/atomate2/common/jobs/pheasy.py | 10 ++++++---- tests/common/jobs/test_pheasy.py | 4 ++-- 2 files changed, 8 insertions(+), 6 deletions(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 580567bb2b..3dcc46e6dc 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -303,8 +303,8 @@ def _run_harmonic_fit( num_har: int Number of displaced supercells in the fit. use_lasso: bool - If True, fit with LASSO on standardized data. If False, fit with - pheasy's default least squares. + If True, fit with LASSO on standardized data, converged to --tol 1e-8. + If False, fit with pheasy's default least squares. rotational_sum_rule: str | None Rotational sum rule passed to pheasy with --rasr, or None for none. alpha_min: int | None @@ -319,7 +319,9 @@ def _run_harmonic_fit( base = f"pheasy --scell SPOSCAR --dim {dim} -w 2 --symprec {float(symprec)}" fit = f"{base} -f --full_ifc" if use_lasso: - fit += " -l LASSO --std" + # pheasy's default --tol of 1e-4 leaves the fit unconverged, so the force + # constants change between machines and package versions + fit += " -l LASSO --std --tol 1e-8" if alpha_min is not None: fit += f" --alpha_min {int(alpha_min)}" if random_seed is not None: @@ -1026,7 +1028,7 @@ def generate_frequencies_eigenvectors( f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --c2 10.0 " f"--full_ifc -w 2 --symprec {float(symprec)} " - f"-l LASSO --std --rasr BHH --ndata {int(num_har)} " + f"-l LASSO --std --tol 1e-8 --rasr BHH --ndata {int(num_har)} " f"--force_matrix_file {_DEFAULT_FILE_PATHS['harmonic_force_matrix']}" ) diff --git a/tests/common/jobs/test_pheasy.py b/tests/common/jobs/test_pheasy.py index e91fad382e..056b1e47a7 100644 --- a/tests/common/jobs/test_pheasy.py +++ b/tests/common/jobs/test_pheasy.py @@ -278,7 +278,7 @@ def fake_run(args, check): assert all(check for _, check in calls) assert [args[11] for args, _ in calls] == ["-s", "-c", "-d", "-f"] fit = " ".join(calls[-1][0]) - assert "-l LASSO --std --seed 103 --rasr BHH --ndata 5" in fit + assert "-l LASSO --std --tol 1e-8 --seed 103 --rasr BHH --ndata 5" in fit assert "--alpha_min" not in fit assert " -o " not in fit @@ -286,7 +286,7 @@ def fake_run(args, check): _run_harmonic_fit(matrix, 1e-3, 3, use_lasso=False) fit = " ".join(calls[-1][0]) assert "-f --full_ifc --rasr BHH --ndata 3" in fit - for flag in ("-l", "--std", "--seed"): + for flag in ("-l", "--std", "--tol", "--seed"): assert flag not in calls[-1][0] calls.clear() From 165584427d946c2bbef239a74cc15dcf57ad7dfb Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sat, 3 Oct 2026 16:49:20 -0700 Subject: [PATCH 15/43] Add a tutorial for the finite-temperature phonon workflow --- .github/workflows/testing.yml | 2 +- tutorials/finite_temperature_phonons.ipynb | 940 +++++++++++++++++++++ tutorials/tutorials.md | 1 + 3 files changed, 942 insertions(+), 1 deletion(-) create mode 100644 tutorials/finite_temperature_phonons.ipynb diff --git a/.github/workflows/testing.yml b/.github/workflows/testing.yml index 7405467740..7175d33825 100644 --- a/.github/workflows/testing.yml +++ b/.github/workflows/testing.yml @@ -303,7 +303,7 @@ jobs: MP_API_KEY: ${{ secrets.MP_API_KEY }} run: | micromamba activate a2 - pytest --durations=5 -n auto --nbmake ./tutorials --ignore=./tutorials/openmm_tutorial.ipynb --ignore=./tutorials/force_fields --ignore=./tutorials/torchsim_tutorial.ipynb --ignore=./tutorials/lammps_workflow.ipynb --ignore=./tutorials/pheasy_workflow.ipynb --ignore=./tutorials/hiphive_workflow.ipynb --ignore=./tutorials/cte_workflow.ipynb + pytest --durations=5 -n auto --nbmake ./tutorials --ignore=./tutorials/openmm_tutorial.ipynb --ignore=./tutorials/force_fields --ignore=./tutorials/torchsim_tutorial.ipynb --ignore=./tutorials/lammps_workflow.ipynb --ignore=./tutorials/pheasy_workflow.ipynb --ignore=./tutorials/hiphive_workflow.ipynb --ignore=./tutorials/cte_workflow.ipynb --ignore=./tutorials/finite_temperature_phonons.ipynb - name: Test ASE env: diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb new file mode 100644 index 0000000000..8bccb3558e --- /dev/null +++ b/tutorials/finite_temperature_phonons.ipynb @@ -0,0 +1,940 @@ +{ + "cells": [ + { + "cell_type": "markdown", + "id": "0", + "metadata": {}, + "source": [ + "# Finite-temperature phonons with pheasy and machine-learned potentials\n", + "\n", + "This notebook computes phonons at a finite temperature with the\n", + "`ForceFieldFiniteTemperaturePhononMaker` workflow. The forces come from three\n", + "MACE potentials, so no DFT is needed.\n", + "\n", + "Section 1 runs five materials at 100, 300, 500, 700 and 900 K. Ca3Ir4Sn13 is\n", + "worked through step by step. Section 2 tests the length of the MD and the number\n", + "of snapshots for KNaICl.\n", + "\n", + "This workflow is new. It is less tested than the other phonon workflows in\n", + "atomate2, and its defaults and output may still change." + ] + }, + { + "cell_type": "markdown", + "id": "1", + "metadata": {}, + "source": [ + "## Background\n", + "\n", + "Harmonic phonons from finite displacements describe the crystal at 0 K. Many\n", + "materials have imaginary modes at 0 K. The anharmonic motion of the atoms can\n", + "stabilize these modes at higher temperature. This workflow fits effective\n", + "harmonic force constants to an MD trajectory at the temperature of interest, as\n", + "in the temperature-dependent effective potential (TDEP) method of Hellman et\n", + "al., Phys. Rev. B 84, 180301 (2011). These force constants include the\n", + "anharmonic effects at that temperature.\n", + "\n", + "The flow has these steps:\n", + "\n", + "1. The structure is relaxed. The relaxation can be switched off, as done below.\n", + "2. A diagonal supercell is built. Its lattice vectors are at least `min_length`\n", + " long, 12 Å by default. A supercell matrix can also be given.\n", + "3. An NVT MD run of the supercell at the temperature. The defaults are 8 ps with\n", + " a 1 fs time step and a Nose-Hoover thermostat.\n", + "4. The first 1 ps of the MD is left out. 50 snapshots are picked, evenly spread\n", + " over the rest of the trajectory.\n", + "5. The forces on the snapshots and on the undisplaced supercell are computed.\n", + "6. pheasy fits the second-order force constants with LASSO. The displacements\n", + " are measured from the undisplaced supercell. The forces of the undisplaced\n", + " supercell are subtracted from the forces of each snapshot.\n", + "7. The band structure and the density of states (DOS) follow from the force\n", + " constants. Imaginary modes are reported. They are not removed.\n", + "\n", + "The MD trajectory is also checked. The check looks for melting and for a move\n", + "away from the starting structure. It also looks at the drift of the potential\n", + "energy late in the run. The result is stored in the output. A warning is raised\n", + "if the check fails, but the fit is still done.\n", + "\n", + "The volume stays that of the starting structure, so thermal expansion is not\n", + "included. The same workflow runs with VASP as\n", + "`atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`.\n", + "`atomate2.forcefields.flows.finite_temperature_phonons` also has two mixed\n", + "versions. One runs the MD with VASP and the force calculations with a force\n", + "field. The other one does the reverse." + ] + }, + { + "cell_type": "markdown", + "id": "2", + "metadata": {}, + "source": [ + "## Installation\n", + "\n", + "The `pheasy` and `ase` extras are needed, plus MACE and the Materials Project\n", + "client:\n", + "\n", + "```\n", + "pip install 'atomate2[pheasy,ase]'\n", + "pip install 'mace-torch>=0.3.16' mp-api\n", + "```\n", + "\n", + "The `pheasy` extra pulls in pheasy and ALM. ALM is compiled from source. The\n", + "hiPhive tutorial and the atomate2 VASP documentation list what the build needs." + ] + }, + { + "cell_type": "markdown", + "id": "3", + "metadata": {}, + "source": [ + "## The potentials\n", + "\n", + "The notebook uses three MACE foundation models. All three are released under the\n", + "Academic Software License.\n", + "\n", + "- **MACE-OMAT-0-medium.** `mace_mp(model=\"medium-omat-0\")` downloads it once and\n", + " caches it under `~/.cache/mace`.\n", + "- **MACE-MATPES-PBE-0** and **MACE-MATPES-r2SCAN-0.** These are MACE-OMAT-0\n", + " fine-tuned on the MatPES data set at the PBE and r2SCAN levels. They need\n", + " `mace-torch>=0.3.10`. Download the two files from the `mace_matpes_0` release of\n", + " [mace-foundations](https://github.com/ACEsuit/mace-foundations/releases/tag/mace_matpes_0):\n", + " - [MACE-matpes-pbe-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-pbe-omat-ft.model)\n", + " - [MACE-matpes-r2scan-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-r2scan-omat-ft.model)\n", + "\n", + "Set the paths to the two downloaded files in the next cell. The Ca3Ir4Sn13\n", + "example below only needs MACE-OMAT-0-medium.\n", + "\n", + "The MD takes most of the time, so a GPU helps a lot. The next cell uses one if\n", + "PyTorch finds it. All our runs used `float64` on one NVIDIA A100 GPU of a\n", + "Perlmutter node." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "4", + "metadata": {}, + "outputs": [], + "source": [ + "import os\n", + "import warnings\n", + "\n", + "# macOS: conda's llvm-openmp and torch's bundled libomp both load and the\n", + "# duplicate aborts the process. This must be set before torch is imported.\n", + "os.environ.setdefault(\"KMP_DUPLICATE_LIB_OK\", \"TRUE\")\n", + "warnings.filterwarnings(\"ignore\")\n", + "\n", + "import torch # noqa: E402\n", + "from mace.calculators import mace_mp # noqa: E402\n", + "\n", + "# Replace the two paths with the files you downloaded.\n", + "MODEL_FILES = {\n", + " \"OMAT-0-medium\": \"medium-omat-0\",\n", + " \"MATPES-PBE-0\": \"/path/to/MACE-matpes-pbe-omat-ft.model\",\n", + " \"MATPES-r2SCAN-0\": \"/path/to/MACE-matpes-r2scan-omat-ft.model\",\n", + "}\n", + "DEVICE = \"cuda\" if torch.cuda.is_available() else \"cpu\"\n", + "\n", + "\n", + "def calc_kwargs(model: str) -> dict:\n", + " \"\"\"Return the calculator settings for one of the models above.\"\"\"\n", + " return {\"model\": MODEL_FILES[model], \"device\": DEVICE, \"default_dtype\": \"float64\"}\n", + "\n", + "\n", + "_ = mace_mp(**calc_kwargs(\"OMAT-0-medium\")) # downloads and caches on first use" + ] + }, + { + "cell_type": "markdown", + "id": "5", + "metadata": {}, + "source": [ + "## One calculator for all jobs\n", + "\n", + "Every force field job builds its own calculator. `run_locally` runs all of\n", + "them in this one Python process, and the workflow has a little over 50 jobs.\n", + "Loading MACE for each of them grows the memory by about 150 MB per job. This\n", + "cell makes the jobs share one calculator. It is only needed when many jobs run\n", + "in one process, not with a workflow manager." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "6", + "metadata": {}, + "outputs": [], + "source": [ + "from ase.calculators.calculator import Calculator\n", + "\n", + "import atomate2.forcefields.utils as ff_utils\n", + "\n", + "_ase_calculator = ff_utils.ase_calculator\n", + "_calculators: dict[str, Calculator] = {}\n", + "\n", + "\n", + "def shared_ase_calculator(calculator_meta: object, **kwargs: object) -> Calculator:\n", + " \"\"\"Build each calculator once and reuse it for every job.\"\"\"\n", + " key = repr((calculator_meta, sorted(kwargs.items())))\n", + " if key not in _calculators:\n", + " _calculators[key] = _ase_calculator(calculator_meta, **kwargs)\n", + " _calculators[key].reset()\n", + " return _calculators[key]\n", + "\n", + "\n", + "ff_utils.ase_calculator = shared_ase_calculator" + ] + }, + { + "cell_type": "markdown", + "id": "7", + "metadata": {}, + "source": [ + "## 1. Five materials from 100 K to 900 K\n", + "\n", + "The first part runs Ca3Ir4Sn13 at 300 K with MACE-OMAT-0-medium step by step.\n", + "The other temperatures, potentials and materials follow with the same code." + ] + }, + { + "cell_type": "markdown", + "id": "8", + "metadata": {}, + "source": [ + "## The structure\n", + "\n", + "Ca3Ir4Sn13 (mp-1200211) is cubic, with 40 atoms in the primitive cell. We start\n", + "from its PBEsol cell in the Materials Project's Harmonic Phonon Database. The\n", + "phonon documents of the Materials Project hold this cell. Set your key first with\n", + "`export MP_API_KEY=...`." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "9", + "metadata": {}, + "outputs": [], + "source": [ + "from mp_api.client import MPRester\n", + "from pymatgen.core import Structure\n", + "\n", + "if not os.environ.get(\"MP_API_KEY\"):\n", + " raise OSError(\"export MP_API_KEY before running this cell\")\n", + "\n", + "\n", + "def get_pheasy_structure(mp_id: str) -> Structure:\n", + " \"\"\"Get the PBEsol cell of a material in the Harmonic Phonon Database.\"\"\"\n", + " with MPRester() as mpr:\n", + " (doc,) = mpr.materials.phonon.search(\n", + " material_ids=[mp_id],\n", + " phonon_method=\"pheasy\",\n", + " fields=[\"structure\"],\n", + " num_chunks=1,\n", + " chunk_size=10,\n", + " )\n", + " return doc.structure\n", + "\n", + "\n", + "structure = get_pheasy_structure(\"mp-1200211\")\n", + "structure.lattice" + ] + }, + { + "cell_type": "markdown", + "id": "10", + "metadata": {}, + "source": [ + "## Building the workflow\n", + "\n", + "`ForceFieldFiniteTemperaturePhononMaker.from_force_field_name` sets one force\n", + "field for the relaxation, the MD and the force calculations. Any MACE model\n", + "routes through `mace_mp`, and the model name in `calculator_kwargs` selects the\n", + "weights.\n", + "\n", + "We skip the relaxation with `relax_initial_structure=False`. The cell is\n", + "already relaxed with PBEsol, and our AIMD reference below uses the same cell. If\n", + "your input cell is not properly relaxed, keep the default\n", + "`relax_initial_structure=True`. The force field then relaxes the cell before\n", + "the MD.\n", + "\n", + "We give the supercell matrix of our AIMD reference, 2x2x2 with 320 atoms.\n", + "Everything else stays at the workflow defaults." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "11", + "metadata": {}, + "outputs": [], + "source": [ + "from atomate2.forcefields.flows.finite_temperature_phonons import (\n", + " ForceFieldFiniteTemperaturePhononMaker,\n", + ")\n", + "\n", + "maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(\n", + " \"MACE-MP-0\",\n", + " calculator_kwargs=calc_kwargs(\"OMAT-0-medium\"),\n", + " relax_initial_structure=False,\n", + " temperature=300,\n", + ")\n", + "flow = maker.make(structure, supercell_matrix=[[2, 0, 0], [0, 2, 0], [0, 0, 2]])\n", + "flow.draw_graph().show()" + ] + }, + { + "cell_type": "markdown", + "id": "12", + "metadata": {}, + "source": [ + "## Running the workflow\n", + "\n", + "The flow has one MD job and 51 force calculations, 50 snapshots and the\n", + "undisplaced supercell. On one A100 GPU the whole run took 11 minutes. The MD\n", + "took 9 minutes, the force calculations 11 seconds and the fit 2 minutes.\n", + "\n", + "`create_folders=True` is needed, because the snapshots are read from the\n", + "trajectory file in the folder of the MD job." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "13", + "metadata": {}, + "outputs": [], + "source": [ + "from jobflow import JobStore, run_locally\n", + "from maggma.stores import MemoryStore\n", + "\n", + "job_store = JobStore(MemoryStore(), additional_stores={\"data\": MemoryStore()})\n", + "responses = run_locally(flow, store=job_store, create_folders=True, ensure_success=True)\n", + "doc = responses[flow.output.uuid][1].output" + ] + }, + { + "cell_type": "markdown", + "id": "14", + "metadata": {}, + "source": [ + "## Results\n", + "\n", + "The output is a `FiniteTemperaturePhononDoc`. It holds the band structure, the\n", + "DOS, the force constants, the fit and the trajectory check." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "15", + "metadata": {}, + "outputs": [], + "source": [ + "import numpy as np\n", + "\n", + "health = doc.trajectory_health\n", + "{\n", + " \"highest frequency in THz\": float(np.max(doc.phonon_bandstructure.bands)),\n", + " \"imaginary modes on the band path\": doc.has_imaginary_modes,\n", + " \"lowest frequency at the commensurate q-points in THz\": doc.min_frequency,\n", + " \"LASSO penalty\": doc.lasso_alpha,\n", + " \"force RMSE in eV/A\": doc.force_rmse,\n", + " \"trajectory check\": health.verdict,\n", + " \"Lindemann ratio\": health.lindemann_ratio,\n", + "}" + ] + }, + { + "cell_type": "markdown", + "id": "16", + "metadata": {}, + "source": [ + "Our run gave a highest frequency of 5.97 THz, no imaginary modes and a stable\n", + "trajectory.\n", + "\n", + "- `has_imaginary_modes` checks the whole band path. `min_frequency` only covers\n", + " the q-points commensurate with the supercell. The fit sets the frequencies at\n", + " these points directly. Everywhere else they are interpolated. Section 2 shows\n", + " why the difference matters.\n", + "- The force RMSE is the part of the forces that the force constants do not\n", + " describe. It grows with temperature, from 0.05 eV/Å at 100 K to 0.29 eV/Å at\n", + " 900 K for Ca3Ir4Sn13.\n", + "- The Lindemann ratio is the root mean square vibration of the atoms around\n", + " their mean positions, divided by the nearest-neighbor distance. Above 0.12 the check reports the trajectory as\n", + " melted." + ] + }, + { + "cell_type": "markdown", + "id": "17", + "metadata": {}, + "source": [ + "## Comparing with 0 K\n", + "\n", + "The Materials Project's Harmonic Phonon Database has the 0 K phonons of the same\n", + "cell, computed with PBEsol (Sahasrabuddhe et al., ChemRxiv (2026),\n", + "doi:10.26434/chemrxiv.15004632/v1). The next cell plots them next to ours. The\n", + "two band structures use different paths through the Brillouin zone, so they are\n", + "drawn side by side." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "18", + "metadata": {}, + "outputs": [], + "source": [ + "import matplotlib.pyplot as plt\n", + "from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine\n", + "from pymatgen.phonon.dos import PhononDos\n", + "\n", + "\n", + "def plot_bands(\n", + " ax: plt.Axes, bs: PhononBandStructureSymmLine, label: str | None = None, **style\n", + ") -> None:\n", + " \"\"\"Plot a phonon band structure, one segment of the path at a time.\"\"\"\n", + " distance = np.array(bs.distance)\n", + " positions, names = [], []\n", + " for idx, branch in enumerate(bs.branches):\n", + " part = slice(branch[\"start_index\"], branch[\"end_index\"] + 1)\n", + " lines = ax.plot(distance[part], bs.bands[:, part].T, **style)\n", + " if idx == 0 and label:\n", + " lines[0].set_label(label)\n", + " start, end = branch[\"name\"].split(\"-\")\n", + " if positions and np.isclose(positions[-1], distance[part.start]):\n", + " if names[-1] != start:\n", + " names[-1] += \"|\" + start\n", + " else:\n", + " positions.append(distance[part.start])\n", + " names.append(start)\n", + " positions.append(distance[branch[\"end_index\"]])\n", + " names.append(end)\n", + " names = [name.replace(\"\\\\Gamma\", \"Γ\").replace(\"GAMMA\", \"Γ\") for name in names]\n", + " ax.set_xticks(positions, names)\n", + " ax.set_xlim(distance[0], distance[-1])\n", + " ax.axhline(0, color=\"gray\", lw=0.5)\n", + "\n", + "\n", + "def plot_dos(ax: plt.Axes, dos: PhononDos, label: str | None = None, **style) -> None:\n", + " \"\"\"Plot a phonon DOS sideways, to sit next to a band structure.\"\"\"\n", + " ax.plot(dos.densities, dos.frequencies, label=label, **style)\n", + " ax.set_xlabel(\"DOS\")\n", + "\n", + "\n", + "with MPRester() as mpr:\n", + " bs_0k = mpr.materials.phonon.get_bandstructure_from_material_id(\n", + " \"mp-1200211\", phonon_method=\"pheasy\"\n", + " ).to_pmg\n", + " dos_0k = mpr.materials.phonon.get_dos_from_material_id(\n", + " \"mp-1200211\", phonon_method=\"pheasy\"\n", + " ).to_pmg\n", + "\n", + "fig, axes = plt.subplots(\n", + " 1, 3, figsize=(13, 4), sharey=True, gridspec_kw={\"width_ratios\": [3, 3, 1]}\n", + ")\n", + "plot_bands(axes[0], bs_0k, color=\"gray\", lw=0.8)\n", + "plot_bands(axes[1], doc.phonon_bandstructure, color=\"C0\", lw=0.8)\n", + "plot_dos(axes[2], dos_0k, label=\"0 K\", color=\"gray\")\n", + "plot_dos(axes[2], doc.phonon_dos, label=\"300 K\", color=\"C0\")\n", + "axes[0].set_title(\"0 K, PBEsol\")\n", + "axes[1].set_title(\"300 K, MACE-OMAT-0-medium\")\n", + "axes[0].set_ylabel(\"Frequency (THz)\")\n", + "axes[2].legend()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "19", + "metadata": {}, + "source": [ + "At 0 K, Ca3Ir4Sn13 has imaginary modes down to about -0.75 THz. At 300 K they\n", + "are gone. The motion of the atoms at 300 K stabilizes them.\n", + "\n", + "To check the force field, we compare with effective harmonic force constants\n", + "fitted to ab initio MD at 300 K. These were computed with PBEsol in the same\n", + "cell and supercell. Their highest frequency is 6.03 THz, against 5.97 THz from\n", + "MACE-OMAT-0-medium. Over the whole band path the frequencies differ by 0.07 THz\n", + "on average." + ] + }, + { + "cell_type": "markdown", + "id": "20", + "metadata": {}, + "source": [ + "## The other temperatures, potentials and materials\n", + "\n", + "The same workflow runs at five temperatures, with all three potentials and for\n", + "four more materials. AlAsPt5, Zn3P2 and Er5Tl3 also have imaginary modes at 0 K.\n", + "Bi4S3N2 is polar. The function below builds and runs one workflow in its own\n", + "folder. Section 2 uses it as well.\n", + "\n", + "The loop runs 75 workflows, so it is off by default. Set `RUN_ALL = True` to\n", + "run it. Each of our runs took 6 to 36 minutes on one A100 GPU." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "21", + "metadata": {}, + "outputs": [], + "source": [ + "from atomate2.common.schemas.finite_temperature_phonons import (\n", + " FiniteTemperaturePhononDoc,\n", + ")\n", + "\n", + "# mp-id and the diagonal of the supercell matrix of our AIMD reference\n", + "MATERIALS = {\n", + " \"Ca3Ir4Sn13\": (\"mp-1200211\", (2, 2, 2)),\n", + " \"AlAsPt5\": (\"mp-1025306\", (4, 4, 2)),\n", + " \"Zn3P2\": (\"mp-2071\", (2, 2, 2)),\n", + " \"Bi4S3N2\": (\"mp-1245549\", (2, 2, 2)),\n", + " \"Er5Tl3\": (\"mp-1105965\", (2, 2, 2)),\n", + " \"KNaICl\": (\"mp-1002081\", (3, 3, 2)),\n", + "}\n", + "TEMPERATURES = (100, 300, 500, 700, 900)\n", + "\n", + "\n", + "def run_ft(\n", + " structure: Structure,\n", + " supercell: tuple[int, int, int],\n", + " model: str,\n", + " root_dir: str,\n", + " temperature: float,\n", + " md_time: float = 8.0,\n", + " n_snapshots: int = 50,\n", + ") -> FiniteTemperaturePhononDoc:\n", + " \"\"\"Run the finite-temperature phonon workflow and return its output.\"\"\"\n", + " maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(\n", + " \"MACE-MP-0\",\n", + " calculator_kwargs=calc_kwargs(model),\n", + " relax_initial_structure=False,\n", + " temperature=temperature,\n", + " md_time=md_time,\n", + " n_snapshots=n_snapshots,\n", + " )\n", + " flow = maker.make(structure, supercell_matrix=np.diag(supercell).tolist())\n", + " os.makedirs(root_dir, exist_ok=True)\n", + " responses = run_locally(\n", + " flow,\n", + " store=JobStore(MemoryStore(), additional_stores={\"data\": MemoryStore()}),\n", + " create_folders=True,\n", + " root_dir=root_dir,\n", + " ensure_success=True,\n", + " )\n", + " return responses[flow.output.uuid][1].output\n", + "\n", + "\n", + "RUN_ALL = False\n", + "docs = {}\n", + "if RUN_ALL:\n", + " for name in (\"Ca3Ir4Sn13\", \"AlAsPt5\", \"Zn3P2\", \"Bi4S3N2\", \"Er5Tl3\"):\n", + " mp_id, supercell = MATERIALS[name]\n", + " unit_cell = get_pheasy_structure(mp_id)\n", + " for model in MODEL_FILES:\n", + " for temperature in TEMPERATURES:\n", + " docs[name, model, temperature] = run_ft(\n", + " unit_cell,\n", + " supercell,\n", + " model,\n", + " f\"runs/{name}_{model}_{temperature}K\",\n", + " temperature,\n", + " )" + ] + }, + { + "cell_type": "markdown", + "id": "22", + "metadata": {}, + "source": [ + "The next cell plots the results of the loop. For each potential it shows the\n", + "band structure at 100, 500 and 900 K. Ca3Ir4Sn13 and Zn3P2 have 40 atoms in the\n", + "primitive cell, so their 120 branches are hard to follow. For these two the DOS\n", + "at all five temperatures is shown as well." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "23", + "metadata": {}, + "outputs": [], + "source": [ + "def plot_temperatures(name: str, with_dos: bool) -> None:\n", + " \"\"\"Plot the band structures of one material at 100, 500 and 900 K.\"\"\"\n", + " ratios = [3, 1] * len(MODEL_FILES) if with_dos else [3] * len(MODEL_FILES)\n", + " fig, axes = plt.subplots(\n", + " 1,\n", + " len(ratios),\n", + " figsize=(4.5 * len(MODEL_FILES), 4),\n", + " sharey=True,\n", + " gridspec_kw={\"width_ratios\": ratios},\n", + " )\n", + " colors = dict(\n", + " zip(TEMPERATURES, plt.cm.plasma(np.linspace(0, 0.85, 5)), strict=True)\n", + " )\n", + " step = 2 if with_dos else 1\n", + " for idx, model in enumerate(MODEL_FILES):\n", + " ax = axes[step * idx]\n", + " for temperature in (100, 500, 900):\n", + " plot_bands(\n", + " ax,\n", + " docs[name, model, temperature].phonon_bandstructure,\n", + " label=f\"{temperature} K\",\n", + " color=colors[temperature],\n", + " lw=0.6,\n", + " )\n", + " ax.set_title(model)\n", + " if with_dos:\n", + " for temperature in TEMPERATURES:\n", + " plot_dos(\n", + " axes[step * idx + 1],\n", + " docs[name, model, temperature].phonon_dos,\n", + " label=f\"{temperature} K\",\n", + " color=colors[temperature],\n", + " )\n", + " axes[0].set_ylabel(\"Frequency (THz)\")\n", + " axes[-1].legend(fontsize=8)\n", + " fig.suptitle(name)\n", + " plt.show()\n", + "\n", + "\n", + "if RUN_ALL:\n", + " for name in (\"Ca3Ir4Sn13\", \"AlAsPt5\", \"Zn3P2\", \"Bi4S3N2\", \"Er5Tl3\"):\n", + " plot_temperatures(name, with_dos=name in (\"Ca3Ir4Sn13\", \"Zn3P2\"))" + ] + }, + { + "cell_type": "markdown", + "id": "24", + "metadata": {}, + "source": [ + "## Our results\n", + "\n", + "The next cell holds the results of our runs. For each material it gives the\n", + "highest frequency on the band path at each temperature. The dashed line is the\n", + "highest frequency of the AIMD reference at 300 K." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "25", + "metadata": {}, + "outputs": [], + "source": [ + "import pandas as pd\n", + "\n", + "# highest frequency on the band path in THz, at 100, 300, 500, 700 and 900 K\n", + "MAX_FREQUENCY = {\n", + " \"Ca3Ir4Sn13\": {\n", + " \"OMAT-0-medium\": (5.98, 5.97, 5.93, 5.90, 5.83),\n", + " \"MATPES-PBE-0\": (5.80, 5.75, 5.67, 5.63, 5.65),\n", + " \"MATPES-r2SCAN-0\": (5.95, 5.98, 5.92, 5.88, 5.78),\n", + " },\n", + " \"AlAsPt5\": {\n", + " \"OMAT-0-medium\": (7.75, 7.73, 7.81, 7.76, 7.71),\n", + " \"MATPES-PBE-0\": (7.65, 7.57, 7.48, 7.59, 7.47),\n", + " \"MATPES-r2SCAN-0\": (7.66, 7.62, 7.77, 7.53, 7.43),\n", + " },\n", + " \"Zn3P2\": {\n", + " \"OMAT-0-medium\": (10.59, 10.36, 10.13, 9.67, 9.17),\n", + " \"MATPES-PBE-0\": (10.33, 10.03, 9.86, 9.53, 8.73),\n", + " \"MATPES-r2SCAN-0\": (11.19, 10.85, 10.66, 10.41, 9.97),\n", + " },\n", + " \"Bi4S3N2\": {\n", + " \"OMAT-0-medium\": (17.15, 16.88, 16.05, 16.26, 15.47),\n", + " \"MATPES-PBE-0\": (15.97, 15.64, 15.40, 14.75, 14.31),\n", + " \"MATPES-r2SCAN-0\": (17.62, 16.94, 17.23, 16.87, 15.54),\n", + " },\n", + " \"Er5Tl3\": {\n", + " \"OMAT-0-medium\": (4.23, 4.22, 4.19, 4.22, 4.23),\n", + " \"MATPES-PBE-0\": (4.11, 4.07, 4.01, 3.93, 3.99),\n", + " \"MATPES-r2SCAN-0\": (4.18, 4.09, 4.08, 3.99, 3.96),\n", + " },\n", + "}\n", + "# AIMD reference at 300 K: highest frequency in THz, and the mean absolute\n", + "# difference of each potential from it over all branches of the band path\n", + "AIMD_MAX_300K = {\n", + " \"Ca3Ir4Sn13\": 6.03,\n", + " \"AlAsPt5\": 7.79,\n", + " \"Zn3P2\": 10.09,\n", + " \"Bi4S3N2\": 17.03,\n", + " \"Er5Tl3\": 3.97,\n", + "}\n", + "MAE_300K = {\n", + " \"Ca3Ir4Sn13\": {\n", + " \"OMAT-0-medium\": 0.07,\n", + " \"MATPES-PBE-0\": 0.17,\n", + " \"MATPES-r2SCAN-0\": 0.10,\n", + " },\n", + " \"AlAsPt5\": {\"OMAT-0-medium\": 0.11, \"MATPES-PBE-0\": 0.21, \"MATPES-r2SCAN-0\": 0.18},\n", + " \"Zn3P2\": {\"OMAT-0-medium\": 0.19, \"MATPES-PBE-0\": 0.09, \"MATPES-r2SCAN-0\": 0.42},\n", + " \"Bi4S3N2\": {\"OMAT-0-medium\": 0.16, \"MATPES-PBE-0\": 0.43, \"MATPES-r2SCAN-0\": 0.17},\n", + " \"Er5Tl3\": {\"OMAT-0-medium\": 0.17, \"MATPES-PBE-0\": 0.16, \"MATPES-r2SCAN-0\": 0.12},\n", + "}\n", + "# runs with imaginary modes on the band path, and runs whose trajectory check\n", + "# was not \"stable\"\n", + "IMAGINARY = {\n", + " (\"Bi4S3N2\", \"OMAT-0-medium\"): (100, 300, 700),\n", + " (\"Bi4S3N2\", \"MATPES-PBE-0\"): (300, 700, 900),\n", + " (\"Bi4S3N2\", \"MATPES-r2SCAN-0\"): (100, 300, 500, 700, 900),\n", + " (\"Zn3P2\", \"MATPES-PBE-0\"): (900,),\n", + "}\n", + "NOT_STABLE = {\n", + " (\"Ca3Ir4Sn13\", \"OMAT-0-medium\", 100): \"shifted_or_diffusing\",\n", + " (\"Ca3Ir4Sn13\", \"MATPES-r2SCAN-0\", 100): \"shifted_or_diffusing\",\n", + " (\"Zn3P2\", \"OMAT-0-medium\", 700): \"melted\",\n", + " (\"Zn3P2\", \"OMAT-0-medium\", 900): \"melted\",\n", + " (\"Zn3P2\", \"MATPES-PBE-0\", 700): \"melted\",\n", + " (\"Zn3P2\", \"MATPES-PBE-0\", 900): \"melted\",\n", + " (\"Zn3P2\", \"MATPES-r2SCAN-0\", 700): \"melted\",\n", + " (\"Zn3P2\", \"MATPES-r2SCAN-0\", 900): \"melted\",\n", + " (\"Bi4S3N2\", \"OMAT-0-medium\", 700): \"melted\",\n", + " (\"Bi4S3N2\", \"OMAT-0-medium\", 900): \"melted\",\n", + " (\"Bi4S3N2\", \"MATPES-PBE-0\", 900): \"melted\",\n", + " (\"Bi4S3N2\", \"MATPES-r2SCAN-0\", 900): \"melted\",\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 5, figsize=(16, 3.4))\n", + "for ax, (name, by_model) in zip(axes, MAX_FREQUENCY.items(), strict=True):\n", + " for model, values in by_model.items():\n", + " ax.plot(TEMPERATURES, values, \"o-\", label=model)\n", + " ax.axhline(AIMD_MAX_300K[name], color=\"black\", ls=\"--\", lw=0.8)\n", + " ax.set_title(name)\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "axes[0].set_ylabel(\"Highest frequency (THz)\")\n", + "axes[0].legend(fontsize=8)\n", + "fig.tight_layout()\n", + "plt.show()\n", + "\n", + "pd.DataFrame(MAE_300K).T.assign(**{\"AIMD highest frequency\": pd.Series(AIMD_MAX_300K)})" + ] + }, + { + "cell_type": "markdown", + "id": "26", + "metadata": {}, + "source": [ + "The table gives the mean absolute difference from the AIMD reference at 300 K\n", + "in THz, over all branches and q-points of the band path.\n", + "\n", + "- No potential is closest to AIMD for all five materials. MACE-OMAT-0-medium is\n", + " closest for Ca3Ir4Sn13, AlAsPt5 and Bi4S3N2, within 0.07 to 0.16 THz.\n", + " MACE-MATPES-r2SCAN-0 is closest for Er5Tl3 and MACE-MATPES-PBE-0 for Zn3P2.\n", + "- MACE-MATPES-PBE-0 gives the lowest frequencies for most materials. For Bi4S3N2 its highest branches lie about\n", + " 1.4 THz below AIMD.\n", + "- Most frequencies soften with temperature. The highest frequency of Bi4S3N2\n", + " drops by 1.7 THz from 100 K to 900 K with MACE-OMAT-0-medium. Er5Tl3 barely\n", + " changes.\n", + "- The imaginary modes at 0 K are gone at every temperature for Ca3Ir4Sn13,\n", + " AlAsPt5, Zn3P2 and Er5Tl3. The one exception is Zn3P2 with MACE-MATPES-PBE-0\n", + " at 900 K, a run that the trajectory check reports as melted. Bi4S3N2 keeps imaginary modes down to -0.7 THz in\n", + " 11 of 15 runs. Its AIMD reference has a small one as well, at -0.12 THz.\n", + " Bi4S3N2 is polar, so these runs and the AIMD reference are compared without\n", + " the non-analytical correction. The force fields give no Born charges.\n", + "\n", + "The trajectory check did not report \"stable\" for 12 runs:\n", + "\n", + "- Zn3P2 and Bi4S3N2 are reported as melted at 700 K or 900 K. The Lindemann\n", + " ratio is above 0.12 there. Zn3P2 melts well above 900 K. The limit of 0.12 is\n", + " a rule of thumb, and we did not check whether these trajectories are liquid.\n", + " Treat these runs with care.\n", + "- Ca3Ir4Sn13 at 100 K is reported as shifted or diffusing with two of the\n", + " potentials. With MACE-OMAT-0-medium the mean positions of the atoms moved\n", + " 0.13 Å away from the starting structure. This is a little more than 1.5\n", + " times their vibration of 0.11 Å. At 300 K the shift is only 0.05 Å, so it\n", + " does not come from the small difference between the PBEsol and the force\n", + " field positions. In experiment, Ca3Ir4Sn13 has a structural transition near\n", + " 40 K, with soft phonons above it (arXiv:1503.08102). The shift at 100 K may\n", + " be the start of this distortion. We did not check this further." + ] + }, + { + "cell_type": "markdown", + "id": "27", + "metadata": {}, + "source": [ + "## 2. MD length and number of snapshots for KNaICl\n", + "\n", + "Two settings control how well the MD samples the temperature:\n", + "\n", + "- `md_time` sets the length of the MD in ps. The default is 8 ps, of which the\n", + " first 1 ps is left out.\n", + "- `n_snapshots` sets the number of snapshots used in the fit. The default is 50.\n", + "\n", + "We tested 4, 8 and 16 ps with 25, 50 and 100 snapshots at 300 K for KNaICl\n", + "(mp-1002081). It has 4 atoms in the primitive cell and 72 in the 3x3x2\n", + "supercell. KNaICl is polar, so it is compared with the AIMD reference without\n", + "the non-analytical correction. The highest frequency of that reference is\n", + "5.51 THz.\n", + "\n", + "The grid runs 27 workflows, so it is off by default." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "28", + "metadata": {}, + "outputs": [], + "source": [ + "RUN_GRID = False\n", + "if RUN_GRID:\n", + " mp_id, supercell = MATERIALS[\"KNaICl\"]\n", + " knaicl = get_pheasy_structure(mp_id)\n", + " for model in MODEL_FILES:\n", + " for md_time in (4, 8, 16):\n", + " for n_snapshots in (25, 50, 100):\n", + " docs[\"KNaICl\", model, md_time, n_snapshots] = run_ft(\n", + " knaicl,\n", + " supercell,\n", + " model,\n", + " f\"runs/KNaICl_{model}_{md_time}ps_{n_snapshots}\",\n", + " 300,\n", + " md_time,\n", + " n_snapshots,\n", + " )" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "29", + "metadata": {}, + "outputs": [], + "source": [ + "MD_TIMES = (4, 8, 16)\n", + "N_SNAPSHOTS = (25, 50, 100)\n", + "# by potential, rows 4, 8 and 16 ps, columns 25, 50 and 100 snapshots\n", + "MAE_GRID = { # mean absolute difference from AIMD at 300 K in THz\n", + " \"OMAT-0-medium\": (\n", + " (0.146, 0.149, 0.150),\n", + " (0.159, 0.145, 0.144),\n", + " (0.156, 0.155, 0.149),\n", + " ),\n", + " \"MATPES-PBE-0\": (\n", + " (0.138, 0.121, 0.121),\n", + " (0.124, 0.129, 0.127),\n", + " (0.127, 0.135, 0.117),\n", + " ),\n", + " \"MATPES-r2SCAN-0\": (\n", + " (0.137, 0.123, 0.123),\n", + " (0.138, 0.131, 0.128),\n", + " (0.147, 0.128, 0.128),\n", + " ),\n", + "}\n", + "MAX_GRID = { # highest frequency on the band path in THz\n", + " \"OMAT-0-medium\": ((5.63, 5.65, 5.63), (5.63, 5.73, 5.70), (5.32, 5.43, 5.44)),\n", + " \"MATPES-PBE-0\": ((5.03, 5.23, 5.26), (5.25, 5.22, 5.33), (5.12, 5.13, 5.27)),\n", + " \"MATPES-r2SCAN-0\": ((5.23, 5.40, 5.40), (5.39, 5.66, 5.56), (5.27, 5.60, 5.54)),\n", + "}\n", + "IMAGINARY_GRID = { # True if the band path has imaginary modes\n", + " \"OMAT-0-medium\": ((False, True, True), (False, False, False), (True, True, False)),\n", + " \"MATPES-PBE-0\": ((True, False, False), (True, True, True), (False, True, False)),\n", + " \"MATPES-r2SCAN-0\": (\n", + " (False, False, False),\n", + " (True, True, False),\n", + " (True, False, False),\n", + " ),\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 3, figsize=(13, 3.6))\n", + "for ax, model in zip(axes, MODEL_FILES, strict=True):\n", + " grid = np.array(MAE_GRID[model])\n", + " image = ax.imshow(grid, cmap=\"viridis\", vmin=0.11, vmax=0.16)\n", + " for i in range(3):\n", + " for j in range(3):\n", + " mark = \" *\" if IMAGINARY_GRID[model][i][j] else \"\"\n", + " ax.text(\n", + " j, i, f\"{grid[i, j]:.3f}{mark}\", ha=\"center\", va=\"center\", color=\"w\"\n", + " )\n", + " ax.set_xticks(range(3), N_SNAPSHOTS)\n", + " ax.set_yticks(range(3), [f\"{t} ps\" for t in MD_TIMES])\n", + " ax.set_xlabel(\"Number of snapshots\")\n", + " ax.set_title(model)\n", + "fig.colorbar(image, ax=axes, label=\"Mean absolute difference from AIMD (THz)\")\n", + "plt.show()\n", + "\n", + "pd.concat(\n", + " {\n", + " model: pd.DataFrame(\n", + " MAX_GRID[model], index=[f\"{t} ps\" for t in MD_TIMES], columns=N_SNAPSHOTS\n", + " )\n", + " for model in MODEL_FILES\n", + " },\n", + " axis=1,\n", + ")" + ] + }, + { + "cell_type": "markdown", + "id": "30", + "metadata": {}, + "source": [ + "In the plot, a star marks a run with imaginary modes on the band path. The\n", + "table gives the highest frequency in THz.\n", + "\n", + "- The mean absolute difference from AIMD lies between 0.12 and 0.16 THz in every\n", + " run. It shows no trend with the MD length or the number of snapshots. Each\n", + " run is one MD trajectory, so these differences are the noise of a single run.\n", + "- The highest frequency changes by up to 0.4 THz between runs, also without a\n", + " trend.\n", + "- 12 of the 27 runs have imaginary modes on the band path, down to -0.9 THz.\n", + " They sit at q-points that are not commensurate with the supercell, such as\n", + " (1/2, 1/2, 0). There the frequencies are interpolated from the fitted force\n", + " constants. The AIMD reference has no imaginary modes in the same supercell. So\n", + " they come from the noise of the fit. They appear in 5 of 9 runs with 25\n", + " snapshots, 5 of 9 with 50 and 2 of 9 with 100.\n", + "- The MD takes most of the time. With MACE-OMAT-0-medium a run took 3.8, 6.0\n", + " and 10.6 minutes for 4, 8 and 16 ps. Going from 50 to 100 snapshots added a\n", + " few seconds of force calculations and fitting.\n", + "\n", + "We also ran Bi4S3N2 and Zn3P2 at 300 K with 100 snapshots. The mean absolute\n", + "difference from AIMD changed by 0.03 THz or less. The fit of Zn3P2 did not take\n", + "longer. Bi4S3N2 kept its imaginary modes with all three potentials, so these are\n", + "unlikely to be noise of the fit.\n", + "\n", + "With a force field the force calculations cost little next to the MD, so 100\n", + "snapshots are worth using. The default stays at 50, because with VASP each\n", + "snapshot is a DFT calculation of the whole supercell. For the MD length, 4 ps\n", + "already gave the same agreement with AIMD for KNaICl. We kept the default of\n", + "8 ps for the other materials." + ] + }, + { + "cell_type": "markdown", + "id": "31", + "metadata": {}, + "source": [ + "## Known limitations\n", + "\n", + "The force constants are those of the starting volume. Thermal expansion is not\n", + "included, so the result is least reliable at high temperature.\n", + "\n", + "A machine-learned potential gives no Born charges, so the non-analytical\n", + "correction is not applied here. With VASP, the `born_maker` computes them.\n", + "\n", + "The trajectory check uses fixed limits. A Lindemann ratio above 0.12 is reported\n", + "as melting. A displacement from the reference of more than 1.5 times the\n", + "vibration around the mean positions is reported as a shift. These are rules of thumb. A warning is raised and\n", + "the fit is still done.\n", + "\n", + "Every result above comes from one MD trajectory. Section 2 shows that two runs\n", + "with different settings can differ by about 0.04 THz on average and by up to\n", + "0.4 THz in the highest frequency." + ] + } + ], + "metadata": { + "language_info": { + "name": "python" + } + }, + "nbformat": 4, + "nbformat_minor": 5 +} diff --git a/tutorials/tutorials.md b/tutorials/tutorials.md index 487c6da5e9..c530f277bc 100644 --- a/tutorials/tutorials.md +++ b/tutorials/tutorials.md @@ -19,6 +19,7 @@ hiphive_workflow force_fields/phonon_workflow grueneisen_workflow cte_workflow +finite_temperature_phonons qha_workflow torchsim_tutorial ``` From 7470fb4b645c79bdcc62ecd7dfde3f6f794eb769 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 10:07:35 -0700 Subject: [PATCH 16/43] Raise the Lindemann limit of the trajectory check to 0.15 and update the tutorial --- .../common/jobs/finite_temperature_phonons.py | 6 +- .../jobs/test_finite_temperature_phonons.py | 4 +- tutorials/finite_temperature_phonons.ipynb | 76 ++++++++++++------- 3 files changed, 55 insertions(+), 31 deletions(-) diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 7999e1add0..22a6228f41 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -62,7 +62,9 @@ # so a large displacement in the first frames means the atom order does not match. _START_LIMIT = 0.5 # Angstrom _RMS_LIMIT = 1.0 # Angstrom -_LINDEMANN_LIMIT = 0.12 +# Lindemann ratio at melting of an fcc solid, Saija et al., J. Chem. Phys. 124, +# 244504 (2006) +_LINDEMANN_LIMIT = 0.15 _SHIFT_RATIO_LIMIT = 1.5 _DRIFT_SIGMA = 3.0 _N_START_FRAMES = 10 @@ -246,7 +248,7 @@ def _assess_trajectory( - A root mean square displacement above 0.5 Angstrom in the first 10 frames means the atoms are not in the order of the reference. - - A root mean square vibration u_vib above 0.12 of the nearest-neighbor + - A root mean square vibration u_vib above 0.15 of the nearest-neighbor distance means the structure melted. - A total displacement u_ref above 1.5 times u_vib means the mean positions moved away from the reference. diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index 699bbf4a7f..d8f755dd30 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -96,8 +96,8 @@ def test_assess_trajectory(cu_supercell): assert health_moved.verdict == "stable" assert health_moved.u_ref == pytest.approx(health.u_ref) - # a vibration of 0.2 A per direction is above the Lindemann limit - frac, energies = _trajectory(cu_supercell, rng, sigma=0.2) + # a vibration of 0.25 A per direction is above the Lindemann limit + frac, energies = _trajectory(cu_supercell, rng, sigma=0.25) assert _verdict(cu_supercell, frac, energies) == "melted" # the mean positions move in the second half, with a flat energy diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 8bccb3558e..4e7f977520 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -55,8 +55,8 @@ "energy late in the run. The result is stored in the output. A warning is raised\n", "if the check fails, but the fit is still done.\n", "\n", - "The volume stays that of the starting structure, so thermal expansion is not\n", - "included. The same workflow runs with VASP as\n", + "The MD runs at constant volume (NVT), at the volume of the starting structure,\n", + "so thermal expansion is not included. The same workflow runs with VASP as\n", "`atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`.\n", "`atomate2.forcefields.flows.finite_temperature_phonons` also has two mixed\n", "versions. One runs the MD with VASP and the force calculations with a force\n", @@ -361,8 +361,12 @@ " describe. It grows with temperature, from 0.05 eV/Å at 100 K to 0.29 eV/Å at\n", " 900 K for Ca3Ir4Sn13.\n", "- The Lindemann ratio is the root mean square vibration of the atoms around\n", - " their mean positions, divided by the nearest-neighbor distance. Above 0.12 the check reports the trajectory as\n", - " melted." + " their mean positions, divided by the nearest-neighbor distance. By the\n", + " Lindemann criterion, a solid melts when this ratio reaches a fixed value\n", + " (Lindemann, Phys. Z. 11, 609 (1910); Gilvarry, Phys. Rev. 102, 308 (1956)).\n", + " The check reports the trajectory as melted above 0.15. This is the ratio at\n", + " melting of fcc solids, defined the same way (Saija et al., J. Chem. Phys. 124,\n", + " 244504 (2006))." ] }, { @@ -386,6 +390,8 @@ "metadata": {}, "outputs": [], "source": [ + "import re\n", + "\n", "import matplotlib.pyplot as plt\n", "from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine\n", "from pymatgen.phonon.dos import PhononDos\n", @@ -412,6 +418,7 @@ " positions.append(distance[branch[\"end_index\"]])\n", " names.append(end)\n", " names = [name.replace(\"\\\\Gamma\", \"Γ\").replace(\"GAMMA\", \"Γ\") for name in names]\n", + " names = [re.sub(r\"_(\\w+)\", r\"$_{\\1}$\", name) for name in names]\n", " ax.set_xticks(positions, names)\n", " ax.set_xlim(distance[0], distance[-1])\n", " ax.axhline(0, color=\"gray\", lw=0.5)\n", @@ -469,8 +476,10 @@ "\n", "The same workflow runs at five temperatures, with all three potentials and for\n", "four more materials. AlAsPt5, Zn3P2 and Er5Tl3 also have imaginary modes at 0 K.\n", - "Bi4S3N2 is polar. The function below builds and runs one workflow in its own\n", - "folder. Section 2 uses it as well.\n", + "Bi4S3N2 is polar. The Materials Project lists AlAsPt5 and Bi4S3N2 as\n", + "theoretical. They are predicted compounds with no known experimental structure.\n", + "\n", + "The function below builds and runs one workflow in its own folder. Section 2 uses it as well.\n", "\n", "The loop runs 75 workflows, so it is off by default. Set `RUN_ALL = True` to\n", "run it. Each of our runs took 6 to 36 minutes on one A100 GPU." @@ -599,7 +608,7 @@ " )\n", " axes[0].set_ylabel(\"Frequency (THz)\")\n", " axes[-1].legend(fontsize=8)\n", - " fig.suptitle(name)\n", + " fig.suptitle(name, y=1.02)\n", " plt.show()\n", "\n", "\n", @@ -688,16 +697,8 @@ "NOT_STABLE = {\n", " (\"Ca3Ir4Sn13\", \"OMAT-0-medium\", 100): \"shifted_or_diffusing\",\n", " (\"Ca3Ir4Sn13\", \"MATPES-r2SCAN-0\", 100): \"shifted_or_diffusing\",\n", - " (\"Zn3P2\", \"OMAT-0-medium\", 700): \"melted\",\n", " (\"Zn3P2\", \"OMAT-0-medium\", 900): \"melted\",\n", - " (\"Zn3P2\", \"MATPES-PBE-0\", 700): \"melted\",\n", " (\"Zn3P2\", \"MATPES-PBE-0\", 900): \"melted\",\n", - " (\"Zn3P2\", \"MATPES-r2SCAN-0\", 700): \"melted\",\n", - " (\"Zn3P2\", \"MATPES-r2SCAN-0\", 900): \"melted\",\n", - " (\"Bi4S3N2\", \"OMAT-0-medium\", 700): \"melted\",\n", - " (\"Bi4S3N2\", \"OMAT-0-medium\", 900): \"melted\",\n", - " (\"Bi4S3N2\", \"MATPES-PBE-0\", 900): \"melted\",\n", - " (\"Bi4S3N2\", \"MATPES-r2SCAN-0\", 900): \"melted\",\n", "}\n", "\n", "fig, axes = plt.subplots(1, 5, figsize=(16, 3.4))\n", @@ -708,8 +709,13 @@ " ax.set_title(name)\n", " ax.set_xlabel(\"Temperature (K)\")\n", "axes[0].set_ylabel(\"Highest frequency (THz)\")\n", - "axes[0].legend(fontsize=8)\n", "fig.tight_layout()\n", + "fig.legend(\n", + " *axes[0].get_legend_handles_labels(),\n", + " loc=\"upper center\",\n", + " ncol=3,\n", + " bbox_to_anchor=(0.5, 0),\n", + ")\n", "plt.show()\n", "\n", "pd.DataFrame(MAE_300K).T.assign(**{\"AIMD highest frequency\": pd.Series(AIMD_MAX_300K)})" @@ -738,12 +744,14 @@ " Bi4S3N2 is polar, so these runs and the AIMD reference are compared without\n", " the non-analytical correction. The force fields give no Born charges.\n", "\n", - "The trajectory check did not report \"stable\" for 12 runs:\n", + "The trajectory check did not report \"stable\" for four runs:\n", "\n", - "- Zn3P2 and Bi4S3N2 are reported as melted at 700 K or 900 K. The Lindemann\n", - " ratio is above 0.12 there. Zn3P2 melts well above 900 K. The limit of 0.12 is\n", - " a rule of thumb, and we did not check whether these trajectories are liquid.\n", - " Treat these runs with care.\n", + "- By the Lindemann criterion, Zn3P2 melts at 900 K with MACE-OMAT-0-medium and\n", + " MACE-MATPES-PBE-0. Its Lindemann ratio there is 0.165 and 0.171. With\n", + " MACE-MATPES-r2SCAN-0 it reaches 0.148 at 900 K, just below the limit of 0.15.\n", + " No other material reaches the limit up to 900 K. The highest ratio among them\n", + " is 0.136, for Bi4S3N2. Every run keeps the volume of the 0 K cell, see the\n", + " known limitations below.\n", "- Ca3Ir4Sn13 at 100 K is reported as shifted or diffusing with two of the\n", " potentials. With MACE-OMAT-0-medium the mean positions of the atoms moved\n", " 0.13 Å away from the starting structure. This is a little more than 1.5\n", @@ -769,7 +777,7 @@ "\n", "We tested 4, 8 and 16 ps with 25, 50 and 100 snapshots at 300 K for KNaICl\n", "(mp-1002081). It has 4 atoms in the primitive cell and 72 in the 3x3x2\n", - "supercell. KNaICl is polar, so it is compared with the AIMD reference without\n", + "supercell. Like AlAsPt5 and Bi4S3N2, KNaICl is a predicted compound. KNaICl is polar, so it is compared with the AIMD reference without\n", "the non-analytical correction. The highest frequency of that reference is\n", "5.51 THz.\n", "\n", @@ -890,6 +898,14 @@ " constants. The AIMD reference has no imaginary modes in the same supercell. So\n", " they come from the noise of the fit. They appear in 5 of 9 runs with 25\n", " snapshots, 5 of 9 with 50 and 2 of 9 with 100.\n", + "- We ran the whole grid a second time. The 4 and 8 ps runs gave the same\n", + " numbers to the third decimal. The 16 ps runs did not. Their highest frequency\n", + " changed by up to 0.2 THz, and imaginary modes appeared or went away in three\n", + " of them. With 100 snapshots, 2 of 9 runs had imaginary modes the first time\n", + " and 3 of 9 the second time. Runs with the same potential and MD length share\n", + " one trajectory. At 16 ps their Lindemann ratios already differed in the first\n", + " round, so the trajectory itself changed. Most likely, tiny numerical\n", + " differences on the GPU grow over a long MD run.\n", "- The MD takes most of the time. With MACE-OMAT-0-medium a run took 3.8, 6.0\n", " and 10.6 minutes for 4, 8 and 16 ps. Going from 50 to 100 snapshots added a\n", " few seconds of force calculations and fitting.\n", @@ -913,16 +929,22 @@ "source": [ "## Known limitations\n", "\n", - "The force constants are those of the starting volume. Thermal expansion is not\n", - "included, so the result is least reliable at high temperature.\n", + "The MD runs at constant volume (NVT). At every temperature it keeps the volume\n", + "of the starting structure, here the 0 K PBEsol cell. A real crystal expands as\n", + "it heats up, and the expansion changes the phonons. At high temperature, the\n", + "volume at each temperature should first be found with an NPT run, and the NVT\n", + "run done at that volume. Without this, thermal expansion is missing from the\n", + "force constants and from the trajectory check.\n", "\n", "A machine-learned potential gives no Born charges, so the non-analytical\n", "correction is not applied here. With VASP, the `born_maker` computes them.\n", "\n", - "The trajectory check uses fixed limits. A Lindemann ratio above 0.12 is reported\n", + "The trajectory check uses fixed limits. A Lindemann ratio above 0.15 is reported\n", "as melting. A displacement from the reference of more than 1.5 times the\n", - "vibration around the mean positions is reported as a shift. These are rules of thumb. A warning is raised and\n", - "the fit is still done.\n", + "vibration around the mean positions is reported as a shift. These are rules of\n", + "thumb, and the Lindemann ratio at melting differs between materials. We did not\n", + "check whether any of the trajectories reported as melted is a liquid. A warning\n", + "is raised and the fit is still done.\n", "\n", "Every result above comes from one MD trajectory. Section 2 shows that two runs\n", "with different settings can differ by about 0.04 THz on average and by up to\n", From 06b10cfb420dd6e67d577e0e6e4ae2f828fdb6f2 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 10:51:45 -0700 Subject: [PATCH 17/43] Add an optional NPT MD that includes thermal expansion in the finite-temperature phonons --- docs/user/codes/vasp.md | 9 +- .../flows/finite_temperature_phonons.py | 92 ++++++++ .../common/jobs/finite_temperature_phonons.py | 222 +++++++++++++++--- .../schemas/finite_temperature_phonons.py | 30 ++- .../flows/finite_temperature_phonons.py | 83 ++++++- .../vasp/flows/finite_temperature_phonons.py | 67 +++++- .../jobs/test_finite_temperature_phonons.py | 119 +++++++++- .../flows/test_finite_temperature_phonons.py | 39 +++ 8 files changed, 606 insertions(+), 55 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 5f3269e240..da73ce9fe1 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -412,7 +412,7 @@ The cluster space grows faster there than the number of displacements the workfl `FiniteTemperaturePhononMaker` fits effective harmonic force constants at a finite temperature, as in the temperature-dependent effective potential ([TDEP](https://doi.org/10.1103/PhysRevB.84.180301)) method. They include the anharmonic effects at that temperature, at the volume of the relaxed structure. -Thermal expansion is not included. +By default, thermal expansion is not included. The structure is relaxed first. An NVT MD run then samples the displacements at the temperature. By default, it runs for 8 ps at 300 K with a time step of 1 fs and a Nosé-Hoover thermostat. @@ -440,6 +440,13 @@ Both set ISPIN from the relaxation directory with `auto_ispin`. Each job continues from the positions and velocities of the previous one. The thermostat variables start again from zero in each job. +An NPT MD can be run first to include thermal expansion. +Set `npt_maker` to a VASP `MDMaker` with an `MDSetGenerator`, and use a larger ENCUT than for the NVT MD, since the cell changes. +The flow runs it at the temperature and at `pressure`, 0 kbar by default, with MDALGO = 3 and ISIF = 3. +Its cell is averaged over the frames after `npt_equilibration_time`, given the symmetry of the relaxed structure, and used for the NVT MD, the statics and the fit. +`fixed_cell_relax_maker` can relax the atoms in this cell, for example with ISIF = 2. +With a force field, `from_force_field_name(..., run_npt=True)` sets both makers. + The trajectory is also checked before the fit. The check looks for melting and for a move away from the reference structure. It also looks at the drift of the potential energy late in the run. diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 332332409a..70db6e1001 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -17,6 +17,7 @@ fit_finite_temperature_phonons, get_md_restart_structure, get_md_supercell, + get_npt_structure, select_md_snapshots, ) from atomate2.common.jobs.pheasy import get_supercell_size @@ -70,6 +71,14 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): give the phonon band structure and density of states. Imaginary modes are reported, not removed. + If npt_maker is set, thermal expansion is included. An NPT MD run at the + temperature and pressure first starts from the undisplaced supercell of the + relaxed structure. Its cell, averaged over the frames after + npt_equilibration_time, gives the unit cell at the temperature, see + :obj:`.get_npt_structure`. If fixed_cell_relax_maker is set, it relaxes the + atoms in this cell. The NVT MD, the phonon displacement calculations and the + fit then use this cell. + The MD maker and the phonon displacement maker are independent. Either can be a VASP or a force field maker, so the forces can come from a different level of theory than the trajectory. The residual forces of the undisplaced @@ -109,6 +118,13 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): Number of consecutive MD jobs that make up the trajectory. Each job continues from the positions and velocities of the previous one. The thermostat variables start again from zero in each job. + npt_time: float + Length of the NPT MD in ps, if there is one. + npt_equilibration_time: float + Time at the start of the NPT trajectory that is left out of the average + cell, in ps. + pressure: float + Pressure of the NPT MD in kbar. min_length: float Each lattice vector of the diagonal supercell is at least min_length long, in Angstrom. @@ -140,6 +156,13 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): born_maker: Maker | None VASP maker for the Born effective charges and the dielectric tensor, used for the non-analytical correction. None skips it. + npt_maker: Maker | None + Maker for the NPT MD. The flow sets its temperature, pressure, time + step and number of steps. None skips the NPT MD. + fixed_cell_relax_maker: Maker | None + Maker for the relaxation of the atoms in the cell from the NPT MD. It + must keep the cell. None keeps the fractional coordinates of the relaxed + structure. Only used with npt_maker. md_maker: Maker Maker for the MD. The flow sets its temperature, time step, number of steps and thermostat. @@ -156,6 +179,9 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): n_snapshots: int = 50 thermostat: Literal["nose-hoover", "langevin"] = "nose-hoover" md_runs: int = 1 + npt_time: float = 8.0 + npt_equilibration_time: float = 2.0 + pressure: float = 0.0 min_length: float = 12.0 symprec: float = SETTINGS.PHONON_SYMPREC rotational_sum_rule: Literal["BH", "H", "BHH"] | None = "BHH" @@ -168,6 +194,8 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): socket: bool = False bulk_relax_maker: Maker | None = None born_maker: Maker | None = None + npt_maker: Maker | None = None + fixed_cell_relax_maker: Maker | None = None md_maker: Maker | None = None phonon_displacement_maker: Maker | None = None @@ -219,6 +247,15 @@ def __post_init__(self) -> None: raise ValueError( f"md_runs ({self.md_runs}) is larger than the {n_steps} MD steps." ) + if self.npt_maker is not None and not ( + 0 <= self.npt_equilibration_time < self.npt_time + ): + raise ValueError( + "npt_equilibration_time must be at least zero and shorter than " + "npt_time." + ) + if self.fixed_cell_relax_maker is not None and self.npt_maker is None: + raise ValueError("fixed_cell_relax_maker is only used with npt_maker.") def get_md_steps(self) -> list[int]: """Get the number of MD steps of each MD job.""" @@ -269,6 +306,7 @@ def make( jobs: list[Job | Flow] = [] optimization_run_job_dir = optimization_run_uuid = None born_run_job_dir = born_run_uuid = None + npt_kwargs: dict = {} if self.bulk_relax_maker is not None: relax = self.bulk_relax_maker.make(structure, prev_dir=prev_dir) @@ -291,6 +329,44 @@ def make( jobs.append(supercell_job) supercell_matrix = supercell_job.output + if self.npt_maker is not None: + start_job = get_md_supercell( + structure, supercell_matrix, self.symprec, self.code + ) + n_steps = round(self.npt_time * 1000 / self.md_time_step) + npt_job = self.get_npt_maker(n_steps).make( + start_job.output, prev_dir=prev_dir + ) + npt_job.append_name(" NPT") + npt_cell_job = get_npt_structure( + npt_job.output.dir_name, + self.md_code, + structure, + supercell_matrix, + start_job.output, + self.temperature, + self.md_time_step, + self.npt_equilibration_time, + self.symprec, + ) + jobs.extend([start_job, npt_job, npt_cell_job]) + npt_kwargs = { + "npt_input_structure": structure, + "pressure": self.pressure, + "npt_time": self.npt_time, + "npt_equilibration_time": self.npt_equilibration_time, + "npt_trajectory_health": npt_cell_job.output["trajectory_health"], + "npt_uuid": npt_job.uuid, + "npt_dir": npt_job.output.dir_name, + } + structure = npt_cell_job.output["structure"] + if self.fixed_cell_relax_maker is not None: + relax = self.fixed_cell_relax_maker.make(structure, prev_dir=prev_dir) + jobs.append(relax) + npt_kwargs["fixed_cell_relax_uuid"] = relax.uuid + npt_kwargs["fixed_cell_relax_job_dir"] = relax.output.dir_name + structure = relax.output.structure + if self.born_maker is not None and (born is None or epsilon_static is None): born_job = self.born_maker.make(structure, prev_dir=prev_dir) jobs.append(born_job) @@ -367,6 +443,7 @@ def make( born=born, epsilon_static=epsilon_static, store_force_constants=self.store_force_constants, + **npt_kwargs, ) jobs.append(fit_job) return Flow(jobs, fit_job.output, name=self.name) @@ -421,6 +498,21 @@ def prev_calc_dir_argname(self) -> str | None: As this differs between codes, it is implemented by the inheriting class. """ + @abstractmethod + def get_npt_maker(self, n_steps: int) -> Maker: + """ + Get the maker of the NPT MD job, with the settings of this flow. + + Parameters + ---------- + n_steps: int + Number of MD steps. + + Returns + ------- + Maker + """ + @abstractmethod def get_md_maker(self, n_steps: int) -> Maker: """ diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 22a6228f41..9e1b2a24f4 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -22,6 +22,7 @@ from pymatgen.io.vasp import Incar, Kpoints, Poscar, Xdatcar from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine from pymatgen.phonon.dos import PhononDos +from pymatgen.symmetry.analyzer import SpacegroupAnalyzer from atomate2.common.jobs.pheasy import ( _DEFAULT_FILE_PATHS, @@ -184,11 +185,14 @@ def get_md_restart_structure( return structure -def _read_vasp_md(directory: Path) -> tuple[np.ndarray, np.ndarray, list[str], float]: - """Read the frames, energies and time step of a VASP MD run.""" +def _read_vasp_md( + directory: Path, +) -> tuple[np.ndarray, np.ndarray, np.ndarray, list[str], float]: + """Read the frames, cells, energies and time step of a VASP MD run.""" incar = Incar.from_file(zpath(str(directory / "INCAR"))) xdatcar = Xdatcar(zpath(str(directory / "XDATCAR"))) frac_coords = np.array([frame.frac_coords for frame in xdatcar.structures]) + cells = np.array([frame.lattice.matrix for frame in xdatcar.structures]) species = [str(site.specie) for site in xdatcar.structures[0]] # the free energy F of each ionic step @@ -204,20 +208,67 @@ def _read_vasp_md(directory: Path) -> tuple[np.ndarray, np.ndarray, list[str], f f"{len(energies)} MD steps in OSZICAR. XDATCAR must have a frame at " "every step, with NBLOCK = 1." ) - return frac_coords, np.array(energies), species, float(incar["POTIM"]) + return frac_coords, cells, np.array(energies), species, float(incar["POTIM"]) def _read_ase_md( directory: Path, time_step: float, skip_first: bool -) -> tuple[np.ndarray, np.ndarray, list[str], float]: - """Read the frames and energies of a force field MD run.""" +) -> tuple[np.ndarray, np.ndarray, np.ndarray, list[str], float]: + """Read the frames, cells and energies of a force field MD run.""" frames = ase_read(directory / ASE_TRAJECTORY_FILE, index=":") if skip_first: # the starting structure is the last frame of the previous MD run frames = frames[1:] frac_coords = np.array([atoms.get_scaled_positions() for atoms in frames]) + cells = np.array([atoms.cell[:] for atoms in frames]) energies = np.array([atoms.get_potential_energy() for atoms in frames]) - return frac_coords, energies, frames[0].get_chemical_symbols(), time_step + return frac_coords, cells, energies, frames[0].get_chemical_symbols(), time_step + + +def _read_md( + md_dirs: Sequence[str], md_code: str, reference: Structure, md_time_step: float +) -> tuple[np.ndarray, np.ndarray, np.ndarray, float]: + """ + Read and join the trajectories of MD runs, in order. + + For VASP, XDATCAR, OSZICAR and the POTIM of INCAR are read from each run + directory. For force fields, the ASE trajectory file is read, and + md_time_step is the time step. Returns the fractional coordinates, the cell + and the potential energy of each frame, and the time step in fs. + """ + directories = [Path(strip_hostname(md_dir)) for md_dir in md_dirs] + if len(set(directories)) != len(directories): + raise ValueError( + f"Each MD run must have its own directory, but the directories are " + f"{md_dirs}." + ) + frac_coords, cells, energies, time_steps = [], [], [], set() + for idx, directory in enumerate(directories): + if md_code == "vasp": + coords, cell, energy, species, time_step = _read_vasp_md(directory) + elif md_code == "forcefields": + coords, cell, energy, species, time_step = _read_ase_md( + directory, md_time_step, skip_first=idx > 0 + ) + else: + raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") + if species != [str(site.specie) for site in reference]: + raise ValueError( + f"The atoms of the MD in {directory} are not in the order of the " + "reference supercell." + ) + frac_coords.append(coords) + cells.append(cell) + energies.append(energy) + time_steps.add(time_step) + if len(time_steps) != 1: + raise ValueError(f"The MD runs have different time steps: {time_steps} fs.") + return ( + np.concatenate(frac_coords), + np.concatenate(cells), + np.concatenate(energies), + time_steps.pop(), + ) def _get_displacements(frac_coords: np.ndarray, reference: Structure) -> np.ndarray: @@ -343,6 +394,94 @@ def _assess_trajectory( ) +@job +def get_npt_structure( + npt_dir: str, + md_code: str, + structure: Structure, + supercell_matrix: Matrix3D, + reference: Structure, + temperature: float, + md_time_step: float, + equilibration_time: float, + symprec: float, +) -> dict: + """ + Get the unit cell at the temperature from an NPT MD run. + + The metric tensor L L^T of the supercell, with the lattice vectors as the + rows of L, is averaged over the frames after equilibration_time. Unlike the + lattice vectors, it does not change when the cell rotates. It is converted + to the metric tensor of the unit cell with the supercell matrix and averaged + over the point group of the structure, so that the cell keeps its symmetry. + The new lattice is the stretch of the lattice of the structure, without a + rotation, that has this metric tensor. The atoms keep their fractional + coordinates. The NPT trajectory is checked as in :obj:`select_md_snapshots`. + + Parameters + ---------- + npt_dir: str + Directory of the NPT MD run. + md_code: str + Code of the MD, "vasp" or "forcefields". + structure: Structure + Unit cell whose supercell the NPT MD started from. + supercell_matrix: Matrix3D + Supercell matrix. + reference: Structure + The undisplaced supercell the NPT MD started from. + temperature: float + MD temperature in K. + md_time_step: float + MD time step in fs. Only used for force field trajectories. + equilibration_time: float + Time at the start of the trajectory that is left out, in ps. + symprec: float + Symmetry precision for the point group of the structure. + + Returns + ------- + dict + The unit cell at the temperature and the check of the NPT trajectory. + """ + frac_coords, cells, energies, time_step = _read_md( + [npt_dir], md_code, reference, md_time_step + ) + n_equil = round(equilibration_time * 1000 / time_step) + if n_equil >= len(cells): + raise ValueError( + f"The NPT trajectory has {len(cells)} frames of {time_step} fs, none " + f"of them after the {equilibration_time} ps that are left out." + ) + metric = np.mean([cell @ cell.T for cell in cells[n_equil:]], axis=0) + inv_matrix = np.linalg.inv(np.array(supercell_matrix, dtype=float)) + metric = inv_matrix @ metric @ inv_matrix.T + # a rotation W of fractional coordinates leaves the metric tensor of the + # symmetric cell unchanged, W^T G W = G + analyzer = SpacegroupAnalyzer(structure, symprec=symprec) + rotations = [op.rotation_matrix for op in analyzer.get_symmetry_operations()] + metric = np.mean([rot.T @ metric @ rot for rot in rotations], axis=0) + lattice = structure.lattice.matrix + inv_lattice = np.linalg.inv(lattice) + eigvals, eigvecs = np.linalg.eigh(inv_lattice @ metric @ inv_lattice.T) + stretch = eigvecs @ np.diag(np.sqrt(eigvals)) @ eigvecs.T + npt_structure = Structure( + lattice @ stretch, + structure.species, + structure.frac_coords, + site_properties=structure.site_properties, + ) + + health = _assess_trajectory(frac_coords, energies, reference, temperature) + if not health.is_stable: + warnings.warn( + f"The NPT trajectory did not stay at the reference structure (verdict: " + f"{health.verdict}). The averaged cell may not describe it.", + stacklevel=2, + ) + return {"structure": npt_structure, "trajectory_health": health.model_dump()} + + @job(data=["structures"]) def select_md_snapshots( md_dirs: Sequence[str], @@ -390,35 +529,9 @@ def select_md_snapshots( root mean square displacement of the snapshots in Angstrom, with the displacement of the center of mass removed. The trajectory check. """ - directories = [Path(strip_hostname(md_dir)) for md_dir in md_dirs] - if len(set(directories)) != len(directories): - raise ValueError( - f"Each MD run must have its own directory, but the directories are " - f"{md_dirs}." - ) - frac_coords, energies, time_steps = [], [], set() - for idx, directory in enumerate(directories): - if md_code == "vasp": - coords, energy, species, time_step = _read_vasp_md(directory) - elif md_code == "forcefields": - coords, energy, species, time_step = _read_ase_md( - directory, md_time_step, skip_first=idx > 0 - ) - else: - raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") - if species != [str(site.specie) for site in reference]: - raise ValueError( - f"The atoms of the MD in {directory} are not in the order of the " - "reference supercell." - ) - frac_coords.append(coords) - energies.append(energy) - time_steps.add(time_step) - if len(time_steps) != 1: - raise ValueError(f"The MD runs have different time steps: {time_steps} fs.") - time_step = time_steps.pop() - all_coords = np.concatenate(frac_coords) - all_energies = np.concatenate(energies) + all_coords, _, all_energies, time_step = _read_md( + md_dirs, md_code, reference, md_time_step + ) n_frames = len(all_coords) n_equil = round(equilibration_time * 1000 / time_step) @@ -513,6 +626,15 @@ def fit_finite_temperature_phonons( optimization_run_job_dir: str | None = None, born_run_uuid: str | None = None, born_run_job_dir: str | None = None, + npt_input_structure: Structure | None = None, + pressure: float | None = None, + npt_time: float | None = None, + npt_equilibration_time: float | None = None, + npt_trajectory_health: dict | None = None, + npt_uuid: str | None = None, + npt_dir: str | None = None, + fixed_cell_relax_uuid: str | None = None, + fixed_cell_relax_job_dir: str | None = None, rotational_sum_rule: str | None = "BHH", alpha_min: int = -6, random_seed: int | None = 103, @@ -537,7 +659,8 @@ def fit_finite_temperature_phonons( Parameters ---------- structure: Structure - Relaxed unit cell. This job sorts its atoms by electronegativity. + Unit cell of the NVT MD, the relaxed unit cell or the cell from the NPT + MD. This job sorts its atoms by electronegativity. supercell_matrix: Matrix3D Diagonal supercell matrix. snapshot_data: dict @@ -580,6 +703,24 @@ def fit_finite_temperature_phonons( UUID of the Born charge calculation. born_run_job_dir: str | None Directory of the Born charge calculation. + npt_input_structure: Structure | None + Unit cell whose supercell the NPT MD started from, if there was one. + pressure: float | None + Pressure of the NPT MD in kbar. + npt_time: float | None + Length of the NPT MD in ps. + npt_equilibration_time: float | None + Time at the start of the NPT trajectory that was left out, in ps. + npt_trajectory_health: dict | None + Check of the NPT trajectory. + npt_uuid: str | None + UUID of the NPT MD job. + npt_dir: str | None + Directory of the NPT MD job. + fixed_cell_relax_uuid: str | None + UUID of the relaxation of the atoms in the cell from the NPT MD. + fixed_cell_relax_job_dir: str | None + Directory of the relaxation of the atoms in the cell from the NPT MD. rotational_sum_rule: str | None Rotational sum rule passed to pheasy with --rasr, or None for none. alpha_min: int @@ -753,6 +894,15 @@ def fit_finite_temperature_phonons( epsilon_static=epsilon.tolist() if epsilon is not None else None, md_uuids=md_uuids, md_dirs=md_dirs, + npt_input_structure=npt_input_structure, + pressure=pressure, + npt_time=npt_time, + npt_equilibration_time=npt_equilibration_time, + npt_trajectory_health=npt_trajectory_health, + npt_uuid=npt_uuid, + npt_dir=npt_dir, + fixed_cell_relax_uuid=fixed_cell_relax_uuid, + fixed_cell_relax_job_dir=fixed_cell_relax_job_dir, uuids=PhononUUIDs( optimization_run_uuid=optimization_run_uuid, displacements_uuids=displacement_data["uuids"], diff --git a/src/atomate2/common/schemas/finite_temperature_phonons.py b/src/atomate2/common/schemas/finite_temperature_phonons.py index eae1e3f6c6..e46ea52490 100644 --- a/src/atomate2/common/schemas/finite_temperature_phonons.py +++ b/src/atomate2/common/schemas/finite_temperature_phonons.py @@ -100,7 +100,9 @@ class FiniteTemperaturePhononDoc(StructureMetadata): structure: Structure | None = Field( None, - description="Relaxed unit cell, with its atoms sorted by electronegativity.", + description="Unit cell of the NVT MD and the fit, with its atoms sorted by " + "electronegativity. It is the relaxed unit cell, or the cell from the NPT MD " + "if there was one.", ) temperature: float | None = Field(None, description="MD temperature in K.") code: str | None = Field( @@ -221,6 +223,32 @@ class FiniteTemperaturePhononDoc(StructureMetadata): ) md_uuids: list[str] | None = Field(None, description="UUIDs of the MD jobs.") md_dirs: list[str] | None = Field(None, description="Directories of the MD jobs.") + npt_input_structure: Structure | None = Field( + None, + description="Unit cell whose supercell the NPT MD started from. None without " + "an NPT MD.", + ) + pressure: float | None = Field(None, description="Pressure of the NPT MD in kbar.") + npt_time: float | None = Field(None, description="Length of the NPT MD in ps.") + npt_equilibration_time: float | None = Field( + None, + description="Time at the start of the NPT trajectory left out of the " + "average cell, in ps.", + ) + npt_trajectory_health: TrajectoryHealth | None = Field( + None, description="Check of the NPT trajectory." + ) + npt_uuid: str | None = Field(None, description="UUID of the NPT MD job.") + npt_dir: str | None = Field(None, description="Directory of the NPT MD job.") + fixed_cell_relax_uuid: str | None = Field( + None, + description="UUID of the relaxation of the atoms in the cell from the NPT MD.", + ) + fixed_cell_relax_job_dir: str | None = Field( + None, + description="Directory of the relaxation of the atoms in the cell from the " + "NPT MD.", + ) uuids: PhononUUIDs | None = Field( None, description="UUIDs of the relaxation, the phonon displacement calculations " diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index 354c7494c8..32e41b3182 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -29,6 +29,8 @@ # period of about 40 time steps. With ASE's thermostat mass Q = 3 N k_B T tdamp**2, the # linearised Nose-Hoover period is close to pi * sqrt(2) * tdamp. _NOSE_HOOVER_TDAMP_STEPS = 40 / (math.pi * math.sqrt(2)) +# time constant of the barostat of the NPT MD +_BAROSTAT_PDAMP_STEPS = 1000 def _get_md_maker( @@ -44,7 +46,7 @@ def _get_md_maker( def _get_force_field_md_maker( - maker: BaseFiniteTemperaturePhononMaker, n_steps: int + maker: BaseFiniteTemperaturePhononMaker, n_steps: int, npt: bool = False ) -> ForceFieldMDMaker: """ Get the force field MD maker of one MD job of a finite-temperature flow. @@ -57,35 +59,42 @@ def _get_force_field_md_maker( The finite-temperature phonon maker. n_steps: int Number of MD steps of the job. + npt: bool + If True, get the NPT MD maker from maker.npt_maker. If False, get the + NVT MD maker from maker.md_maker. Returns ------- ForceFieldMDMaker """ - md_maker = maker.md_maker + md_maker = maker.npt_maker if npt else maker.md_maker + name = "NPT maker" if npt else "MD maker" if not isinstance(md_maker, ForceFieldMDMaker): raise TypeError( - f"The MD maker must be a ForceFieldMDMaker, not {type(md_maker).__name__}." + f"The {name} must be a ForceFieldMDMaker, not {type(md_maker).__name__}." ) if md_maker.dynamics is not None or md_maker.ase_md_kwargs: raise ValueError( - "The flow sets the thermostat. The MD maker must not set dynamics or " + f"The flow sets the thermostat. The {name} must not set dynamics or " "ase_md_kwargs." ) - if maker.thermostat == "nose-hoover": + if npt or maker.thermostat == "nose-hoover": dynamics = "nose-hoover-chain" md_kwargs = { "tdamp": _NOSE_HOOVER_TDAMP_STEPS * maker.md_time_step * units.fs, "tchain": 1, } + if npt: + md_kwargs["pdamp"] = _BAROSTAT_PDAMP_STEPS * maker.md_time_step * units.fs else: # AseMDMaker sets its default friction of 10 ps^-1 dynamics = "langevin" md_kwargs = {} return replace( md_maker, - ensemble=MDEnsemble.nvt, + ensemble=MDEnsemble.npt if npt else MDEnsemble.nvt, temperature=maker.temperature, + pressure=maker.pressure if npt else md_maker.pressure, n_steps=n_steps, time_step=maker.md_time_step, dynamics=dynamics, @@ -113,7 +122,11 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): 0 in VASP. The Langevin thermostat has the default friction of :obj:`.AseMDMaker`, 10 ps^-1. The initial velocities of the first MD job follow the Maxwell-Boltzmann distribution, seeded with random_seed, with - zero total momentum. + zero total momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover + chain thermostat and barostat that change the whole cell, whatever the + thermostat setting. Its thermostat time constant is that of the + Nose-Hoover thermostat above, and its barostat time constant is 1000 time + steps. See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. @@ -127,6 +140,12 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): born_maker: .Maker | None Maker for the Born effective charges and the dielectric tensor. It is None by default, as in the force field pheasy phonon workflow. + npt_maker: .ForceFieldMDMaker | None + Maker for the NPT MD. It must not set dynamics or ase_md_kwargs. None + skips the NPT MD. + fixed_cell_relax_maker: .ForceFieldRelaxMaker | None + Maker for the relaxation of the atoms in the cell from the NPT MD. It + must keep the cell. md_maker: .ForceFieldMDMaker Maker for the MD. It must not set dynamics or ase_md_kwargs, since the flow sets the thermostat. @@ -181,12 +200,28 @@ def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: """ return _get_force_field_md_maker(self, n_steps) + def get_npt_maker(self, n_steps: int) -> ForceFieldMDMaker: + """ + Get the force field maker of the NPT MD job. + + Parameters + ---------- + n_steps: int + Number of MD steps. + + Returns + ------- + ForceFieldMDMaker + """ + return _get_force_field_md_maker(self, n_steps, npt=True) + @classmethod def from_force_field_name( cls, force_field_name: str | MLFF | dict, calculator_kwargs: dict | None = None, relax_initial_structure: bool = True, + run_npt: bool = False, **kwargs, ) -> Self: """ @@ -204,6 +239,9 @@ def from_force_field_name( The keyword arguments to pass to the calculator. relax_initial_structure: bool = True Whether to relax the initial structure. + run_npt: bool = False + Whether to run an NPT MD with the force field first. The NVT MD then + uses its average cell, with the atoms relaxed in that cell. **kwargs Additional kwargs to pass to ForceFieldFiniteTemperaturePhononMaker. @@ -216,7 +254,20 @@ def from_force_field_name( force_field_name=force_field_name, calculator_kwargs=calculator_kwargs, ) + npt_maker: ForceFieldMDMaker | None = None + fixed_cell_relax_maker: ForceFieldRelaxMaker | None = None + if run_npt: + npt_maker = _get_md_maker(force_field_name, calculator_kwargs) + fixed_cell_relax_maker = ForceFieldRelaxMaker( + force_field_name=force_field_name, + calculator_kwargs=calculator_kwargs, + relax_cell=False, + relax_kwargs={"fmax": 1e-5}, + fix_symmetry=True, + ) kwargs.update( + npt_maker=npt_maker, + fixed_cell_relax_maker=fixed_cell_relax_maker, bulk_relax_maker=( ForceFieldRelaxMaker( force_field_name=force_field_name, @@ -353,6 +404,9 @@ class MLFFMDVaspStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) md_maker: .ForceFieldMDMaker Maker for the MD. It must not set dynamics or ase_md_kwargs, since the flow sets the thermostat. + npt_maker: .ForceFieldMDMaker | None + Maker for the NPT MD, under the same conditions as md_maker. None skips + the NPT MD. phonon_displacement_maker: .BaseVaspMaker Maker for the static calculations on the snapshots and the undisplaced supercell. @@ -379,6 +433,21 @@ def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: """ return _get_force_field_md_maker(self, n_steps) + def get_npt_maker(self, n_steps: int) -> ForceFieldMDMaker: + """ + Get the force field maker of the NPT MD job. + + Parameters + ---------- + n_steps: int + Number of MD steps. + + Returns + ------- + ForceFieldMDMaker + """ + return _get_force_field_md_maker(self, n_steps, npt=True) + @classmethod def from_force_field_name( cls, diff --git a/src/atomate2/vasp/flows/finite_temperature_phonons.py b/src/atomate2/vasp/flows/finite_temperature_phonons.py index a82e3335ba..97e89f1ac2 100644 --- a/src/atomate2/vasp/flows/finite_temperature_phonons.py +++ b/src/atomate2/vasp/flows/finite_temperature_phonons.py @@ -77,6 +77,16 @@ ) +def _check_md_incar(user_incar: dict, name: str) -> None: + """Check that an MD maker leaves the INCAR tags that the flow sets alone.""" + if tags := sorted(set(_MD_FLOW_TAGS) & set(user_incar)): + raise ValueError(f"The flow sets {tags}. Remove them from the {name}.") + if int(user_incar.get("NBLOCK", 1)) != 1: + raise ValueError( + "The MD must write every step to XDATCAR, so NBLOCK must be 1." + ) + + def _get_relax_maker() -> DoubleRelaxMaker: """Get a tight relaxation with the basis set and smearing of the statics.""" return DoubleRelaxMaker.from_relax_maker( @@ -147,6 +157,14 @@ class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): user_incar_settings must not contain IBRION, ISIF, LANGEVIN_GAMMA, MDALGO, NSW, POTIM, SMASS, TEBEG or TEEND, since the flow sets them. NBLOCK must be 1 if it is set. + npt_maker: .MDMaker | None + Maker for the NPT MD, with an :obj:`.MDSetGenerator`, under the same + conditions as md_maker. It must not set PSTRESS either. Its ENCUT should + be larger than that of the NVT MD, since the cell changes. None skips + the NPT MD. + fixed_cell_relax_maker: .Maker | None + Maker for the relaxation of the atoms in the cell from the NPT MD, for + example with ISIF = 2. phonon_displacement_maker: .BaseVaspMaker Maker for the static calculations on the snapshots and the undisplaced supercell. @@ -196,13 +214,7 @@ def get_md_maker(self, n_steps: int) -> MDMaker: "The MD maker must be a VASP MDMaker with an MDSetGenerator." ) generator = md_maker.input_set_generator - user_incar = generator.user_incar_settings - if tags := sorted(set(_MD_FLOW_TAGS) & set(user_incar)): - raise ValueError(f"The flow sets {tags}. Remove them from the MD maker.") - if int(user_incar.get("NBLOCK", 1)) != 1: - raise ValueError( - "The MD must write every step to XDATCAR, so NBLOCK must be 1." - ) + _check_md_incar(generator.user_incar_settings, "MD maker") if isinstance(generator, LangevinMDSetGenerator): if self.thermostat != "langevin": raise ValueError( @@ -223,3 +235,44 @@ def get_md_maker(self, n_steps: int) -> MDMaker: time_step=self.md_time_step, ) return replace(md_maker, input_set_generator=generator) + + def get_npt_maker(self, n_steps: int) -> MDMaker: + """ + Get the VASP maker of the NPT MD job. + + The NPT MD uses the Langevin thermostat with the Parrinello-Rahman + barostat of VASP, MDALGO = 3 with ISIF = 3, as MDSetGenerator sets them + for ensemble="npt". PSTRESS is the pressure of the flow. + + Parameters + ---------- + n_steps: int + Number of MD steps. + + Returns + ------- + MDMaker + """ + md_maker = self.npt_maker + if ( + not isinstance(md_maker, MDMaker) + or type(md_maker.input_set_generator) is not MDSetGenerator + ): + raise TypeError( + "The NPT maker must be a VASP MDMaker with an MDSetGenerator." + ) + generator = md_maker.input_set_generator + user_incar = generator.user_incar_settings + _check_md_incar(user_incar, "NPT maker") + if "PSTRESS" in user_incar: + raise ValueError("The flow sets PSTRESS. Remove it from the NPT maker.") + generator = replace( + generator, + ensemble="npt", + start_temp=self.temperature, + end_temp=self.temperature, + nsteps=n_steps, + time_step=self.md_time_step, + user_incar_settings={**user_incar, "PSTRESS": self.pressure}, + ) + return replace(md_maker, input_set_generator=generator) diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index d8f755dd30..8bc2833929 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -22,6 +22,7 @@ from pymatgen.io.ase import AseAtomsAdaptor from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure +from atomate2.ase.md import MDEnsemble from atomate2.common.jobs.finite_temperature_phonons import ( ASE_TRAJECTORY_FILE, _assess_trajectory, @@ -30,13 +31,14 @@ fit_finite_temperature_phonons, get_md_restart_structure, get_md_supercell, + get_npt_structure, select_md_snapshots, ) from atomate2.forcefields.flows.finite_temperature_phonons import ( ForceFieldFiniteTemperaturePhononMaker, _get_force_field_md_maker, ) -from atomate2.forcefields.jobs import ForceFieldStaticMaker +from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker from atomate2.forcefields.md import ForceFieldMDMaker EMT_CALCULATOR = {"@module": "ase.calculators.emt", "@callable": "EMT"} @@ -231,10 +233,12 @@ def test_select_md_snapshots_vasp(cu_supercell): ) -def _write_ase_md(directory, reference, frac, energies): +def _write_ase_md(directory, reference, frac, energies, cells=None): frames = [] - for coords, energy in zip(frac, energies, strict=True): + for idx, (coords, energy) in enumerate(zip(frac, energies, strict=True)): atoms = AseAtomsAdaptor.get_atoms(reference) + if cells is not None: + atoms.set_cell(cells[idx]) atoms.set_scaled_positions(coords) atoms.calc = SinglePointCalculator(atoms, energy=energy) frames.append(atoms) @@ -293,6 +297,39 @@ def test_select_md_snapshots_forcefields(cu_supercell): assert output["trajectory_health"]["verdict"] == "melted" +def test_get_npt_structure(cu_supercell): + unit_cell = AseAtomsAdaptor.get_structure(bulk("Cu", "fcc", a=3.61, cubic=True)) + rng = np.random.default_rng(4) + n_frames = 201 + frac = _frames(cu_supercell, n_frames, 0.05, rng) + # the cell is 2% longer in each direction, with random strains, and it + # rotates about the z axis + cells = [] + for angle in rng.uniform(0, 2 * np.pi, n_frames): + strain = np.eye(3) + rng.normal(0, 0.005, (3, 3)) + cos, sin = np.cos(angle), np.sin(angle) + rotation = np.array([[cos, -sin, 0], [sin, cos, 0], [0, 0, 1]]) + cells.append(1.02 * cu_supercell.lattice.matrix @ strain @ rotation.T) + energies = rng.normal(0, 0.01, n_frames) + _write_ase_md(Path("npt"), cu_supercell, frac, energies, cells=cells) + + args = ("forcefields", unit_cell, (2 * np.eye(3)).tolist(), cu_supercell, 300) + output = get_npt_structure.original( + str(Path("npt").resolve()), *args, 2.0, 0.02, 1e-4 + ) + structure = output["structure"] + # the cell stays cubic and keeps the orientation of the unit cell + assert np.allclose( + structure.lattice.matrix, 1.02 * unit_cell.lattice.matrix, atol=5e-3 + ) + assert structure.lattice.abc == pytest.approx([structure.lattice.a] * 3) + assert np.allclose(structure.frac_coords, unit_cell.frac_coords) + assert output["trajectory_health"]["verdict"] == "stable" + + with pytest.raises(ValueError, match="none of them after"): + get_npt_structure.original(str(Path("npt").resolve()), *args, 2.0, 1.0, 1e-4) + + def test_get_md_supercell(): """The supercell has the atom order of phonopy and the magnetic moments.""" structure = Structure( @@ -431,6 +468,14 @@ def test_rms_displacement_matches_mode_sampling(): ({"md_maker": None}, "md_maker and phonon_displacement_maker must be set"), ({"code": "aims"}, "code must be one of"), ({"md_code": None}, "md_code must be one of"), + ( + {"npt_maker": ForceFieldMDMaker(), "npt_equilibration_time": 8.0}, + "npt_equilibration_time must be", + ), + ( + {"fixed_cell_relax_maker": ForceFieldRelaxMaker()}, + "only used with npt_maker", + ), ], ) def test_maker_checks(kwargs, match): @@ -491,6 +536,35 @@ def test_force_field_md_maker(cu_supercell): ) +def test_force_field_npt_maker(cu_supercell): + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT_CALCULATOR, run_npt=True, md_time_step=2.0, pressure=10.0 + ) + npt_maker = maker.get_npt_maker(100) + assert npt_maker.ensemble == MDEnsemble.npt + assert npt_maker.dynamics == "nose-hoover-chain" + assert npt_maker.n_steps == 100 + assert npt_maker.pressure == 10.0 + # a barostat time constant of 1000 steps + assert npt_maker.ase_md_kwargs["pdamp"] / units.fs == pytest.approx(2000) + assert maker.get_md_maker(100).ensemble == MDEnsemble.nvt + # the atoms are relaxed in the cell from the NPT MD + assert not maker.fixed_cell_relax_maker.relax_cell + assert maker.fixed_cell_relax_maker.fix_symmetry + + flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) + names = [job.name for job in flow.jobs] + assert "ASE MD NPT" in names + assert "get_npt_structure" in names + + # no NPT MD by default + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(EMT_CALCULATOR) + assert maker.npt_maker is None + assert maker.fixed_cell_relax_maker is None + flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) + assert not any("NPT" in job.name for job in flow.jobs) + + def _commensurate_frequencies(phonon): matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix phonon.run_qpoints(get_commensurate_points(np.rint(matrix).astype(int))) @@ -661,3 +735,42 @@ def test_finite_temperature_phonon_maker_emt(clean_dir): freqs = _commensurate_frequencies(phonon) top = len(freqs) // 3 assert freqs[-top:].mean() == pytest.approx(freqs_0k[-top:].mean(), rel=0.15) + + +def test_finite_temperature_phonon_maker_emt_npt(clean_dir): + """Run the force field workflow with an NPT MD first, with EMT on Cu3Au.""" + structure = Structure( + Lattice.cubic(3.75), + ["Au", "Cu", "Cu", "Cu"], + [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], + ) + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT_CALCULATOR, + run_npt=True, + min_length=7.0, + npt_time=2.0, + npt_equilibration_time=0.5, + md_time=1.0, + md_time_step=2.0, + equilibration_time=0.2, + n_snapshots=10, + ) + flow = maker.make(structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + doc = responses[flow.output.uuid][1].output + + assert doc.pressure == 0.0 + assert doc.npt_time == 2.0 + assert doc.npt_equilibration_time == 0.5 + assert doc.npt_trajectory_health.verdict == "stable" + assert doc.npt_uuid is not None + assert doc.npt_dir is not None + assert doc.fixed_cell_relax_uuid is not None + # the NVT MD and the fit use the cubic cell from the NPT MD + assert doc.structure.lattice.abc == pytest.approx([doc.structure.lattice.a] * 3) + assert doc.structure.lattice.angles == pytest.approx((90, 90, 90)) + ratio = doc.structure.volume / doc.npt_input_structure.volume + assert ratio != 1 + assert ratio == pytest.approx(1, abs=0.05) + assert doc.trajectory_health.verdict == "stable" + assert not doc.has_imaginary_modes diff --git a/tests/vasp/flows/test_finite_temperature_phonons.py b/tests/vasp/flows/test_finite_temperature_phonons.py index b29e691af6..df64306ed8 100644 --- a/tests/vasp/flows/test_finite_temperature_phonons.py +++ b/tests/vasp/flows/test_finite_temperature_phonons.py @@ -223,6 +223,45 @@ def test_md_maker_checks(): FiniteTemperaturePhononMaker(md_maker=StaticMaker()).get_md_maker(10) +def test_npt_maker(si_structure, nio_supercell): + npt_maker = MDMaker( + input_set_generator=MDSetGenerator(user_incar_settings={"ENCUT": 700}) + ) + maker = FiniteTemperaturePhononMaker( + temperature=600, pressure=5.0, npt_maker=npt_maker + ) + incar = ( + maker.get_npt_maker(100) + .input_set_generator.get_input_set(nio_supercell, potcar_spec=True) + .incar + ) + assert incar["ISIF"] == 3 + assert incar["MDALGO"] == 3 + assert incar["PSTRESS"] == 5.0 + assert incar["TEBEG"] == incar["TEEND"] == 600 + assert incar["NSW"] == 100 + assert incar["ENCUT"] == 700 + flow = maker.make(si_structure) + assert any(job.name.endswith(" NPT") for job in flow.jobs) + + maker = FiniteTemperaturePhononMaker( + npt_maker=MDMaker( + input_set_generator=MDSetGenerator(user_incar_settings={"PSTRESS": 1}) + ) + ) + with pytest.raises(ValueError, match="The flow sets PSTRESS"): + maker.get_npt_maker(10) + maker = FiniteTemperaturePhononMaker( + npt_maker=MDMaker(input_set_generator=LangevinMDSetGenerator()) + ) + with pytest.raises(TypeError, match="VASP MDMaker with an MDSetGenerator"): + maker.get_npt_maker(10) + + # a force field MD gets a force field NPT MD + maker = MLFFMDVaspStaticFiniteTemperaturePhononMaker(npt_maker=ForceFieldMDMaker()) + assert maker.get_npt_maker(10).pressure == 0.0 + + def test_from_force_field_name(): maker = VaspMDMLFFStaticFiniteTemperaturePhononMaker.from_force_field_name( "MACE-MP-0", From cfa5430086a25e8ffd2a331203740069da265fa4 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 12:17:00 -0700 Subject: [PATCH 18/43] Add the NPT section to the finite-temperature phonon tutorial --- tutorials/finite_temperature_phonons.ipynb | 398 +++++++++++++++++++-- 1 file changed, 366 insertions(+), 32 deletions(-) diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 4e7f977520..77dd110a4a 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -11,9 +11,10 @@ "`ForceFieldFiniteTemperaturePhononMaker` workflow. The forces come from three\n", "MACE potentials, so no DFT is needed.\n", "\n", - "Section 1 runs five materials at 100, 300, 500, 700 and 900 K. Ca3Ir4Sn13 is\n", - "worked through step by step. Section 2 tests the length of the MD and the number\n", - "of snapshots for KNaICl.\n", + "Section 1 runs five materials at 100, 300, 500, 700 and 900 K, in the 0 K cell.\n", + "Ca3Ir4Sn13 is worked through step by step. Section 2 runs the same materials in\n", + "the cell at each temperature, found with an NPT MD. Section 3 tests the length\n", + "of the MD and the number of snapshots for KNaICl.\n", "\n", "This workflow is new. It is less tested than the other phonon workflows in\n", "atomate2, and its defaults and output may still change." @@ -39,15 +40,17 @@ "1. The structure is relaxed. The relaxation can be switched off, as done below.\n", "2. A diagonal supercell is built. Its lattice vectors are at least `min_length`\n", " long, 12 Å by default. A supercell matrix can also be given.\n", - "3. An NVT MD run of the supercell at the temperature. The defaults are 8 ps with\n", + "3. Optional, off by default: an NPT MD gives the cell at the temperature.\n", + " Section 2 explains this step.\n", + "4. An NVT MD run of the supercell at the temperature. The defaults are 8 ps with\n", " a 1 fs time step and a Nose-Hoover thermostat.\n", - "4. The first 1 ps of the MD is left out. 50 snapshots are picked, evenly spread\n", + "5. The first 1 ps of the MD is left out. 50 snapshots are picked, evenly spread\n", " over the rest of the trajectory.\n", - "5. The forces on the snapshots and on the undisplaced supercell are computed.\n", - "6. pheasy fits the second-order force constants with LASSO. The displacements\n", + "6. The forces on the snapshots and on the undisplaced supercell are computed.\n", + "7. pheasy fits the second-order force constants with LASSO. The displacements\n", " are measured from the undisplaced supercell. The forces of the undisplaced\n", " supercell are subtracted from the forces of each snapshot.\n", - "7. The band structure and the density of states (DOS) follow from the force\n", + "8. The band structure and the density of states (DOS) follow from the force\n", " constants. Imaginary modes are reported. They are not removed.\n", "\n", "The MD trajectory is also checked. The check looks for melting and for a move\n", @@ -55,8 +58,8 @@ "energy late in the run. The result is stored in the output. A warning is raised\n", "if the check fails, but the fit is still done.\n", "\n", - "The MD runs at constant volume (NVT), at the volume of the starting structure,\n", - "so thermal expansion is not included. The same workflow runs with VASP as\n", + "Without the NPT step, the MD runs at constant volume (NVT), at the volume of\n", + "the starting structure, so thermal expansion is not included. The same workflow runs with VASP as\n", "`atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`.\n", "`atomate2.forcefields.flows.finite_temperature_phonons` also has two mixed\n", "versions. One runs the MD with VASP and the force calculations with a force\n", @@ -355,7 +358,7 @@ "\n", "- `has_imaginary_modes` checks the whole band path. `min_frequency` only covers\n", " the q-points commensurate with the supercell. The fit sets the frequencies at\n", - " these points directly. Everywhere else they are interpolated. Section 2 shows\n", + " these points directly. Everywhere else they are interpolated. Section 3 shows\n", " why the difference matters.\n", "- The force RMSE is the part of the forces that the force constants do not\n", " describe. It grows with temperature, from 0.05 eV/Å at 100 K to 0.29 eV/Å at\n", @@ -479,7 +482,8 @@ "Bi4S3N2 is polar. The Materials Project lists AlAsPt5 and Bi4S3N2 as\n", "theoretical. They are predicted compounds with no known experimental structure.\n", "\n", - "The function below builds and runs one workflow in its own folder. Section 2 uses it as well.\n", + "The function below builds and runs one workflow in its own folder. Sections 2\n", + "and 3 use it as well.\n", "\n", "The loop runs 75 workflows, so it is off by default. Set `RUN_ALL = True` to\n", "run it. Each of our runs took 6 to 36 minutes on one A100 GPU." @@ -516,12 +520,15 @@ " temperature: float,\n", " md_time: float = 8.0,\n", " n_snapshots: int = 50,\n", + " relax: bool = False,\n", + " run_npt: bool = False,\n", ") -> FiniteTemperaturePhononDoc:\n", " \"\"\"Run the finite-temperature phonon workflow and return its output.\"\"\"\n", " maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(\n", " \"MACE-MP-0\",\n", " calculator_kwargs=calc_kwargs(model),\n", - " relax_initial_structure=False,\n", + " relax_initial_structure=relax,\n", + " run_npt=run_npt,\n", " temperature=temperature,\n", " md_time=md_time,\n", " n_snapshots=n_snapshots,\n", @@ -750,16 +757,16 @@ " MACE-MATPES-PBE-0. Its Lindemann ratio there is 0.165 and 0.171. With\n", " MACE-MATPES-r2SCAN-0 it reaches 0.148 at 900 K, just below the limit of 0.15.\n", " No other material reaches the limit up to 900 K. The highest ratio among them\n", - " is 0.136, for Bi4S3N2. Every run keeps the volume of the 0 K cell, see the\n", - " known limitations below.\n", + " is 0.136, for Bi4S3N2. Every run keeps the volume of the 0 K cell. Section 2\n", + " adds thermal expansion.\n", "- Ca3Ir4Sn13 at 100 K is reported as shifted or diffusing with two of the\n", " potentials. With MACE-OMAT-0-medium the mean positions of the atoms moved\n", " 0.13 Å away from the starting structure. This is a little more than 1.5\n", - " times their vibration of 0.11 Å. At 300 K the shift is only 0.05 Å, so it\n", - " does not come from the small difference between the PBEsol and the force\n", - " field positions. In experiment, Ca3Ir4Sn13 has a structural transition near\n", - " 40 K, with soft phonons above it (arXiv:1503.08102). The shift at 100 K may\n", - " be the start of this distortion. We did not check this further." + " times their vibration of 0.11 Å. At 300 K the shift is only 0.05 Å. In\n", + " Section 2 the force field first relaxes the cell and the atoms, and the runs\n", + " at 100 K are stable. So the shift comes from running the force field in a\n", + " cell, and with positions, that are not its own. We did not check which\n", + " distortion the atoms move to." ] }, { @@ -767,7 +774,335 @@ "id": "27", "metadata": {}, "source": [ - "## 2. MD length and number of snapshots for KNaICl\n", + "## 2. Thermal expansion with an NPT MD\n", + "\n", + "In Section 1 every MD ran in the PBEsol cell at 0 K. Two things change this\n", + "cell. Each force field has its own 0 K cell, a little different from the PBEsol\n", + "one. And the crystal expands as it heats up. With `run_npt=True` the workflow\n", + "includes both:\n", + "\n", + "1. The force field relaxes the structure. Keep the default\n", + " `relax_initial_structure=True`, so that the NPT MD starts from the force\n", + " field's own 0 K cell.\n", + "2. An NPT MD of the supercell runs at the temperature and at `pressure`, 0 kbar\n", + " by default. It runs for `npt_time`, 8 ps by default, with the same\n", + " thermostat as the NVT MD and a Martyna-Tobias-Klein barostat.\n", + "3. The cell is averaged over the NPT MD after `npt_equilibration_time`, 2 ps by\n", + " default. The average keeps the symmetry of the structure. The atoms keep\n", + " their fractional coordinates and are then relaxed in the new cell, with the\n", + " cell fixed.\n", + "4. The NVT MD, the snapshots, the fit and the trajectory check follow as in\n", + " Section 1, in the new cell. The relaxed structure in the new cell is the\n", + " undisplaced supercell of the fit.\n", + "\n", + "The NPT trajectory is checked like the NVT one, and the result is stored as\n", + "`npt_trajectory_health`. `structure` holds the cell of the NVT MD and\n", + "`npt_input_structure` the cell that the NPT MD started from.\n", + "\n", + "We run Ca3Ir4Sn13 at 900 K with MACE-OMAT-0-medium." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "28", + "metadata": {}, + "outputs": [], + "source": [ + "maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(\n", + " \"MACE-MP-0\",\n", + " calculator_kwargs=calc_kwargs(\"OMAT-0-medium\"),\n", + " run_npt=True,\n", + " temperature=900,\n", + ")\n", + "flow = maker.make(structure, supercell_matrix=[[2, 0, 0], [0, 2, 0], [0, 0, 2]])\n", + "responses = run_locally(\n", + " flow,\n", + " store=JobStore(MemoryStore(), additional_stores={\"data\": MemoryStore()}),\n", + " create_folders=True,\n", + " ensure_success=True,\n", + ")\n", + "doc_npt = responses[flow.output.uuid][1].output\n", + "{\n", + " \"lattice at 0 K in A\": doc_npt.npt_input_structure.lattice.abc,\n", + " \"lattice at 900 K in A\": doc_npt.structure.lattice.abc,\n", + " \"volume ratio\": doc_npt.structure.volume / doc_npt.npt_input_structure.volume,\n", + " \"NPT trajectory check\": doc_npt.npt_trajectory_health.verdict,\n", + " \"highest frequency in THz\": float(np.max(doc_npt.phonon_bandstructure.bands)),\n", + " \"imaginary modes on the band path\": doc_npt.has_imaginary_modes,\n", + " \"trajectory check\": doc_npt.trajectory_health.verdict,\n", + "}" + ] + }, + { + "cell_type": "markdown", + "id": "29", + "metadata": {}, + "source": [ + "Our run took 20 minutes. The NPT MD and the NVT MD took about 8 minutes each\n", + "and the fit 2 minutes. The 0 K cell of MACE-OMAT-0-medium has a lattice\n", + "parameter of 9.825 Å, and its volume is 3.8% larger than that of the PBEsol\n", + "cell. At 900 K the lattice parameter is 9.964 Å, 4.3% more volume. Both\n", + "trajectories were stable. The highest frequency is 4.95 THz, against 5.83 THz\n", + "in the PBEsol cell in Section 1." + ] + }, + { + "cell_type": "markdown", + "id": "30", + "metadata": {}, + "source": [ + "## The other temperatures, potentials and materials\n", + "\n", + "We ran all 75 settings of Section 1 again with `run_npt=True`. To tell the two\n", + "effects apart, we also ran them with the relaxation but without the NPT MD,\n", + "that is in the force field's own 0 K cell. `run_ft` takes both options. The two\n", + "loops run 150 workflows, so they are off by default. Each of our runs took 6 to\n", + "38 minutes on one A100 GPU." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "31", + "metadata": {}, + "outputs": [], + "source": [ + "RUN_NPT = False\n", + "if RUN_NPT:\n", + " for name in (\"Ca3Ir4Sn13\", \"AlAsPt5\", \"Zn3P2\", \"Bi4S3N2\", \"Er5Tl3\"):\n", + " mp_id, supercell = MATERIALS[name]\n", + " unit_cell = get_pheasy_structure(mp_id)\n", + " for model in MODEL_FILES:\n", + " for temperature in TEMPERATURES:\n", + " for label, run_npt in ((\"relaxed\", False), (\"npt\", True)):\n", + " docs[name, model, temperature, label] = run_ft(\n", + " unit_cell,\n", + " supercell,\n", + " model,\n", + " f\"runs/{name}_{model}_{temperature}K_{label}\",\n", + " temperature,\n", + " relax=True,\n", + " run_npt=run_npt,\n", + " )" + ] + }, + { + "cell_type": "markdown", + "id": "32", + "metadata": {}, + "source": [ + "## Our results\n", + "\n", + "The next cell holds the results of our runs. The first plot gives the volume\n", + "relative to the PBEsol cell. The point at 0 K is the force field's relaxed cell.\n", + "The second plot gives the highest frequency for each potential in three cells:\n", + "the PBEsol cell of Section 1, the force field's 0 K cell, and the cell from the\n", + "NPT MD." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "33", + "metadata": {}, + "outputs": [], + "source": [ + "# volume relative to the PBEsol cell: the force field's relaxed 0 K cell, then\n", + "# the NPT cell at 100, 300, 500, 700 and 900 K\n", + "VOLUME = {\n", + " \"Ca3Ir4Sn13\": {\n", + " \"OMAT-0-medium\": (1.0382, 1.0420, 1.0517, 1.0612, 1.0716, 1.0828),\n", + " \"MATPES-PBE-0\": (1.0432, 1.0475, 1.0568, 1.0665, 1.0774, 1.0890),\n", + " \"MATPES-r2SCAN-0\": (1.0192, 1.0227, 1.0311, 1.0398, 1.0491, 1.0591),\n", + " },\n", + " \"AlAsPt5\": {\n", + " \"OMAT-0-medium\": (1.0341, 1.0382, 1.0463, 1.0551, 1.0642, 1.0744),\n", + " \"MATPES-PBE-0\": (1.0175, 1.0229, 1.0313, 1.0400, 1.0501, 1.0501),\n", + " \"MATPES-r2SCAN-0\": (1.0021, 1.0061, 1.0133, 1.0210, 1.0302, 1.0392),\n", + " },\n", + " \"Zn3P2\": {\n", + " \"OMAT-0-medium\": (1.0533, 1.0585, 1.0681, 1.0780, 1.0884, 1.1012),\n", + " \"MATPES-PBE-0\": (1.0510, 1.0551, 1.0636, 1.0723, 1.0813, 1.0934),\n", + " \"MATPES-r2SCAN-0\": (1.0087, 1.0125, 1.0211, 1.0301, 1.0387, 1.0491),\n", + " },\n", + " \"Bi4S3N2\": {\n", + " \"OMAT-0-medium\": (1.1075, 1.1153, 1.1269, 1.1424, 1.1515, 1.1741),\n", + " \"MATPES-PBE-0\": (1.0457, 1.0594, 1.0764, 1.0967, 1.1515, 1.1625),\n", + " \"MATPES-r2SCAN-0\": (1.0292, 1.0381, 1.0502, 1.0656, 1.0807, 1.0861),\n", + " },\n", + " \"Er5Tl3\": {\n", + " \"OMAT-0-medium\": (1.0291, 1.0356, 1.0465, 1.0573, 1.0684, 1.0801),\n", + " \"MATPES-PBE-0\": (1.1224, 1.1283, 1.1431, 1.1589, 1.1744, 1.1939),\n", + " \"MATPES-r2SCAN-0\": (1.0646, 1.0697, 1.0806, 1.0925, 1.1034, 1.1164),\n", + " },\n", + "}\n", + "# highest frequency on the band path in THz, at 100, 300, 500, 700 and 900 K,\n", + "# in the force field's relaxed 0 K cell\n", + "MAX_RELAXED = {\n", + " \"Ca3Ir4Sn13\": {\n", + " \"OMAT-0-medium\": (5.57, 5.55, 5.51, 5.45, 5.37),\n", + " \"MATPES-PBE-0\": (5.38, 5.32, 5.25, 5.20, 5.14),\n", + " \"MATPES-r2SCAN-0\": (5.75, 5.74, 5.68, 5.59, 5.56),\n", + " },\n", + " \"AlAsPt5\": {\n", + " \"OMAT-0-medium\": (6.98, 7.07, 7.08, 7.20, 7.21),\n", + " \"MATPES-PBE-0\": (7.15, 7.30, 7.16, 7.04, 8.46),\n", + " \"MATPES-r2SCAN-0\": (7.52, 7.52, 7.49, 7.52, 7.44),\n", + " },\n", + " \"Zn3P2\": {\n", + " \"OMAT-0-medium\": (10.37, 9.96, 9.74, 9.18, 8.45),\n", + " \"MATPES-PBE-0\": (9.97, 9.65, 9.51, 8.96, 7.97),\n", + " \"MATPES-r2SCAN-0\": (11.14, 10.85, 10.62, 10.18, 9.94),\n", + " },\n", + " \"Bi4S3N2\": {\n", + " \"OMAT-0-medium\": (16.73, 15.92, 15.19, 14.78, 14.15),\n", + " \"MATPES-PBE-0\": (15.48, 15.44, 14.61, 14.41, 14.09),\n", + " \"MATPES-r2SCAN-0\": (17.23, 16.61, 16.17, 16.08, 14.72),\n", + " },\n", + " \"Er5Tl3\": {\n", + " \"OMAT-0-medium\": (4.08, 4.00, 3.94, 3.96, 4.02),\n", + " \"MATPES-PBE-0\": (3.67, 3.61, 3.57, 3.52, 3.52),\n", + " \"MATPES-r2SCAN-0\": (3.83, 3.83, 3.72, 3.68, 3.69),\n", + " },\n", + "}\n", + "# the same in the NPT cell\n", + "MAX_NPT = {\n", + " \"Ca3Ir4Sn13\": {\n", + " \"OMAT-0-medium\": (5.50, 5.44, 5.25, 5.12, 4.95),\n", + " \"MATPES-PBE-0\": (5.32, 5.16, 5.02, 4.84, 4.71),\n", + " \"MATPES-r2SCAN-0\": (5.68, 5.65, 5.45, 5.24, 5.10),\n", + " },\n", + " \"AlAsPt5\": {\n", + " \"OMAT-0-medium\": (6.92, 6.95, 6.65, 6.75, 6.60),\n", + " \"MATPES-PBE-0\": (7.15, 7.13, 7.02, 6.75, 6.55),\n", + " \"MATPES-r2SCAN-0\": (7.42, 7.27, 6.97, 6.90, 6.89),\n", + " },\n", + " \"Zn3P2\": {\n", + " \"OMAT-0-medium\": (10.20, 9.99, 9.52, 8.93, 8.26),\n", + " \"MATPES-PBE-0\": (9.90, 9.53, 9.15, 8.74, 7.85),\n", + " \"MATPES-r2SCAN-0\": (11.11, 10.63, 10.45, 9.95, 9.53),\n", + " },\n", + " \"Bi4S3N2\": {\n", + " \"OMAT-0-medium\": (16.61, 15.66, 14.93, 14.28, 14.05),\n", + " \"MATPES-PBE-0\": (15.26, 15.19, 14.34, 13.64, 12.86),\n", + " \"MATPES-r2SCAN-0\": (17.18, 16.15, 15.71, 15.17, 14.13),\n", + " },\n", + " \"Er5Tl3\": {\n", + " \"OMAT-0-medium\": (4.04, 3.88, 3.83, 3.72, 3.72),\n", + " \"MATPES-PBE-0\": (3.65, 3.55, 3.48, 3.34, 3.13),\n", + " \"MATPES-r2SCAN-0\": (3.75, 3.67, 3.63, 3.50, 3.44),\n", + " },\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 5, figsize=(16, 3.4))\n", + "for ax, (name, by_model) in zip(axes, VOLUME.items(), strict=True):\n", + " for model, values in by_model.items():\n", + " ax.plot((0, *TEMPERATURES), values, \"o-\", label=model)\n", + " ax.axhline(1, color=\"black\", ls=\"--\", lw=0.8)\n", + " ax.set_title(name)\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "axes[0].set_ylabel(\"Volume / PBEsol volume\")\n", + "fig.tight_layout()\n", + "fig.legend(\n", + " *axes[0].get_legend_handles_labels(),\n", + " loc=\"upper center\",\n", + " ncol=3,\n", + " bbox_to_anchor=(0.5, 0),\n", + ")\n", + "plt.show()\n", + "\n", + "fig, axes = plt.subplots(3, 5, figsize=(16, 8.5), sharex=True)\n", + "for col, name in enumerate(VOLUME):\n", + " for row, model in enumerate(MODEL_FILES):\n", + " ax = axes[row, col]\n", + " for label, values, style in (\n", + " (\"PBEsol cell\", MAX_FREQUENCY, \"o-\"),\n", + " (\"relaxed 0 K cell\", MAX_RELAXED, \"s--\"),\n", + " (\"NPT cell\", MAX_NPT, \"^:\"),\n", + " ):\n", + " ax.plot(TEMPERATURES, values[name][model], style, label=label)\n", + " if row == 0:\n", + " ax.set_title(name)\n", + " if col == 0:\n", + " ax.set_ylabel(f\"{model}\\nHighest frequency (THz)\")\n", + " if row == 2:\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "fig.tight_layout()\n", + "fig.legend(\n", + " *axes[0, 0].get_legend_handles_labels(),\n", + " loc=\"upper center\",\n", + " ncol=3,\n", + " bbox_to_anchor=(0.5, 0),\n", + ")\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "34", + "metadata": {}, + "source": [ + "We do not compare these runs with the AIMD reference. It used the PBEsol cell\n", + "at every temperature.\n", + "\n", + "- The 0 K cells of the force fields are larger than the PBEsol cell, by up to\n", + " 12% in volume. MACE-OMAT-0-medium and MACE-MATPES-PBE-0 are trained on PBE\n", + " data, and PBE gives larger cells than PBEsol. MACE-MATPES-r2SCAN-0 gives the\n", + " cell closest to PBEsol for four of the five materials. For AlAsPt5 the two\n", + " differ by 0.2%.\n", + "- From 0 K to 900 K the volume grows by 3 to 6.5%. Bi4S3N2 with\n", + " MACE-MATPES-PBE-0 is the exception, with 11%.\n", + "- The larger 0 K cell alone lowers the frequencies. At 300 K the highest\n", + " frequency of Ca3Ir4Sn13 drops from 5.97 THz in the PBEsol cell to 5.55 THz\n", + " in the cell of MACE-OMAT-0-medium. With MACE-MATPES-PBE-0 the 0 K cell of Er5Tl3 is 12% larger, and its\n", + " highest frequency at 300 K drops from 4.07 to 3.61 THz. With\n", + " MACE-MATPES-r2SCAN-0 the cell of Zn3P2 grows by less than 1%, and its highest\n", + " frequency at 300 K stays at 10.85 THz.\n", + "- Thermal expansion lowers the frequencies further. At 100 K the NPT cell\n", + " changes the highest frequency by about 0.2 THz or less. At 900 K it lowers\n", + " it by 0.1 to 0.6 THz in most runs.\n", + "- At constant volume a frequency can also rise with temperature. In the 0 K\n", + " cell, the highest frequency of AlAsPt5 with MACE-OMAT-0-medium rises from\n", + " 6.98 THz at 100 K to 7.21 THz at 900 K. In the NPT cell it falls from 6.92 to\n", + " 6.60 THz.\n", + "\n", + "The trajectory check did not report \"stable\" for these runs:\n", + "\n", + "- Zn3P2 at 900 K melts with all three potentials, in the NPT MD and in the NVT\n", + " MD that follows. With MACE-MATPES-r2SCAN-0, its Lindemann ratio in Section 1\n", + " stayed just below the limit, at 0.148. In the NPT cell it is 0.153.\n", + "- Bi4S3N2 melts in the larger cells. In the PBEsol cell of Section 1 none of\n", + " its runs melted. With MACE-OMAT-0-medium the NVT MD is reported as melted\n", + " from 700 K, in the 0 K cell and in the NPT cell. With MACE-MATPES-PBE-0 it\n", + " melts at 900 K in both cells. Its NPT MD is also reported as melted at 500 K\n", + " and as shifted at 700 K, and its volume jumps by 5% between these two\n", + " temperatures. With MACE-MATPES-r2SCAN-0 it melts at 900 K in the NPT cell,\n", + " just above the limit.\n", + "- AlAsPt5 at 900 K with MACE-MATPES-PBE-0 is reported as shifted, in the NVT MD\n", + " in the 0 K cell and in the NPT MD. In the 0 K cell its highest frequency\n", + " jumps to 8.46 THz. In the NPT MD its volume does not grow from 700 to 900 K.\n", + " The atoms move away from the starting structure, so the phonons of these two\n", + " runs do not describe it.\n", + "- Ca3Ir4Sn13 at 100 K is stable in both cells, unlike in Section 1.\n", + "\n", + "Bi4S3N2 has imaginary modes on the band path in all 30 runs. Ca3Ir4Sn13 with\n", + "MACE-MATPES-r2SCAN-0 at 100 K has small ones in both cells, and Er5Tl3 with the\n", + "same potential at 100 K in the 0 K cell. So does the run of Zn3P2 with\n", + "MACE-OMAT-0-medium at 900 K in the 0 K cell, which melted.\n", + "\n", + "A run with the NPT MD took 11 to 38 minutes, against 6 to 30 minutes in the\n", + "0 K cell. To compare a force field with DFT phonons in a given cell, run in\n", + "that cell, as in Section 1. To predict the phonons at a temperature with the\n", + "force field alone, use `run_npt=True`." + ] + }, + { + "cell_type": "markdown", + "id": "35", + "metadata": {}, + "source": [ + "## 3. MD length and number of snapshots for KNaICl\n", "\n", "Two settings control how well the MD samples the temperature:\n", "\n", @@ -787,7 +1122,7 @@ { "cell_type": "code", "execution_count": null, - "id": "28", + "id": "36", "metadata": {}, "outputs": [], "source": [ @@ -812,7 +1147,7 @@ { "cell_type": "code", "execution_count": null, - "id": "29", + "id": "37", "metadata": {}, "outputs": [], "source": [ @@ -881,7 +1216,7 @@ }, { "cell_type": "markdown", - "id": "30", + "id": "38", "metadata": {}, "source": [ "In the plot, a star marks a run with imaginary modes on the band path. The\n", @@ -924,17 +1259,16 @@ }, { "cell_type": "markdown", - "id": "31", + "id": "39", "metadata": {}, "source": [ "## Known limitations\n", "\n", - "The MD runs at constant volume (NVT). At every temperature it keeps the volume\n", - "of the starting structure, here the 0 K PBEsol cell. A real crystal expands as\n", - "it heats up, and the expansion changes the phonons. At high temperature, the\n", - "volume at each temperature should first be found with an NPT run, and the NVT\n", - "run done at that volume. Without this, thermal expansion is missing from the\n", - "force constants and from the trajectory check.\n", + "By default the MD runs at constant volume (NVT). At every temperature it keeps\n", + "the volume of the starting structure, as in Section 1. A real crystal expands as\n", + "it heats up, and the expansion changes the phonons. At high temperature, use\n", + "`run_npt=True` as in Section 2. The NPT cell is the average over one MD run, so\n", + "it carries the noise of that run.\n", "\n", "A machine-learned potential gives no Born charges, so the non-analytical\n", "correction is not applied here. With VASP, the `born_maker` computes them.\n", @@ -946,7 +1280,7 @@ "check whether any of the trajectories reported as melted is a liquid. A warning\n", "is raised and the fit is still done.\n", "\n", - "Every result above comes from one MD trajectory. Section 2 shows that two runs\n", + "Every result above comes from one MD trajectory. Section 3 shows that two runs\n", "with different settings can differ by about 0.04 THz on average and by up to\n", "0.4 THz in the highest frequency." ] From d0cb4bc5baccd3ae45f1a775134b439a1a9c75b7 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 23:10:10 -0700 Subject: [PATCH 19/43] Use a Langevin thermostat for the NVT MD --- docs/user/codes/vasp.md | 42 +- .../flows/finite_temperature_phonons.py | 81 ++-- .../common/jobs/finite_temperature_phonons.py | 149 +++--- src/atomate2/common/jobs/pheasy.py | 6 +- .../schemas/finite_temperature_phonons.py | 21 +- .../flows/finite_temperature_phonons.py | 25 +- .../vasp/flows/finite_temperature_phonons.py | 41 +- src/atomate2/vasp/sets/core.py | 7 +- .../jobs/test_finite_temperature_phonons.py | 337 ++----------- .../flows/test_finite_temperature_phonons.py | 238 +++++++++ .../flows/test_finite_temperature_phonons.py | 11 +- tutorials/finite_temperature_phonons.ipynb | 454 ++++++++++-------- 12 files changed, 702 insertions(+), 710 deletions(-) create mode 100644 tests/forcefields/flows/test_finite_temperature_phonons.py diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index da73ce9fe1..da6fae4fe6 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -415,14 +415,19 @@ They include the anharmonic effects at that temperature, at the volume of the re By default, thermal expansion is not included. The structure is relaxed first. An NVT MD run then samples the displacements at the temperature. -By default, it runs for 8 ps at 300 K with a time step of 1 fs and a Nosé-Hoover thermostat. +By default, it runs for 8 ps at 300 K with a time step of 1 fs and a Langevin thermostat. The first 1 ps is left out, and 50 snapshots are picked evenly spread over the rest. Static calculations give the forces on the snapshots and on the undisplaced supercell. -The displacements are measured from the relaxed positions. +The displacements are measured from the undisplaced supercell. Pheasy then fits the second-order force constants to them with LASSO. As in the pheasy phonon workflow, a `DielectricMaker` computes the Born charges and the dielectric tensor for the non-analytical correction. It needs the `pheasy` extra, like the pheasy phonon workflow above. +```{warning} +This workflow is new and has not been tested widely. +It might still change in future versions. +``` + ```python from atomate2.vasp.flows.finite_temperature_phonons import ( FiniteTemperaturePhononMaker, @@ -431,6 +436,12 @@ from atomate2.vasp.flows.finite_temperature_phonons import ( flow = FiniteTemperaturePhononMaker(temperature=300).make(structure) ``` +The fit only uses the positions of the MD, not its dynamics. +What matters is that the MD samples the canonical ensemble. +A Langevin thermostat does this for every mode ([Bussi and Parrinello](https://doi.org/10.1103/PhysRevE.75.056707)). +A Nosé-Hoover thermostat can leave nearly harmonic modes out of equilibrium ([Legoll et al.](https://doi.org/10.1007/s00205-006-0029-1)), most of all at low temperature. +`thermostat="nose-hoover"` switches to it, but this is not recommended. + The MD uses looser settings than the statics, for example ENCUT = 500 eV instead of 600 eV. Only the forces of the statics enter the fit. The relaxation, the MD and the statics use the same functional, +U, smearing and k-point settings. @@ -439,18 +450,20 @@ Both set ISPIN from the relaxation directory with `auto_ispin`. `md_runs` splits the MD into consecutive jobs, for example to stay within the walltime of a queue. Each job continues from the positions and velocities of the previous one. The thermostat variables start again from zero in each job. +The MD files are read by the job that picks the snapshots, so the MD run directories must be on a file system that this job can read. An NPT MD can be run first to include thermal expansion. Set `npt_maker` to a VASP `MDMaker` with an `MDSetGenerator`, and use a larger ENCUT than for the NVT MD, since the cell changes. The flow runs it at the temperature and at `pressure`, 0 kbar by default, with MDALGO = 3 and ISIF = 3. -Its cell is averaged over the frames after `npt_equilibration_time`, given the symmetry of the relaxed structure, and used for the NVT MD, the statics and the fit. +VASP only runs NPT MD with its Langevin thermostat. +The cell is averaged over the frames after `npt_equilibration_time`, given the symmetry of the relaxed structure, and used for the NVT MD, the statics and the fit. `fixed_cell_relax_maker` can relax the atoms in this cell, for example with ISIF = 2. -With a force field, `from_force_field_name(..., run_npt=True)` sets both makers. The trajectory is also checked before the fit. The check looks for melting and for a move away from the reference structure. It also looks at the drift of the potential energy late in the run. The result is stored in `trajectory_health` of the output `FiniteTemperaturePhononDoc`, and a warning is raised when the check fails. +The limits of the check are rules of thumb, except for the Lindemann ratio of 0.15 at melting ([Saija et al.](https://doi.org/10.1063/1.2208357)). Imaginary modes are counted at the q-points commensurate with the supercell. They are reported and not removed. @@ -462,6 +475,27 @@ Three more makers are in `atomate2.forcefields.flows.finite_temperature_phonons` Each has a `from_force_field_name` method to choose the force field. They need the package of the force field, for example `mace-torch` for MACE. All of them use the same fit. +A force field NPT MD uses ASE's `MTKNPT`, a Nosé-Hoover chain thermostat with the barostat of [Martyna et al.](https://doi.org/10.1063/1.467468). + +```python +from atomate2.forcefields.flows.finite_temperature_phonons import ( + ForceFieldFiniteTemperaturePhononMaker, +) + +maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + "MACE-MP-0", temperature=600, run_npt=True +) +flow = maker.make(structure) +``` + +`run_npt=True` sets the NPT MD and the relaxation of the atoms in its cell. + +Known limitations: + +- pheasy needs a diagonal supercell matrix. +- The MD is classical, so there is no zero-point motion. +- Each result comes from one MD trajectory, so it carries the noise of that trajectory. +- With a force field MD and VASP statics, the trajectory and the forces come from different potential energy surfaces. ### Grüneisen parameter workflow diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 70db6e1001..27507812cd 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -2,7 +2,6 @@ from __future__ import annotations -import numbers from abc import ABC, abstractmethod from dataclasses import dataclass from enum import Enum @@ -31,8 +30,6 @@ from pymatgen.core import Structure SUPPORTED_CODES = frozenset(("vasp", "forcefields")) -_THERMOSTATS = ("nose-hoover", "langevin") -_ROTATIONAL_SUM_RULES = ("BH", "H", "BHH") def _get_force_field(maker: Maker, code: str) -> tuple[str | None, dict | None]: @@ -53,6 +50,18 @@ def _get_force_field(maker: Maker, code: str) -> tuple[str | None, dict | None]: Doi("10.1103/PhysRevB.84.180301"), description="Effective harmonic force constants fitted to MD, as in TDEP.", ) +@due.dcite( + Doi("10.1103/PhysRevB.87.104111"), + description="Temperature dependent effective potential method.", +) +@due.dcite( + Doi("10.1088/1361-648X/acd831"), + description="Implementation strategies in phonopy and phono3py.", +) +@due.dcite( + Doi("10.7566/JPSJ.92.012001"), + description="Phonopy and phono3py.", +) @dataclass class BaseFiniteTemperaturePhononMaker(Maker, ABC): """ @@ -89,6 +98,9 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): potential energy late in the run. The result is stored in the output document. A warning is raised if the check fails, but the fit is still done. + This workflow is new and has not been tested widely. It might still change + in future versions. + .. Note:: The atoms of the relaxed structure are sorted by electronegativity before the supercell is built, as the VASP input sets do. The atoms are @@ -113,7 +125,11 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): n_snapshots: int Number of MD snapshots in the fit. thermostat: Literal["nose-hoover", "langevin"] - Thermostat of the NVT MD. + Thermostat of the NVT MD. Langevin, the default, samples the canonical + ensemble also for nearly harmonic modes (Bussi and Parrinello, Phys. Rev. + E 75, 056707 (2007)). A Nose-Hoover thermostat may leave such modes out + of equilibrium (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 + (2007)). The NPT MD does not use this setting. md_runs: int Number of consecutive MD jobs that make up the trajectory. Each job continues from the positions and velocities of the previous one. The @@ -177,7 +193,7 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): md_time_step: float = 1.0 equilibration_time: float = 1.0 n_snapshots: int = 50 - thermostat: Literal["nose-hoover", "langevin"] = "nose-hoover" + thermostat: Literal["nose-hoover", "langevin"] = "langevin" md_runs: int = 1 npt_time: float = 8.0 npt_equilibration_time: float = 2.0 @@ -209,31 +225,12 @@ def __post_init__(self) -> None: f"{key} must be one of {sorted(SUPPORTED_CODES)}, not " f"{getattr(self, key)!r}." ) - if self.thermostat not in _THERMOSTATS: - raise ValueError( - f"thermostat must be one of {_THERMOSTATS}, not {self.thermostat!r}." - ) - if self.rotational_sum_rule not in (*_ROTATIONAL_SUM_RULES, None): - raise ValueError( - f"rotational_sum_rule must be one of {_ROTATIONAL_SUM_RULES} or " - f"None, not {self.rotational_sum_rule!r}." - ) - for key in ("md_runs", "n_snapshots"): - value = getattr(self, key) - if ( - isinstance(value, bool) - or not isinstance(value, numbers.Integral) - or value < 1 - ): - raise ValueError(f"{key} must be a positive integer, not {value!r}.") - if ( - isinstance(self.alpha_min, bool) - or not isinstance(self.alpha_min, numbers.Integral) - or self.alpha_min >= -2 - ): - raise ValueError( - f"alpha_min must be an integer below -2, not {self.alpha_min!r}." - ) + if self.socket and self.code == "vasp": + raise ValueError("socket is not supported by VASP.") + if min(self.md_runs, self.n_snapshots) < 1: + raise ValueError("md_runs and n_snapshots must be at least 1.") + if self.alpha_min >= -2: + raise ValueError(f"alpha_min must be below -2, not {self.alpha_min}.") if min(self.temperature, self.md_time, self.md_time_step) <= 0: raise ValueError("temperature, md_time and md_time_step must be positive.") n_steps = round(self.md_time * 1000 / self.md_time_step) @@ -267,9 +264,9 @@ def make( self, structure: Structure, prev_dir: str | Path | None = None, - supercell_matrix: Matrix3D | None = None, born: list[Matrix3D] | None = None, epsilon_static: Matrix3D | None = None, + supercell_matrix: Matrix3D | None = None, ) -> Flow: """ Make a flow to calculate effective harmonic phonons at a temperature. @@ -280,17 +277,17 @@ def make( The unit cell. prev_dir: str | Path | None A previous calculation directory. It is passed to the relaxation. - The born job, the MD jobs and the phonon displacement calculations - get the relaxation directory, or this directory if there is no - relaxation. - supercell_matrix: Matrix3D | None - Diagonal supercell matrix. If None, it is chosen from min_length. + All later jobs get the relaxation directory, or this directory if + there is no relaxation. born: list[Matrix3D] | None - Born effective charges of the relaxed structure with its atoms - sorted by electronegativity. If given with epsilon_static, the - born_maker is not run. + Born effective charges of the structure the NVT MD runs in, with its + atoms sorted by electronegativity. This is the relaxed structure, or + the structure at the temperature with npt_maker. If given with + epsilon_static, the born_maker is not run. epsilon_static: Matrix3D | None High-frequency dielectric tensor. + supercell_matrix: Matrix3D | None + Diagonal supercell matrix. If None, it is chosen from min_length. Returns ------- @@ -344,7 +341,6 @@ def make( structure, supercell_matrix, start_job.output, - self.temperature, self.md_time_step, self.npt_equilibration_time, self.symprec, @@ -357,7 +353,7 @@ def make( "npt_equilibration_time": self.npt_equilibration_time, "npt_trajectory_health": npt_cell_job.output["trajectory_health"], "npt_uuid": npt_job.uuid, - "npt_dir": npt_job.output.dir_name, + "npt_job_dir": npt_job.output.dir_name, } structure = npt_cell_job.output["structure"] if self.fixed_cell_relax_maker is not None: @@ -389,7 +385,6 @@ def make( md_dirs, self.md_code, reference, - self.temperature, self.md_time_step, self.equilibration_time, self.n_snapshots, @@ -431,7 +426,7 @@ def make( md_force_field_name=md_force_field_name, md_force_field_kwargs=md_force_field_kwargs, md_uuids=[md_job.uuid for md_job in md_jobs], - md_dirs=md_dirs, + md_job_dirs=md_dirs, optimization_run_uuid=optimization_run_uuid, optimization_run_job_dir=optimization_run_job_dir, born_run_uuid=born_run_uuid, diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 9e1b2a24f4..58eb86448b 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -39,12 +39,7 @@ FiniteTemperaturePhononDoc, TrajectoryHealth, ) -from atomate2.common.schemas.phonons import ( - ForceConstants, - PhononJobDirs, - PhononUUIDs, - get_factor, -) +from atomate2.common.schemas.phonons import ForceConstants, PhononJobDirs, PhononUUIDs from atomate2.utils.path import strip_hostname if TYPE_CHECKING: @@ -59,16 +54,26 @@ ASE_TRAJECTORY_FILE = "md_trajectory.traj" _KPATH_SCHEME = "seekpath" -# Thresholds of the trajectory check. The MD starts from the reference structure, -# so a large displacement in the first frames means the atom order does not match. +# Limits of the trajectory check +# Rule of thumb: in the first 10 steps thermal motion moves an atom by about a +# tenth of an Angstrom or less, while a wrong atom order moves it by a bond length. +_N_START_FRAMES = 10 _START_LIMIT = 0.5 # Angstrom -_RMS_LIMIT = 1.0 # Angstrom -# Lindemann ratio at melting of an fcc solid, Saija et al., J. Chem. Phys. 124, -# 244504 (2006) +# Lindemann ratio at melting of an fcc solid. It is about 0.18 for a bcc solid. +# Saija et al., J. Chem. Phys. 124, 244504 (2006) _LINDEMANN_LIMIT = 0.15 +# Rule of thumb: u_ref / u_vib = 1.5 means the mean positions moved by about as +# much as the atoms vibrate (u_shift = 1.1 u_vib). _SHIFT_RATIO_LIMIT = 1.5 +# Rule of thumb: the mean positions are only checked if the second half of the +# trajectory lasts at least one period of a 1 THz vibration. +_MIN_SHIFT_WINDOW = 1.0 # ps +# Three sigma rule: without a drift, a change this large has a probability below +# 5% for any unimodal distribution. Pukelsheim, Am. Stat. 48, 88 (1994) _DRIFT_SIGMA = 3.0 -_N_START_FRAMES = 10 +# Rule of thumb: a third of a typical nearest-neighbor distance of 3 Angstrom, +# about twice the vibration at the Lindemann limit for that distance. +_RMS_LIMIT = 1.0 # Angstrom def _get_phonopy( @@ -169,7 +174,7 @@ def get_md_restart_structure( directory = Path(strip_hostname(md_dir)) if md_code == "vasp": structure = Poscar.from_file(zpath(str(directory / "CONTCAR"))).structure - elif md_code == "forcefields": + else: atoms = ase_read(directory / ASE_TRAJECTORY_FILE, index=-1) structure = Structure( atoms.cell[:], @@ -178,8 +183,6 @@ def get_md_restart_structure( coords_are_cartesian=True, site_properties={"velocities": atoms.get_velocities().tolist()}, ) - else: - raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") for key, values in _get_site_properties(reference).items(): structure.add_site_property(key, values) return structure @@ -212,13 +215,12 @@ def _read_vasp_md( def _read_ase_md( - directory: Path, time_step: float, skip_first: bool + directory: Path, time_step: float ) -> tuple[np.ndarray, np.ndarray, np.ndarray, list[str], float]: """Read the frames, cells and energies of a force field MD run.""" - frames = ase_read(directory / ASE_TRAJECTORY_FILE, index=":") - if skip_first: - # the starting structure is the last frame of the previous MD run - frames = frames[1:] + # the first frame is the starting structure, before the first step, which + # XDATCAR leaves out as well + frames = ase_read(directory / ASE_TRAJECTORY_FILE, index=":")[1:] frac_coords = np.array([atoms.get_scaled_positions() for atoms in frames]) cells = np.array([atoms.cell[:] for atoms in frames]) energies = np.array([atoms.get_potential_energy() for atoms in frames]) @@ -236,22 +238,15 @@ def _read_md( md_time_step is the time step. Returns the fractional coordinates, the cell and the potential energy of each frame, and the time step in fs. """ - directories = [Path(strip_hostname(md_dir)) for md_dir in md_dirs] - if len(set(directories)) != len(directories): - raise ValueError( - f"Each MD run must have its own directory, but the directories are " - f"{md_dirs}." - ) - frac_coords, cells, energies, time_steps = [], [], [], set() - for idx, directory in enumerate(directories): + frac_coords, cells, energies = [], [], [] + for md_dir in md_dirs: + directory = Path(strip_hostname(md_dir)) if md_code == "vasp": coords, cell, energy, species, time_step = _read_vasp_md(directory) - elif md_code == "forcefields": + else: coords, cell, energy, species, time_step = _read_ase_md( - directory, md_time_step, skip_first=idx > 0 + directory, md_time_step ) - else: - raise ValueError(f"MD code must be 'vasp' or 'forcefields', not {md_code}.") if species != [str(site.specie) for site in reference]: raise ValueError( f"The atoms of the MD in {directory} are not in the order of the " @@ -260,14 +255,11 @@ def _read_md( frac_coords.append(coords) cells.append(cell) energies.append(energy) - time_steps.add(time_step) - if len(time_steps) != 1: - raise ValueError(f"The MD runs have different time steps: {time_steps} fs.") return ( np.concatenate(frac_coords), np.concatenate(cells), np.concatenate(energies), - time_steps.pop(), + time_step, ) @@ -289,20 +281,22 @@ def _assess_trajectory( frac_coords: np.ndarray, energies: np.ndarray, reference: Structure, - temperature: float, + time_step: float, ) -> TrajectoryHealth: """ Check whether the MD trajectory stayed at the reference structure. The displacement of the center of mass of each frame is removed from its - displacements. The checks are applied in this order. + displacements. The checks are applied in this order. The limits are rules + of thumb, except where a source is given next to them in this module. - A root mean square displacement above 0.5 Angstrom in the first 10 frames means the atoms are not in the order of the reference. - A root mean square vibration u_vib above 0.15 of the nearest-neighbor distance means the structure melted. - A total displacement u_ref above 1.5 times u_vib means the mean - positions moved away from the reference. + positions moved away from the reference. This check is skipped if the + second half of the trajectory is shorter than 1 ps. - A change of the mean potential energy from the second to the last quarter of the frames above 3 times the standard deviation of the energy in the last fifth means the structure transformed (falling energy) @@ -322,8 +316,8 @@ def _assess_trajectory( Potential energy of each frame in eV. reference: Structure The undisplaced supercell. - temperature: float - MD temperature in K. + time_step: float + MD time step in fs. Returns ------- @@ -352,6 +346,10 @@ def _assess_trajectory( d_nn = float(distances.min(axis=1).mean()) lindemann_ratio = u_vib / d_nn shift_ratio = u_ref / max(u_vib, 1e-9) + shifted = ( + shift_ratio > _SHIFT_RATIO_LIMIT + and len(tail) * time_step / 1000 >= _MIN_SHIFT_WINDOW + ) energy = energies / n_atoms quarter = len(energy) // 4 @@ -367,7 +365,7 @@ def _assess_trajectory( verdict = "reference_mismatch" elif lindemann_ratio > _LINDEMANN_LIMIT: verdict = "melted" - elif shift_ratio > _SHIFT_RATIO_LIMIT: + elif shifted: verdict = "transformed" if big_drift and drift < 0 else "shifted_or_diffusing" elif big_drift: verdict = "transformed" if drift < 0 else "disordering" @@ -378,7 +376,6 @@ def _assess_trajectory( return TrajectoryHealth( verdict=verdict, - is_stable=verdict == "stable", n_frames=n_frames, rms_displacement_start=rms_start, rms_displacement_end=rms_end, @@ -390,7 +387,6 @@ def _assess_trajectory( shift_ratio=shift_ratio, energy_drift=drift, energy_fluctuation=fluctuation, - equipartition_rise=1.5 * kB * temperature, ) @@ -401,7 +397,6 @@ def get_npt_structure( structure: Structure, supercell_matrix: Matrix3D, reference: Structure, - temperature: float, md_time_step: float, equilibration_time: float, symprec: float, @@ -430,8 +425,6 @@ def get_npt_structure( Supercell matrix. reference: Structure The undisplaced supercell the NPT MD started from. - temperature: float - MD temperature in K. md_time_step: float MD time step in fs. Only used for force field trajectories. equilibration_time: float @@ -472,8 +465,8 @@ def get_npt_structure( site_properties=structure.site_properties, ) - health = _assess_trajectory(frac_coords, energies, reference, temperature) - if not health.is_stable: + health = _assess_trajectory(frac_coords, energies, reference, time_step) + if health.verdict != "stable": warnings.warn( f"The NPT trajectory did not stay at the reference structure (verdict: " f"{health.verdict}). The averaged cell may not describe it.", @@ -487,7 +480,6 @@ def select_md_snapshots( md_dirs: Sequence[str], md_code: str, reference: Structure, - temperature: float, md_time_step: float, equilibration_time: float, n_snapshots: int, @@ -495,11 +487,11 @@ def select_md_snapshots( """ Pick snapshots from the MD trajectory and check the trajectory. - The trajectories of all MD runs are joined in order, with a frame at every - time step. The time of a frame is its index in the joined trajectory times - the time step, so the first frame is at time zero. The frames of the first - equilibration_time are left out, and n_snapshots frames are picked evenly - spread over the rest. For VASP, XDATCAR, OSZICAR and the POTIM of INCAR are + The trajectories of all MD runs are joined in order, with a frame after + every time step. The time of a frame is its step number times the time + step. The frames of the first equilibration_time are left out, and + n_snapshots frames are picked evenly spread over the rest, from the first + to the last. For VASP, XDATCAR, OSZICAR and the POTIM of INCAR are read from each run directory. For force fields, the ASE trajectory file is read. The run directories must be readable from where this job runs. @@ -511,8 +503,6 @@ def select_md_snapshots( Code of the MD, "vasp" or "forcefields". reference: Structure The undisplaced supercell the MD started from. - temperature: float - MD temperature in K. md_time_step: float MD time step in fs. Only used for force field trajectories. equilibration_time: float @@ -542,8 +532,7 @@ def select_md_snapshots( f"leaving out {equilibration_time} ps, {max(n_left, 0)} frames are " f"left, fewer than the {n_snapshots} snapshots." ) - stride = n_left // n_snapshots - indices = list(range(n_equil, n_frames, stride))[:n_snapshots] + indices = np.linspace(n_equil, n_frames - 1, n_snapshots).round().astype(int) site_properties = _get_site_properties(reference) snapshots = [ @@ -559,8 +548,8 @@ def select_md_snapshots( np.array([_get_displacements(all_coords[idx], reference) for idx in indices]), reference, ) - health = _assess_trajectory(all_coords, all_energies, reference, temperature) - if not health.is_stable: + health = _assess_trajectory(all_coords, all_energies, reference, time_step) + if health.verdict != "stable": warnings.warn( f"The MD trajectory did not stay at the reference structure (verdict: " f"{health.verdict}). The fitted force constants may not describe it.", @@ -568,7 +557,7 @@ def select_md_snapshots( ) return { "structures": [*snapshots, reference], - "snapshot_times": [idx * time_step / 1000 for idx in indices], + "snapshot_times": [(idx + 1) * time_step / 1000 for idx in indices], "md_time": n_frames * time_step / 1000, "rms_displacement": float(np.sqrt(np.mean(np.sum(disps**2, axis=2)))), "trajectory_health": health.model_dump(), @@ -593,7 +582,9 @@ def _get_rms_displacement(phonon: Phonopy, temperature: float, tol: float) -> fl inv_sqrt_mass = 1 / np.sqrt(masses) dynmat = force_constants * np.outer(inv_sqrt_mass, inv_sqrt_mass) eigvals, eigvecs = np.linalg.eigh((dynmat + dynmat.T) / 2) - frequencies = np.sign(eigvals) * np.sqrt(np.abs(eigvals)) * get_factor("vasp") + frequencies = ( + np.sign(eigvals) * np.sqrt(np.abs(eigvals)) * phonon.unit_conversion_factor + ) keep = frequencies > tol weights = np.sum(eigvecs[:, keep] ** 2 / masses[:, None], axis=0) msd = kB * temperature * np.sum(weights / eigvals[keep]) @@ -621,7 +612,7 @@ def fit_finite_temperature_phonons( md_force_field_name: str | None = None, md_force_field_kwargs: dict | None = None, md_uuids: list[str] | None = None, - md_dirs: list[str] | None = None, + md_job_dirs: list[str] | None = None, optimization_run_uuid: str | None = None, optimization_run_job_dir: str | None = None, born_run_uuid: str | None = None, @@ -632,7 +623,7 @@ def fit_finite_temperature_phonons( npt_equilibration_time: float | None = None, npt_trajectory_health: dict | None = None, npt_uuid: str | None = None, - npt_dir: str | None = None, + npt_job_dir: str | None = None, fixed_cell_relax_uuid: str | None = None, fixed_cell_relax_job_dir: str | None = None, rotational_sum_rule: str | None = "BHH", @@ -693,7 +684,7 @@ def fit_finite_temperature_phonons( Keyword arguments of the force field calculator of the MD. md_uuids: list[str] | None UUIDs of the MD jobs. - md_dirs: list[str] | None + md_job_dirs: list[str] | None Directories of the MD jobs. optimization_run_uuid: str | None UUID of the relaxation. @@ -715,7 +706,7 @@ def fit_finite_temperature_phonons( Check of the NPT trajectory. npt_uuid: str | None UUID of the NPT MD job. - npt_dir: str | None + npt_job_dir: str | None Directory of the NPT MD job. fixed_cell_relax_uuid: str | None UUID of the relaxation of the atoms in the cell from the NPT MD. @@ -746,9 +737,6 @@ def fit_finite_temperature_phonons( FiniteTemperaturePhononDoc """ supercell_matrix = np.array(supercell_matrix) - if not np.allclose(supercell_matrix, np.diag(np.diag(supercell_matrix))): - raise ValueError("pheasy needs a diagonal supercell matrix.") - structure = structure.get_sorted_structure() if born is not None and len(born) != len(structure): raise ValueError("The number of Born charges is not the number of atoms.") @@ -757,15 +745,6 @@ def fit_finite_temperature_phonons( forces = np.array(displacement_data["forces"]) structures = displacement_data["displaced_structures"] - if len(structures) != len(snapshot_data["snapshot_times"]) + 1: - raise ValueError( - "The phonon displacement calculations must be the snapshots followed " - "by the undisplaced supercell." - ) - if not np.allclose(structures[-1].frac_coords, supercell.frac_coords, atol=1e-6): - raise ValueError( - "The last phonon displacement calculation is not the undisplaced supercell." - ) residual_forces = forces[-1] fit_forces = forces[:-1] - residual_forces disps = np.array( @@ -778,12 +757,8 @@ def fit_finite_temperature_phonons( np.save(_DEFAULT_FILE_PATHS["harmonic_displacements"], disps) np.save(_DEFAULT_FILE_PATHS["harmonic_force_matrix"], fit_forces) - # Remove the files of an earlier fit. pheasy appends to its log, and a failed - # fit would leave the old force constants behind. log_file = Path(_DEFAULT_FILE_PATHS["harmonic_fit_log"]) - log_file.unlink(missing_ok=True) fc_file = Path(_DEFAULT_FILE_PATHS["force_constants"]) - fc_file.unlink(missing_ok=True) _run_harmonic_fit( supercell_matrix, symprec, @@ -815,6 +790,8 @@ def fit_finite_temperature_phonons( supercell_matrix=phonon.supercell_matrix, ) if not np.all(np.isclose(borns, 0.0)): + # the factor is for forces in eV/Angstrom, as from VASP and the force + # fields phonon.nac_params = { "born": borns, "dielectric": epsilon, @@ -884,7 +861,7 @@ def fit_finite_temperature_phonons( tol_imaginary_modes=tol_imaginary_modes, has_imaginary_modes=has_imaginary_modes, n_imaginary_modes=int(np.sum(frequencies < -tol_imaginary_modes)), - min_frequency=float(frequencies.min()), + lowest_frequency=float(frequencies.min()), phonon_bandstructure=bs_symm_line, phonon_dos=dos, force_constants=ForceConstants(phonon.force_constants.tolist()) @@ -893,14 +870,14 @@ def fit_finite_temperature_phonons( born=borns.tolist() if borns is not None else None, epsilon_static=epsilon.tolist() if epsilon is not None else None, md_uuids=md_uuids, - md_dirs=md_dirs, + md_job_dirs=md_job_dirs, npt_input_structure=npt_input_structure, pressure=pressure, npt_time=npt_time, npt_equilibration_time=npt_equilibration_time, npt_trajectory_health=npt_trajectory_health, npt_uuid=npt_uuid, - npt_dir=npt_dir, + npt_job_dir=npt_job_dir, fixed_cell_relax_uuid=fixed_cell_relax_uuid, fixed_cell_relax_job_dir=fixed_cell_relax_job_dir, uuids=PhononUUIDs( diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 3dcc46e6dc..f64d380b76 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -290,9 +290,9 @@ def _run_harmonic_fit( Fit the second-order force constants with pheasy in the current folder. pheasy reads POSCAR, SPOSCAR and the harmonic displacement and force - matrices, and writes FORCE_CONSTANTS. The caller removes the files of an - earlier fit and checks the result, since the pheasy phonon workflow and - the finite-temperature workflow check different things. + matrices, and writes FORCE_CONSTANTS. The caller checks the result, since + the pheasy phonon workflow and the finite-temperature workflow check + different things. Parameters ---------- diff --git a/src/atomate2/common/schemas/finite_temperature_phonons.py b/src/atomate2/common/schemas/finite_temperature_phonons.py index e46ea52490..db1614a58c 100644 --- a/src/atomate2/common/schemas/finite_temperature_phonons.py +++ b/src/atomate2/common/schemas/finite_temperature_phonons.py @@ -40,7 +40,6 @@ class TrajectoryHealth(BaseModel): "the MD are not in the order of the reference. Every other verdict except " "'stable' means the trajectory left the reference structure.", ) - is_stable: bool | None = Field(None, description="True if the verdict is 'stable'.") n_frames: int | None = Field(None, description="Number of MD frames analysed.") rms_displacement_start: float | None = Field( None, @@ -88,11 +87,6 @@ class TrajectoryHealth(BaseModel): description="Standard deviation of the potential energy in the last fifth of " "the frames, in eV/atom.", ) - equipartition_rise: float | None = Field( - None, - description="Potential energy per atom that a harmonic MD run gains when " - "it starts from the reference structure, 3/2 k_B T, in eV/atom.", - ) class FiniteTemperaturePhononDoc(StructureMetadata): @@ -133,7 +127,8 @@ class FiniteTemperaturePhononDoc(StructureMetadata): md_time_step: float | None = Field(None, description="MD time step in fs.") md_time: float | None = Field( None, - description="Number of MD frames read from disk times the time step, in ps.", + description="Length of the joined MD trajectory, the number of frames times " + "the time step, in ps.", ) equilibration_time: float | None = Field( None, description="Time at the start of the trajectory left out, in ps." @@ -143,8 +138,8 @@ class FiniteTemperaturePhononDoc(StructureMetadata): ) snapshot_times: list[float] | None = Field( None, - description="MD time of each snapshot in ps, with the first frame of the " - "trajectory at time zero.", + description="MD time of each snapshot in ps, its step number times the time " + "step.", ) supercell_matrix: Matrix3D | None = Field( None, description="Supercell matrix of the MD and the statics." @@ -195,7 +190,7 @@ class FiniteTemperaturePhononDoc(StructureMetadata): description="Number of imaginary modes at the q-points commensurate with the " "supercell.", ) - min_frequency: float | None = Field( + lowest_frequency: float | None = Field( None, description="Lowest frequency at the q-points commensurate with the " "supercell, in THz. Imaginary frequencies are negative.", @@ -222,7 +217,9 @@ class FiniteTemperaturePhononDoc(StructureMetadata): "non-analytical correction together with born.", ) md_uuids: list[str] | None = Field(None, description="UUIDs of the MD jobs.") - md_dirs: list[str] | None = Field(None, description="Directories of the MD jobs.") + md_job_dirs: list[str] | None = Field( + None, description="Directories of the MD jobs." + ) npt_input_structure: Structure | None = Field( None, description="Unit cell whose supercell the NPT MD started from. None without " @@ -239,7 +236,7 @@ class FiniteTemperaturePhononDoc(StructureMetadata): None, description="Check of the NPT trajectory." ) npt_uuid: str | None = Field(None, description="UUID of the NPT MD job.") - npt_dir: str | None = Field(None, description="Directory of the NPT MD job.") + npt_job_dir: str | None = Field(None, description="Directory of the NPT MD job.") fixed_cell_relax_uuid: str | None = Field( None, description="UUID of the relaxation of the atoms in the cell from the NPT MD.", diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index 32e41b3182..704d6522a3 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -102,6 +102,7 @@ def _get_force_field_md_maker( traj_file=ASE_TRAJECTORY_FILE, traj_file_fmt="ase", traj_interval=1, + store_trajectory="no", mb_velocity_seed=maker.random_seed, zero_linear_momentum=True, ) @@ -116,17 +117,19 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): force field, MACE-MP-0 by default. Use :obj:`from_force_field_name` to use another one. The MD writes an ASE trajectory file with a frame at every time step. The snapshots are read from this file, and the trajectory is not - stored in the output document of the MD job. The Nose-Hoover thermostat is - ASE's NoseHooverChainNVT with one thermostat variable, like MDALGO = 2 in - VASP. Its time constant gives a period of about 40 time steps, like SMASS = - 0 in VASP. The Langevin thermostat has the default friction of - :obj:`.AseMDMaker`, 10 ps^-1. The initial velocities of the first MD job - follow the Maxwell-Boltzmann distribution, seeded with random_seed, with - zero total momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover - chain thermostat and barostat that change the whole cell, whatever the - thermostat setting. Its thermostat time constant is that of the - Nose-Hoover thermostat above, and its barostat time constant is 1000 time - steps. + stored in the output document of the MD job. The Langevin thermostat has + the default friction of :obj:`.AseMDMaker`, 10 ps^-1. Its random forces + come from numpy's global random number generator, so two runs give + different trajectories. The Nose-Hoover thermostat is ASE's + NoseHooverChainNVT with one thermostat variable, like MDALGO = 2 in VASP. + Its time constant gives a period of about 40 time steps, like SMASS = 0 in + VASP. The initial velocities of the first MD job follow the + Maxwell-Boltzmann distribution, seeded with random_seed, with zero total + momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover chain + thermostat and barostat that change the whole cell, whatever the + thermostat setting (Martyna et al., J. Chem. Phys. 101, 4177 (1994)). Its + thermostat time constant is that of the Nose-Hoover thermostat above, and + its barostat time constant is 1000 time steps. See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. diff --git a/src/atomate2/vasp/flows/finite_temperature_phonons.py b/src/atomate2/vasp/flows/finite_temperature_phonons.py index 97e89f1ac2..725da4ea83 100644 --- a/src/atomate2/vasp/flows/finite_temperature_phonons.py +++ b/src/atomate2/vasp/flows/finite_temperature_phonons.py @@ -15,7 +15,6 @@ from atomate2.vasp.sets.core import ( LangevinMDSetGenerator, MDSetGenerator, - StaticSetGenerator, TightRelaxSetGenerator, ) @@ -34,28 +33,19 @@ _MD_INCAR = { "ENCUT": 500, "EDIFF": 1e-5, - "PREC": "Normal", "ALGO": "Normal", "LREAL": "Auto", "NBLOCK": 1, "LWAVE": False, - "LCHARG": False, **_ELECTRONIC_INCAR, } +# changes to the INCAR of PhononDisplacementMaker _STATIC_INCAR = { - "IBRION": 2, - "ISIF": 3, - "NSW": 0, "ENCUT": 600, "ENAUG": 1360, - "EDIFF": 1e-7, "PREC": "Accurate", - "ALGO": "Normal", "LASPH": True, "NELM": 200, - "LREAL": False, - "LAECHG": False, - "LCHARG": False, "LWAVE": False, **_ELECTRONIC_INCAR, } @@ -111,13 +101,9 @@ def _get_md_maker() -> MDMaker: def _get_phonon_displacement_maker() -> PhononDisplacementMaker: """Get the static maker for the forces on the snapshots.""" - return PhononDisplacementMaker( - input_set_generator=StaticSetGenerator( - user_incar_settings=dict(_STATIC_INCAR), - user_kpoints_settings=dict(_KPOINTS), - auto_ispin=True, - ) - ) + maker = PhononDisplacementMaker() + maker.input_set_generator.user_incar_settings.update(_STATIC_INCAR) + return maker @dataclass @@ -130,15 +116,16 @@ class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): All three use ISMEAR = 0 with SIGMA = 0.05 and the same reciprocal_density setting of 100. The relaxation is a double tight relaxation with ENCUT = 600 eV, ENAUG = 1360 eV and PREC = Accurate, as in the phonon displacement - calculations. These also use EDIFF = 1e-7. The MD uses ENCUT = 500 eV, - EDIFF = 1e-5 and PREC = Normal, and writes every step to XDATCAR with - NBLOCK = 1. The Nose-Hoover thermostat uses MDALGO = 2 and SMASS = 0. The - Langevin thermostat uses MDALGO = 3 with LANGEVIN_GAMMA = 10 ps^-1 for each - species. VASP draws the initial velocities of the first MD job. The MD and - the phonon displacement calculations start from the magnetic moments of the - relaxed structure, if it has any. They all get the same prev_dir, the - relaxation directory by default. auto_ispin of the MD and of the phonon - displacement calculations sets ISPIN from it. + calculations. These otherwise keep the settings of PhononDisplacementMaker, + such as EDIFF = 1e-7. The MD uses ENCUT = 500 eV, EDIFF = 1e-5 and PREC = + Normal, and writes every step to XDATCAR with NBLOCK = 1. The Langevin + thermostat uses MDALGO = 3 with LANGEVIN_GAMMA = 10 ps^-1 for each species. + The Nose-Hoover thermostat uses MDALGO = 2 and SMASS = 0. VASP draws the + initial velocities of the first MD job. The MD and the phonon displacement + calculations start from the magnetic moments of the relaxed structure, if + it has any. They all get the same prev_dir, the relaxation directory by + default. auto_ispin of the MD and of the phonon displacement calculations + sets ISPIN from it. See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. diff --git a/src/atomate2/vasp/sets/core.py b/src/atomate2/vasp/sets/core.py index 19a50ba702..5594d35a89 100644 --- a/src/atomate2/vasp/sets/core.py +++ b/src/atomate2/vasp/sets/core.py @@ -10,7 +10,6 @@ import numpy as np from pymatgen.core.periodic_table import Element -from pymatgen.io.vasp import Poscar try: from pymatgen.io.vasp.sets import LobsterSet # type: ignore[attr-defined] @@ -754,9 +753,9 @@ def incar_updates(self) -> dict: updates = super().incar_updates # the Nose mass is only used by the Nose-Hoover thermostat updates.pop("SMASS", None) - # one value for each species block of the POSCAR - n_species = len(Poscar(self.structure).site_symbols) - updates.update(MDALGO=3, LANGEVIN_GAMMA=[self.langevin_gamma] * n_species) + # one value for each element, as for ensemble="npt" + n_elements = len(self.structure.composition) + updates.update(MDALGO=3, LANGEVIN_GAMMA=[self.langevin_gamma] * n_elements) return updates diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index 8bc2833929..262dbddabd 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -1,8 +1,6 @@ -"""Tests of the finite-temperature phonon workflow. +"""Tests of the jobs of the finite-temperature phonon workflow. -The end-to-end test runs the force field workflow with ASE's EMT potential, so -it needs no reference data. It lives here and not under tests/forcefields, -because pheasy is only installed in the test-non-ase CI job. +The tests of the whole force field workflow are in tests/forcefields/flows. """ import gzip @@ -15,14 +13,11 @@ from ase.calculators import emt from ase.calculators.singlepoint import SinglePointCalculator from ase.io import write as ase_write -from jobflow import run_locally from phonopy import Phonopy -from phonopy.harmonic.dynmat_to_fc import get_commensurate_points from pymatgen.core import Lattice, Structure from pymatgen.io.ase import AseAtomsAdaptor from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure -from atomate2.ase.md import MDEnsemble from atomate2.common.jobs.finite_temperature_phonons import ( ASE_TRAJECTORY_FILE, _assess_trajectory, @@ -34,15 +29,11 @@ get_npt_structure, select_md_snapshots, ) -from atomate2.forcefields.flows.finite_temperature_phonons import ( - ForceFieldFiniteTemperaturePhononMaker, - _get_force_field_md_maker, -) -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker -from atomate2.forcefields.md import ForceFieldMDMaker -EMT_CALCULATOR = {"@module": "ase.calculators.emt", "@callable": "EMT"} TEMPERATURE = 300.0 +# a long time step, so that the second half of the synthetic trajectories of 400 +# frames lasts 2 ps and the mean positions are checked +TIME_STEP = 10.0 TEST_DIR = Path(__file__).resolve().parents[2] / "test_data" @@ -73,8 +64,8 @@ def _trajectory(reference, rng, sigma=0.05, shift=None, energies=None): return frac, energies -def _verdict(reference, frac, energies): - return _assess_trajectory(frac, energies, reference, TEMPERATURE).verdict +def _verdict(reference, frac, energies, time_step=TIME_STEP): + return _assess_trajectory(frac, energies, reference, time_step).verdict def test_assess_trajectory(cu_supercell): @@ -82,19 +73,17 @@ def test_assess_trajectory(cu_supercell): n_atoms = len(cu_supercell) frac, energies = _trajectory(cu_supercell, rng) - health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + health = _assess_trajectory(frac, energies, cu_supercell, TIME_STEP) assert health.verdict == "stable" - assert health.is_stable assert health.n_frames == 400 # u_vib is sqrt(3) sigma for Gaussian displacements assert health.u_vib == pytest.approx(np.sqrt(3) * 0.05, rel=0.05) assert health.u_ref**2 == pytest.approx(health.u_shift**2 + health.u_vib**2) assert health.nearest_neighbor_distance == pytest.approx(3.61 / np.sqrt(2)) - assert health.equipartition_rise == pytest.approx(1.5 * units.kB * TEMPERATURE) # a translation of the whole cell is not a displacement moved = frac + np.array([0.1, 0.05, 0]) - health_moved = _assess_trajectory(moved, energies, cu_supercell, TEMPERATURE) + health_moved = _assess_trajectory(moved, energies, cu_supercell, TIME_STEP) assert health_moved.verdict == "stable" assert health_moved.u_ref == pytest.approx(health.u_ref) @@ -105,9 +94,11 @@ def test_assess_trajectory(cu_supercell): # the mean positions move in the second half, with a flat energy shift = rng.normal(0, 0.4, size=(n_atoms, 3)) frac, energies = _trajectory(cu_supercell, rng, shift=shift) - health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + health = _assess_trajectory(frac, energies, cu_supercell, TIME_STEP) assert health.verdict == "shifted_or_diffusing" assert health.shift_ratio > 1.5 + # in a second half shorter than 1 ps the mean positions are not checked + assert _verdict(cu_supercell, frac, energies, time_step=1.0) == "stable" # the same move with a falling energy is a transformation falling = np.concatenate([np.zeros(200), np.linspace(0, -0.1, 200)]) * n_atoms @@ -121,7 +112,7 @@ def test_assess_trajectory(cu_supercell): # a rising energy at the reference is disordering rising = np.linspace(0, 0.1, 400) * n_atoms frac, energies = _trajectory(cu_supercell, rng, energies=rising) - health = _assess_trajectory(frac, energies, cu_supercell, TEMPERATURE) + health = _assess_trajectory(frac, energies, cu_supercell, TIME_STEP) assert health.verdict == "disordering" assert health.energy_drift == pytest.approx(0.05, rel=0.05) @@ -131,7 +122,7 @@ def test_assess_trajectory(cu_supercell): frac, energies = _trajectory(sparse, rng) move = rng.choice([-2.2, 2.2], size=(len(sparse), 3)) / np.sqrt(3) frac[360:] = _frames(sparse, 40, 0.05, rng, shift=move) - health = _assess_trajectory(frac, energies, sparse, TEMPERATURE) + health = _assess_trajectory(frac, energies, sparse, TIME_STEP) assert health.verdict == "diffusing_or_soft" assert health.rms_displacement_end > 1.0 @@ -141,7 +132,7 @@ def test_assess_trajectory(cu_supercell): assert _verdict(cu_supercell, frac, energies) == "reference_mismatch" # too few frames to compare the quarters - health = _assess_trajectory(frac[:15], energies[:15], cu_supercell, TEMPERATURE) + health = _assess_trajectory(frac[:15], energies[:15], cu_supercell, TIME_STEP) assert health.energy_drift is None @@ -185,43 +176,31 @@ def test_select_md_snapshots_vasp(cu_supercell): md_dirs = ["host:" + str(Path("md1").resolve()), str(Path("md2").resolve())] # 0.1 ps is 50 frames of 2 fs, so 250 frames are left for 10 snapshots - output = select_md_snapshots.original( - md_dirs, "vasp", cu_supercell, TEMPERATURE, 1.0, 0.1, 10 - ) + output = select_md_snapshots.original(md_dirs, "vasp", cu_supercell, 1.0, 0.1, 10) structures = output["structures"] assert len(structures) == 11 assert structures[-1] == cu_supercell - indices = range(50, 300, 25) + # from the first to the last frame after 0.1 ps + indices = [50, 78, 105, 133, 161, 188, 216, 244, 271, 299] for structure, idx in zip(structures[:-1], indices, strict=True): diff = structure.frac_coords - frac[idx] assert np.allclose(diff - np.round(diff), 0, atol=1e-8) - assert output["snapshot_times"] == pytest.approx([idx * 0.002 for idx in indices]) + # XDATCAR has the frames after steps 1 to 300 + assert output["snapshot_times"] == pytest.approx( + [(idx + 1) * 0.002 for idx in indices] + ) assert output["md_time"] == pytest.approx(0.6) assert output["rms_displacement"] == pytest.approx(np.sqrt(3) * 0.05, rel=0.1) assert output["trajectory_health"]["n_frames"] == 300 with pytest.raises(ValueError, match="fewer than the 300 snapshots"): - select_md_snapshots.original( - md_dirs[:1], "vasp", cu_supercell, 300, 1, 0.1, 300 - ) + select_md_snapshots.original(md_dirs[:1], "vasp", cu_supercell, 1, 0.1, 300) # atoms of another species at the same positions other = cu_supercell.copy() other.replace_species({"Cu": "Ag"}) with pytest.raises(ValueError, match="not in the order of the reference"): - select_md_snapshots.original(md_dirs[:1], "vasp", other, 300, 1, 0.1, 10) - - # the same run twice, once with a host name - with pytest.raises(ValueError, match="its own directory"): - select_md_snapshots.original( - [md_dirs[0], str(Path("md1").resolve())], - "vasp", - cu_supercell, - 300, - 1, - 0.1, - 10, - ) + select_md_snapshots.original(md_dirs[:1], "vasp", other, 1, 0.1, 10) Path("md4").mkdir() for name in ("INCAR", "XDATCAR"): @@ -229,7 +208,7 @@ def test_select_md_snapshots_vasp(cu_supercell): (Path("md4") / "OSZICAR").write_text("") with pytest.raises(ValueError, match=r"0 MD steps in OSZICAR\..*NBLOCK = 1"): select_md_snapshots.original( - [str(Path("md4").resolve())], "vasp", cu_supercell, 300, 1, 0.1, 10 + [str(Path("md4").resolve())], "vasp", cu_supercell, 1, 0.1, 10 ) @@ -258,24 +237,24 @@ def test_select_md_snapshots_forcefields(cu_supercell): [str(Path(name).resolve()) for name in ("md1", "md2")], "forcefields", cu_supercell, - 300, 2.0, 0.02, 14, ) - assert output["trajectory_health"]["n_frames"] == 151 - # 10 frames of 2 fs are left out, and 141 frames are left for 14 snapshots - indices = range(10, 150, 10) - assert output["snapshot_times"] == pytest.approx([idx * 0.002 for idx in indices]) + # the starting structure of each run is left out, so frame 0 is step 1 + assert output["trajectory_health"]["n_frames"] == 150 + # 10 frames of 2 fs are left out, and 140 frames are left for 14 snapshots + indices = np.linspace(10, 149, 14).round().astype(int) + assert output["snapshot_times"] == pytest.approx((indices + 1) * 0.002) for structure, idx in zip(output["structures"][:-1], indices, strict=True): - diff = structure.frac_coords - frac[idx] + diff = structure.frac_coords - frac[idx + 1] assert np.allclose(diff - np.round(diff), 0, atol=1e-8) # the snapshots keep the magnetic moments of the reference magmoms = [1.0] * len(cu_supercell) magnetic = cu_supercell.copy(site_properties={"magmom": magmoms}) output = select_md_snapshots.original( - [str(Path("md1").resolve())], "forcefields", magnetic, 300, 2.0, 0.02, 14 + [str(Path("md1").resolve())], "forcefields", magnetic, 2.0, 0.02, 14 ) for structure in output["structures"]: assert structure.site_properties == {"magmom": magmoms} @@ -289,7 +268,6 @@ def test_select_md_snapshots_forcefields(cu_supercell): [str(Path("md3").resolve())], "forcefields", cu_supercell, - 300, 2.0, 0.02, 14, @@ -313,7 +291,7 @@ def test_get_npt_structure(cu_supercell): energies = rng.normal(0, 0.01, n_frames) _write_ase_md(Path("npt"), cu_supercell, frac, energies, cells=cells) - args = ("forcefields", unit_cell, (2 * np.eye(3)).tolist(), cu_supercell, 300) + args = ("forcefields", unit_cell, (2 * np.eye(3)).tolist(), cu_supercell) output = get_npt_structure.original( str(Path("npt").resolve()), *args, 2.0, 0.02, 1e-4 ) @@ -391,9 +369,6 @@ def test_get_md_restart_structure(cu_supercell): assert np.allclose(restart.cart_coords, cu_supercell.cart_coords) assert restart.site_properties["magmom"] == [1.0] * 32 - with pytest.raises(ValueError, match="MD code must be"): - get_md_restart_structure.original("ase", "lammps", reference) - def test_get_rms_displacement(): """An Einstein crystal has = 3 k_B T / k per atom.""" @@ -449,128 +424,6 @@ def test_rms_displacement_matches_mode_sampling(): assert not np.allclose(unweighted, removed, atol=1e-3) -@pytest.mark.parametrize( - ("kwargs", "match"), - [ - ({"thermostat": "berendsen"}, "thermostat must be one of"), - ({"rotational_sum_rule": "X"}, "rotational_sum_rule must be one of"), - ({"md_runs": 0}, "md_runs must be a positive integer"), - ({"n_snapshots": 2.5}, "n_snapshots must be a positive integer"), - ({"alpha_min": -2}, "alpha_min must be an integer below -2"), - ({"alpha_min": -6.0}, "alpha_min must be an integer below -2"), - ({"md_time_step": 0}, "must be positive"), - ({"equilibration_time": 8.0}, "fewer than the 50 snapshots"), - ({"equilibration_time": -1.0}, "fewer than the 50 snapshots"), - ( - {"md_time": 0.01, "equilibration_time": 0, "n_snapshots": 5, "md_runs": 20}, - "larger than the 10", - ), - ({"md_maker": None}, "md_maker and phonon_displacement_maker must be set"), - ({"code": "aims"}, "code must be one of"), - ({"md_code": None}, "md_code must be one of"), - ( - {"npt_maker": ForceFieldMDMaker(), "npt_equilibration_time": 8.0}, - "npt_equilibration_time must be", - ), - ( - {"fixed_cell_relax_maker": ForceFieldRelaxMaker()}, - "only used with npt_maker", - ), - ], -) -def test_maker_checks(kwargs, match): - with pytest.raises(ValueError, match=match): - ForceFieldFiniteTemperaturePhononMaker(**kwargs) - - -def test_force_field_md_maker(cu_supercell): - maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( - EMT_CALCULATOR, - md_time=1.0, - md_time_step=2.0, - equilibration_time=0.5, - md_runs=3, - random_seed=5, - ) - assert maker.get_md_steps() == [167, 167, 166] - md_maker = maker.get_md_maker(167) - assert md_maker.n_steps == 167 - assert md_maker.time_step == 2.0 - assert md_maker.temperature == TEMPERATURE - assert md_maker.mb_velocity_seed == 5 - assert md_maker.dynamics == "nose-hoover-chain" - assert md_maker.ase_md_kwargs["tchain"] == 1 - # a thermostat period of 40 steps, 80 fs - period = np.pi * np.sqrt(2) * md_maker.ase_md_kwargs["tdamp"] / units.fs - assert period == pytest.approx(80.0) - # the maker of the flow is not changed - assert maker.md_maker.n_steps == 1000 - assert maker.md_maker.dynamics is None - # the force field relaxation keeps the symmetry - assert maker.bulk_relax_maker.fix_symmetry - assert ForceFieldFiniteTemperaturePhononMaker().bulk_relax_maker.fix_symmetry - - # the MD jobs have a number only when there are several - flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) - md_names = [job.name for job in flow.jobs if "MD" in job.name] - assert md_names == ["ASE MD 1/3", "ASE MD 2/3", "ASE MD 3/3"] - maker = ForceFieldFiniteTemperaturePhononMaker(md_time=2.0) - flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) - assert [job.name for job in flow.jobs if "MD" in job.name] == ["ASE MD"] - - langevin = ForceFieldFiniteTemperaturePhononMaker( - thermostat="langevin" - ).get_md_maker(10) - # AseMDMaker sets its default friction when the job runs - assert langevin.dynamics == "langevin" - assert langevin.ase_md_kwargs == {} - - maker = ForceFieldFiniteTemperaturePhononMaker( - md_maker=ForceFieldMDMaker(ase_md_kwargs={"tdamp": 10}) - ) - with pytest.raises(ValueError, match="must not set dynamics or ase_md_kwargs"): - maker.get_md_maker(10) - with pytest.raises(TypeError, match="must be a ForceFieldMDMaker"): - _get_force_field_md_maker( - ForceFieldFiniteTemperaturePhononMaker(md_maker=ForceFieldStaticMaker()), 10 - ) - - -def test_force_field_npt_maker(cu_supercell): - maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( - EMT_CALCULATOR, run_npt=True, md_time_step=2.0, pressure=10.0 - ) - npt_maker = maker.get_npt_maker(100) - assert npt_maker.ensemble == MDEnsemble.npt - assert npt_maker.dynamics == "nose-hoover-chain" - assert npt_maker.n_steps == 100 - assert npt_maker.pressure == 10.0 - # a barostat time constant of 1000 steps - assert npt_maker.ase_md_kwargs["pdamp"] / units.fs == pytest.approx(2000) - assert maker.get_md_maker(100).ensemble == MDEnsemble.nvt - # the atoms are relaxed in the cell from the NPT MD - assert not maker.fixed_cell_relax_maker.relax_cell - assert maker.fixed_cell_relax_maker.fix_symmetry - - flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) - names = [job.name for job in flow.jobs] - assert "ASE MD NPT" in names - assert "get_npt_structure" in names - - # no NPT MD by default - maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(EMT_CALCULATOR) - assert maker.npt_maker is None - assert maker.fixed_cell_relax_maker is None - flow = maker.make(cu_supercell, supercell_matrix=np.eye(3).tolist()) - assert not any("NPT" in job.name for job in flow.jobs) - - -def _commensurate_frequencies(phonon): - matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix - phonon.run_qpoints(get_commensurate_points(np.rint(matrix).astype(int))) - return np.sort(phonon.qpoints.frequencies.ravel()) - - def _emt_phonon(structure, supercell_matrix): """0 K phonopy object of EMT, with its force constants.""" phonon = Phonopy( @@ -627,7 +480,7 @@ def test_fit_recovers_harmonic_force_constants(): "snapshot_data": snapshot_data, "displacement_data": displacement_data, "temperature": TEMPERATURE, - "thermostat": "nose-hoover", + "thermostat": "langevin", "md_time_step": 1.0, "equilibration_time": 0.5, "code": "forcefields", @@ -652,125 +505,3 @@ def test_fit_recovers_harmonic_force_constants(): with pytest.raises(ValueError, match="number of Born charges"): fit_finite_temperature_phonons.original(born=born[:3], **fit_kwargs) assert Path("FORCE_CONSTANTS").stat().st_mtime_ns == fc_time - - with pytest.raises(ValueError, match="diagonal supercell matrix"): - fit_finite_temperature_phonons.original( - **{**fit_kwargs, "supercell_matrix": [[1, 1, 0], [0, 1, 0], [0, 0, 1]]} - ) - with pytest.raises(ValueError, match="snapshots followed by the undisplaced"): - fit_finite_temperature_phonons.original( - **{**fit_kwargs, "snapshot_data": {"snapshot_times": [0.0] * 19}} - ) - shuffled = { - **displacement_data, - "displaced_structures": [supercell, *snapshots], - } - with pytest.raises(ValueError, match="not the undisplaced supercell"): - fit_finite_temperature_phonons.original( - **{**fit_kwargs, "displacement_data": shuffled} - ) - - -def test_finite_temperature_phonon_maker_emt(clean_dir): - """Run the whole force field workflow with EMT on L1_2 Cu3Au at 300 K.""" - # Au first, so that sorting the atoms by electronegativity reorders them - structure = Structure( - Lattice.cubic(3.75), - ["Au", "Cu", "Cu", "Cu"], - [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], - ) - # a 2x2x2 supercell of the cubic cell, 32 atoms, and 2 ps of MD at 2 fs in - # two MD jobs - maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( - EMT_CALCULATOR, - min_length=7.0, - md_time=2.0, - md_time_step=2.0, - md_runs=2, - equilibration_time=0.5, - n_snapshots=12, - ) - flow = maker.make(structure) - responses = run_locally(flow, create_folders=True, ensure_success=True) - doc = responses[flow.output.uuid][1].output - - assert [str(site.specie) for site in doc.structure] == ["Cu", "Cu", "Cu", "Au"] - assert doc.temperature == TEMPERATURE - assert doc.thermostat == "nose-hoover" - assert doc.md_code == doc.code == "forcefields" - assert doc.md_force_field_name == doc.force_field_name == "ase.calculators.emt.EMT" - assert doc.force_field_kwargs == {} - # 1000 steps and the starting structure - assert doc.md_time == pytest.approx(2.002) - assert doc.n_snapshots == 12 - assert len(doc.snapshot_times) == 12 - assert min(doc.snapshot_times) == pytest.approx(0.5) - assert len(doc.md_uuids) == len(doc.md_dirs) == 2 - assert len(doc.uuids.displacements_uuids) == 13 - assert doc.uuids.optimization_run_uuid is not None - assert doc.uuids.born_run_uuid is None - assert doc.supercell_matrix == ((2, 0, 0), (0, 2, 0), (0, 0, 2)) - assert doc.trajectory_health.verdict == "stable" - assert doc.max_residual_force < 1e-8 - assert 0 < doc.force_rmse < 0.2 - assert doc.lasso_alpha > 0 - # Cu3Au is stable at 300 K - assert not doc.has_imaginary_modes - assert doc.n_imaginary_modes == 0 - assert doc.min_frequency > -0.1 - # the snapshot amplitude agrees with the one of the fitted force constants - assert doc.rms_displacement == pytest.approx( - doc.rms_displacement_from_force_constants, rel=0.25 - ) - force_constants = np.array(doc.force_constants.force_constants) - assert force_constants.shape == (32, 32, 3, 3) - fit_dir = Path(doc.jobdirs.taskdoc_run_job_dir) - for name in ("FORCE_CONSTANTS", "phonopy.yaml", "pheasy_harmonic_fit.log"): - assert (fit_dir / name).exists() - - # at a fixed volume, the frequencies stay close to the 0 K ones of EMT - phonon = _emt_phonon(doc.structure, np.array(doc.supercell_matrix)) - freqs_0k = _commensurate_frequencies(phonon) - phonon.force_constants = force_constants - freqs = _commensurate_frequencies(phonon) - top = len(freqs) // 3 - assert freqs[-top:].mean() == pytest.approx(freqs_0k[-top:].mean(), rel=0.15) - - -def test_finite_temperature_phonon_maker_emt_npt(clean_dir): - """Run the force field workflow with an NPT MD first, with EMT on Cu3Au.""" - structure = Structure( - Lattice.cubic(3.75), - ["Au", "Cu", "Cu", "Cu"], - [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], - ) - maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( - EMT_CALCULATOR, - run_npt=True, - min_length=7.0, - npt_time=2.0, - npt_equilibration_time=0.5, - md_time=1.0, - md_time_step=2.0, - equilibration_time=0.2, - n_snapshots=10, - ) - flow = maker.make(structure) - responses = run_locally(flow, create_folders=True, ensure_success=True) - doc = responses[flow.output.uuid][1].output - - assert doc.pressure == 0.0 - assert doc.npt_time == 2.0 - assert doc.npt_equilibration_time == 0.5 - assert doc.npt_trajectory_health.verdict == "stable" - assert doc.npt_uuid is not None - assert doc.npt_dir is not None - assert doc.fixed_cell_relax_uuid is not None - # the NVT MD and the fit use the cubic cell from the NPT MD - assert doc.structure.lattice.abc == pytest.approx([doc.structure.lattice.a] * 3) - assert doc.structure.lattice.angles == pytest.approx((90, 90, 90)) - ratio = doc.structure.volume / doc.npt_input_structure.volume - assert ratio != 1 - assert ratio == pytest.approx(1, abs=0.05) - assert doc.trajectory_health.verdict == "stable" - assert not doc.has_imaginary_modes diff --git a/tests/forcefields/flows/test_finite_temperature_phonons.py b/tests/forcefields/flows/test_finite_temperature_phonons.py new file mode 100644 index 0000000000..4540b24150 --- /dev/null +++ b/tests/forcefields/flows/test_finite_temperature_phonons.py @@ -0,0 +1,238 @@ +"""Tests for the force field finite-temperature phonon workflow. + +The tests run the workflow with ASE's EMT potential, so they need no reference +data and no machine-learned force field. pheasy is only installed in the +numpy-limited forcefield CI job, so the tests are skipped in the other +forcefield jobs. +""" + +import pytest + +pytest.importorskip("pheasy") + +import numpy as np +from ase import units +from jobflow import run_locally +from pymatgen.core import Lattice, Structure + +from atomate2.ase.md import MDEnsemble +from atomate2.forcefields.flows.finite_temperature_phonons import ( + ForceFieldFiniteTemperaturePhononMaker, + _get_force_field_md_maker, +) +from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.md import ForceFieldMDMaker + +EMT = {"@module": "ase.calculators.emt", "@callable": "EMT"} + + +@pytest.fixture +def cu3au(): + """L1_2 Cu3Au with Au first, so that sorting by electronegativity reorders it.""" + return Structure( + Lattice.cubic(3.75), + ["Au", "Cu", "Cu", "Cu"], + [[0, 0, 0], [0, 0.5, 0.5], [0.5, 0, 0.5], [0.5, 0.5, 0]], + ) + + +def run_emt_flow(structure, **kwargs): + """Run the force field workflow with EMT and return its output document.""" + # the Langevin thermostat of ASE draws from numpy's global generator + np.random.seed(103) # noqa: NPY002 + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT, min_length=7.0, md_time_step=2.0, **kwargs + ) + flow = maker.make(structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + return responses[flow.output.uuid][1].output + + +@pytest.mark.parametrize( + ("kwargs", "match"), + [ + ({"md_runs": 0}, "md_runs and n_snapshots must be at least 1"), + ({"alpha_min": -2}, "alpha_min must be below -2"), + ({"md_time_step": 0}, "must be positive"), + ({"equilibration_time": 8.0}, "fewer than the 50 snapshots"), + ({"equilibration_time": -1.0}, "fewer than the 50 snapshots"), + ( + {"md_time": 0.01, "equilibration_time": 0, "n_snapshots": 5, "md_runs": 20}, + "larger than the 10", + ), + ({"md_maker": None}, "md_maker and phonon_displacement_maker must be set"), + ({"code": "aims"}, "code must be one of"), + ({"md_code": None}, "md_code must be one of"), + ({"code": "vasp", "socket": True}, "socket is not supported by VASP"), + ( + {"npt_maker": ForceFieldMDMaker(), "npt_equilibration_time": 8.0}, + "npt_equilibration_time must be", + ), + ( + {"fixed_cell_relax_maker": ForceFieldRelaxMaker()}, + "only used with npt_maker", + ), + ], +) +def test_maker_checks(kwargs, match): + with pytest.raises(ValueError, match=match): + ForceFieldFiniteTemperaturePhononMaker(**kwargs) + + +def test_force_field_md_maker(cu3au): + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT, + md_time=1.0, + md_time_step=2.0, + equilibration_time=0.5, + md_runs=3, + random_seed=5, + ) + assert maker.get_md_steps() == [167, 167, 166] + md_maker = maker.get_md_maker(167) + assert md_maker.n_steps == 167 + assert md_maker.time_step == 2.0 + assert md_maker.temperature == 300 + assert md_maker.mb_velocity_seed == 5 + assert md_maker.store_trajectory == "no" + # Langevin by default, with the default friction of AseMDMaker + assert md_maker.dynamics == "langevin" + assert md_maker.ase_md_kwargs == {} + # the maker of the flow is not changed + assert maker.md_maker.n_steps == 1000 + assert maker.md_maker.dynamics is None + # the force field relaxation keeps the symmetry + assert maker.bulk_relax_maker.fix_symmetry + assert ForceFieldFiniteTemperaturePhononMaker().bulk_relax_maker.fix_symmetry + + # the MD jobs have a number only when there are several + flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) + md_names = [job.name for job in flow.jobs if "MD" in job.name] + assert md_names == ["ASE MD 1/3", "ASE MD 2/3", "ASE MD 3/3"] + maker = ForceFieldFiniteTemperaturePhononMaker(md_time=2.0) + flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) + assert [job.name for job in flow.jobs if "MD" in job.name] == ["ASE MD"] + + nose_hoover = ForceFieldFiniteTemperaturePhononMaker( + thermostat="nose-hoover", md_time_step=2.0 + ).get_md_maker(10) + assert nose_hoover.dynamics == "nose-hoover-chain" + assert nose_hoover.ase_md_kwargs["tchain"] == 1 + # a thermostat period of 40 steps, 80 fs + period = np.pi * np.sqrt(2) * nose_hoover.ase_md_kwargs["tdamp"] / units.fs + assert period == pytest.approx(80.0) + + maker = ForceFieldFiniteTemperaturePhononMaker( + md_maker=ForceFieldMDMaker(ase_md_kwargs={"tdamp": 10}) + ) + with pytest.raises(ValueError, match="must not set dynamics or ase_md_kwargs"): + maker.get_md_maker(10) + with pytest.raises(TypeError, match="must be a ForceFieldMDMaker"): + _get_force_field_md_maker( + ForceFieldFiniteTemperaturePhononMaker(md_maker=ForceFieldStaticMaker()), 10 + ) + + with pytest.raises(ValueError, match="diagonal supercell matrix"): + maker.make(cu3au, supercell_matrix=[[1, 1, 0], [0, 1, 0], [0, 0, 1]]) + + +def test_force_field_npt_maker(cu3au): + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT, run_npt=True, md_time_step=2.0, pressure=10.0 + ) + npt_maker = maker.get_npt_maker(100) + assert npt_maker.ensemble == MDEnsemble.npt + assert npt_maker.dynamics == "nose-hoover-chain" + assert npt_maker.n_steps == 100 + assert npt_maker.pressure == 10.0 + # a barostat time constant of 1000 steps + assert npt_maker.ase_md_kwargs["pdamp"] / units.fs == pytest.approx(2000) + assert maker.get_md_maker(100).ensemble == MDEnsemble.nvt + # the atoms are relaxed in the cell from the NPT MD + assert not maker.fixed_cell_relax_maker.relax_cell + assert maker.fixed_cell_relax_maker.fix_symmetry + + flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) + names = [job.name for job in flow.jobs] + assert "ASE MD NPT" in names + assert "get_npt_structure" in names + + # no NPT MD by default + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(EMT) + assert maker.npt_maker is None + assert maker.fixed_cell_relax_maker is None + flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) + assert not any("NPT" in job.name for job in flow.jobs) + + +def test_finite_temperature_phonon_maker_emt(clean_dir, cu3au): + """Run the whole workflow with EMT on Cu3Au at 300 K.""" + # a 2x2x2 supercell of the cubic cell, 32 atoms, and 2 ps of MD at 2 fs in + # two MD jobs + doc = run_emt_flow( + cu3au, md_time=2.0, md_runs=2, equilibration_time=0.5, n_snapshots=12 + ) + + assert [str(site.specie) for site in doc.structure] == ["Cu", "Cu", "Cu", "Au"] + assert doc.temperature == 300 + assert doc.thermostat == "langevin" + assert doc.md_code == doc.code == "forcefields" + assert doc.md_force_field_name == doc.force_field_name == "ase.calculators.emt.EMT" + assert doc.force_field_kwargs == {} + assert doc.md_time == pytest.approx(2.0) + assert doc.n_snapshots == 12 + # 250 steps of 2 fs are left out + assert doc.snapshot_times[0] == pytest.approx(0.502) + assert doc.snapshot_times[-1] == pytest.approx(2.0) + assert len(doc.md_uuids) == len(doc.md_job_dirs) == 2 + assert len(doc.uuids.displacements_uuids) == 13 + assert doc.uuids.optimization_run_uuid is not None + assert doc.uuids.born_run_uuid is None + assert doc.supercell_matrix == ((2, 0, 0), (0, 2, 0), (0, 0, 2)) + assert doc.trajectory_health.verdict == "stable" + assert doc.max_residual_force < 1e-8 + assert np.array(doc.force_constants.force_constants).shape == (32, 32, 3, 3) + # Cu3Au is stable at 300 K + assert not doc.has_imaginary_modes + assert doc.n_imaginary_modes == 0 + # the snapshot amplitude agrees with the one of the fitted force constants + assert doc.rms_displacement == pytest.approx( + doc.rms_displacement_from_force_constants, rel=0.25 + ) + # values of this run, to catch changes of the results + assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(6.815, rel=0.05) + # the acoustic modes at Gamma + assert doc.lowest_frequency == pytest.approx(0, abs=1e-3) + assert doc.rms_displacement == pytest.approx(0.1235, rel=0.05) + assert doc.force_rmse == pytest.approx(0.1045, rel=0.15) + + +def test_finite_temperature_phonon_maker_emt_npt(clean_dir, cu3au): + """Run the workflow with an NPT MD first, with EMT on Cu3Au at 300 K.""" + doc = run_emt_flow( + cu3au, + run_npt=True, + npt_time=2.0, + npt_equilibration_time=0.5, + md_time=1.0, + equilibration_time=0.2, + n_snapshots=10, + ) + + assert doc.pressure == 0.0 + assert doc.npt_time == 2.0 + assert doc.npt_equilibration_time == 0.5 + assert doc.npt_trajectory_health.verdict == "stable" + assert doc.npt_uuid is not None + assert doc.npt_job_dir is not None + assert doc.fixed_cell_relax_uuid is not None + # the atoms are relaxed in the cell from the NPT MD + assert doc.max_residual_force < 1e-3 + # the NVT MD and the fit use the cubic cell from the NPT MD, which expanded + assert doc.structure.lattice.abc == pytest.approx([doc.structure.lattice.a] * 3) + assert doc.structure.lattice.angles == pytest.approx((90, 90, 90)) + assert doc.structure.volume > doc.npt_input_structure.volume + assert doc.structure.lattice.a == pytest.approx(3.7328, rel=2e-3) + assert doc.trajectory_health.verdict == "stable" + assert not doc.has_imaginary_modes + assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(6.554, rel=0.05) diff --git a/tests/vasp/flows/test_finite_temperature_phonons.py b/tests/vasp/flows/test_finite_temperature_phonons.py index df64306ed8..8bc48c7c9e 100644 --- a/tests/vasp/flows/test_finite_temperature_phonons.py +++ b/tests/vasp/flows/test_finite_temperature_phonons.py @@ -72,7 +72,7 @@ def test_vasp_flows(si_structure, maker_cls, md_code, code): args = snapshots.function_args assert [ref.uuid for ref in args[0]] == [md_1.uuid, md_2.uuid] - assert args[1:] == (md_code, reference.output, 300.0, 1.0, 1.0, 50) + assert args[1:] == (md_code, reference.output, 1.0, 1.0, 50) # the statics get the snapshots followed by the undisplaced supercell, and # only VASP statics get the relaxation directory @@ -127,7 +127,9 @@ def test_non_diagonal_supercell_matrix(si_structure): def test_relax_md_and_static_settings_match(nio_supercell, test_dir): """The relaxation, the MD and the statics must see the same Hamiltonian.""" - maker = FiniteTemperaturePhononMaker(md_time=4.0, md_time_step=0.5) + maker = FiniteTemperaturePhononMaker( + md_time=4.0, md_time_step=0.5, thermostat="nose-hoover" + ) md_generator = maker.get_md_maker(maker.get_md_steps()[0]).input_set_generator static_generator = maker.phonon_displacement_maker.input_set_generator relax_generator = maker.bulk_relax_maker.relax_maker1.input_set_generator @@ -181,7 +183,8 @@ def test_relax_md_and_static_settings_match(nio_supercell, test_dir): def test_langevin_thermostat(nio_supercell): - maker = FiniteTemperaturePhononMaker(thermostat="langevin", temperature=600) + # Langevin by default + maker = FiniteTemperaturePhononMaker(temperature=600) md_maker = maker.get_md_maker(100) assert isinstance(md_maker.input_set_generator, LangevinMDSetGenerator) incar = md_maker.input_set_generator.get_input_set( @@ -195,7 +198,7 @@ def test_langevin_thermostat(nio_supercell): assert type(maker.md_maker.input_set_generator) is MDSetGenerator # a Langevin MD maker needs the Langevin thermostat - maker = FiniteTemperaturePhononMaker(md_maker=md_maker) + maker = FiniteTemperaturePhononMaker(md_maker=md_maker, thermostat="nose-hoover") with pytest.raises(ValueError, match="Set thermostat to 'langevin'"): maker.get_md_maker(100) maker = FiniteTemperaturePhononMaker(md_maker=md_maker, thermostat="langevin") diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 77dd110a4a..02876f9844 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -43,7 +43,7 @@ "3. Optional, off by default: an NPT MD gives the cell at the temperature.\n", " Section 2 explains this step.\n", "4. An NVT MD run of the supercell at the temperature. The defaults are 8 ps with\n", - " a 1 fs time step and a Nose-Hoover thermostat.\n", + " a 1 fs time step and a Langevin thermostat.\n", "5. The first 1 ps of the MD is left out. 50 snapshots are picked, evenly spread\n", " over the rest of the trajectory.\n", "6. The forces on the snapshots and on the undisplaced supercell are computed.\n", @@ -70,6 +70,40 @@ "cell_type": "markdown", "id": "2", "metadata": {}, + "source": [ + "## Thermostats\n", + "\n", + "The fit only uses the positions of the atoms in the MD, not how they move. What\n", + "matters is that the snapshots follow the canonical distribution, so that every\n", + "phonon mode holds its share of the thermal energy.\n", + "\n", + "The NVT MD uses a Langevin thermostat. It adds a friction and a random force to\n", + "every atom, and it samples the canonical distribution (Bussi and Parrinello,\n", + "Phys. Rev. E 75, 056707 (2007)). The friction is 10 ps^-1. A Nose-Hoover\n", + "thermostat acts on the whole crystal through one extra variable. It changes the\n", + "motion of the atoms less, which matters for vibrational spectra or diffusion.\n", + "But in a nearly harmonic crystal the modes barely exchange energy, and a\n", + "Nose-Hoover thermostat can leave them out of equilibrium. This is proven for a\n", + "harmonic oscillator (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 (2007)).\n", + "The problem is worst at low temperature, where the crystal is closest to\n", + "harmonic.\n", + "\n", + "The NPT MD of Section 2 uses ASE's `MTKNPT`. It combines a Nose-Hoover\n", + "thermostat with the barostat of Martyna, Tobias and Klein, which samples the\n", + "isothermal-isobaric ensemble (J. Chem. Phys. 101, 4177 (1994)). Only its\n", + "average cell is used. With VASP, the NPT MD uses VASP's Langevin thermostat\n", + "and Parrinello-Rahman barostat, since VASP only runs NPT MD with these.\n", + "\n", + "`thermostat=\"nose-hoover\"` switches the NVT MD to a Nose-Hoover thermostat. We\n", + "do not recommend it. The random forces of the Langevin thermostat come from\n", + "numpy's random number generator, so two runs with the same settings give\n", + "different trajectories." + ] + }, + { + "cell_type": "markdown", + "id": "3", + "metadata": {}, "source": [ "## Installation\n", "\n", @@ -87,7 +121,7 @@ }, { "cell_type": "markdown", - "id": "3", + "id": "4", "metadata": {}, "source": [ "## The potentials\n", @@ -115,7 +149,7 @@ { "cell_type": "code", "execution_count": null, - "id": "4", + "id": "5", "metadata": {}, "outputs": [], "source": [ @@ -149,7 +183,7 @@ }, { "cell_type": "markdown", - "id": "5", + "id": "6", "metadata": {}, "source": [ "## One calculator for all jobs\n", @@ -164,7 +198,7 @@ { "cell_type": "code", "execution_count": null, - "id": "6", + "id": "7", "metadata": {}, "outputs": [], "source": [ @@ -190,7 +224,7 @@ }, { "cell_type": "markdown", - "id": "7", + "id": "8", "metadata": {}, "source": [ "## 1. Five materials from 100 K to 900 K\n", @@ -201,7 +235,7 @@ }, { "cell_type": "markdown", - "id": "8", + "id": "9", "metadata": {}, "source": [ "## The structure\n", @@ -215,7 +249,7 @@ { "cell_type": "code", "execution_count": null, - "id": "9", + "id": "10", "metadata": {}, "outputs": [], "source": [ @@ -245,7 +279,7 @@ }, { "cell_type": "markdown", - "id": "10", + "id": "11", "metadata": {}, "source": [ "## Building the workflow\n", @@ -268,7 +302,7 @@ { "cell_type": "code", "execution_count": null, - "id": "11", + "id": "12", "metadata": {}, "outputs": [], "source": [ @@ -288,14 +322,14 @@ }, { "cell_type": "markdown", - "id": "12", + "id": "13", "metadata": {}, "source": [ "## Running the workflow\n", "\n", "The flow has one MD job and 51 force calculations, 50 snapshots and the\n", - "undisplaced supercell. On one A100 GPU the whole run took 11 minutes. The MD\n", - "took 9 minutes, the force calculations 11 seconds and the fit 2 minutes.\n", + "undisplaced supercell. On one A100 GPU the whole run took 12 minutes. The MD\n", + "took 9 minutes, the force calculations 12 seconds and the fit 2 minutes.\n", "\n", "`create_folders=True` is needed, because the snapshots are read from the\n", "trajectory file in the folder of the MD job." @@ -304,7 +338,7 @@ { "cell_type": "code", "execution_count": null, - "id": "13", + "id": "14", "metadata": {}, "outputs": [], "source": [ @@ -318,7 +352,7 @@ }, { "cell_type": "markdown", - "id": "14", + "id": "15", "metadata": {}, "source": [ "## Results\n", @@ -330,7 +364,7 @@ { "cell_type": "code", "execution_count": null, - "id": "15", + "id": "16", "metadata": {}, "outputs": [], "source": [ @@ -340,7 +374,7 @@ "{\n", " \"highest frequency in THz\": float(np.max(doc.phonon_bandstructure.bands)),\n", " \"imaginary modes on the band path\": doc.has_imaginary_modes,\n", - " \"lowest frequency at the commensurate q-points in THz\": doc.min_frequency,\n", + " \"lowest frequency at the commensurate q-points in THz\": doc.lowest_frequency,\n", " \"LASSO penalty\": doc.lasso_alpha,\n", " \"force RMSE in eV/A\": doc.force_rmse,\n", " \"trajectory check\": health.verdict,\n", @@ -350,13 +384,13 @@ }, { "cell_type": "markdown", - "id": "16", + "id": "17", "metadata": {}, "source": [ "Our run gave a highest frequency of 5.97 THz, no imaginary modes and a stable\n", "trajectory.\n", "\n", - "- `has_imaginary_modes` checks the whole band path. `min_frequency` only covers\n", + "- `has_imaginary_modes` checks the whole band path. `lowest_frequency` only covers\n", " the q-points commensurate with the supercell. The fit sets the frequencies at\n", " these points directly. Everywhere else they are interpolated. Section 3 shows\n", " why the difference matters.\n", @@ -374,7 +408,7 @@ }, { "cell_type": "markdown", - "id": "17", + "id": "18", "metadata": {}, "source": [ "## Comparing with 0 K\n", @@ -389,7 +423,7 @@ { "cell_type": "code", "execution_count": null, - "id": "18", + "id": "19", "metadata": {}, "outputs": [], "source": [ @@ -457,7 +491,7 @@ }, { "cell_type": "markdown", - "id": "19", + "id": "20", "metadata": {}, "source": [ "At 0 K, Ca3Ir4Sn13 has imaginary modes down to about -0.75 THz. At 300 K they\n", @@ -472,7 +506,7 @@ }, { "cell_type": "markdown", - "id": "20", + "id": "21", "metadata": {}, "source": [ "## The other temperatures, potentials and materials\n", @@ -486,13 +520,13 @@ "and 3 use it as well.\n", "\n", "The loop runs 75 workflows, so it is off by default. Set `RUN_ALL = True` to\n", - "run it. Each of our runs took 6 to 36 minutes on one A100 GPU." + "run it. Each of our runs took 6 to 22 minutes on one A100 GPU." ] }, { "cell_type": "code", "execution_count": null, - "id": "21", + "id": "22", "metadata": {}, "outputs": [], "source": [ @@ -564,7 +598,7 @@ }, { "cell_type": "markdown", - "id": "22", + "id": "23", "metadata": {}, "source": [ "The next cell plots the results of the loop. For each potential it shows the\n", @@ -576,7 +610,7 @@ { "cell_type": "code", "execution_count": null, - "id": "23", + "id": "24", "metadata": {}, "outputs": [], "source": [ @@ -626,7 +660,7 @@ }, { "cell_type": "markdown", - "id": "24", + "id": "25", "metadata": {}, "source": [ "## Our results\n", @@ -639,7 +673,7 @@ { "cell_type": "code", "execution_count": null, - "id": "25", + "id": "26", "metadata": {}, "outputs": [], "source": [ @@ -648,29 +682,29 @@ "# highest frequency on the band path in THz, at 100, 300, 500, 700 and 900 K\n", "MAX_FREQUENCY = {\n", " \"Ca3Ir4Sn13\": {\n", - " \"OMAT-0-medium\": (5.98, 5.97, 5.93, 5.90, 5.83),\n", - " \"MATPES-PBE-0\": (5.80, 5.75, 5.67, 5.63, 5.65),\n", - " \"MATPES-r2SCAN-0\": (5.95, 5.98, 5.92, 5.88, 5.78),\n", + " \"OMAT-0-medium\": (6.03, 5.97, 5.94, 5.89, 5.78),\n", + " \"MATPES-PBE-0\": (5.80, 5.75, 5.74, 5.66, 5.64),\n", + " \"MATPES-r2SCAN-0\": (6.03, 5.95, 5.91, 5.89, 5.78),\n", " },\n", " \"AlAsPt5\": {\n", - " \"OMAT-0-medium\": (7.75, 7.73, 7.81, 7.76, 7.71),\n", - " \"MATPES-PBE-0\": (7.65, 7.57, 7.48, 7.59, 7.47),\n", - " \"MATPES-r2SCAN-0\": (7.66, 7.62, 7.77, 7.53, 7.43),\n", + " \"OMAT-0-medium\": (7.80, 7.76, 7.70, 7.77, 7.78),\n", + " \"MATPES-PBE-0\": (7.58, 7.66, 7.68, 7.67, 7.80),\n", + " \"MATPES-r2SCAN-0\": (7.65, 7.58, 7.54, 7.68, 7.58),\n", " },\n", " \"Zn3P2\": {\n", - " \"OMAT-0-medium\": (10.59, 10.36, 10.13, 9.67, 9.17),\n", - " \"MATPES-PBE-0\": (10.33, 10.03, 9.86, 9.53, 8.73),\n", - " \"MATPES-r2SCAN-0\": (11.19, 10.85, 10.66, 10.41, 9.97),\n", + " \"OMAT-0-medium\": (10.73, 10.44, 10.05, 9.80, 9.42),\n", + " \"MATPES-PBE-0\": (10.42, 10.08, 9.91, 9.63, 9.27),\n", + " \"MATPES-r2SCAN-0\": (11.26, 10.91, 10.69, 10.33, 10.14),\n", " },\n", " \"Bi4S3N2\": {\n", - " \"OMAT-0-medium\": (17.15, 16.88, 16.05, 16.26, 15.47),\n", - " \"MATPES-PBE-0\": (15.97, 15.64, 15.40, 14.75, 14.31),\n", - " \"MATPES-r2SCAN-0\": (17.62, 16.94, 17.23, 16.87, 15.54),\n", + " \"OMAT-0-medium\": (17.35, 16.93, 15.98, 15.85, 15.12),\n", + " \"MATPES-PBE-0\": (15.64, 15.21, 15.28, 14.56, 14.53),\n", + " \"MATPES-r2SCAN-0\": (17.60, 17.23, 16.52, 16.00, 15.73),\n", " },\n", " \"Er5Tl3\": {\n", - " \"OMAT-0-medium\": (4.23, 4.22, 4.19, 4.22, 4.23),\n", - " \"MATPES-PBE-0\": (4.11, 4.07, 4.01, 3.93, 3.99),\n", - " \"MATPES-r2SCAN-0\": (4.18, 4.09, 4.08, 3.99, 3.96),\n", + " \"OMAT-0-medium\": (4.36, 4.25, 4.28, 4.24, 4.19),\n", + " \"MATPES-PBE-0\": (4.15, 4.12, 4.05, 3.91, 3.86),\n", + " \"MATPES-r2SCAN-0\": (4.18, 4.14, 4.15, 4.11, 3.98),\n", " },\n", "}\n", "# AIMD reference at 300 K: highest frequency in THz, and the mean absolute\n", @@ -688,22 +722,23 @@ " \"MATPES-PBE-0\": 0.17,\n", " \"MATPES-r2SCAN-0\": 0.10,\n", " },\n", - " \"AlAsPt5\": {\"OMAT-0-medium\": 0.11, \"MATPES-PBE-0\": 0.21, \"MATPES-r2SCAN-0\": 0.18},\n", - " \"Zn3P2\": {\"OMAT-0-medium\": 0.19, \"MATPES-PBE-0\": 0.09, \"MATPES-r2SCAN-0\": 0.42},\n", - " \"Bi4S3N2\": {\"OMAT-0-medium\": 0.16, \"MATPES-PBE-0\": 0.43, \"MATPES-r2SCAN-0\": 0.17},\n", - " \"Er5Tl3\": {\"OMAT-0-medium\": 0.17, \"MATPES-PBE-0\": 0.16, \"MATPES-r2SCAN-0\": 0.12},\n", + " \"AlAsPt5\": {\"OMAT-0-medium\": 0.11, \"MATPES-PBE-0\": 0.19, \"MATPES-r2SCAN-0\": 0.17},\n", + " \"Zn3P2\": {\"OMAT-0-medium\": 0.21, \"MATPES-PBE-0\": 0.10, \"MATPES-r2SCAN-0\": 0.44},\n", + " \"Bi4S3N2\": {\"OMAT-0-medium\": 0.15, \"MATPES-PBE-0\": 0.46, \"MATPES-r2SCAN-0\": 0.16},\n", + " \"Er5Tl3\": {\"OMAT-0-medium\": 0.18, \"MATPES-PBE-0\": 0.17, \"MATPES-r2SCAN-0\": 0.13},\n", "}\n", "# runs with imaginary modes on the band path, and runs whose trajectory check\n", "# was not \"stable\"\n", "IMAGINARY = {\n", - " (\"Bi4S3N2\", \"OMAT-0-medium\"): (100, 300, 700),\n", - " (\"Bi4S3N2\", \"MATPES-PBE-0\"): (300, 700, 900),\n", + " (\"AlAsPt5\", \"MATPES-PBE-0\"): (100,),\n", + " (\"Bi4S3N2\", \"OMAT-0-medium\"): (100, 300, 500),\n", + " (\"Bi4S3N2\", \"MATPES-PBE-0\"): (300, 500, 700, 900),\n", " (\"Bi4S3N2\", \"MATPES-r2SCAN-0\"): (100, 300, 500, 700, 900),\n", - " (\"Zn3P2\", \"MATPES-PBE-0\"): (900,),\n", "}\n", "NOT_STABLE = {\n", " (\"Ca3Ir4Sn13\", \"OMAT-0-medium\", 100): \"shifted_or_diffusing\",\n", " (\"Ca3Ir4Sn13\", \"MATPES-r2SCAN-0\", 100): \"shifted_or_diffusing\",\n", + " (\"Er5Tl3\", \"MATPES-r2SCAN-0\", 100): \"shifted_or_diffusing\",\n", " (\"Zn3P2\", \"OMAT-0-medium\", 900): \"melted\",\n", " (\"Zn3P2\", \"MATPES-PBE-0\", 900): \"melted\",\n", "}\n", @@ -730,48 +765,50 @@ }, { "cell_type": "markdown", - "id": "26", + "id": "27", "metadata": {}, "source": [ "The table gives the mean absolute difference from the AIMD reference at 300 K\n", "in THz, over all branches and q-points of the band path.\n", "\n", "- No potential is closest to AIMD for all five materials. MACE-OMAT-0-medium is\n", - " closest for Ca3Ir4Sn13, AlAsPt5 and Bi4S3N2, within 0.07 to 0.16 THz.\n", + " closest for Ca3Ir4Sn13, AlAsPt5 and Bi4S3N2, within 0.07 to 0.15 THz.\n", " MACE-MATPES-r2SCAN-0 is closest for Er5Tl3 and MACE-MATPES-PBE-0 for Zn3P2.\n", - "- MACE-MATPES-PBE-0 gives the lowest frequencies for most materials. For Bi4S3N2 its highest branches lie about\n", - " 1.4 THz below AIMD.\n", + "- MACE-MATPES-PBE-0 gives the lowest frequencies for most materials. For\n", + " Bi4S3N2 its highest branches lie about 1.8 THz below AIMD.\n", "- Most frequencies soften with temperature. The highest frequency of Bi4S3N2\n", - " drops by 1.7 THz from 100 K to 900 K with MACE-OMAT-0-medium. Er5Tl3 barely\n", + " drops by 2.2 THz from 100 K to 900 K with MACE-OMAT-0-medium. AlAsPt5 barely\n", " changes.\n", - "- The imaginary modes at 0 K are gone at every temperature for Ca3Ir4Sn13,\n", - " AlAsPt5, Zn3P2 and Er5Tl3. The one exception is Zn3P2 with MACE-MATPES-PBE-0\n", - " at 900 K, a run that the trajectory check reports as melted. Bi4S3N2 keeps imaginary modes down to -0.7 THz in\n", - " 11 of 15 runs. Its AIMD reference has a small one as well, at -0.12 THz.\n", - " Bi4S3N2 is polar, so these runs and the AIMD reference are compared without\n", - " the non-analytical correction. The force fields give no Born charges.\n", + "- The imaginary modes at 0 K are gone at every temperature for Ca3Ir4Sn13, Zn3P2\n", + " and Er5Tl3. AlAsPt5 keeps a small one, -0.12 THz, with MACE-MATPES-PBE-0 at\n", + " 100 K. Bi4S3N2 keeps imaginary modes down to -0.8 THz in 12 of 15 runs. Its\n", + " AIMD reference has a small one as well, at -0.12 THz. Bi4S3N2 is polar, so\n", + " these runs and the AIMD reference are compared without the non-analytical\n", + " correction. The force fields give no Born charges.\n", "\n", - "The trajectory check did not report \"stable\" for four runs:\n", + "The trajectory check did not report \"stable\" for five runs:\n", "\n", "- By the Lindemann criterion, Zn3P2 melts at 900 K with MACE-OMAT-0-medium and\n", - " MACE-MATPES-PBE-0. Its Lindemann ratio there is 0.165 and 0.171. With\n", - " MACE-MATPES-r2SCAN-0 it reaches 0.148 at 900 K, just below the limit of 0.15.\n", - " No other material reaches the limit up to 900 K. The highest ratio among them\n", - " is 0.136, for Bi4S3N2. Every run keeps the volume of the 0 K cell. Section 2\n", - " adds thermal expansion.\n", - "- Ca3Ir4Sn13 at 100 K is reported as shifted or diffusing with two of the\n", - " potentials. With MACE-OMAT-0-medium the mean positions of the atoms moved\n", - " 0.13 Å away from the starting structure. This is a little more than 1.5\n", - " times their vibration of 0.11 Å. At 300 K the shift is only 0.05 Å. In\n", - " Section 2 the force field first relaxes the cell and the atoms, and the runs\n", - " at 100 K are stable. So the shift comes from running the force field in a\n", - " cell, and with positions, that are not its own. We did not check which\n", - " distortion the atoms move to." + " MACE-MATPES-PBE-0. Its Lindemann ratio there is 0.161 and 0.157. With\n", + " MACE-MATPES-r2SCAN-0 it reaches 0.144 at 900 K, below the limit of 0.15. No\n", + " other material reaches the limit up to 900 K. The highest ratio among them is\n", + " 0.127, for Bi4S3N2. Every run keeps the volume of the 0 K cell. Section 2 adds\n", + " thermal expansion.\n", + "- At 100 K three runs are reported as shifted or diffusing: Ca3Ir4Sn13 with\n", + " MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0, and Er5Tl3 with\n", + " MACE-MATPES-r2SCAN-0. The mean positions of the atoms moved away from the\n", + " starting structure by more than they vibrate. Both materials have imaginary\n", + " modes at 0 K. Section 2 shows the same at 100 K in the force field's own cell,\n", + " for Ca3Ir4Sn13 and AlAsPt5. From 300 K on, their NVT runs are stable.\n", + " Most likely the atoms stay in a slightly distorted structure at 100 K and\n", + " move between such structures at higher temperature. We did not check which\n", + " distortion it is. The force constants of these runs describe vibrations\n", + " around the symmetric structure, so use them with care." ] }, { "cell_type": "markdown", - "id": "27", + "id": "28", "metadata": {}, "source": [ "## 2. Thermal expansion with an NPT MD\n", @@ -785,8 +822,8 @@ " `relax_initial_structure=True`, so that the NPT MD starts from the force\n", " field's own 0 K cell.\n", "2. An NPT MD of the supercell runs at the temperature and at `pressure`, 0 kbar\n", - " by default. It runs for `npt_time`, 8 ps by default, with the same\n", - " thermostat as the NVT MD and a Martyna-Tobias-Klein barostat.\n", + " by default. It runs for `npt_time`, 8 ps by default, with a Nose-Hoover\n", + " thermostat and a Martyna-Tobias-Klein barostat.\n", "3. The cell is averaged over the NPT MD after `npt_equilibration_time`, 2 ps by\n", " default. The average keeps the symmetry of the structure. The atoms keep\n", " their fractional coordinates and are then relaxed in the new cell, with the\n", @@ -805,7 +842,7 @@ { "cell_type": "code", "execution_count": null, - "id": "28", + "id": "29", "metadata": {}, "outputs": [], "source": [ @@ -836,20 +873,20 @@ }, { "cell_type": "markdown", - "id": "29", + "id": "30", "metadata": {}, "source": [ - "Our run took 20 minutes. The NPT MD and the NVT MD took about 8 minutes each\n", + "Our run took 19 minutes. The NPT MD and the NVT MD took about 8 minutes each\n", "and the fit 2 minutes. The 0 K cell of MACE-OMAT-0-medium has a lattice\n", "parameter of 9.825 Å, and its volume is 3.8% larger than that of the PBEsol\n", "cell. At 900 K the lattice parameter is 9.964 Å, 4.3% more volume. Both\n", - "trajectories were stable. The highest frequency is 4.95 THz, against 5.83 THz\n", + "trajectories were stable. The highest frequency is 4.91 THz, against 5.78 THz\n", "in the PBEsol cell in Section 1." ] }, { "cell_type": "markdown", - "id": "30", + "id": "31", "metadata": {}, "source": [ "## The other temperatures, potentials and materials\n", @@ -858,13 +895,13 @@ "effects apart, we also ran them with the relaxation but without the NPT MD,\n", "that is in the force field's own 0 K cell. `run_ft` takes both options. The two\n", "loops run 150 workflows, so they are off by default. Each of our runs took 6 to\n", - "38 minutes on one A100 GPU." + "29 minutes on one A100 GPU." ] }, { "cell_type": "code", "execution_count": null, - "id": "31", + "id": "32", "metadata": {}, "outputs": [], "source": [ @@ -889,7 +926,7 @@ }, { "cell_type": "markdown", - "id": "32", + "id": "33", "metadata": {}, "source": [ "## Our results\n", @@ -904,7 +941,7 @@ { "cell_type": "code", "execution_count": null, - "id": "33", + "id": "34", "metadata": {}, "outputs": [], "source": [ @@ -941,57 +978,57 @@ "# in the force field's relaxed 0 K cell\n", "MAX_RELAXED = {\n", " \"Ca3Ir4Sn13\": {\n", - " \"OMAT-0-medium\": (5.57, 5.55, 5.51, 5.45, 5.37),\n", - " \"MATPES-PBE-0\": (5.38, 5.32, 5.25, 5.20, 5.14),\n", - " \"MATPES-r2SCAN-0\": (5.75, 5.74, 5.68, 5.59, 5.56),\n", + " \"OMAT-0-medium\": (5.58, 5.58, 5.51, 5.47, 5.40),\n", + " \"MATPES-PBE-0\": (5.37, 5.31, 5.26, 5.19, 5.17),\n", + " \"MATPES-r2SCAN-0\": (5.78, 5.76, 5.69, 5.59, 5.54),\n", " },\n", " \"AlAsPt5\": {\n", - " \"OMAT-0-medium\": (6.98, 7.07, 7.08, 7.20, 7.21),\n", - " \"MATPES-PBE-0\": (7.15, 7.30, 7.16, 7.04, 8.46),\n", - " \"MATPES-r2SCAN-0\": (7.52, 7.52, 7.49, 7.52, 7.44),\n", + " \"OMAT-0-medium\": (7.19, 7.07, 7.09, 7.20, 7.17),\n", + " \"MATPES-PBE-0\": (7.23, 7.24, 7.11, 7.09, 7.30),\n", + " \"MATPES-r2SCAN-0\": (7.52, 7.43, 7.42, 7.49, 7.45),\n", " },\n", " \"Zn3P2\": {\n", - " \"OMAT-0-medium\": (10.37, 9.96, 9.74, 9.18, 8.45),\n", - " \"MATPES-PBE-0\": (9.97, 9.65, 9.51, 8.96, 7.97),\n", - " \"MATPES-r2SCAN-0\": (11.14, 10.85, 10.62, 10.18, 9.94),\n", + " \"OMAT-0-medium\": (10.25, 9.82, 9.67, 9.39, 8.91),\n", + " \"MATPES-PBE-0\": (9.99, 9.73, 9.35, 9.06, 8.70),\n", + " \"MATPES-r2SCAN-0\": (11.19, 10.92, 10.46, 10.40, 9.84),\n", " },\n", " \"Bi4S3N2\": {\n", - " \"OMAT-0-medium\": (16.73, 15.92, 15.19, 14.78, 14.15),\n", - " \"MATPES-PBE-0\": (15.48, 15.44, 14.61, 14.41, 14.09),\n", - " \"MATPES-r2SCAN-0\": (17.23, 16.61, 16.17, 16.08, 14.72),\n", + " \"OMAT-0-medium\": (16.74, 15.80, 15.47, 14.80, 14.41),\n", + " \"MATPES-PBE-0\": (15.40, 15.02, 14.32, 14.55, 14.42),\n", + " \"MATPES-r2SCAN-0\": (17.27, 16.95, 16.22, 15.74, 15.42),\n", " },\n", " \"Er5Tl3\": {\n", - " \"OMAT-0-medium\": (4.08, 4.00, 3.94, 3.96, 4.02),\n", - " \"MATPES-PBE-0\": (3.67, 3.61, 3.57, 3.52, 3.52),\n", - " \"MATPES-r2SCAN-0\": (3.83, 3.83, 3.72, 3.68, 3.69),\n", + " \"OMAT-0-medium\": (4.10, 4.07, 4.06, 4.00, 4.01),\n", + " \"MATPES-PBE-0\": (3.70, 3.62, 3.56, 3.57, 3.40),\n", + " \"MATPES-r2SCAN-0\": (3.83, 3.83, 3.77, 3.78, 3.72),\n", " },\n", "}\n", "# the same in the NPT cell\n", "MAX_NPT = {\n", " \"Ca3Ir4Sn13\": {\n", - " \"OMAT-0-medium\": (5.50, 5.44, 5.25, 5.12, 4.95),\n", - " \"MATPES-PBE-0\": (5.32, 5.16, 5.02, 4.84, 4.71),\n", - " \"MATPES-r2SCAN-0\": (5.68, 5.65, 5.45, 5.24, 5.10),\n", + " \"OMAT-0-medium\": (5.56, 5.39, 5.26, 5.11, 4.91),\n", + " \"MATPES-PBE-0\": (5.33, 5.19, 5.03, 4.89, 4.71),\n", + " \"MATPES-r2SCAN-0\": (5.72, 5.59, 5.44, 5.26, 5.06),\n", " },\n", " \"AlAsPt5\": {\n", - " \"OMAT-0-medium\": (6.92, 6.95, 6.65, 6.75, 6.60),\n", - " \"MATPES-PBE-0\": (7.15, 7.13, 7.02, 6.75, 6.55),\n", - " \"MATPES-r2SCAN-0\": (7.42, 7.27, 6.97, 6.90, 6.89),\n", + " \"OMAT-0-medium\": (7.18, 6.90, 6.90, 6.51, 6.88),\n", + " \"MATPES-PBE-0\": (7.15, 6.94, 6.90, 6.63, 6.64),\n", + " \"MATPES-r2SCAN-0\": (7.39, 7.27, 7.26, 7.11, 6.77),\n", " },\n", " \"Zn3P2\": {\n", - " \"OMAT-0-medium\": (10.20, 9.99, 9.52, 8.93, 8.26),\n", - " \"MATPES-PBE-0\": (9.90, 9.53, 9.15, 8.74, 7.85),\n", - " \"MATPES-r2SCAN-0\": (11.11, 10.63, 10.45, 9.95, 9.53),\n", + " \"OMAT-0-medium\": (10.23, 9.82, 9.31, 8.91, 8.42),\n", + " \"MATPES-PBE-0\": (9.97, 9.68, 9.19, 8.86, 8.19),\n", + " \"MATPES-r2SCAN-0\": (11.16, 10.72, 10.39, 9.87, 9.66),\n", " },\n", " \"Bi4S3N2\": {\n", - " \"OMAT-0-medium\": (16.61, 15.66, 14.93, 14.28, 14.05),\n", - " \"MATPES-PBE-0\": (15.26, 15.19, 14.34, 13.64, 12.86),\n", - " \"MATPES-r2SCAN-0\": (17.18, 16.15, 15.71, 15.17, 14.13),\n", + " \"OMAT-0-medium\": (16.39, 15.58, 15.15, 13.75, 13.63),\n", + " \"MATPES-PBE-0\": (15.50, 15.04, 14.74, 13.39, 12.34),\n", + " \"MATPES-r2SCAN-0\": (17.38, 16.63, 16.28, 15.33, 14.67),\n", " },\n", " \"Er5Tl3\": {\n", - " \"OMAT-0-medium\": (4.04, 3.88, 3.83, 3.72, 3.72),\n", - " \"MATPES-PBE-0\": (3.65, 3.55, 3.48, 3.34, 3.13),\n", - " \"MATPES-r2SCAN-0\": (3.75, 3.67, 3.63, 3.50, 3.44),\n", + " \"OMAT-0-medium\": (4.04, 3.99, 3.79, 3.77, 3.66),\n", + " \"MATPES-PBE-0\": (3.67, 3.56, 3.46, 3.32, 3.25),\n", + " \"MATPES-r2SCAN-0\": (3.78, 3.72, 3.64, 3.56, 3.44),\n", " },\n", "}\n", "\n", @@ -1040,7 +1077,7 @@ }, { "cell_type": "markdown", - "id": "34", + "id": "35", "metadata": {}, "source": [ "We do not compare these runs with the AIMD reference. It used the PBEsol cell\n", @@ -1054,44 +1091,47 @@ "- From 0 K to 900 K the volume grows by 3 to 6.5%. Bi4S3N2 with\n", " MACE-MATPES-PBE-0 is the exception, with 11%.\n", "- The larger 0 K cell alone lowers the frequencies. At 300 K the highest\n", - " frequency of Ca3Ir4Sn13 drops from 5.97 THz in the PBEsol cell to 5.55 THz\n", - " in the cell of MACE-OMAT-0-medium. With MACE-MATPES-PBE-0 the 0 K cell of Er5Tl3 is 12% larger, and its\n", - " highest frequency at 300 K drops from 4.07 to 3.61 THz. With\n", - " MACE-MATPES-r2SCAN-0 the cell of Zn3P2 grows by less than 1%, and its highest\n", - " frequency at 300 K stays at 10.85 THz.\n", + " frequency of Ca3Ir4Sn13 drops from 5.97 THz in the PBEsol cell to 5.58 THz\n", + " in the cell of MACE-OMAT-0-medium. With MACE-MATPES-PBE-0 the 0 K cell of\n", + " Er5Tl3 is 12% larger, and its highest frequency at 300 K drops from 4.12 to\n", + " 3.62 THz. With MACE-MATPES-r2SCAN-0 the cell of Zn3P2 grows by less than 1%,\n", + " and its highest frequency at 300 K stays at 10.9 THz.\n", "- Thermal expansion lowers the frequencies further. At 100 K the NPT cell\n", - " changes the highest frequency by about 0.2 THz or less. At 900 K it lowers\n", - " it by 0.1 to 0.6 THz in most runs.\n", - "- At constant volume a frequency can also rise with temperature. In the 0 K\n", - " cell, the highest frequency of AlAsPt5 with MACE-OMAT-0-medium rises from\n", - " 6.98 THz at 100 K to 7.21 THz at 900 K. In the NPT cell it falls from 6.92 to\n", - " 6.60 THz.\n", + " changes the highest frequency by 0.15 THz or less, except for Bi4S3N2. At\n", + " 900 K it lowers it by 0.15 to 0.8 THz. For Bi4S3N2 with MACE-MATPES-PBE-0,\n", + " whose cell grows by 11%, it lowers it by 2.1 THz.\n", + "- At constant volume a frequency can also rise with temperature. In the PBEsol\n", + " cell, the highest frequency of AlAsPt5 with MACE-MATPES-PBE-0 rises from\n", + " 7.58 THz at 100 K to 7.80 THz at 900 K. In the NPT cell it falls from 7.15 to\n", + " 6.64 THz.\n", "\n", "The trajectory check did not report \"stable\" for these runs:\n", "\n", - "- Zn3P2 at 900 K melts with all three potentials, in the NPT MD and in the NVT\n", - " MD that follows. With MACE-MATPES-r2SCAN-0, its Lindemann ratio in Section 1\n", - " stayed just below the limit, at 0.148. In the NPT cell it is 0.153.\n", - "- Bi4S3N2 melts in the larger cells. In the PBEsol cell of Section 1 none of\n", - " its runs melted. With MACE-OMAT-0-medium the NVT MD is reported as melted\n", - " from 700 K, in the 0 K cell and in the NPT cell. With MACE-MATPES-PBE-0 it\n", - " melts at 900 K in both cells. Its NPT MD is also reported as melted at 500 K\n", - " and as shifted at 700 K, and its volume jumps by 5% between these two\n", - " temperatures. With MACE-MATPES-r2SCAN-0 it melts at 900 K in the NPT cell,\n", - " just above the limit.\n", - "- AlAsPt5 at 900 K with MACE-MATPES-PBE-0 is reported as shifted, in the NVT MD\n", - " in the 0 K cell and in the NPT MD. In the 0 K cell its highest frequency\n", - " jumps to 8.46 THz. In the NPT MD its volume does not grow from 700 to 900 K.\n", - " The atoms move away from the starting structure, so the phonons of these two\n", - " runs do not describe it.\n", - "- Ca3Ir4Sn13 at 100 K is stable in both cells, unlike in Section 1.\n", - "\n", - "Bi4S3N2 has imaginary modes on the band path in all 30 runs. Ca3Ir4Sn13 with\n", - "MACE-MATPES-r2SCAN-0 at 100 K has small ones in both cells, and Er5Tl3 with the\n", - "same potential at 100 K in the 0 K cell. So does the run of Zn3P2 with\n", - "MACE-OMAT-0-medium at 900 K in the 0 K cell, which melted.\n", - "\n", - "A run with the NPT MD took 11 to 38 minutes, against 6 to 30 minutes in the\n", + "- Zn3P2 at 900 K melts with all three potentials in the NPT MD and in the NVT MD\n", + " that follows. With MACE-MATPES-r2SCAN-0, its Lindemann ratio in Section 1\n", + " stayed below the limit, at 0.144. In the NVT MD in the NPT cell it is 0.150,\n", + " just above the limit. In the 0 K cell it melts at 900 K with MACE-OMAT-0-medium and\n", + " MACE-MATPES-PBE-0.\n", + "- Bi4S3N2 melts at 900 K in the NPT cell. The NPT MD is reported as melted with\n", + " all three potentials, and the NVT MD that follows with MACE-OMAT-0-medium and\n", + " MACE-MATPES-PBE-0. With MACE-MATPES-PBE-0 the NPT MD is also reported as\n", + " melted at 500 K and as shifted at 700 K, and the volume jumps by 5% between\n", + " these two temperatures. In the PBEsol cell and in the 0 K cell none of its\n", + " runs melted.\n", + "- AlAsPt5 at 900 K with MACE-MATPES-PBE-0: the NPT MD is reported as shifted,\n", + " and its volume does not grow from 700 to 900 K. The cell of this run is not\n", + " reliable, even though the NVT MD that follows is stable.\n", + "- At 100 K, the shift check fires for Ca3Ir4Sn13 and AlAsPt5. In the 0 K cell\n", + " this happens with MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0 for both. In the\n", + " NPT cell it happens for Ca3Ir4Sn13 with MACE-MATPES-r2SCAN-0 and for AlAsPt5\n", + " with all three potentials. Section 1 discusses this.\n", + "\n", + "Bi4S3N2 has imaginary modes on the band path in all 30 runs. A few runs at\n", + "100 K have small ones too: Ca3Ir4Sn13 with MACE-MATPES-r2SCAN-0 in both cells,\n", + "and AlAsPt5 in the NPT cell with MACE-OMAT-0-medium and MACE-MATPES-PBE-0. The\n", + "check reports all of these runs as shifted.\n", + "\n", + "A run with the NPT MD took 12 to 29 minutes, against 6 to 21 minutes in the\n", "0 K cell. To compare a force field with DFT phonons in a given cell, run in\n", "that cell, as in Section 1. To predict the phonons at a temperature with the\n", "force field alone, use `run_npt=True`." @@ -1099,7 +1139,7 @@ }, { "cell_type": "markdown", - "id": "35", + "id": "36", "metadata": {}, "source": [ "## 3. MD length and number of snapshots for KNaICl\n", @@ -1122,7 +1162,7 @@ { "cell_type": "code", "execution_count": null, - "id": "36", + "id": "37", "metadata": {}, "outputs": [], "source": [ @@ -1147,7 +1187,7 @@ { "cell_type": "code", "execution_count": null, - "id": "37", + "id": "38", "metadata": {}, "outputs": [], "source": [ @@ -1156,40 +1196,36 @@ "# by potential, rows 4, 8 and 16 ps, columns 25, 50 and 100 snapshots\n", "MAE_GRID = { # mean absolute difference from AIMD at 300 K in THz\n", " \"OMAT-0-medium\": (\n", - " (0.146, 0.149, 0.150),\n", - " (0.159, 0.145, 0.144),\n", - " (0.156, 0.155, 0.149),\n", + " (0.179, 0.181, 0.147),\n", + " (0.167, 0.170, 0.148),\n", + " (0.162, 0.171, 0.158),\n", " ),\n", " \"MATPES-PBE-0\": (\n", - " (0.138, 0.121, 0.121),\n", - " (0.124, 0.129, 0.127),\n", - " (0.127, 0.135, 0.117),\n", + " (0.158, 0.137, 0.133),\n", + " (0.129, 0.108, 0.120),\n", + " (0.142, 0.089, 0.105),\n", " ),\n", " \"MATPES-r2SCAN-0\": (\n", - " (0.137, 0.123, 0.123),\n", - " (0.138, 0.131, 0.128),\n", - " (0.147, 0.128, 0.128),\n", + " (0.188, 0.161, 0.162),\n", + " (0.191, 0.184, 0.136),\n", + " (0.152, 0.154, 0.169),\n", " ),\n", "}\n", "MAX_GRID = { # highest frequency on the band path in THz\n", - " \"OMAT-0-medium\": ((5.63, 5.65, 5.63), (5.63, 5.73, 5.70), (5.32, 5.43, 5.44)),\n", - " \"MATPES-PBE-0\": ((5.03, 5.23, 5.26), (5.25, 5.22, 5.33), (5.12, 5.13, 5.27)),\n", - " \"MATPES-r2SCAN-0\": ((5.23, 5.40, 5.40), (5.39, 5.66, 5.56), (5.27, 5.60, 5.54)),\n", + " \"OMAT-0-medium\": ((5.48, 5.52, 5.66), (5.35, 5.56, 5.63), (5.57, 5.62, 5.61)),\n", + " \"MATPES-PBE-0\": ((5.20, 5.18, 5.13), (5.07, 5.22, 5.33), (5.05, 5.31, 5.24)),\n", + " \"MATPES-r2SCAN-0\": ((5.64, 5.51, 5.57), (5.32, 5.58, 5.42), (5.42, 5.53, 5.53)),\n", "}\n", "IMAGINARY_GRID = { # True if the band path has imaginary modes\n", - " \"OMAT-0-medium\": ((False, True, True), (False, False, False), (True, True, False)),\n", - " \"MATPES-PBE-0\": ((True, False, False), (True, True, True), (False, True, False)),\n", - " \"MATPES-r2SCAN-0\": (\n", - " (False, False, False),\n", - " (True, True, False),\n", - " (True, False, False),\n", - " ),\n", + " \"OMAT-0-medium\": ((False, True, True), (True, True, False), (True, True, False)),\n", + " \"MATPES-PBE-0\": ((True, True, True), (False, True, False), (False, False, True)),\n", + " \"MATPES-r2SCAN-0\": ((True, True, True), (True, True, False), (True, True, True)),\n", "}\n", "\n", "fig, axes = plt.subplots(1, 3, figsize=(13, 3.6))\n", "for ax, model in zip(axes, MODEL_FILES, strict=True):\n", " grid = np.array(MAE_GRID[model])\n", - " image = ax.imshow(grid, cmap=\"viridis\", vmin=0.11, vmax=0.16)\n", + " image = ax.imshow(grid, cmap=\"viridis\", vmin=0.08, vmax=0.20)\n", " for i in range(3):\n", " for j in range(3):\n", " mark = \" *\" if IMAGINARY_GRID[model][i][j] else \"\"\n", @@ -1216,50 +1252,41 @@ }, { "cell_type": "markdown", - "id": "38", + "id": "39", "metadata": {}, "source": [ "In the plot, a star marks a run with imaginary modes on the band path. The\n", "table gives the highest frequency in THz.\n", "\n", - "- The mean absolute difference from AIMD lies between 0.12 and 0.16 THz in every\n", - " run. It shows no trend with the MD length or the number of snapshots. Each\n", - " run is one MD trajectory, so these differences are the noise of a single run.\n", - "- The highest frequency changes by up to 0.4 THz between runs, also without a\n", + "- The mean absolute difference from AIMD lies between 0.09 and 0.19 THz. It\n", + " shows no trend with the MD length or the number of snapshots. Each run is one\n", + " MD trajectory, so these differences are the noise of a single run.\n", + "- The highest frequency changes by up to 0.3 THz between runs, also without a\n", " trend.\n", - "- 12 of the 27 runs have imaginary modes on the band path, down to -0.9 THz.\n", - " They sit at q-points that are not commensurate with the supercell, such as\n", - " (1/2, 1/2, 0). There the frequencies are interpolated from the fitted force\n", - " constants. The AIMD reference has no imaginary modes in the same supercell. So\n", - " they come from the noise of the fit. They appear in 5 of 9 runs with 25\n", - " snapshots, 5 of 9 with 50 and 2 of 9 with 100.\n", - "- We ran the whole grid a second time. The 4 and 8 ps runs gave the same\n", - " numbers to the third decimal. The 16 ps runs did not. Their highest frequency\n", - " changed by up to 0.2 THz, and imaginary modes appeared or went away in three\n", - " of them. With 100 snapshots, 2 of 9 runs had imaginary modes the first time\n", - " and 3 of 9 the second time. Runs with the same potential and MD length share\n", - " one trajectory. At 16 ps their Lindemann ratios already differed in the first\n", - " round, so the trajectory itself changed. Most likely, tiny numerical\n", - " differences on the GPU grow over a long MD run.\n", - "- The MD takes most of the time. With MACE-OMAT-0-medium a run took 3.8, 6.0\n", - " and 10.6 minutes for 4, 8 and 16 ps. Going from 50 to 100 snapshots added a\n", - " few seconds of force calculations and fitting.\n", - "\n", - "We also ran Bi4S3N2 and Zn3P2 at 300 K with 100 snapshots. The mean absolute\n", - "difference from AIMD changed by 0.03 THz or less. The fit of Zn3P2 did not take\n", - "longer. Bi4S3N2 kept its imaginary modes with all three potentials, so these are\n", - "unlikely to be noise of the fit.\n", - "\n", - "With a force field the force calculations cost little next to the MD, so 100\n", - "snapshots are worth using. The default stays at 50, because with VASP each\n", - "snapshot is a DFT calculation of the whole supercell. For the MD length, 4 ps\n", - "already gave the same agreement with AIMD for KNaICl. We kept the default of\n", - "8 ps for the other materials." + "- 19 of the 27 runs have imaginary modes on the band path, down to -1.5 THz. In\n", + " all but two of them they only appear at q-points that are not commensurate\n", + " with the supercell, where the frequencies are interpolated from the fitted\n", + " force constants. The AIMD reference has no imaginary modes in the same\n", + " supercell. They appear in 6 of 9 runs with 25 snapshots, 8 of 9 with 50 and\n", + " 5 of 9 with 100. In an earlier round of the same grid with a Nose-Hoover\n", + " thermostat, 12 of the 27 runs had them.\n", + "- The random forces of the Langevin thermostat are not seeded, so a second run\n", + " of the grid would not give the same numbers.\n", + "- The MD takes most of the time. With MACE-OMAT-0-medium a run with 50\n", + " snapshots took 3.5, 6.1 and 10.8 minutes for 4, 8 and 16 ps. Going from 50 to\n", + " 100 snapshots added a few seconds of force calculations and fitting.\n", + "\n", + "With a force field the force calculations cost little next to the MD, so more\n", + "snapshots are cheap. In this test they did not remove the imaginary modes,\n", + "though. The default stays at 50, because with VASP each snapshot is a DFT\n", + "calculation of the whole supercell. For the MD length, 4 ps gave about the same\n", + "agreement with AIMD as 8 and 16 ps for KNaICl. We kept the default of 8 ps for\n", + "the other materials." ] }, { "cell_type": "markdown", - "id": "39", + "id": "40", "metadata": {}, "source": [ "## Known limitations\n", @@ -1280,9 +1307,10 @@ "check whether any of the trajectories reported as melted is a liquid. A warning\n", "is raised and the fit is still done.\n", "\n", - "Every result above comes from one MD trajectory. Section 3 shows that two runs\n", - "with different settings can differ by about 0.04 THz on average and by up to\n", - "0.4 THz in the highest frequency." + "Every result above comes from one MD trajectory. Section 3 shows that runs with\n", + "different settings differ by up to 0.1 THz on average and by up to 0.3 THz in\n", + "the highest frequency. The Langevin thermostat is not seeded, so a second run\n", + "gives somewhat different numbers." ] } ], From c84d02980ee42fae8a9aeb61438765f818d4ae23 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 23:15:43 -0700 Subject: [PATCH 20/43] Say in the docs how to include thermal expansion in the finite-temperature workflow --- docs/user/codes/vasp.md | 5 +++-- 1 file changed, 3 insertions(+), 2 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index da6fae4fe6..5b966d87b9 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -411,8 +411,9 @@ The cluster space grows faster there than the number of displacements the workfl #### Finite-temperature phonons `FiniteTemperaturePhononMaker` fits effective harmonic force constants at a finite temperature, as in the temperature-dependent effective potential ([TDEP](https://doi.org/10.1103/PhysRevB.84.180301)) method. -They include the anharmonic effects at that temperature, at the volume of the relaxed structure. -By default, thermal expansion is not included. +They include the anharmonic effects at that temperature. +By default, the MD runs at the volume of the relaxed structure, so thermal expansion is not included. +It can be switched on with an NPT MD before the NVT MD, see below. The structure is relaxed first. An NVT MD run then samples the displacements at the temperature. By default, it runs for 8 ps at 300 K with a time step of 1 fs and a Langevin thermostat. From 0faae0249903ab7359d9f21811dfd5cca456f3fa Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Sun, 4 Oct 2026 23:42:58 -0700 Subject: [PATCH 21/43] inline the VASP defaults, share the NAC setup, add PHEASY_CMD --- docs/user/codes/vasp.md | 14 +- .../flows/finite_temperature_phonons.py | 9 +- .../common/jobs/finite_temperature_phonons.py | 103 +++++++++------ src/atomate2/common/jobs/pheasy.py | 23 +++- src/atomate2/common/jobs/phonons.py | 45 +++++++ .../flows/finite_temperature_phonons.py | 2 +- src/atomate2/settings.py | 2 + .../vasp/flows/finite_temperature_phonons.py | 121 +++++++++--------- .../jobs/test_finite_temperature_phonons.py | 18 +++ .../flows/test_finite_temperature_phonons.py | 10 ++ 10 files changed, 232 insertions(+), 115 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 5b966d87b9..3bfb713367 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -346,6 +346,8 @@ phonon_flow = PhononMaker(min_length=15.0, store_force_constants=False).make( Alternatively, users can accelerate the calculation of interatomic force constants using the machine-learning-based [Pheasy code](https://doi.org/10.48550/arXiv.2508.01020). The `pheasy` extra, `pip install "atomate2[pheasy]"`, installs the pheasy version this workflow needs, together with phonopy and ALM. +The workflows call the `pheasy` command. +A different command can be set with `PHEASY_CMD` in the atomate2 settings. ALM is compiled from source. If that build fails, see the ALM instructions below. By design, these workflows have the same basic structure as the harmonic forcefield workflows and use [Phonopy](https://doi.org/10.7566/JPSJ.92.012001) in part to compute the phonon spectrum. To use `Pheasy` in the previous example, we would replace the import string to `from atomate2.vasp.flows.pheasy import PhononMaker`. @@ -476,7 +478,7 @@ Three more makers are in `atomate2.forcefields.flows.finite_temperature_phonons` Each has a `from_force_field_name` method to choose the force field. They need the package of the force field, for example `mace-torch` for MACE. All of them use the same fit. -A force field NPT MD uses ASE's `MTKNPT`, a Nosé-Hoover chain thermostat with the barostat of [Martyna et al.](https://doi.org/10.1063/1.467468). +A force field NPT MD uses ASE's `MTKNPT`, a Nosé-Hoover thermostat with the barostat of [Martyna et al.](https://doi.org/10.1063/1.467468). ```python from atomate2.forcefields.flows.finite_temperature_phonons import ( @@ -491,6 +493,16 @@ flow = maker.make(structure) `run_npt=True` sets the NPT MD and the relaxation of the atoms in its cell. +A force field gives no Born charges, so the force field makers skip the non-analytical correction by default. +The Born charges and the dielectric tensor can still come from VASP. +Either pass `born` and `epsilon_static` to `make`, or set a VASP `born_maker`: + +```python +from atomate2.vasp.jobs.core import DielectricMaker + +maker.born_maker = DielectricMaker() +``` + Known limitations: - pheasy needs a diagonal supercell matrix. diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 27507812cd..3d53f9d8d6 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -364,7 +364,12 @@ def make( structure = relax.output.structure if self.born_maker is not None and (born is None or epsilon_static is None): - born_job = self.born_maker.make(structure, prev_dir=prev_dir) + # as in the phonon workflow, so that a VASP born_maker can run after a + # force field relaxation, whose folder has no VASP files + born_kwargs = {} + if self.prev_calc_dir_argname is not None: + born_kwargs[self.prev_calc_dir_argname] = prev_dir + born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) born = born_job.output.calcs_reversed[0].output.outcar["born"] epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static @@ -488,7 +493,7 @@ def make_md( @property @abstractmethod def prev_calc_dir_argname(self) -> str | None: - """Name of the argument that passes prev_dir to the phonon displacement maker. + """Name of the prev_dir argument of the phonon displacement and Born makers. As this differs between codes, it is implemented by the inheriting class. """ diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 58eb86448b..2e8413289a 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -16,7 +16,6 @@ from phonopy.file_IO import parse_FORCE_CONSTANTS from phonopy.harmonic.dynmat_to_fc import get_commensurate_points from phonopy.interface.vasp import write_vasp -from phonopy.structure.symmetry import symmetrize_borns_and_epsilon from pymatgen.core import Structure from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure from pymatgen.io.vasp import Incar, Kpoints, Poscar, Xdatcar @@ -34,6 +33,7 @@ _get_kpath, _run_band_structure_and_plot, _run_total_dos_and_plot, + _set_nac_params, ) from atomate2.common.schemas.finite_temperature_phonons import ( FiniteTemperaturePhononDoc, @@ -390,6 +390,60 @@ def _assess_trajectory( ) +def average_npt_structure( + cells: np.ndarray, + structure: Structure, + supercell_matrix: Matrix3D, + symprec: float, +) -> Structure: + """ + Average the supercell lattices of an NPT MD into a unit cell. + + The metric tensor L L^T of the supercell, with the lattice vectors as the + rows of L, is averaged over the cells. Unlike the lattice vectors, it does + not change when the cell rotates. It is converted to the metric tensor of + the unit cell with the supercell matrix and averaged over the point group of + the structure, so that the cell keeps its symmetry. The new lattice is the + stretch of the lattice of the structure, without a rotation, that has this + metric tensor. The atoms keep their fractional coordinates. + + Parameters + ---------- + cells: np.ndarray + Supercell lattices of the frames to average, with the lattice vectors + as rows, in Angstrom. + structure: Structure + Unit cell whose supercell the NPT MD started from. + supercell_matrix: Matrix3D + Supercell matrix. + symprec: float + Symmetry precision for the point group of the structure. + + Returns + ------- + Structure + The unit cell with the averaged lattice. + """ + metric = np.mean([cell @ cell.T for cell in cells], axis=0) + inv_matrix = np.linalg.inv(np.array(supercell_matrix, dtype=float)) + metric = inv_matrix @ metric @ inv_matrix.T + # a rotation W of fractional coordinates leaves the metric tensor of the + # symmetric cell unchanged, W^T G W = G + analyzer = SpacegroupAnalyzer(structure, symprec=symprec) + rotations = [op.rotation_matrix for op in analyzer.get_symmetry_operations()] + metric = np.mean([rot.T @ metric @ rot for rot in rotations], axis=0) + lattice = structure.lattice.matrix + inv_lattice = np.linalg.inv(lattice) + eigvals, eigvecs = np.linalg.eigh(inv_lattice @ metric @ inv_lattice.T) + stretch = eigvecs @ np.diag(np.sqrt(eigvals)) @ eigvecs.T + return Structure( + lattice @ stretch, + structure.species, + structure.frac_coords, + site_properties=structure.site_properties, + ) + + @job def get_npt_structure( npt_dir: str, @@ -404,14 +458,9 @@ def get_npt_structure( """ Get the unit cell at the temperature from an NPT MD run. - The metric tensor L L^T of the supercell, with the lattice vectors as the - rows of L, is averaged over the frames after equilibration_time. Unlike the - lattice vectors, it does not change when the cell rotates. It is converted - to the metric tensor of the unit cell with the supercell matrix and averaged - over the point group of the structure, so that the cell keeps its symmetry. - The new lattice is the stretch of the lattice of the structure, without a - rotation, that has this metric tensor. The atoms keep their fractional - coordinates. The NPT trajectory is checked as in :obj:`select_md_snapshots`. + The cells after equilibration_time are averaged with + :obj:`average_npt_structure`. The NPT trajectory is checked as in + :obj:`select_md_snapshots`. Parameters ---------- @@ -446,23 +495,8 @@ def get_npt_structure( f"The NPT trajectory has {len(cells)} frames of {time_step} fs, none " f"of them after the {equilibration_time} ps that are left out." ) - metric = np.mean([cell @ cell.T for cell in cells[n_equil:]], axis=0) - inv_matrix = np.linalg.inv(np.array(supercell_matrix, dtype=float)) - metric = inv_matrix @ metric @ inv_matrix.T - # a rotation W of fractional coordinates leaves the metric tensor of the - # symmetric cell unchanged, W^T G W = G - analyzer = SpacegroupAnalyzer(structure, symprec=symprec) - rotations = [op.rotation_matrix for op in analyzer.get_symmetry_operations()] - metric = np.mean([rot.T @ metric @ rot for rot in rotations], axis=0) - lattice = structure.lattice.matrix - inv_lattice = np.linalg.inv(lattice) - eigvals, eigvecs = np.linalg.eigh(inv_lattice @ metric @ inv_lattice.T) - stretch = eigvecs @ np.diag(np.sqrt(eigvals)) @ eigvecs.T - npt_structure = Structure( - lattice @ stretch, - structure.species, - structure.frac_coords, - site_properties=structure.site_properties, + npt_structure = average_npt_structure( + cells[n_equil:], structure, supercell_matrix, symprec ) health = _assess_trajectory(frac_coords, energies, reference, time_step) @@ -781,22 +815,7 @@ def fit_finite_temperature_phonons( borns = epsilon = None if born is not None and epsilon_static is not None: - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - ) - if not np.all(np.isclose(borns, 0.0)): - # the factor is for forces in eV/Angstrom, as from VASP and the force - # fields - phonon.nac_params = { - "born": borns, - "dielectric": epsilon, - "factor": 14.399652, - } + borns, epsilon = _set_nac_params(phonon, born, epsilon_static, symprec) # frequencies at the q-points commensurate with the supercell matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index f64d380b76..7096f997e5 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -38,6 +38,7 @@ CubicSupercellTransformation, ) +from atomate2 import SETTINGS from atomate2.common.jobs.phonons import ( ANGSTROM_TO_BOHR, _generate_phonon_object, @@ -316,7 +317,10 @@ def _run_harmonic_fit( Log file of the fit. None keeps pheasy's default. """ dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) - base = f"pheasy --scell SPOSCAR --dim {dim} -w 2 --symprec {float(symprec)}" + base = ( + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR --dim {dim} -w 2 " + f"--symprec {float(symprec)}" + ) fit = f"{base} -f --full_ifc" if use_lasso: # pheasy's default --tol of 1e-4 leaves the fit unconverged, so the force @@ -401,7 +405,7 @@ def _run_anharmonic_fit( """ dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) base = ( - f"pheasy --scell SPOSCAR --dim {dim} -w {anhar_max_order} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR --dim {dim} -w {anhar_max_order} " f"--symprec {float(symprec)}" ) cutoffs = f"--c3 {float(fcs_cutoff_radius[1] / ANGSTROM_TO_BOHR)}" @@ -997,7 +1001,8 @@ def generate_frequencies_eigenvectors( shutil.copy(filename, refit_dir / filename) pheasy_cmd_11 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR " + f"--dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -s -w 2 --c2 " f"10.0 --symprec {float(symprec)} " @@ -1005,14 +1010,16 @@ def generate_frequencies_eigenvectors( ) pheasy_cmd_12 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR " + f"--dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -c --symprec " f"{float(symprec)} --c2 10.0 -w 2" ) pheasy_cmd_13 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR " + f"--dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -w 2 -d --symprec " f"{float(symprec)} --c2 10.0 " @@ -1024,7 +1031,8 @@ def generate_frequencies_eigenvectors( if len(phonon.displacements) > 3: pheasy_cmd_14 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR " + f"--dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --c2 10.0 " f"--full_ifc -w 2 --symprec {float(symprec)} " @@ -1034,7 +1042,8 @@ def generate_frequencies_eigenvectors( else: pheasy_cmd_14 = ( - f"pheasy --scell SPOSCAR --dim {int(supercell_matrix[0][0])} " + f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR " + f"--dim {int(supercell_matrix[0][0])} " f"{int(supercell_matrix[1][1])} " f"{int(supercell_matrix[2][2])} -f --full_ifc " f"--c2 10.0 -w 2 --symprec {float(symprec)} " diff --git a/src/atomate2/common/jobs/phonons.py b/src/atomate2/common/jobs/phonons.py index a148f047d0..3935d2f840 100644 --- a/src/atomate2/common/jobs/phonons.py +++ b/src/atomate2/common/jobs/phonons.py @@ -164,6 +164,51 @@ def _get_num_harmonic_supercells( return int(np.ceil(num_disp_sc * multiplier)) + 1 +def _set_nac_params( + phonon: Phonopy, + born: Sequence[Matrix3D], + epsilon_static: Matrix3D, + symprec: float, + is_symmetry: bool = True, +) -> tuple[np.ndarray, np.ndarray]: + """ + Symmetrize the Born charges and the dielectric tensor and set the NAC. + + The non-analytical correction is only set if a Born charge is not zero. + + Parameters + ---------- + phonon: Phonopy + Phonopy object whose unit cell the Born charges belong to. + born: Sequence[Matrix3D] + Born effective charges, one per atom of the unit cell. + epsilon_static: Matrix3D + High-frequency dielectric tensor. + symprec: float + Symmetry precision. + is_symmetry: bool + Whether to symmetrize the Born charges and the dielectric tensor. + + Returns + ------- + tuple[np.ndarray, np.ndarray] + The Born charges and the dielectric tensor. + """ + borns, epsilon = symmetrize_borns_and_epsilon( + ucell=phonon.unitcell, + borns=np.array(born), + epsilon=np.array(epsilon_static), + symprec=symprec, + primitive_matrix=phonon.primitive_matrix, + supercell_matrix=phonon.supercell_matrix, + is_symmetry=is_symmetry, + ) + if not np.all(np.isclose(borns, 0.0)): + # e^2 / (4 pi epsilon_0) in eV Angstrom, for forces in eV/Angstrom + phonon.nac_params = {"born": borns, "dielectric": epsilon, "factor": 14.399652} + return borns, epsilon + + def _get_kpath( structure: Structure, kpath_scheme: str, symprec: float, **kpath_kwargs ) -> tuple: diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index 704d6522a3..ff395ac975 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -125,7 +125,7 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): Its time constant gives a period of about 40 time steps, like SMASS = 0 in VASP. The initial velocities of the first MD job follow the Maxwell-Boltzmann distribution, seeded with random_seed, with zero total - momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover chain + momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover thermostat and barostat that change the whole cell, whatever the thermostat setting (Martyna et al., J. Chem. Phys. 101, 4177 (1994)). Its thermostat time constant is that of the Nose-Hoover thermostat above, and diff --git a/src/atomate2/settings.py b/src/atomate2/settings.py index 32bcbf2da2..99c21f13c1 100644 --- a/src/atomate2/settings.py +++ b/src/atomate2/settings.py @@ -258,6 +258,8 @@ class Atomate2Settings(BaseSettings): "GBRV_v1.5", description="location of JDFTX pseudopotentials." ) + PHEASY_CMD: str = Field("pheasy", description="The command to run pheasy.") + LAMMPS_CMD: str = Field("lmp", description="The command to run LAMMPS.") LAMMPS_MPICMD: str | None = Field( diff --git a/src/atomate2/vasp/flows/finite_temperature_phonons.py b/src/atomate2/vasp/flows/finite_temperature_phonons.py index 725da4ea83..1c22f2fc98 100644 --- a/src/atomate2/vasp/flows/finite_temperature_phonons.py +++ b/src/atomate2/vasp/flows/finite_temperature_phonons.py @@ -15,6 +15,7 @@ from atomate2.vasp.sets.core import ( LangevinMDSetGenerator, MDSetGenerator, + StaticSetGenerator, TightRelaxSetGenerator, ) @@ -23,36 +24,6 @@ from atomate2.vasp.jobs.base import BaseVaspMaker -# The relaxation, the MD and the phonon displacement calculations use the same -# smearing and k-point density. -_ELECTRONIC_INCAR = {"ISMEAR": 0, "SIGMA": 0.05} -_KPOINTS = {"reciprocal_density": 100} - -# The MD only samples the displacements. The forces of the fit come from the -# phonon displacement calculations, which use tighter settings. -_MD_INCAR = { - "ENCUT": 500, - "EDIFF": 1e-5, - "ALGO": "Normal", - "LREAL": "Auto", - "NBLOCK": 1, - "LWAVE": False, - **_ELECTRONIC_INCAR, -} -# changes to the INCAR of PhononDisplacementMaker -_STATIC_INCAR = { - "ENCUT": 600, - "ENAUG": 1360, - "PREC": "Accurate", - "LASPH": True, - "NELM": 200, - "LWAVE": False, - **_ELECTRONIC_INCAR, -} -_RELAX_INCAR = { - key: _STATIC_INCAR[key] for key in ("ENCUT", "ENAUG", "PREC", "LASPH") -} | _ELECTRONIC_INCAR - # INCAR tags of the MD that the flow sets _MD_FLOW_TAGS = ( "IBRION", @@ -77,35 +48,6 @@ def _check_md_incar(user_incar: dict, name: str) -> None: ) -def _get_relax_maker() -> DoubleRelaxMaker: - """Get a tight relaxation with the basis set and smearing of the statics.""" - return DoubleRelaxMaker.from_relax_maker( - TightRelaxMaker( - input_set_generator=TightRelaxSetGenerator( - user_incar_settings=dict(_RELAX_INCAR), - user_kpoints_settings=dict(_KPOINTS), - ) - ) - ) - - -def _get_md_maker() -> MDMaker: - """Get the MD maker, whose temperature, steps and thermostat the flow sets.""" - return MDMaker( - input_set_generator=MDSetGenerator( - user_incar_settings=dict(_MD_INCAR), - user_kpoints_settings=dict(_KPOINTS), - ) - ) - - -def _get_phonon_displacement_maker() -> PhononDisplacementMaker: - """Get the static maker for the forces on the snapshots.""" - maker = PhononDisplacementMaker() - maker.input_set_generator.user_incar_settings.update(_STATIC_INCAR) - return maker - - @dataclass class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): """ @@ -161,11 +103,66 @@ class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): Code of the MD. """ - bulk_relax_maker: Maker | None = field(default_factory=_get_relax_maker) + bulk_relax_maker: Maker | None = field( + default_factory=lambda: DoubleRelaxMaker.from_relax_maker( + TightRelaxMaker( + input_set_generator=TightRelaxSetGenerator( + user_incar_settings={ + "ENCUT": 600, + "ENAUG": 1360, + "PREC": "Accurate", + "LASPH": True, + "ISMEAR": 0, + "SIGMA": 0.05, + }, + user_kpoints_settings={"reciprocal_density": 100}, + ) + ) + ) + ) born_maker: BaseVaspMaker | None = field(default_factory=DielectricMaker) - md_maker: Maker = field(default_factory=_get_md_maker) + md_maker: Maker = field( + default_factory=lambda: MDMaker( + input_set_generator=MDSetGenerator( + user_incar_settings={ + "ENCUT": 500, + "EDIFF": 1e-5, + "ALGO": "Normal", + "LREAL": "Auto", + "NBLOCK": 1, + "LWAVE": False, + "ISMEAR": 0, + "SIGMA": 0.05, + }, + user_kpoints_settings={"reciprocal_density": 100}, + ) + ) + ) phonon_displacement_maker: Maker = field( - default_factory=_get_phonon_displacement_maker + default_factory=lambda: PhononDisplacementMaker( + input_set_generator=StaticSetGenerator( + user_incar_settings={ + "IBRION": 2, + "ISIF": 3, + "NSW": 0, + "ENCUT": 600, + "ENAUG": 1360, + "EDIFF": 1e-7, + "PREC": "Accurate", + "ALGO": "Normal", + "LASPH": True, + "NELM": 200, + "LREAL": False, + "LAECHG": False, + "LCHARG": False, + "LWAVE": False, + "ISMEAR": 0, + "SIGMA": 0.05, + }, + user_kpoints_settings={"reciprocal_density": 100}, + auto_ispin=True, + ) + ) ) code: str = "vasp" md_code: str = "vasp" diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index 262dbddabd..d241f28ee3 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -23,6 +23,7 @@ _assess_trajectory, _get_rms_displacement, _remove_center_of_mass, + average_npt_structure, fit_finite_temperature_phonons, get_md_restart_structure, get_md_supercell, @@ -275,6 +276,23 @@ def test_select_md_snapshots_forcefields(cu_supercell): assert output["trajectory_health"]["verdict"] == "melted" +def test_average_npt_structure(): + """Rotated cells of an expanded tetragonal supercell average to its unit cell.""" + structure = Structure( + Lattice.tetragonal(3.0, 5.0), ["Si", "Si"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ) + matrix = np.diag([2, 2, 1]) + supercell = np.diag([1.01, 1.01, 1.03]) @ matrix @ structure.lattice.matrix + rng = np.random.default_rng(7) + cells = [] + for _ in range(5): + rotation, _ = np.linalg.qr(rng.normal(size=(3, 3))) + cells.append(supercell @ rotation.T) + averaged = average_npt_structure(np.array(cells), structure, matrix, 1e-3) + assert np.allclose(averaged.lattice.matrix, np.diag([3.03, 3.03, 5.15])) + assert np.allclose(averaged.frac_coords, structure.frac_coords) + + def test_get_npt_structure(cu_supercell): unit_cell = AseAtomsAdaptor.get_structure(bulk("Cu", "fcc", a=3.61, cubic=True)) rng = np.random.default_rng(4) diff --git a/tests/forcefields/flows/test_finite_temperature_phonons.py b/tests/forcefields/flows/test_finite_temperature_phonons.py index 4540b24150..6e2895357b 100644 --- a/tests/forcefields/flows/test_finite_temperature_phonons.py +++ b/tests/forcefields/flows/test_finite_temperature_phonons.py @@ -22,6 +22,7 @@ ) from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker from atomate2.forcefields.md import ForceFieldMDMaker +from atomate2.vasp.jobs.core import DielectricMaker EMT = {"@module": "ase.calculators.emt", "@callable": "EMT"} @@ -165,6 +166,15 @@ def test_force_field_npt_maker(cu3au): assert not any("NPT" in job.name for job in flow.jobs) +def test_force_field_with_vasp_born_charges(cu3au): + """A VASP born_maker after a force field relaxation gets no prev_dir.""" + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name(EMT) + maker.born_maker = DielectricMaker() + flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) + born_job = next(job for job in flow.jobs if job.name == "dielectric") + assert born_job.function_kwargs.get("prev_dir") is None + + def test_finite_temperature_phonon_maker_emt(clean_dir, cu3au): """Run the whole workflow with EMT on Cu3Au at 300 K.""" # a 2x2x2 supercell of the cubic cell, 32 atoms, and 2 ps of MD at 2 fs in From 42e6b4818e95bbf65a9ad4fe9037de2b00f82a6d Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 11:07:18 -0700 Subject: [PATCH 22/43] Add force field Born charges and dielectric tensors with MACE-Field --- .github/workflows/testing.yml | 6 +- docs/user/codes/forcefields.md | 32 +++++++++ pyproject.toml | 5 ++ src/atomate2/common/flows/hiphive.py | 10 ++- src/atomate2/common/flows/pheasy.py | 10 ++- src/atomate2/common/flows/phonons.py | 33 +++++---- src/atomate2/common/jobs/hiphive.py | 33 +++------ src/atomate2/common/jobs/pheasy.py | 33 +++------ src/atomate2/common/jobs/phonons.py | 32 +++------ src/atomate2/common/schemas/phonons.py | 81 ++++++++++++++++------ src/atomate2/forcefields/flows/hiphive.py | 12 ++-- src/atomate2/forcefields/flows/pheasy.py | 12 ++-- src/atomate2/forcefields/flows/phonons.py | 12 ++-- src/atomate2/forcefields/jobs.py | 84 +++++++++++++++++++++-- src/atomate2/forcefields/schemas.py | 22 +++++- src/atomate2/forcefields/utils.py | 21 +++++- tests/forcefields/conftest.py | 36 ++++++++++ tests/forcefields/flows/test_phonon.py | 32 ++++++++- tests/forcefields/test_jobs.py | 24 ++++++- tests/forcefields/test_mace_field.py | 55 +++++++++++++++ 20 files changed, 452 insertions(+), 133 deletions(-) create mode 100644 tests/forcefields/test_mace_field.py diff --git a/.github/workflows/testing.yml b/.github/workflows/testing.yml index 7405467740..2f8a35a073 100644 --- a/.github/workflows/testing.yml +++ b/.github/workflows/testing.yml @@ -41,7 +41,7 @@ jobs: fail-fast: false matrix: python-version: ["3.12"] - dep-group: ["generic", "torch-limited", "e3nn-limited", "numpy-limited"] + dep-group: ["generic", "torch-limited", "e3nn-limited", "numpy-limited", "mace-field"] steps: - name: Check out repo @@ -91,9 +91,11 @@ jobs: # torch-limited loads the heaviest MLIP stack (matgl + nequip + torch); # running it single-process avoids the OOM that kills the runner when # xdist spawns multiple workers each holding a copy of the models. + # The MACE-Field fork replaces mace-torch, so its group only runs the + # MACE-Field tests. run: | micromamba activate a2 - pytest -v --durations=5 -n ${{ matrix.dep-group == 'torch-limited' && '1' || 'auto' }} --cov=atomate2 --cov-report=xml tests/forcefields + pytest -v --durations=5 -n ${{ matrix.dep-group == 'torch-limited' && '1' || 'auto' }} --cov=atomate2 --cov-report=xml ${{ matrix.dep-group == 'mace-field' && 'tests/forcefields/test_mace_field.py' || 'tests/forcefields' }} - name: Forcefield tutorial if: matrix.dep-group == 'torch-limited' diff --git a/docs/user/codes/forcefields.md b/docs/user/codes/forcefields.md index c926c04b37..dbd04b8783 100644 --- a/docs/user/codes/forcefields.md +++ b/docs/user/codes/forcefields.md @@ -38,6 +38,7 @@ Support is provided for the following models, which can be selected using `atoma | MACE-MP-0 | `MACE` or `MACE_MP_0` (recommended) | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MP-0b3 | `MACE_MP_0B3` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MPA-0 | `MACE_MPA_0` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | +| MACE-Field | `MACE_Field` | [10.1103/b116-xy8k](https://doi.org/10.1103/b116-xy8k) | Born effective charges and dielectric tensor only, via `ForceFieldDielectricMaker`. Needs the MACE-Field fork of `mace_torch` and a model file. [See notes below.](#mace-field-notes) | | MatPES-PBE | `MATPES_PBE` | [10.48550/arXiv.2503.04070](https://doi.org/10.48550/arXiv.2503.04070) | Relies on `matgl`. Defaults to TensorNet architecture, but can also use M3GNet or CHGNet architectures via kwargs. See `atomate2.forcefields.utils._DEFAULT_CALCULATOR_KWARGS` for more options. | | MatPES-r2SCAN | `MATPES_R2SCAN`| [10.48550/arXiv.2503.04070](https://doi.org/10.48550/arXiv.2503.04070) | Relies on `matgl`. Defaults to TensorNet architecture, but can also use M3GNet or CHGNet architectures via kwargs. See `atomate2.forcefields.utils._DEFAULT_CALCULATOR_KWARGS` for more options. | | MatterSim | `MatterSim` | [arXiv:2405.04967](https://arxiv.org/abs/2405.04967) | Requires the `mattersim` package | @@ -73,6 +74,37 @@ However, this may not be preserved in future versions, and `calculator_meta` is [^calculator-meta-type-annotation]: In this context, the type annotation of the decoded dict should be either `Type[Calculator]` or `Callable[..., Calculator]`, where `Calculator` is from `ase.calculators.calculator`. +## Notes on MACE-Field {#mace-field-notes} + +[MACE-Field](https://doi.org/10.1103/b116-xy8k) gives the Born effective charges and the high-frequency dielectric tensor of inorganic crystals. +`ForceFieldDielectricMaker` computes them, and the phonon workflows use them for the non-analytical correction when it is set as `born_maker`. +MACE-Field is a fork of MACE that installs as `mace_torch`, so it cannot be installed together with MACE. +It is in the `strict-forcefields-mace-field` extra. +The model file has to be downloaded from the [MACE-Field releases](https://github.com/mdi-group/mace-field/releases) and passed as `model`: + +```py +from atomate2.forcefields.flows.phonons import PhononMaker +from atomate2.forcefields.jobs import ForceFieldDielectricMaker + +born_maker = ForceFieldDielectricMaker( + calculator_kwargs={"model": "MACEField-MH-0-omat-dielectric.model"} +) +flow = PhononMaker(born_maker=born_maker).make(structure) +``` + +The model head "mp-dielectric" is used by default. +The dielectric tensor is 1 + chi, with chi the electronic susceptibility of the model. + +```{warning} +This feature is new and has not been tested widely. +It might still change in future versions. +``` + +We compared it with the DFPT results in the Materials Project's Harmonic Phonon Database for NaCl, KCl, MgO and Bi4S3N2. +For NaCl, KCl and MgO, which are likely in its training data, the Born charges agree to 0.02 e and the dielectric constants to about 5%. +For Bi4S3N2, the Born charges are about 15% too small and the dielectric tensor is off by up to 10%. +The authors report a dielectric constant about 10% too large for alpha-quartz. + ## Notes on FairChem (Meta) models {#fairchem-notes} The FAIRChem models provided by Meta require extra authentication via HuggingFace: diff --git a/pyproject.toml b/pyproject.toml index 179e3ed325..74987aee39 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -138,6 +138,11 @@ strict-forcefields-e3nn-limited = [ strict-forcefields-numpy-limited = [ "nequip-allegro==0.8.3", ] +# MACE-Field is a fork of MACE that installs as mace-torch, so it cannot share +# a group with mace-torch. Remove this group once ACEsuit/mace#1177 is released. +strict-forcefields-mace-field = [ + "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64", +] strict = [ "atomate2[cclib, phonons, lobster, openmm, mp, defects, ase, ase-ext]", diff --git a/src/atomate2/common/flows/hiphive.py b/src/atomate2/common/flows/hiphive.py index 37bbd9a543..c8f84bf643 100644 --- a/src/atomate2/common/flows/hiphive.py +++ b/src/atomate2/common/flows/hiphive.py @@ -24,7 +24,11 @@ from pymatgen.core.structure import Structure from atomate2.aims.jobs.base import BaseAimsMaker - from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker + from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, + ) from atomate2.vasp.jobs.base import BaseVaspMaker SUPPORTED_CODES = frozenset(("vasp", "aims", "forcefields")) @@ -138,7 +142,7 @@ class BasePhononMaker(PurePhonopyMaker, ABC): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker, .BaseAsimsMaker, .BaseVaspMaker, or None + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None Maker to compute the BORN charges. phonon_displacement_maker: .ForceFieldStaticMaker, .BaseAimsMaker, .BaseVaspMaker Maker used to compute the forces for a supercell. @@ -182,7 +186,7 @@ class BasePhononMaker(PurePhonopyMaker, ABC): static_energy_maker: ForceFieldRelaxMaker | BaseVaspMaker | BaseAimsMaker | None = ( None ) - born_maker: ForceFieldStaticMaker | BaseVaspMaker | None = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None phonon_displacement_maker: ForceFieldStaticMaker | BaseVaspMaker | BaseAimsMaker = ( None ) diff --git a/src/atomate2/common/flows/pheasy.py b/src/atomate2/common/flows/pheasy.py index 8e3d5f64a9..910b606866 100644 --- a/src/atomate2/common/flows/pheasy.py +++ b/src/atomate2/common/flows/pheasy.py @@ -26,7 +26,11 @@ from pymatgen.core.structure import Structure from atomate2.aims.jobs.base import BaseAimsMaker - from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker + from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, + ) from atomate2.vasp.jobs.base import BaseVaspMaker SUPPORTED_CODES = frozenset(("vasp", "aims", "forcefields")) @@ -180,7 +184,7 @@ class BasePhononMaker(PurePhonopyMaker, ABC): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker, .BaseAsimsMaker, .BaseVaspMaker, or None + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None Maker to compute the BORN charges. phonon_displacement_maker: .ForceFieldStaticMaker, .BaseAimsMaker, .BaseVaspMaker Maker used to compute the forces for a supercell. @@ -231,7 +235,7 @@ class BasePhononMaker(PurePhonopyMaker, ABC): static_energy_maker: ForceFieldRelaxMaker | BaseVaspMaker | BaseAimsMaker | None = ( None ) - born_maker: ForceFieldStaticMaker | BaseVaspMaker | None = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None phonon_displacement_maker: ForceFieldStaticMaker | BaseVaspMaker | BaseAimsMaker = ( None ) diff --git a/src/atomate2/common/flows/phonons.py b/src/atomate2/common/flows/phonons.py index 9f30cc8c80..557c162b98 100644 --- a/src/atomate2/common/flows/phonons.py +++ b/src/atomate2/common/flows/phonons.py @@ -27,7 +27,11 @@ from pymatgen.core.structure import Structure from atomate2.aims.jobs.base import BaseAimsMaker - from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker + from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, + ) from atomate2.torchsim.core import TorchSimOptimizeMaker, TorchSimStaticMaker from atomate2.vasp.jobs.base import BaseVaspMaker @@ -106,8 +110,8 @@ class BasePhononMaker(Maker, ABC): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker, .BaseAsimsMaker, .BaseVaspMaker, - .TorchSimStaticMaker, or None + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, .TorchSimStaticMaker, + or None Maker to compute the BORN charges. phonon_displacement_maker: .ForceFieldStaticMaker, .BaseAimsMaker, .BaseVaspMaker, .TorchSimStaticMaker @@ -167,9 +171,9 @@ class BasePhononMaker(Maker, ABC): | TorchSimStaticMaker | None ) = None - born_maker: ForceFieldStaticMaker | BaseVaspMaker | TorchSimStaticMaker | None = ( - None - ) + born_maker: ( + ForceFieldDielectricMaker | BaseVaspMaker | TorchSimStaticMaker | None + ) = None phonon_displacement_maker: ( ForceFieldStaticMaker | BaseVaspMaker | BaseAimsMaker | TorchSimStaticMaker ) = None @@ -339,12 +343,17 @@ def make( born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - # I am not happy how we currently access "born" charges - # This is very vasp specific code aims and forcefields - # do not support this at the moment, if this changes we have - # to update this section - epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static - born = born_job.output.calcs_reversed[0].output.outcar["born"] + # a force field dielectric document has the Born charges and the + # dielectric tensor as fields, a VASP task document has them in its + # last calculation + schema = born_job.output_schema + if schema is not None and "born" in schema.model_fields: + epsilon_static = born_job.output.epsilon_static + born = born_job.output.born + else: + calc_output = born_job.output.calcs_reversed[0].output + epsilon_static = calc_output.epsilon_static + born = calc_output.outcar["born"] born_run_job_dir = born_job.output.dir_name born_run_uuid = born_job.output.uuid diff --git a/src/atomate2/common/jobs/hiphive.py b/src/atomate2/common/jobs/hiphive.py index f1b073707e..8d5791d03e 100644 --- a/src/atomate2/common/jobs/hiphive.py +++ b/src/atomate2/common/jobs/hiphive.py @@ -22,7 +22,6 @@ from packaging.version import parse as parse_version from phonopy.file_IO import parse_FORCE_CONSTANTS from phonopy.interface.vasp import write_vasp -from phonopy.structure.symmetry import symmetrize_borns_and_epsilon from pymatgen.core import Structure from pymatgen.io.ase import AseAtomsAdaptor from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure @@ -43,6 +42,7 @@ _run_band_structure_and_plot, _run_total_dos_and_plot, ) +from atomate2.common.schemas.phonons import _set_nac_params if TYPE_CHECKING: from ase.atoms import Atoms @@ -525,29 +525,14 @@ def generate_frequencies_eigenvectors( # get the born charges and dielectric constant if born is not None and epsilon_static is not None: - if len(structure) == len(born): - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - raise ValueError( - "Number of born charges does not agree with number of atoms" - ) - - if code == "vasp" and not np.all(np.isclose(borns, 0.0)): - phonon.nac_params = { - "born": borns, - "dielectric": epsilon, - "factor": 14.399652, - } - # Other codes could be added here - + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) else: borns = None epsilon = None diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 6c69ca1176..4564e1ea57 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -28,7 +28,6 @@ from packaging.version import parse as parse_version from phonopy.file_IO import parse_FORCE_CONSTANTS from phonopy.interface.vasp import write_vasp -from phonopy.structure.symmetry import symmetrize_borns_and_epsilon from pymatgen.core import Structure from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure from pymatgen.io.vasp import Kpoints @@ -47,6 +46,7 @@ _run_band_structure_and_plot, _run_total_dos_and_plot, ) +from atomate2.common.schemas.phonons import _set_nac_params if TYPE_CHECKING: from collections.abc import Sequence @@ -717,29 +717,14 @@ def generate_frequencies_eigenvectors( # get the born charges and dielectric constant if born is not None and epsilon_static is not None: - if len(structure) == len(born): - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - raise ValueError( - "Number of born charges does not agree with number of atoms" - ) - - if code == "vasp" and not np.all(np.isclose(borns, 0.0)): - phonon.nac_params = { - "born": borns, - "dielectric": epsilon, - "factor": 14.399652, - } - # Other codes could be added here - + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) else: borns = None epsilon = None diff --git a/src/atomate2/common/jobs/phonons.py b/src/atomate2/common/jobs/phonons.py index a148f047d0..7130f10279 100644 --- a/src/atomate2/common/jobs/phonons.py +++ b/src/atomate2/common/jobs/phonons.py @@ -23,7 +23,6 @@ from packaging.version import parse as parse_version from phonopy import Phonopy from phonopy.phonon.band_structure import get_band_qpoints_and_path_connections -from phonopy.structure.symmetry import symmetrize_borns_and_epsilon from pymatgen.core import Structure from pymatgen.io.phonopy import ( get_ph_bs_symm_line, @@ -39,7 +38,7 @@ from pymatgen.symmetry.kpath import KPathSeek from atomate2.common.schemas.phonons import PhononBSDOSDoc as Atomate2PhononBSDOSDoc -from atomate2.common.schemas.phonons import get_factor +from atomate2.common.schemas.phonons import _set_nac_params, get_factor from atomate2.common.utils import check_class_name, get_supercell_matrix from atomate2.vasp.jobs.base import BaseVaspMaker @@ -544,27 +543,14 @@ def generate_frequencies_eigenvectors( set_of_forces = [np.array(forces) for forces in displacement_data["forces"]] if born is not None and epsilon_static is not None: - if len(structure) == len(born): - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - raise ValueError( - "Number of Born charges does not agree with number of atoms" - ) - if code == "vasp" and not np.all(np.isclose(borns, 0.0)): - phonon.nac_params = { - "born": borns, - "dielectric": epsilon, - "factor": 14.399652, # TODO: where is this magic number coming from? - } - # Other codes could be added here + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) else: borns = None epsilon = None diff --git a/src/atomate2/common/schemas/phonons.py b/src/atomate2/common/schemas/phonons.py index 30d4a645d0..5d728fa238 100644 --- a/src/atomate2/common/schemas/phonons.py +++ b/src/atomate2/common/schemas/phonons.py @@ -62,6 +62,58 @@ def get_factor(code: str) -> float: raise ValueError(f"Frequency conversion factor for code ({code}) not defined.") +def _set_nac_params( + phonon: Phonopy, + born: Sequence[Matrix3D], + epsilon_static: Matrix3D, + symprec: float, + code: str, + is_symmetry: bool = True, +) -> tuple[np.ndarray, np.ndarray]: + """ + Symmetrize the Born charges and the dielectric tensor and set the NAC. + + The non-analytical correction is only set for VASP and force field + calculations, whose forces are in eV/Angstrom, and only if a Born charge + is not zero. + + Parameters + ---------- + phonon: Phonopy + Phonopy object whose unit cell the Born charges belong to. + born: Sequence[Matrix3D] + Born effective charges, one per atom of the unit cell. + epsilon_static: Matrix3D + High-frequency dielectric tensor. + symprec: float + Symmetry precision. + code: str + Code of the force calculations. + is_symmetry: bool + Whether to symmetrize the Born charges and the dielectric tensor. + + Returns + ------- + tuple[np.ndarray, np.ndarray] + The Born charges and the dielectric tensor. + """ + if len(born) != len(phonon.unitcell): + raise ValueError("Number of Born charges does not agree with number of atoms") + borns, epsilon = symmetrize_borns_and_epsilon( + ucell=phonon.unitcell, + borns=np.array(born), + epsilon=np.array(epsilon_static), + symprec=symprec, + primitive_matrix=phonon.primitive_matrix, + supercell_matrix=phonon.supercell_matrix, + is_symmetry=is_symmetry, + ) + if code in ("vasp", "forcefields") and not np.all(np.isclose(borns, 0.0)): + # e^2 / (4 pi epsilon_0) in eV Angstrom, for forces in eV/Angstrom + phonon.nac_params = {"born": borns, "dielectric": epsilon, "factor": 14.399652} + return borns, epsilon + + class PhononComputationalSettings(BaseModel): """Collection to store computational settings for the phonon computation.""" @@ -360,27 +412,14 @@ def from_forces_born( set_of_forces = [np.array(forces) for forces in displacement_data["forces"]] if born is not None and epsilon_static is not None: - if len(structure) == len(born): - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - raise ValueError( - "Number of Born charges does not agree with number of atoms" - ) - if code == "vasp" and not np.all(np.isclose(borns, 0.0)): - phonon.nac_params = { - "born": borns, - "dielectric": epsilon, - "factor": 14.399652, - } - # Other codes could be added here + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) else: borns = None epsilon = None diff --git a/src/atomate2/forcefields/flows/hiphive.py b/src/atomate2/forcefields/flows/hiphive.py index f074f2a172..21ad8b60e3 100644 --- a/src/atomate2/forcefields/flows/hiphive.py +++ b/src/atomate2/forcefields/flows/hiphive.py @@ -7,7 +7,11 @@ from atomate2 import SETTINGS from atomate2.common.flows.hiphive import BasePhononMaker -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) @dataclass @@ -80,8 +84,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker or None - Maker to compute the BORN charges. + born_maker: .ForceFieldDielectricMaker or None + Maker to compute the BORN charges, for example with MACE-Field. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -130,7 +134,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldStaticMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/pheasy.py b/src/atomate2/forcefields/flows/pheasy.py index d9db491809..03e46f0f5a 100644 --- a/src/atomate2/forcefields/flows/pheasy.py +++ b/src/atomate2/forcefields/flows/pheasy.py @@ -7,7 +7,11 @@ from atomate2 import SETTINGS from atomate2.common.flows.pheasy import BasePhononMaker -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) @dataclass @@ -80,8 +84,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker or None - Maker to compute the BORN charges. + born_maker: .ForceFieldDielectricMaker or None + Maker to compute the BORN charges, for example with MACE-Field. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -130,7 +134,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldStaticMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/phonons.py b/src/atomate2/forcefields/flows/phonons.py index dfc428a5cb..b55b0bee0b 100644 --- a/src/atomate2/forcefields/flows/phonons.py +++ b/src/atomate2/forcefields/flows/phonons.py @@ -7,7 +7,11 @@ from atomate2 import SETTINGS from atomate2.common.flows.phonons import BasePhononMaker -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) from atomate2.forcefields.utils import MLFF if TYPE_CHECKING: @@ -88,8 +92,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldStaticMaker or None - Maker to compute the BORN charges. + born_maker: .ForceFieldDielectricMaker or None + Maker to compute the BORN charges, for example with MACE-Field. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -139,7 +143,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldStaticMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/jobs.py b/src/atomate2/forcefields/jobs.py index 6ac7295b39..b617089c20 100644 --- a/src/atomate2/forcefields/jobs.py +++ b/src/atomate2/forcefields/jobs.py @@ -5,17 +5,29 @@ import logging import warnings from dataclasses import dataclass, field +from pathlib import Path from typing import TYPE_CHECKING -from jobflow import job +import numpy as np +from jobflow import Maker, job +from pymatgen.io.ase import AseAtomsAdaptor +from pymatgen.util.due import Doi, due from atomate2.ase.jobs import AseRelaxMaker -from atomate2.forcefields.schemas import ForceFieldTaskDocument -from atomate2.forcefields.utils import _FORCEFIELD_DATA_OBJECTS, MLFF, ForceFieldMixin +from atomate2.forcefields.schemas import ( + ForceFieldDielectricDocument, + ForceFieldTaskDocument, +) +from atomate2.forcefields.utils import ( + _FORCEFIELD_DATA_OBJECTS, + MLFF, + ForceFieldMixin, + _get_pkg_version, + revert_default_dtype, +) if TYPE_CHECKING: from collections.abc import Callable - from pathlib import Path from pymatgen.core.structure import Molecule, Structure @@ -213,3 +225,67 @@ class ForceFieldStaticMaker(ForceFieldRelaxMaker): optimizer_kwargs: dict = field(default_factory=dict) calculator_kwargs: dict = field(default_factory=dict) task_document_kwargs: dict = field(default_factory=dict) + + +@due.dcite( + Doi("10.1103/b116-xy8k"), + description="MACE-Field: Born effective charges and dielectric tensor", +) +@dataclass +class ForceFieldDielectricMaker(ForceFieldMixin, Maker): + """ + Maker for the Born effective charges and the dielectric tensor from a force field. + + The force field must give the Born effective charges and the electronic + susceptibility chi as the results "becs" and "polarizability", as MACE-Field + does. The high-frequency dielectric tensor is 1 + chi. Unless an electric + field is set in calculator_kwargs, both are computed at zero field. + + Parameters + ---------- + name : str + The job name. + force_field_name : str or .MLFF or dict + The name of the force field. + calculator_kwargs : dict + Keyword arguments that will get passed to the ASE calculator. For + MACE-Field, "model" is the path of the model file. + """ + + name: str = "Force field dielectric" + force_field_name: str | MLFF | dict = MLFF.MACE_Field + calculator_kwargs: dict = field(default_factory=dict) + + @job(output_schema=ForceFieldDielectricDocument) + def make( + self, structure: Structure, prev_dir: str | Path | None = None + ) -> ForceFieldDielectricDocument: + """ + Compute the Born effective charges and the dielectric tensor. + + Parameters + ---------- + structure: .Structure + A pymatgen structure. + prev_dir : str or Path or None + A previous calculation directory. Unused, just added to match the + method signature of other makers. + + Returns + ------- + ForceFieldDielectricDocument + """ + atoms = AseAtomsAdaptor.get_atoms(structure) + with revert_default_dtype(): + atoms.calc = self._get_calculator() + atoms.get_potential_energy() + return ForceFieldDielectricDocument( + structure=structure, + born=atoms.calc.results["becs"].tolist(), + epsilon_static=( + np.eye(3) + atoms.calc.results["polarizability"].reshape(3, 3) + ).tolist(), + forcefield_name=self.force_field_name, + forcefield_version=_get_pkg_version(self.calculator_meta), + dir_name=str(Path.cwd()), + ) diff --git a/src/atomate2/forcefields/schemas.py b/src/atomate2/forcefields/schemas.py index 51a0e67308..2283112883 100644 --- a/src/atomate2/forcefields/schemas.py +++ b/src/atomate2/forcefields/schemas.py @@ -5,9 +5,10 @@ import warnings from typing import TYPE_CHECKING, Any +from emmet.core.math import Matrix3D from emmet.core.types.enums import StoreTrajectoryOption from pydantic import BaseModel, Field -from pymatgen.core import Molecule +from pymatgen.core import Molecule, Structure from atomate2.ase.schemas import ( AseMoleculeTaskDoc, @@ -178,3 +179,22 @@ def from_ase_compatible_result( if isinstance(result.final_mol_or_struct, Molecule) else cls ).from_ase_task_doc(ase_task_doc, **ff_kwargs) + + +class ForceFieldDielectricDocument(BaseModel): + """Born effective charges and dielectric tensor from a force field.""" + + structure: Structure = Field(description="The structure of the calculation.") + born: list[Matrix3D] = Field( + description="Born effective charges, one per site, in units of e." + ) + epsilon_static: Matrix3D = Field( + description="The high-frequency dielectric tensor." + ) + forcefield_name: str | None = Field(None, description="Name of the force field.") + forcefield_version: str | None = Field( + None, description="Version of the force field package." + ) + dir_name: str | None = Field( + None, description="Directory where the calculation was performed." + ) diff --git a/src/atomate2/forcefields/utils.py b/src/atomate2/forcefields/utils.py index 2cd486e43e..19636fe628 100644 --- a/src/atomate2/forcefields/utils.py +++ b/src/atomate2/forcefields/utils.py @@ -40,6 +40,7 @@ class MLFF(Enum): # TODO inherit from StrEnum when 3.11+ MACE_MP_0 = "MACE-MP-0" MACE_MPA_0 = "MACE-MPA-0" MACE_MP_0B3 = "MACE-MP-0b3" + MACE_Field = "MACE-Field" GAP = "GAP" M3GNet = "M3GNet" CHGNet = "CHGNet" @@ -78,6 +79,7 @@ def _missing_(cls, value: Any) -> Any: MLFF.MACE_MP_0: {"model": "medium"}, MLFF.MACE_MP_0B3: {"model": "medium-0b3"}, MLFF.MACE_MPA_0: {"model": "medium-mpa-0"}, + MLFF.MACE_Field: {"head": "mp-dielectric", "default_dtype": "float64"}, MLFF.MATPES_PBE: { "architecture": "TensorNet", "version": "2025.2", @@ -428,6 +430,17 @@ def ase_calculator( else: calculator = mace_mp(default_dtype=default_dtype or "", **kwargs) + case MLFF.MACE_Field: + # needs the MACE-Field fork of mace and the path of a model file + from mace.calculators import MACECalculator + + calculator = MACECalculator( + model_paths=kwargs.pop("model"), + model_type="MACEField", + default_dtype=default_dtype or "", + **kwargs, + ) + case MLFF.Nequip | MLFF.Allegro: from nequip.integrations.ase import NequIPCalculator @@ -541,7 +554,13 @@ def _get_pkg_name(calculator_meta: MLFF | str | dict[str, Any]) -> str | None: ff_pkg = "fairchem.core" case MLFF.GAP: ff_pkg = "quippy-ase" - case MLFF.MACE | MLFF.MACE_MP_0 | MLFF.MACE_MPA_0 | MLFF.MACE_MP_0B3: + case ( + MLFF.MACE + | MLFF.MACE_MP_0 + | MLFF.MACE_MPA_0 + | MLFF.MACE_MP_0B3 + | MLFF.MACE_Field + ): ff_pkg = "mace-torch" case MLFF.MatterSim: ff_pkg = "mattersim" diff --git a/tests/forcefields/conftest.py b/tests/forcefields/conftest.py index 5646bc08e1..dd1dd901fd 100644 --- a/tests/forcefields/conftest.py +++ b/tests/forcefields/conftest.py @@ -3,13 +3,18 @@ import hashlib import tempfile import urllib.request +from importlib import import_module +from importlib.util import find_spec from pathlib import Path from typing import TYPE_CHECKING +import numpy as np import pytest import torch +from ase.calculators.calculator import Calculator, all_changes from emmet.core.utils import get_hash_blocked +from atomate2.forcefields.jobs import ForceFieldDielectricMaker from atomate2.forcefields.utils import MLFF, _get_pkg_version if TYPE_CHECKING: @@ -21,6 +26,10 @@ ) for mlff in MLFF } +# the MACE-Field fork installs as mace-torch, so only its model class tells them apart +_INSTALLED_MLFF["MACE_Field"] = find_spec("mace") is not None and hasattr( + import_module("mace.modules.extensions"), "MACEField" +) def mlff_is_installed(mlff: str | MLFF) -> bool: @@ -53,3 +62,30 @@ def get_deepmd_pretrained_model_path(test_dir: Path) -> Path: raise RuntimeError(f"MD5 mismatch: {file_md5} != {ref_md5}") yield Path(local_path.name) local_path.close() + + +class FakeDielectricCalculator(Calculator): + """Born charges of +2 and -2 and a susceptibility of 3, as MACE-Field gives them. + + The atoms of the first species get +2, all others -2. + """ + + implemented_properties = ("energy", "becs", "polarizability") + + def calculate(self, atoms=None, properties=None, system_changes=all_changes): + super().calculate(atoms, properties, system_changes) + sign = np.where(self.atoms.numbers == self.atoms.numbers[0], 1.0, -1.0) + self.results = { + "energy": 0.0, + "becs": 2 * sign[:, None, None] * np.eye(3), + "polarizability": 3 * np.eye(3), + } + + +@pytest.fixture +def fake_dielectric_calculator(monkeypatch): + monkeypatch.setattr( + ForceFieldDielectricMaker, + "_get_calculator", + lambda _self: FakeDielectricCalculator(), + ) diff --git a/tests/forcefields/flows/test_phonon.py b/tests/forcefields/flows/test_phonon.py index 71765c4fdb..708ac1d0ee 100644 --- a/tests/forcefields/flows/test_phonon.py +++ b/tests/forcefields/flows/test_phonon.py @@ -16,10 +16,15 @@ ) from jobflow import Flow, JobStore, run_locally from numpy.testing import assert_allclose +from pymatgen.core import Lattice from pymatgen.core.structure import Structure from atomate2.forcefields.flows.phonons import PhononMaker -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) from atomate2.forcefields.utils import MLFF from ..conftest import mlff_is_installed # noqa: TID252 @@ -286,3 +291,28 @@ def test_ext_load_phonon_initialization(): assert maker.bulk_relax_maker.ase_calculator_name == "mace_mp" assert maker.static_energy_maker.ase_calculator_name == "mace_mp" assert maker.phonon_displacement_maker.ase_calculator_name == "mace_mp" + + +def test_phonon_wf_force_field_born_charges(clean_dir, fake_dielectric_calculator): + """Born charges from a force field dielectric job enter the NAC.""" + structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(4.17), ["Ni", "O"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ).get_primitive_structure() + emt = {"@module": "ase.calculators.emt", "@callable": "EMT"} + flow = PhononMaker( + bulk_relax_maker=None, + static_energy_maker=None, + phonon_displacement_maker=ForceFieldStaticMaker(force_field_name=emt), + born_maker=ForceFieldDielectricMaker(), + min_length=8, + create_thermal_displacements=False, + store_force_constants=False, + ).make(structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + doc = responses[flow[-1].uuid][1].output + + assert np.array(doc.born) == pytest.approx( + np.array([2, -2])[:, None, None] * np.eye(3) + ) + assert np.array(doc.epsilon_static) == pytest.approx(4 * np.eye(3)) + assert doc.phonon_bandstructure.has_nac diff --git a/tests/forcefields/test_jobs.py b/tests/forcefields/test_jobs.py index 92accf3033..2591070d7b 100644 --- a/tests/forcefields/test_jobs.py +++ b/tests/forcefields/test_jobs.py @@ -6,13 +6,18 @@ import numpy as np import pytest from jobflow import run_locally -from pymatgen.core import Molecule, Structure +from pymatgen.core import Lattice, Molecule, Structure from pymatgen.symmetry.analyzer import SpacegroupAnalyzer from pytest import approx from atomate2.forcefields import MLFF -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) from atomate2.forcefields.schemas import ( + ForceFieldDielectricDocument, ForceFieldMoleculeTaskDocument, ForceFieldTaskDocument, ) @@ -909,3 +914,18 @@ def test_roundtrip_legacy(si_structure: Structure, import_str: str): assert deser.maker.mlff == MLFF.Forcefield assert isinstance(deser.maker.calculator, MACECalculator) assert isinstance(deser.maker.calculator, Calculator) + + +def test_dielectric_maker(fake_dielectric_calculator, clean_dir): + structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(5.6), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ).get_primitive_structure() + job = ForceFieldDielectricMaker(force_field_name="MACE-Field").make(structure) + output = run_locally(job, ensure_success=True)[job.uuid][1].output + + assert isinstance(output, ForceFieldDielectricDocument) + assert output.structure == structure + assert np.array(output.born) == approx(np.array([2, -2])[:, None, None] * np.eye(3)) + # eps_inf = 1 + chi + assert np.array(output.epsilon_static) == approx(4 * np.eye(3)) + assert output.forcefield_name == "MLFF.MACE_Field" diff --git a/tests/forcefields/test_mace_field.py b/tests/forcefields/test_mace_field.py new file mode 100644 index 0000000000..0e734c81e4 --- /dev/null +++ b/tests/forcefields/test_mace_field.py @@ -0,0 +1,55 @@ +"""Test the Born charges and the dielectric tensor of the MACE-Field model. + +The MACE-Field fork of mace installs as mace-torch, so these tests only run in +the mace-field CI group. +""" + +import hashlib +import urllib.request + +import numpy as np +import pytest +from emmet.core.utils import get_hash_blocked +from jobflow import run_locally +from pymatgen.core import Lattice, Structure + +from atomate2.forcefields.jobs import ForceFieldDielectricMaker + +from .conftest import mlff_is_installed + +pytestmark = pytest.mark.skipif( + not mlff_is_installed("MACE_Field"), reason="MACE-Field is not installed" +) + +MODEL_URL = ( + "https://github.com/mdi-group/mace-field/releases/download/1.0.2/" + "MACEField-MH-0-omat-dielectric.model" +) +MODEL_MD5 = "1dac204204e368d94b2b8a597c9fdf8d" + + +@pytest.fixture(scope="module") +def mace_field_model(tmp_path_factory): + path = tmp_path_factory.mktemp("mace_field") / MODEL_URL.rsplit("/", 1)[-1] + urllib.request.urlretrieve(MODEL_URL, path) + assert get_hash_blocked(str(path), hasher=hashlib.md5()) == MODEL_MD5 + return path + + +def test_mace_field_dielectric_maker(mace_field_model, clean_dir): + structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(5.64), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ).get_primitive_structure() + job = ForceFieldDielectricMaker( + calculator_kwargs={"model": str(mace_field_model)} + ).make(structure) + output = run_locally(job, ensure_success=True)[job.uuid][1].output + + born = np.array(output.born) + # the acoustic sum rule holds by construction + assert born.sum(axis=0) == pytest.approx(np.zeros((3, 3)), abs=1e-6) + # cubic, so the tensors are isotropic. DFPT gives about 1.09 and 2.5. + species = [str(site.specie) for site in output.structure] + assert born[species.index("Na")] == pytest.approx(1.0898 * np.eye(3), abs=1e-3) + epsilon = np.array(output.epsilon_static) + assert epsilon == pytest.approx(2.5845 * np.eye(3), abs=1e-3) From ac2d733a01794725657c22c937729c7e4c2af378 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 11:26:26 -0700 Subject: [PATCH 23/43] Reshape the flattened MACE-Field Born charges to 3x3 tensors --- src/atomate2/forcefields/jobs.py | 3 ++- tests/forcefields/conftest.py | 2 +- 2 files changed, 3 insertions(+), 2 deletions(-) diff --git a/src/atomate2/forcefields/jobs.py b/src/atomate2/forcefields/jobs.py index b617089c20..ba767b9862 100644 --- a/src/atomate2/forcefields/jobs.py +++ b/src/atomate2/forcefields/jobs.py @@ -281,7 +281,8 @@ def make( atoms.get_potential_energy() return ForceFieldDielectricDocument( structure=structure, - born=atoms.calc.results["becs"].tolist(), + # MACE-Field returns the Born charges flattened, one row of 9 per atom + born=atoms.calc.results["becs"].reshape(-1, 3, 3).tolist(), epsilon_static=( np.eye(3) + atoms.calc.results["polarizability"].reshape(3, 3) ).tolist(), diff --git a/tests/forcefields/conftest.py b/tests/forcefields/conftest.py index dd1dd901fd..532cbd383a 100644 --- a/tests/forcefields/conftest.py +++ b/tests/forcefields/conftest.py @@ -77,7 +77,7 @@ def calculate(self, atoms=None, properties=None, system_changes=all_changes): sign = np.where(self.atoms.numbers == self.atoms.numbers[0], 1.0, -1.0) self.results = { "energy": 0.0, - "becs": 2 * sign[:, None, None] * np.eye(3), + "becs": (2 * sign[:, None, None] * np.eye(3)).reshape(-1, 9), "polarizability": 3 * np.eye(3), } From 81067e90f9d6542182fb51eb478e63bd25b5c1c2 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 11:38:17 -0700 Subject: [PATCH 24/43] Use the force field Born charges of #1573 in the finite-temperature workflow --- docs/user/codes/vasp.md | 12 +++-- .../flows/finite_temperature_phonons.py | 17 ++++++- .../common/jobs/finite_temperature_phonons.py | 10 +++-- src/atomate2/common/jobs/phonons.py | 45 ------------------- .../flows/finite_temperature_phonons.py | 6 ++- .../flows/test_finite_temperature_phonons.py | 34 +++++++++++++- 6 files changed, 68 insertions(+), 56 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 3bfb713367..881c089397 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -493,13 +493,19 @@ flow = maker.make(structure) `run_npt=True` sets the NPT MD and the relaxation of the atoms in its cell. -A force field gives no Born charges, so the force field makers skip the non-analytical correction by default. -The Born charges and the dielectric tensor can still come from VASP. -Either pass `born` and `epsilon_static` to `make`, or set a VASP `born_maker`: +Most force fields give no Born charges, so the force field makers skip the non-analytical correction by default. +The Born charges and the dielectric tensor can come from MACE-Field, see the [force field notes](forcefields.md#mace-field-notes), or from VASP. +Either pass `born` and `epsilon_static` to `make`, or set a `born_maker`: ```python +from atomate2.forcefields.jobs import ForceFieldDielectricMaker from atomate2.vasp.jobs.core import DielectricMaker +# with MACE-Field +maker.born_maker = ForceFieldDielectricMaker( + calculator_kwargs={"model": "MACEField-MH-0-omat-dielectric.model"} +) +# or with VASP maker.born_maker = DielectricMaker() ``` diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 3d53f9d8d6..45dbc88b95 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -300,6 +300,11 @@ def make( if not np.allclose(matrix, np.diag(np.diag(matrix))): raise ValueError("pheasy needs a diagonal supercell matrix.") + # VASP sorts the atoms by electronegativity. Sorting here as well keeps + # the Born charges of a force field born_maker in the order of the fit. + if not isinstance(structure, OutputReference): + structure = structure.get_sorted_structure() + jobs: list[Job | Flow] = [] optimization_run_job_dir = optimization_run_uuid = None born_run_job_dir = born_run_uuid = None @@ -371,8 +376,16 @@ def make( born_kwargs[self.prev_calc_dir_argname] = prev_dir born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - born = born_job.output.calcs_reversed[0].output.outcar["born"] - epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static + # as in the phonon workflow, a force field dielectric document has the + # Born charges as fields, a VASP task document in its last calculation + schema = born_job.output_schema + if schema is not None and "born" in schema.model_fields: + born = born_job.output.born + epsilon_static = born_job.output.epsilon_static + else: + calc_output = born_job.output.calcs_reversed[0].output + born = calc_output.outcar["born"] + epsilon_static = calc_output.epsilon_static born_run_job_dir = born_job.output.dir_name born_run_uuid = born_job.output.uuid diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 2e8413289a..4dc39e4f09 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -33,13 +33,17 @@ _get_kpath, _run_band_structure_and_plot, _run_total_dos_and_plot, - _set_nac_params, ) from atomate2.common.schemas.finite_temperature_phonons import ( FiniteTemperaturePhononDoc, TrajectoryHealth, ) -from atomate2.common.schemas.phonons import ForceConstants, PhononJobDirs, PhononUUIDs +from atomate2.common.schemas.phonons import ( + ForceConstants, + PhononJobDirs, + PhononUUIDs, + _set_nac_params, +) from atomate2.utils.path import strip_hostname if TYPE_CHECKING: @@ -815,7 +819,7 @@ def fit_finite_temperature_phonons( borns = epsilon = None if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params(phonon, born, epsilon_static, symprec) + borns, epsilon = _set_nac_params(phonon, born, epsilon_static, symprec, code) # frequencies at the q-points commensurate with the supercell matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix diff --git a/src/atomate2/common/jobs/phonons.py b/src/atomate2/common/jobs/phonons.py index 67d8207579..7130f10279 100644 --- a/src/atomate2/common/jobs/phonons.py +++ b/src/atomate2/common/jobs/phonons.py @@ -163,51 +163,6 @@ def _get_num_harmonic_supercells( return int(np.ceil(num_disp_sc * multiplier)) + 1 -def _set_nac_params( - phonon: Phonopy, - born: Sequence[Matrix3D], - epsilon_static: Matrix3D, - symprec: float, - is_symmetry: bool = True, -) -> tuple[np.ndarray, np.ndarray]: - """ - Symmetrize the Born charges and the dielectric tensor and set the NAC. - - The non-analytical correction is only set if a Born charge is not zero. - - Parameters - ---------- - phonon: Phonopy - Phonopy object whose unit cell the Born charges belong to. - born: Sequence[Matrix3D] - Born effective charges, one per atom of the unit cell. - epsilon_static: Matrix3D - High-frequency dielectric tensor. - symprec: float - Symmetry precision. - is_symmetry: bool - Whether to symmetrize the Born charges and the dielectric tensor. - - Returns - ------- - tuple[np.ndarray, np.ndarray] - The Born charges and the dielectric tensor. - """ - borns, epsilon = symmetrize_borns_and_epsilon( - ucell=phonon.unitcell, - borns=np.array(born), - epsilon=np.array(epsilon_static), - symprec=symprec, - primitive_matrix=phonon.primitive_matrix, - supercell_matrix=phonon.supercell_matrix, - is_symmetry=is_symmetry, - ) - if not np.all(np.isclose(borns, 0.0)): - # e^2 / (4 pi epsilon_0) in eV Angstrom, for forces in eV/Angstrom - phonon.nac_params = {"born": borns, "dielectric": epsilon, "factor": 14.399652} - return borns, epsilon - - def _get_kpath( structure: Structure, kpath_scheme: str, symprec: float, **kpath_kwargs ) -> tuple: diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index ff395ac975..d36ca047a3 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -141,8 +141,10 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): Maker for the relaxation of the unit cell. It keeps the symmetry of the structure. None skips the relaxation. born_maker: .Maker | None - Maker for the Born effective charges and the dielectric tensor. It is - None by default, as in the force field pheasy phonon workflow. + Maker for the Born effective charges and the dielectric tensor, for + example a ForceFieldDielectricMaker with MACE-Field or a VASP + DielectricMaker. It is None by default, as in the force field pheasy + phonon workflow. npt_maker: .ForceFieldMDMaker | None Maker for the NPT MD. It must not set dynamics or ase_md_kwargs. None skips the NPT MD. diff --git a/tests/forcefields/flows/test_finite_temperature_phonons.py b/tests/forcefields/flows/test_finite_temperature_phonons.py index 6e2895357b..0ae2877705 100644 --- a/tests/forcefields/flows/test_finite_temperature_phonons.py +++ b/tests/forcefields/flows/test_finite_temperature_phonons.py @@ -20,7 +20,11 @@ ForceFieldFiniteTemperaturePhononMaker, _get_force_field_md_maker, ) -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) from atomate2.forcefields.md import ForceFieldMDMaker from atomate2.vasp.jobs.core import DielectricMaker @@ -246,3 +250,31 @@ def test_finite_temperature_phonon_maker_emt_npt(clean_dir, cu3au): assert doc.trajectory_health.verdict == "stable" assert not doc.has_imaginary_modes assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(6.554, rel=0.05) + + +def test_finite_temperature_phonon_maker_emt_born_charges( + clean_dir, cu3au, fake_dielectric_calculator +): + """Born charges from a force field dielectric job enter the NAC.""" + np.random.seed(103) # noqa: NPY002 + maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( + EMT, + min_length=7.0, + md_time_step=2.0, + md_time=1.0, + equilibration_time=0.2, + n_snapshots=10, + ) + maker.born_maker = ForceFieldDielectricMaker() + flow = maker.make(cu3au) + responses = run_locally(flow, create_folders=True, ensure_success=True) + doc = responses[flow.output.uuid][1].output + + # the fake calculator gives +2 to the first species of the sorted cell, Cu + born = np.array(doc.born) + assert born.shape == (4, 3, 3) + assert np.all(np.diagonal(born[:3], axis1=1, axis2=2) > 0) + assert np.all(np.diagonal(born[3:], axis1=1, axis2=2) < 0) + assert np.array(doc.epsilon_static) == pytest.approx(4 * np.eye(3)) + assert doc.uuids.born_run_uuid is not None + assert doc.phonon_bandstructure.has_nac From 79b5d4ff341d6b89cd7770daf991d58e5e5ffeed Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 12:12:31 -0700 Subject: [PATCH 25/43] some more force field Born charges --- .github/workflows/testing.yml | 9 +++- docs/user/codes/forcefields.md | 49 ++++++++++++++++------ pyproject.toml | 10 ++--- src/atomate2/common/flows/phonons.py | 15 +++---- src/atomate2/common/jobs/hiphive.py | 20 ++++----- src/atomate2/common/jobs/pheasy.py | 20 ++++----- src/atomate2/common/jobs/phonons.py | 20 ++++----- src/atomate2/common/schemas/phonons.py | 51 ++++++++++++----------- src/atomate2/forcefields/flows/hiphive.py | 11 +++-- src/atomate2/forcefields/flows/pheasy.py | 11 +++-- src/atomate2/forcefields/flows/phonons.py | 7 ++-- src/atomate2/forcefields/jobs.py | 6 +-- src/atomate2/forcefields/schemas.py | 9 +--- tests/common/schemas/test_phonons.py | 40 ++++++++++++++++++ tests/forcefields/conftest.py | 17 ++++---- tests/forcefields/flows/test_phonon.py | 28 +++++++++---- tests/forcefields/test_jobs.py | 2 +- tests/forcefields/test_mace_field.py | 3 +- tests/forcefields/test_md.py | 3 +- 19 files changed, 201 insertions(+), 130 deletions(-) diff --git a/.github/workflows/testing.yml b/.github/workflows/testing.yml index 2f8a35a073..12207d1b93 100644 --- a/.github/workflows/testing.yml +++ b/.github/workflows/testing.yml @@ -78,6 +78,11 @@ jobs: micromamba activate a2 uv pip install .[strict,strict-forcefields-${{ matrix.dep-group }},abinit,approxneb,aims,pheasy,phono3py] --group tests + # without the fork, the MACE-Field tests would be skipped + - name: Check that the MACE-Field fork is installed + if: matrix.dep-group == 'mace-field' + run: micromamba run -n a2 python -c "from mace.modules.extensions import MACEField" + - name: Install pymatgen from master if triggered by pymatgen repo dispatch if: github.event_name == 'repository_dispatch' && github.event.action == 'pymatgen-ci-trigger' run: | @@ -92,10 +97,10 @@ jobs: # running it single-process avoids the OOM that kills the runner when # xdist spawns multiple workers each holding a copy of the models. # The MACE-Field fork replaces mace-torch, so its group only runs the - # MACE-Field tests. + # MACE-Field tests, in one process. run: | micromamba activate a2 - pytest -v --durations=5 -n ${{ matrix.dep-group == 'torch-limited' && '1' || 'auto' }} --cov=atomate2 --cov-report=xml ${{ matrix.dep-group == 'mace-field' && 'tests/forcefields/test_mace_field.py' || 'tests/forcefields' }} + pytest -v --durations=5 -n ${{ (matrix.dep-group == 'torch-limited' || matrix.dep-group == 'mace-field') && '1' || 'auto' }} --cov=atomate2 --cov-report=xml ${{ matrix.dep-group == 'mace-field' && 'tests/forcefields/test_mace_field.py' || 'tests/forcefields' }} - name: Forcefield tutorial if: matrix.dep-group == 'torch-limited' diff --git a/docs/user/codes/forcefields.md b/docs/user/codes/forcefields.md index dbd04b8783..e9fefde698 100644 --- a/docs/user/codes/forcefields.md +++ b/docs/user/codes/forcefields.md @@ -35,10 +35,10 @@ Support is provided for the following models, which can be selected using `atoma | FAIRChem | `FAIRChem` | [Meta's FAIRChem Github](https://github.com/facebookresearch/fairchem) | Proprietary, requires extra authentication. [See notes below.](#fairchem-notes) | | Gaussian Approximation Potential (GAP) | `GAP` | [10.1103/PhysRevLett.104.136403](https://doi.org/10.1103/PhysRevLett.104.136403) | Relies on `quippy-ase` package | | M3GNet | `M3GNet` | [10.1038/s43588-022-00349-3](https://doi.org/10.1038/s43588-022-00349-3) | Relies on `matgl` package | +| MACE-Field | `MACE_Field` | [10.1103/b116-xy8k](https://doi.org/10.1103/b116-xy8k) | Born effective charges and dielectric tensor only, via `ForceFieldDielectricMaker`. Needs the MACE-Field fork of `mace_torch` and a model file. [See notes below.](#mace-field-notes) | | MACE-MP-0 | `MACE` or `MACE_MP_0` (recommended) | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MP-0b3 | `MACE_MP_0B3` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MPA-0 | `MACE_MPA_0` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | -| MACE-Field | `MACE_Field` | [10.1103/b116-xy8k](https://doi.org/10.1103/b116-xy8k) | Born effective charges and dielectric tensor only, via `ForceFieldDielectricMaker`. Needs the MACE-Field fork of `mace_torch` and a model file. [See notes below.](#mace-field-notes) | | MatPES-PBE | `MATPES_PBE` | [10.48550/arXiv.2503.04070](https://doi.org/10.48550/arXiv.2503.04070) | Relies on `matgl`. Defaults to TensorNet architecture, but can also use M3GNet or CHGNet architectures via kwargs. See `atomate2.forcefields.utils._DEFAULT_CALCULATOR_KWARGS` for more options. | | MatPES-r2SCAN | `MATPES_R2SCAN`| [10.48550/arXiv.2503.04070](https://doi.org/10.48550/arXiv.2503.04070) | Relies on `matgl`. Defaults to TensorNet architecture, but can also use M3GNet or CHGNet architectures via kwargs. See `atomate2.forcefields.utils._DEFAULT_CALCULATOR_KWARGS` for more options. | | MatterSim | `MatterSim` | [arXiv:2405.04967](https://arxiv.org/abs/2405.04967) | Requires the `mattersim` package | @@ -77,33 +77,56 @@ However, this may not be preserved in future versions, and `calculator_meta` is ## Notes on MACE-Field {#mace-field-notes} [MACE-Field](https://doi.org/10.1103/b116-xy8k) gives the Born effective charges and the high-frequency dielectric tensor of inorganic crystals. -`ForceFieldDielectricMaker` computes them, and the phonon workflows use them for the non-analytical correction when it is set as `born_maker`. -MACE-Field is a fork of MACE that installs as `mace_torch`, so it cannot be installed together with MACE. -It is in the `strict-forcefields-mace-field` extra. -The model file has to be downloaded from the [MACE-Field releases](https://github.com/mdi-group/mace-field/releases) and passed as `model`: +`ForceFieldDielectricMaker` computes them. +The phonon workflows use them for the non-analytical correction when it is set as `born_maker`. + +MACE-Field is a fork of MACE that installs as `mace_torch`, so it replaces MACE. +Install it with `pip install 'atomate2[mace-field]'`. +The fork still runs the MACE foundation models, so the forces can come from MACE in the same environment. +The model file has to be downloaded from the [MACE-Field releases](https://github.com/mdi-group/mace-field/releases). +There is no default model, so `model` must be set. +Give its absolute path, since each job runs in its own folder: ```py +from pymatgen.core import Lattice, Structure + from atomate2.forcefields.flows.phonons import PhononMaker from atomate2.forcefields.jobs import ForceFieldDielectricMaker -born_maker = ForceFieldDielectricMaker( - calculator_kwargs={"model": "MACEField-MH-0-omat-dielectric.model"} +structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(5.64), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] +).get_primitive_structure() + +maker = PhononMaker.from_force_field_name( + "MACE_MP_0", calculator_kwargs={"model": "medium-omat-0"} +) +# from_force_field_name sets born_maker to None +maker.born_maker = ForceFieldDielectricMaker( + calculator_kwargs={"model": "/path/to/MACEField-MH-0-omat-dielectric.model"} ) -flow = PhononMaker(born_maker=born_maker).make(structure) +flow = maker.make(structure) ``` -The model head "mp-dielectric" is used by default. -The dielectric tensor is 1 + chi, with chi the electronic susceptibility of the model. +The Born charges can also come from VASP. +Pass them to `make` as `born` and `epsilon_static`, or set a VASP maker such as `atomate2.vasp.jobs.core.DielectricMaker` as `born_maker`. + +Limitations: + +- Both tensors are computed at zero electric field. The dielectric tensor is the clamped-ion one, 1 + chi, with chi the electronic susceptibility of the model. +- The model has the heads "mp-dielectric", "mp-ferroelectric" and "pt_head". "mp-dielectric" is used by default. +- The model runs on the CPU unless `device` is set in `calculator_kwargs`. +- The fork reports itself as `mace-torch` 0.3.15, so this is the `forcefield_version` in the output. ```{warning} This feature is new and has not been tested widely. It might still change in future versions. ``` -We compared it with the DFPT results in the Materials Project's Harmonic Phonon Database for NaCl, KCl, MgO and Bi4S3N2. -For NaCl, KCl and MgO, which are likely in its training data, the Born charges agree to 0.02 e and the dielectric constants to about 5%. +As a spot check, we compared the "mp-dielectric" head with the DFPT results in the Materials Project's Harmonic Phonon Database for NaCl, KCl, MgO and Bi4S3N2. +NaCl, KCl and MgO are in the training data of MACE-Field. +For them, the Born charges agree to 0.02 e and the high-frequency dielectric constants to 5%. For Bi4S3N2, the Born charges are about 15% too small and the dielectric tensor is off by up to 10%. -The authors report a dielectric constant about 10% too large for alpha-quartz. +For alpha-quartz, the authors report a high-frequency dielectric constant of 2.64 along the c axis, against 2.41 from PBE DFPT. ## Notes on FairChem (Meta) models {#fairchem-notes} diff --git a/pyproject.toml b/pyproject.toml index 74987aee39..0afabfc6e7 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -70,6 +70,8 @@ defects = [ ase = ["ase>=3.26.0"] ase-ext = ["tblite>=0.3.0; platform_system=='Linux'"] forcefields-demo = ["chgnet>=0.3.8","atomate2[ase]"] +# the MACE-Field fork of MACE replaces mace-torch +mace-field = ["atomate2[ase]", "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64"] torchsim = [ "torch-sim-atomistic[symmetry]==0.6.1; python_version >= '3.12'" @@ -138,11 +140,9 @@ strict-forcefields-e3nn-limited = [ strict-forcefields-numpy-limited = [ "nequip-allegro==0.8.3", ] -# MACE-Field is a fork of MACE that installs as mace-torch, so it cannot share -# a group with mace-torch. Remove this group once ACEsuit/mace#1177 is released. -strict-forcefields-mace-field = [ - "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64", -] +# MACE-Field installs as mace-torch, so it cannot share a group with mace-torch. +# Remove this group once MACE-Field is in a mace-torch release (ACEsuit/mace#1177). +strict-forcefields-mace-field = ["atomate2[mace-field]"] strict = [ "atomate2[cclib, phonons, lobster, openmm, mp, defects, ase, ase-ext]", diff --git a/src/atomate2/common/flows/phonons.py b/src/atomate2/common/flows/phonons.py index 557c162b98..6a4861cac7 100644 --- a/src/atomate2/common/flows/phonons.py +++ b/src/atomate2/common/flows/phonons.py @@ -110,8 +110,7 @@ class BasePhononMaker(Maker, ABC): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, .TorchSimStaticMaker, - or None + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None Maker to compute the BORN charges. phonon_displacement_maker: .ForceFieldStaticMaker, .BaseAimsMaker, .BaseVaspMaker, .TorchSimStaticMaker @@ -171,9 +170,7 @@ class BasePhononMaker(Maker, ABC): | TorchSimStaticMaker | None ) = None - born_maker: ( - ForceFieldDielectricMaker | BaseVaspMaker | TorchSimStaticMaker | None - ) = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None phonon_displacement_maker: ( ForceFieldStaticMaker | BaseVaspMaker | BaseAimsMaker | TorchSimStaticMaker ) = None @@ -343,10 +340,10 @@ def make( born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - # a force field dielectric document has the Born charges and the - # dielectric tensor as fields, a VASP task document has them in its - # last calculation - schema = born_job.output_schema + # A force field dielectric document has the Born charges and the + # dielectric tensor as fields. A VASP task document has them in its + # last calculation. + schema = getattr(born_job, "output_schema", None) if schema is not None and "born" in schema.model_fields: epsilon_static = born_job.output.epsilon_static born = born_job.output.born diff --git a/src/atomate2/common/jobs/hiphive.py b/src/atomate2/common/jobs/hiphive.py index 8d5791d03e..3d56b1125b 100644 --- a/src/atomate2/common/jobs/hiphive.py +++ b/src/atomate2/common/jobs/hiphive.py @@ -524,18 +524,14 @@ def generate_frequencies_eigenvectors( ) # get the born charges and dielectric constant - if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params( - phonon, - born, - epsilon_static, - symprec, - code, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - borns = None - epsilon = None + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) prim = ase_read("POSCAR") supercell = ase_read("SPOSCAR") diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 4564e1ea57..3389d8f689 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -716,18 +716,14 @@ def generate_frequencies_eigenvectors( ) # get the born charges and dielectric constant - if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params( - phonon, - born, - epsilon_static, - symprec, - code, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - borns = None - epsilon = None + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) prim = ase_read("POSCAR") supercell = ase_read("SPOSCAR") diff --git a/src/atomate2/common/jobs/phonons.py b/src/atomate2/common/jobs/phonons.py index 7130f10279..332b3aace9 100644 --- a/src/atomate2/common/jobs/phonons.py +++ b/src/atomate2/common/jobs/phonons.py @@ -542,18 +542,14 @@ def generate_frequencies_eigenvectors( ) set_of_forces = [np.array(forces) for forces in displacement_data["forces"]] - if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params( - phonon, - born, - epsilon_static, - symprec, - code, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - borns = None - epsilon = None + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) # Produces all force constants phonon.produce_force_constants(forces=set_of_forces) diff --git a/src/atomate2/common/schemas/phonons.py b/src/atomate2/common/schemas/phonons.py index 5d728fa238..ccb955c5b6 100644 --- a/src/atomate2/common/schemas/phonons.py +++ b/src/atomate2/common/schemas/phonons.py @@ -35,6 +35,9 @@ logger = logging.getLogger(__name__) +# codes whose forces are in eV/Angstrom +_EV_ANGSTROM_CODES = ("ase", "forcefields", "vasp", "torchsim") + def get_factor(code: str) -> float: """ @@ -55,7 +58,7 @@ def get_factor(code: str) -> float: ValueError If code is not defined """ - if code in ["ase", "forcefields", "vasp", "torchsim"]: + if code in _EV_ANGSTROM_CODES: return VaspToTHz if code == "aims": return omegaToTHz # Based on CODATA 2002 @@ -64,26 +67,25 @@ def get_factor(code: str) -> float: def _set_nac_params( phonon: Phonopy, - born: Sequence[Matrix3D], - epsilon_static: Matrix3D, + born: Sequence[Matrix3D] | None, + epsilon_static: Matrix3D | None, symprec: float, code: str, is_symmetry: bool = True, -) -> tuple[np.ndarray, np.ndarray]: +) -> tuple[np.ndarray | None, np.ndarray | None]: """ Symmetrize the Born charges and the dielectric tensor and set the NAC. - The non-analytical correction is only set for VASP and force field - calculations, whose forces are in eV/Angstrom, and only if a Born charge - is not zero. + The non-analytical correction is set unless all Born charges are zero. Its + factor assumes forces in eV/Angstrom, so it is only set for those codes. Parameters ---------- phonon: Phonopy Phonopy object whose unit cell the Born charges belong to. - born: Sequence[Matrix3D] + born: Sequence[Matrix3D] | None Born effective charges, one per atom of the unit cell. - epsilon_static: Matrix3D + epsilon_static: Matrix3D | None High-frequency dielectric tensor. symprec: float Symmetry precision. @@ -94,9 +96,12 @@ def _set_nac_params( Returns ------- - tuple[np.ndarray, np.ndarray] - The Born charges and the dielectric tensor. + tuple[np.ndarray | None, np.ndarray | None] + The Born charges and the dielectric tensor, or None if either was not + given. """ + if born is None or epsilon_static is None: + return None, None if len(born) != len(phonon.unitcell): raise ValueError("Number of Born charges does not agree with number of atoms") borns, epsilon = symmetrize_borns_and_epsilon( @@ -108,8 +113,8 @@ def _set_nac_params( supercell_matrix=phonon.supercell_matrix, is_symmetry=is_symmetry, ) - if code in ("vasp", "forcefields") and not np.all(np.isclose(borns, 0.0)): - # e^2 / (4 pi epsilon_0) in eV Angstrom, for forces in eV/Angstrom + if code in _EV_ANGSTROM_CODES and not np.all(np.isclose(borns, 0.0)): + # e^2 / (4 pi epsilon_0) in eV Angstrom phonon.nac_params = {"born": borns, "dielectric": epsilon, "factor": 14.399652} return borns, epsilon @@ -411,18 +416,14 @@ def from_forces_born( phonon.generate_displacements(distance=displacement) set_of_forces = [np.array(forces) for forces in displacement_data["forces"]] - if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params( - phonon, - born, - epsilon_static, - symprec, - code, - is_symmetry=kwargs.get("symmetrize_born", True), - ) - else: - borns = None - epsilon = None + borns, epsilon = _set_nac_params( + phonon, + born, + epsilon_static, + symprec, + code, + is_symmetry=kwargs.get("symmetrize_born", True), + ) # Produces all force constants phonon.produce_force_constants(forces=set_of_forces) diff --git a/src/atomate2/forcefields/flows/hiphive.py b/src/atomate2/forcefields/flows/hiphive.py index 21ad8b60e3..4aa00353fd 100644 --- a/src/atomate2/forcefields/flows/hiphive.py +++ b/src/atomate2/forcefields/flows/hiphive.py @@ -3,7 +3,7 @@ from __future__ import annotations from dataclasses import dataclass, field -from typing import Literal +from typing import TYPE_CHECKING, Literal from atomate2 import SETTINGS from atomate2.common.flows.hiphive import BasePhononMaker @@ -13,6 +13,9 @@ ForceFieldStaticMaker, ) +if TYPE_CHECKING: + from atomate2.vasp.jobs.base import BaseVaspMaker + @dataclass class PhononMaker(BasePhononMaker): @@ -84,8 +87,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker or None - Maker to compute the BORN charges, for example with MACE-Field. + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -134,7 +137,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | None = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/pheasy.py b/src/atomate2/forcefields/flows/pheasy.py index 03e46f0f5a..227dfe0045 100644 --- a/src/atomate2/forcefields/flows/pheasy.py +++ b/src/atomate2/forcefields/flows/pheasy.py @@ -3,7 +3,7 @@ from __future__ import annotations from dataclasses import dataclass, field -from typing import Literal +from typing import TYPE_CHECKING, Literal from atomate2 import SETTINGS from atomate2.common.flows.pheasy import BasePhononMaker @@ -13,6 +13,9 @@ ForceFieldStaticMaker, ) +if TYPE_CHECKING: + from atomate2.vasp.jobs.base import BaseVaspMaker + @dataclass class PhononMaker(BasePhononMaker): @@ -84,8 +87,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker or None - Maker to compute the BORN charges, for example with MACE-Field. + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -134,7 +137,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | None = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/phonons.py b/src/atomate2/forcefields/flows/phonons.py index b55b0bee0b..a912629fb8 100644 --- a/src/atomate2/forcefields/flows/phonons.py +++ b/src/atomate2/forcefields/flows/phonons.py @@ -18,6 +18,7 @@ from typing_extensions import Self from atomate2.forcefields import MLFF + from atomate2.vasp.jobs.base import BaseVaspMaker @dataclass @@ -92,8 +93,8 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker or None - Maker to compute the BORN charges, for example with MACE-Field. + born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. generate_frequencies_eigenvectors_kwargs : dict @@ -143,7 +144,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | None = None + born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/jobs.py b/src/atomate2/forcefields/jobs.py index ba767b9862..4e9be27bc4 100644 --- a/src/atomate2/forcefields/jobs.py +++ b/src/atomate2/forcefields/jobs.py @@ -238,8 +238,8 @@ class ForceFieldDielectricMaker(ForceFieldMixin, Maker): The force field must give the Born effective charges and the electronic susceptibility chi as the results "becs" and "polarizability", as MACE-Field - does. The high-frequency dielectric tensor is 1 + chi. Unless an electric - field is set in calculator_kwargs, both are computed at zero field. + does. The high-frequency dielectric tensor is 1 + chi. Both are computed at + zero electric field by default. Parameters ---------- @@ -286,7 +286,7 @@ def make( epsilon_static=( np.eye(3) + atoms.calc.results["polarizability"].reshape(3, 3) ).tolist(), - forcefield_name=self.force_field_name, + forcefield_name=self.ase_calculator_name, forcefield_version=_get_pkg_version(self.calculator_meta), dir_name=str(Path.cwd()), ) diff --git a/src/atomate2/forcefields/schemas.py b/src/atomate2/forcefields/schemas.py index 2283112883..1a47531303 100644 --- a/src/atomate2/forcefields/schemas.py +++ b/src/atomate2/forcefields/schemas.py @@ -181,7 +181,7 @@ def from_ase_compatible_result( ).from_ase_task_doc(ase_task_doc, **ff_kwargs) -class ForceFieldDielectricDocument(BaseModel): +class ForceFieldDielectricDocument(ForceFieldMeta): """Born effective charges and dielectric tensor from a force field.""" structure: Structure = Field(description="The structure of the calculation.") @@ -191,10 +191,3 @@ class ForceFieldDielectricDocument(BaseModel): epsilon_static: Matrix3D = Field( description="The high-frequency dielectric tensor." ) - forcefield_name: str | None = Field(None, description="Name of the force field.") - forcefield_version: str | None = Field( - None, description="Version of the force field package." - ) - dir_name: str | None = Field( - None, description="Directory where the calculation was performed." - ) diff --git a/tests/common/schemas/test_phonons.py b/tests/common/schemas/test_phonons.py index f0ddd9315f..38884f933d 100644 --- a/tests/common/schemas/test_phonons.py +++ b/tests/common/schemas/test_phonons.py @@ -3,7 +3,10 @@ import numpy as np import pytest from monty.json import MontyEncoder +from phonopy import Phonopy from pydantic import ValidationError +from pymatgen.core import Lattice, Structure +from pymatgen.io.phonopy import get_phonopy_structure from atomate2.common.schemas.phonons import ( PhononBSDOSDoc, @@ -11,6 +14,7 @@ PhononJobDirs, PhononUUIDs, ThermalDisplacementData, + _set_nac_params, ) @@ -58,3 +62,39 @@ def test_phonon_bs_dos_doc(): def test_model_validate(model_cls): validated = model_cls.model_validate_json(json.dumps(model_cls(), cls=MontyEncoder)) assert isinstance(validated, model_cls) + + +def get_nacl_phonon(): + structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(5.6), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ).get_primitive_structure() + return Phonopy(get_phonopy_structure(structure), supercell_matrix=np.eye(3)) + + +@pytest.mark.parametrize( + ("code", "charge", "has_nac"), + [ + ("vasp", 1, True), + ("forcefields", 1, True), + ("aims", 1, False), + ("vasp", 0, False), + ], +) +def test_set_nac_params(code, charge, has_nac): + phonon = get_nacl_phonon() + born = charge * np.array([1, -1])[:, None, None] * np.eye(3) + borns, epsilon = _set_nac_params( + phonon, born.tolist(), (2 * np.eye(3)).tolist(), 1e-4, code + ) + + assert borns == pytest.approx(born) + assert epsilon == pytest.approx(2 * np.eye(3)) + assert (phonon.nac_params is not None) == has_nac + + +def test_set_nac_params_without_born(): + phonon = get_nacl_phonon() + assert _set_nac_params(phonon, None, None, 1e-4, "vasp") == (None, None) + assert phonon.nac_params is None + with pytest.raises(ValueError, match="Number of Born charges"): + _set_nac_params(phonon, [np.eye(3).tolist()], np.eye(3).tolist(), 1e-4, "vasp") diff --git a/tests/forcefields/conftest.py b/tests/forcefields/conftest.py index 532cbd383a..3a77b5bdaa 100644 --- a/tests/forcefields/conftest.py +++ b/tests/forcefields/conftest.py @@ -4,7 +4,6 @@ import tempfile import urllib.request from importlib import import_module -from importlib.util import find_spec from pathlib import Path from typing import TYPE_CHECKING @@ -27,9 +26,12 @@ for mlff in MLFF } # the MACE-Field fork installs as mace-torch, so only its model class tells them apart -_INSTALLED_MLFF["MACE_Field"] = find_spec("mace") is not None and hasattr( - import_module("mace.modules.extensions"), "MACEField" -) +try: + _INSTALLED_MLFF["MACE_Field"] = hasattr( + import_module("mace.modules.extensions"), "MACEField" + ) +except ImportError: + _INSTALLED_MLFF["MACE_Field"] = False def mlff_is_installed(mlff: str | MLFF) -> bool: @@ -65,9 +67,10 @@ def get_deepmd_pretrained_model_path(test_dir: Path) -> Path: class FakeDielectricCalculator(Calculator): - """Born charges of +2 and -2 and a susceptibility of 3, as MACE-Field gives them. + """Born charges of +2 and -2 and a susceptibility of 3. - The atoms of the first species get +2, all others -2. + The atoms of the first species get +2, all others -2. Both results are + flattened, as MACE-Field returns them. """ implemented_properties = ("energy", "becs", "polarizability") @@ -78,7 +81,7 @@ def calculate(self, atoms=None, properties=None, system_changes=all_changes): self.results = { "energy": 0.0, "becs": (2 * sign[:, None, None] * np.eye(3)).reshape(-1, 9), - "polarizability": 3 * np.eye(3), + "polarizability": (3 * np.eye(3)).reshape(9), } diff --git a/tests/forcefields/flows/test_phonon.py b/tests/forcefields/flows/test_phonon.py index 708ac1d0ee..83c8fda584 100644 --- a/tests/forcefields/flows/test_phonon.py +++ b/tests/forcefields/flows/test_phonon.py @@ -35,6 +35,7 @@ # skip m3gnet and matpes models due to matcalc requiring # DGL which is PyTorch 2.4 incompatible, raises # "FileNotFoundError: Cannot find DGL C++ libgraphbolt_pytorch_2.4.1.so" +# skip MACE-Field, which needs the path of its model file skip_mlff = set( map( MLFF, @@ -46,6 +47,7 @@ "MATPES_PBE", "Allegro", "FAIRChem", + "MACE_Field", ], ) ) @@ -293,26 +295,36 @@ def test_ext_load_phonon_initialization(): assert maker.phonon_displacement_maker.ase_calculator_name == "mace_mp" -def test_phonon_wf_force_field_born_charges(clean_dir, fake_dielectric_calculator): - """Born charges from a force field dielectric job enter the NAC.""" +@pytest.mark.parametrize("born_by_hand", [False, True]) +def test_phonon_wf_force_field_born_charges( + clean_dir, fake_dielectric_calculator, born_by_hand +): + """Born charges from a force field dielectric job or given by hand enter the NAC.""" structure = Structure.from_spacegroup( "Fm-3m", Lattice.cubic(4.17), ["Ni", "O"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() + born = np.array([2, -2])[:, None, None] * np.eye(3) emt = {"@module": "ase.calculators.emt", "@callable": "EMT"} - flow = PhononMaker( + maker = PhononMaker( bulk_relax_maker=None, static_energy_maker=None, phonon_displacement_maker=ForceFieldStaticMaker(force_field_name=emt), - born_maker=ForceFieldDielectricMaker(), + born_maker=None if born_by_hand else ForceFieldDielectricMaker(), min_length=8, create_thermal_displacements=False, store_force_constants=False, - ).make(structure) + ) + if born_by_hand: + flow = maker.make( + structure, born=born.tolist(), epsilon_static=(4 * np.eye(3)).tolist() + ) + else: + flow = maker.make(structure) responses = run_locally(flow, create_folders=True, ensure_success=True) doc = responses[flow[-1].uuid][1].output - assert np.array(doc.born) == pytest.approx( - np.array([2, -2])[:, None, None] * np.eye(3) - ) + assert np.array(doc.born) == pytest.approx(born) assert np.array(doc.epsilon_static) == pytest.approx(4 * np.eye(3)) assert doc.phonon_bandstructure.has_nac + # the LO-TO splitting raises the highest frequency from about 12.6 THz + assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(17.976, abs=1e-2) diff --git a/tests/forcefields/test_jobs.py b/tests/forcefields/test_jobs.py index 2591070d7b..386b88e73a 100644 --- a/tests/forcefields/test_jobs.py +++ b/tests/forcefields/test_jobs.py @@ -920,7 +920,7 @@ def test_dielectric_maker(fake_dielectric_calculator, clean_dir): structure = Structure.from_spacegroup( "Fm-3m", Lattice.cubic(5.6), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() - job = ForceFieldDielectricMaker(force_field_name="MACE-Field").make(structure) + job = ForceFieldDielectricMaker().make(structure) output = run_locally(job, ensure_success=True)[job.uuid][1].output assert isinstance(output, ForceFieldDielectricDocument) diff --git a/tests/forcefields/test_mace_field.py b/tests/forcefields/test_mace_field.py index 0e734c81e4..48cca063fe 100644 --- a/tests/forcefields/test_mace_field.py +++ b/tests/forcefields/test_mace_field.py @@ -48,7 +48,8 @@ def test_mace_field_dielectric_maker(mace_field_model, clean_dir): born = np.array(output.born) # the acoustic sum rule holds by construction assert born.sum(axis=0) == pytest.approx(np.zeros((3, 3)), abs=1e-6) - # cubic, so the tensors are isotropic. DFPT gives about 1.09 and 2.5. + # cubic, so the tensors are isotropic. The Materials Project's Harmonic Phonon + # Database has 1.09 and 2.56 from DFPT. species = [str(site.specie) for site in output.structure] assert born[species.index("Na")] == pytest.approx(1.0898 * np.eye(3), abs=1e-3) epsilon = np.array(output.epsilon_static) diff --git a/tests/forcefields/test_md.py b/tests/forcefields/test_md.py index 4217896cf8..2aaef9f90f 100644 --- a/tests/forcefields/test_md.py +++ b/tests/forcefields/test_md.py @@ -45,8 +45,9 @@ def test_maker_initialization(mlff): ) +# MACE-Field needs the path of its model file _mlffs_for_test = set(INSTALLED_MLFF).difference( - map(MLFF, ("Forcefield", "Allegro", "M3GNet", "MACE", "Nequip")) + map(MLFF, ("Forcefield", "Allegro", "M3GNet", "MACE", "Nequip", "MACE_Field")) ) _md_test_params = sorted(product(_mlffs_for_test, [True, False]), key=str) From fdb084b65b2d693b4a4d080be273ed0b02a79f0f Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 12:16:20 -0700 Subject: [PATCH 26/43] Use the simplified NAC helper in the finite-temperature workflow --- docs/user/codes/vasp.md | 2 +- .../common/flows/finite_temperature_phonons.py | 12 +++++++----- .../common/jobs/finite_temperature_phonons.py | 4 +--- 3 files changed, 9 insertions(+), 9 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 881c089397..c1755413d2 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -503,7 +503,7 @@ from atomate2.vasp.jobs.core import DielectricMaker # with MACE-Field maker.born_maker = ForceFieldDielectricMaker( - calculator_kwargs={"model": "MACEField-MH-0-omat-dielectric.model"} + calculator_kwargs={"model": "/path/to/MACEField-MH-0-omat-dielectric.model"} ) # or with VASP maker.born_maker = DielectricMaker() diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 45dbc88b95..819ca1eb3d 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -170,8 +170,9 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): bulk_relax_maker: Maker | None Maker for the relaxation of the unit cell. None skips the relaxation. born_maker: Maker | None - VASP maker for the Born effective charges and the dielectric tensor, - used for the non-analytical correction. None skips it. + Maker for the Born effective charges and the dielectric tensor, used + for the non-analytical correction, for example a + ForceFieldDielectricMaker or a VASP DielectricMaker. None skips it. npt_maker: Maker | None Maker for the NPT MD. The flow sets its temperature, pressure, time step and number of steps. None skips the NPT MD. @@ -376,9 +377,10 @@ def make( born_kwargs[self.prev_calc_dir_argname] = prev_dir born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - # as in the phonon workflow, a force field dielectric document has the - # Born charges as fields, a VASP task document in its last calculation - schema = born_job.output_schema + # As in the phonon workflow, a force field dielectric document has the + # Born charges as fields. A VASP task document has them in its last + # calculation. + schema = getattr(born_job, "output_schema", None) if schema is not None and "born" in schema.model_fields: born = born_job.output.born epsilon_static = born_job.output.epsilon_static diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 4dc39e4f09..9fca439b4a 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -817,9 +817,7 @@ def fit_finite_temperature_phonons( predicted = -np.einsum("ijab,mjb->mia", phonon.force_constants, disps) force_rmse = float(np.sqrt(np.mean((fit_forces - predicted) ** 2))) - borns = epsilon = None - if born is not None and epsilon_static is not None: - borns, epsilon = _set_nac_params(phonon, born, epsilon_static, symprec, code) + borns, epsilon = _set_nac_params(phonon, born, epsilon_static, symprec, code) # frequencies at the q-points commensurate with the supercell matrix = np.linalg.inv(phonon.primitive_matrix) @ phonon.supercell_matrix From ea89a2f5199e090889d12604b4f87a043955e5c7 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 13:17:37 -0700 Subject: [PATCH 27/43] more edits to the force field Born charges --- .github/workflows/testing.yml | 3 +- docs/user/codes/forcefields.md | 96 +++++++++++------------ pyproject.toml | 1 - src/atomate2/common/flows/phonons.py | 12 +-- src/atomate2/common/schemas/phonons.py | 24 +++--- src/atomate2/forcefields/flows/hiphive.py | 12 ++- src/atomate2/forcefields/flows/pheasy.py | 12 ++- src/atomate2/forcefields/flows/phonons.py | 9 +-- src/atomate2/forcefields/jobs.py | 21 ++++- src/atomate2/forcefields/utils.py | 8 +- src/atomate2/torchsim/flows/phonons.py | 8 +- tests/common/schemas/test_phonons.py | 2 + tests/forcefields/conftest.py | 4 +- tests/forcefields/flows/test_pheasy.py | 35 ++++++++- tests/forcefields/flows/test_phonon.py | 4 +- tests/forcefields/test_jobs.py | 5 +- tests/forcefields/test_mace_field.py | 52 ++++++++---- tests/forcefields/test_md.py | 2 +- 18 files changed, 183 insertions(+), 127 deletions(-) diff --git a/.github/workflows/testing.yml b/.github/workflows/testing.yml index 12207d1b93..c2bf5e05f0 100644 --- a/.github/workflows/testing.yml +++ b/.github/workflows/testing.yml @@ -96,8 +96,7 @@ jobs: # torch-limited loads the heaviest MLIP stack (matgl + nequip + torch); # running it single-process avoids the OOM that kills the runner when # xdist spawns multiple workers each holding a copy of the models. - # The MACE-Field fork replaces mace-torch, so its group only runs the - # MACE-Field tests, in one process. + # The mace-field group only runs the MACE-Field tests, in one process. run: | micromamba activate a2 pytest -v --durations=5 -n ${{ (matrix.dep-group == 'torch-limited' || matrix.dep-group == 'mace-field') && '1' || 'auto' }} --cov=atomate2 --cov-report=xml ${{ matrix.dep-group == 'mace-field' && 'tests/forcefields/test_mace_field.py' || 'tests/forcefields' }} diff --git a/docs/user/codes/forcefields.md b/docs/user/codes/forcefields.md index e9fefde698..0737695c1b 100644 --- a/docs/user/codes/forcefields.md +++ b/docs/user/codes/forcefields.md @@ -35,7 +35,7 @@ Support is provided for the following models, which can be selected using `atoma | FAIRChem | `FAIRChem` | [Meta's FAIRChem Github](https://github.com/facebookresearch/fairchem) | Proprietary, requires extra authentication. [See notes below.](#fairchem-notes) | | Gaussian Approximation Potential (GAP) | `GAP` | [10.1103/PhysRevLett.104.136403](https://doi.org/10.1103/PhysRevLett.104.136403) | Relies on `quippy-ase` package | | M3GNet | `M3GNet` | [10.1038/s43588-022-00349-3](https://doi.org/10.1038/s43588-022-00349-3) | Relies on `matgl` package | -| MACE-Field | `MACE_Field` | [10.1103/b116-xy8k](https://doi.org/10.1103/b116-xy8k) | Born effective charges and dielectric tensor only, via `ForceFieldDielectricMaker`. Needs the MACE-Field fork of `mace_torch` and a model file. [See notes below.](#mace-field-notes) | +| MACE-Field | `MACE_FIELD` | [10.1103/b116-xy8k](https://doi.org/10.1103/b116-xy8k) | Born effective charges and dielectric tensor only, via `ForceFieldDielectricMaker`. Relies on the MACE-Field fork of `mace_torch` and a model file. [See notes below.](#mace-field-notes) | | MACE-MP-0 | `MACE` or `MACE_MP_0` (recommended) | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MP-0b3 | `MACE_MP_0B3` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | | MACE-MPA-0 | `MACE_MPA_0` | [10.1063/5.0297006](https://doi.org/10.1063/5.0297006) | Relies on `mace_torch` and optionally `torch_dftd` packages | @@ -74,15 +74,45 @@ However, this may not be preserved in future versions, and `calculator_meta` is [^calculator-meta-type-annotation]: In this context, the type annotation of the decoded dict should be either `Type[Calculator]` or `Callable[..., Calculator]`, where `Calculator` is from `ase.calculators.calculator`. +## Notes on FairChem (Meta) models {#fairchem-notes} + +The FAIRChem models provided by Meta require extra authentication via HuggingFace: +1. Request access to the UMA models [via HuggingFace](https://huggingface.co/facebook/UMA). You will need to set up a HuggingFace account. You will need to receive approval for the UMA models to proceed. +2. Install the HuggingFace CLI with `pip install 'huggingface_hub'`. +3. Run `huggingface-cli login` from a shell to authenticate your session. You will need to set up an access token. +4. You can now use the FAIRChem calculators. The general syntax for setting up a FAIRChem calculator in `atomate2` is: +```py +calculator_kwargs = { + "predict_unit": {"model_name": "uma-s-1p1"}, + "task_name": "omat", +} +``` + +`atomate2` will then set up a `FAIRChemCalculator`: +```py +from atomate2.forcefields.utils import MLFF, _DEFAULT_CALCULATOR_KWARGS +from fairchem.core import FAIRChemCalculator, pretrained_mlip + +predict_unit_kwargs = calculator_kwargs.pop( + "predict_unit", _DEFAULT_CALCULATOR_KWARGS[MLFF.FAIRChem]["predict_unit"] +) +calculator = FAIRChemCalculator( + pretrained_mlip.get_predict_unit(predict_unit_kwargs), + **{k: v for k, v in calculator_kwargs.items() if k != "predict_unit"}, +) +``` + +The default in `atomate2` is the OMat24 model with `uma-s-1p1`. + ## Notes on MACE-Field {#mace-field-notes} [MACE-Field](https://doi.org/10.1103/b116-xy8k) gives the Born effective charges and the high-frequency dielectric tensor of inorganic crystals. `ForceFieldDielectricMaker` computes them. -The phonon workflows use them for the non-analytical correction when it is set as `born_maker`. +The phonon workflows use them for the non-analytical correction when `ForceFieldDielectricMaker` is set as `born_maker`. MACE-Field is a fork of MACE that installs as `mace_torch`, so it replaces MACE. Install it with `pip install 'atomate2[mace-field]'`. -The fork still runs the MACE foundation models, so the forces can come from MACE in the same environment. +The fork also runs the MACE foundation models, so the forces can come from MACE-OMAT in the same environment. The model file has to be downloaded from the [MACE-Field releases](https://github.com/mdi-group/mace-field/releases). There is no default model, so `model` must be set. Give its absolute path, since each job runs in its own folder: @@ -97,22 +127,21 @@ structure = Structure.from_spacegroup( "Fm-3m", Lattice.cubic(5.64), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() -maker = PhononMaker.from_force_field_name( - "MACE_MP_0", calculator_kwargs={"model": "medium-omat-0"} -) -# from_force_field_name sets born_maker to None -maker.born_maker = ForceFieldDielectricMaker( - calculator_kwargs={"model": "/path/to/MACEField-MH-0-omat-dielectric.model"} -) -flow = maker.make(structure) +flow = PhononMaker.from_force_field_name( + "MACE_MP_0", + calculator_kwargs={"model": "medium-omat-0"}, + born_maker=ForceFieldDielectricMaker( + calculator_kwargs={"model": "/path/to/MACEField-MH-0-omat-dielectric.model"} + ), +).make(structure) ``` -The Born charges can also come from VASP. -Pass them to `make` as `born` and `epsilon_static`, or set a VASP maker such as `atomate2.vasp.jobs.core.DielectricMaker` as `born_maker`. +Born charges from VASP can be passed to `make` as `born` and `epsilon_static`. +They must be in the same order as the sites of the structure. Limitations: -- Both tensors are computed at zero electric field. The dielectric tensor is the clamped-ion one, 1 + chi, with chi the electronic susceptibility of the model. +- Both tensors are computed at zero electric field by default. The dielectric tensor is the clamped-ion one, 1 + chi, with chi the electronic susceptibility of the model. - The model has the heads "mp-dielectric", "mp-ferroelectric" and "pt_head". "mp-dielectric" is used by default. - The model runs on the CPU unless `device` is set in `calculator_kwargs`. - The fork reports itself as `mace-torch` 0.3.15, so this is the `forcefield_version` in the output. @@ -122,38 +151,7 @@ This feature is new and has not been tested widely. It might still change in future versions. ``` -As a spot check, we compared the "mp-dielectric" head with the DFPT results in the Materials Project's Harmonic Phonon Database for NaCl, KCl, MgO and Bi4S3N2. -NaCl, KCl and MgO are in the training data of MACE-Field. -For them, the Born charges agree to 0.02 e and the high-frequency dielectric constants to 5%. -For Bi4S3N2, the Born charges are about 15% too small and the dielectric tensor is off by up to 10%. -For alpha-quartz, the authors report a high-frequency dielectric constant of 2.64 along the c axis, against 2.41 from PBE DFPT. - -## Notes on FairChem (Meta) models {#fairchem-notes} - -The FAIRChem models provided by Meta require extra authentication via HuggingFace: -1. Request access to the UMA models [via HuggingFace](https://huggingface.co/facebook/UMA). You will need to set up a HuggingFace account. You will need to receive approval for the UMA models to proceed. -2. Install the HuggingFace CLI with `pip install 'huggingface_hub'`. -3. Run `huggingface-cli login` from a shell to authenticate your session. You will need to set up an access token. -4. You can now use the FAIRChem calculators. The general syntax for setting up a FAIRChem calculator in `atomate2` is: -```py -calculator_kwargs = { - "predict_unit": {"model_name": "uma-s-1p1"}, - "task_name": "omat", -} -``` - -`atomate2` will then set up a `FAIRChemCalculator`: -```py -from atomate2.forcefields.utils import MLFF, _DEFAULT_CALCULATOR_KWARGS -from fairchem.core import FAIRChemCalculator, pretrained_mlip - -predict_unit_kwargs = calculator_kwargs.pop( - "predict_unit", _DEFAULT_CALCULATOR_KWARGS[MLFF.FAIRChem]["predict_unit"] -) -calculator = FAIRChemCalculator( - pretrained_mlip.get_predict_unit(predict_unit_kwargs), - **{k: v for k, v in calculator_kwargs.items() if k != "predict_unit"}, -) -``` - -The default in `atomate2` is the OMat24 model with `uma-s-1p1`. +We compared the "mp-dielectric" head with the DFPT results in the Materials Project's Harmonic Phonon Database. +The 50 materials have no Materials Project dielectric data, so they are likely not in the training data of MACE-Field. +The Born charges are off by 0.26 e on average, about 11%. +The high-frequency dielectric constants are off by 8% on average, and by more than 20% for 2 of the 50 materials. diff --git a/pyproject.toml b/pyproject.toml index 0afabfc6e7..eff3fd4516 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -70,7 +70,6 @@ defects = [ ase = ["ase>=3.26.0"] ase-ext = ["tblite>=0.3.0; platform_system=='Linux'"] forcefields-demo = ["chgnet>=0.3.8","atomate2[ase]"] -# the MACE-Field fork of MACE replaces mace-torch mace-field = ["atomate2[ase]", "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64"] torchsim = [ diff --git a/src/atomate2/common/flows/phonons.py b/src/atomate2/common/flows/phonons.py index 6a4861cac7..0846cdfcae 100644 --- a/src/atomate2/common/flows/phonons.py +++ b/src/atomate2/common/flows/phonons.py @@ -17,6 +17,7 @@ run_phonon_displacements, ) from atomate2.common.jobs.utils import structure_to_conventional, structure_to_primitive +from atomate2.common.utils import check_class_name if TYPE_CHECKING: from pathlib import Path @@ -340,17 +341,12 @@ def make( born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - # A force field dielectric document has the Born charges and the - # dielectric tensor as fields. A VASP task document has them in its - # last calculation. - schema = getattr(born_job, "output_schema", None) - if schema is not None and "born" in schema.model_fields: + if check_class_name(self.born_maker, "ForceFieldDielectricMaker"): epsilon_static = born_job.output.epsilon_static born = born_job.output.born else: - calc_output = born_job.output.calcs_reversed[0].output - epsilon_static = calc_output.epsilon_static - born = calc_output.outcar["born"] + epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static + born = born_job.output.calcs_reversed[0].output.outcar["born"] born_run_job_dir = born_job.output.dir_name born_run_uuid = born_job.output.uuid diff --git a/src/atomate2/common/schemas/phonons.py b/src/atomate2/common/schemas/phonons.py index ccb955c5b6..d9a30e5f67 100644 --- a/src/atomate2/common/schemas/phonons.py +++ b/src/atomate2/common/schemas/phonons.py @@ -13,7 +13,7 @@ from phonopy import Phonopy from phonopy.phonon.band_structure import get_band_qpoints_and_path_connections from phonopy.structure.symmetry import symmetrize_borns_and_epsilon -from phonopy.units import VaspToTHz +from phonopy.units import Bohr, Hartree, VaspToTHz from pydantic import BaseModel, Field from pymatgen.core import Structure from pymatgen.io.phonopy import ( @@ -35,9 +35,6 @@ logger = logging.getLogger(__name__) -# codes whose forces are in eV/Angstrom -_EV_ANGSTROM_CODES = ("ase", "forcefields", "vasp", "torchsim") - def get_factor(code: str) -> float: """ @@ -58,7 +55,7 @@ def get_factor(code: str) -> float: ValueError If code is not defined """ - if code in _EV_ANGSTROM_CODES: + if code in ["ase", "forcefields", "vasp", "torchsim"]: return VaspToTHz if code == "aims": return omegaToTHz # Based on CODATA 2002 @@ -76,8 +73,8 @@ def _set_nac_params( """ Symmetrize the Born charges and the dielectric tensor and set the NAC. - The non-analytical correction is set unless all Born charges are zero. Its - factor assumes forces in eV/Angstrom, so it is only set for those codes. + The non-analytical correction is set unless all Born charges are zero or + the code is FHI-aims. Parameters ---------- @@ -97,8 +94,8 @@ def _set_nac_params( Returns ------- tuple[np.ndarray | None, np.ndarray | None] - The Born charges and the dielectric tensor, or None if either was not - given. + The symmetrized Born charges and dielectric tensor, or None if either + was not given. """ if born is None or epsilon_static is None: return None, None @@ -113,9 +110,12 @@ def _set_nac_params( supercell_matrix=phonon.supercell_matrix, is_symmetry=is_symmetry, ) - if code in _EV_ANGSTROM_CODES and not np.all(np.isclose(borns, 0.0)): - # e^2 / (4 pi epsilon_0) in eV Angstrom - phonon.nac_params = {"born": borns, "dielectric": epsilon, "factor": 14.399652} + if code != "aims" and not np.all(np.isclose(borns, 0.0)): + phonon.nac_params = { + "born": borns, + "dielectric": epsilon, + "factor": Hartree * Bohr, + } return borns, epsilon diff --git a/src/atomate2/forcefields/flows/hiphive.py b/src/atomate2/forcefields/flows/hiphive.py index 4aa00353fd..c99eda7603 100644 --- a/src/atomate2/forcefields/flows/hiphive.py +++ b/src/atomate2/forcefields/flows/hiphive.py @@ -3,7 +3,7 @@ from __future__ import annotations from dataclasses import dataclass, field -from typing import TYPE_CHECKING, Literal +from typing import Literal from atomate2 import SETTINGS from atomate2.common.flows.hiphive import BasePhononMaker @@ -13,9 +13,6 @@ ForceFieldStaticMaker, ) -if TYPE_CHECKING: - from atomate2.vasp.jobs.base import BaseVaspMaker - @dataclass class PhononMaker(BasePhononMaker): @@ -28,7 +25,8 @@ class PhononMaker(BasePhononMaker): forces are computed for these structures. With the help of phonopy, these forces are then converted into a dynamical matrix. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can - be performed. The BORN charges can be supplied manually. + be performed. The BORN charges can be supplied manually or computed + with ``born_maker``. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. @@ -87,7 +85,7 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + born_maker: .ForceFieldDielectricMaker or None Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. @@ -137,7 +135,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/pheasy.py b/src/atomate2/forcefields/flows/pheasy.py index 227dfe0045..44b284acd9 100644 --- a/src/atomate2/forcefields/flows/pheasy.py +++ b/src/atomate2/forcefields/flows/pheasy.py @@ -3,7 +3,7 @@ from __future__ import annotations from dataclasses import dataclass, field -from typing import TYPE_CHECKING, Literal +from typing import Literal from atomate2 import SETTINGS from atomate2.common.flows.pheasy import BasePhononMaker @@ -13,9 +13,6 @@ ForceFieldStaticMaker, ) -if TYPE_CHECKING: - from atomate2.vasp.jobs.base import BaseVaspMaker - @dataclass class PhononMaker(BasePhononMaker): @@ -28,7 +25,8 @@ class PhononMaker(BasePhononMaker): forces are computed for these structures. With the help of phonopy, these forces are then converted into a dynamical matrix. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can - be performed. The BORN charges can be supplied manually. + be performed. The BORN charges can be supplied manually or computed + with ``born_maker``. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. @@ -87,7 +85,7 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + born_maker: .ForceFieldDielectricMaker or None Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. @@ -137,7 +135,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: diff --git a/src/atomate2/forcefields/flows/phonons.py b/src/atomate2/forcefields/flows/phonons.py index a912629fb8..0014320b17 100644 --- a/src/atomate2/forcefields/flows/phonons.py +++ b/src/atomate2/forcefields/flows/phonons.py @@ -18,7 +18,6 @@ from typing_extensions import Self from atomate2.forcefields import MLFF - from atomate2.vasp.jobs.base import BaseVaspMaker @dataclass @@ -32,7 +31,8 @@ class PhononMaker(BasePhononMaker): forces are computed for these structures. With the help of phonopy, these forces are then converted into a dynamical matrix. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can - be performed. The BORN charges can be supplied manually. + be performed. The BORN charges can be supplied manually or computed + with ``born_maker``. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. @@ -93,7 +93,7 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .ForceFieldDielectricMaker, .BaseVaspMaker, or None + born_maker: .ForceFieldDielectricMaker or None Maker to compute the BORN charges. phonon_displacement_maker : .ForceFieldStaticMaker or None Maker used to compute the forces for a supercell. @@ -144,7 +144,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" store_force_constants: bool = True code: str = "forcefields" - born_maker: ForceFieldDielectricMaker | BaseVaspMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None @property def prev_calc_dir_argname(self) -> None: @@ -214,7 +214,6 @@ def from_force_field_name( force_field_name=force_field_name, calculator_kwargs=calculator_kwargs, ), - born_maker=None, ) return cls( name=(f"{static_energy_maker.mlff.name} Phonon Maker"), diff --git a/src/atomate2/forcefields/jobs.py b/src/atomate2/forcefields/jobs.py index 4e9be27bc4..b4f49cc5e5 100644 --- a/src/atomate2/forcefields/jobs.py +++ b/src/atomate2/forcefields/jobs.py @@ -3,9 +3,9 @@ from __future__ import annotations import logging +import os import warnings from dataclasses import dataclass, field -from pathlib import Path from typing import TYPE_CHECKING import numpy as np @@ -28,6 +28,7 @@ if TYPE_CHECKING: from collections.abc import Callable + from pathlib import Path from pymatgen.core.structure import Molecule, Structure @@ -231,6 +232,14 @@ class ForceFieldStaticMaker(ForceFieldRelaxMaker): Doi("10.1103/b116-xy8k"), description="MACE-Field: Born effective charges and dielectric tensor", ) +@due.dcite( + Doi("10.1038/sdata.2016.134"), + description="MACE-Field training data: Materials Project dielectric data", +) +@due.dcite( + Doi("10.1038/s41597-020-0407-9"), + description="MACE-Field training data: Materials Project ferroelectric data", +) @dataclass class ForceFieldDielectricMaker(ForceFieldMixin, Maker): """ @@ -241,6 +250,10 @@ class ForceFieldDielectricMaker(ForceFieldMixin, Maker): does. The high-frequency dielectric tensor is 1 + chi. Both are computed at zero electric field by default. + MACE-Field needs the MACE-Field fork of mace-torch and a model file, see the + force field docs. This maker is new and less tested than the other force + field makers. It might still change in future versions. + Parameters ---------- name : str @@ -249,11 +262,11 @@ class ForceFieldDielectricMaker(ForceFieldMixin, Maker): The name of the force field. calculator_kwargs : dict Keyword arguments that will get passed to the ASE calculator. For - MACE-Field, "model" is the path of the model file. + MACE-Field, "model" must be set to the path of the model file. """ name: str = "Force field dielectric" - force_field_name: str | MLFF | dict = MLFF.MACE_Field + force_field_name: str | MLFF | dict = MLFF.MACE_FIELD calculator_kwargs: dict = field(default_factory=dict) @job(output_schema=ForceFieldDielectricDocument) @@ -288,5 +301,5 @@ def make( ).tolist(), forcefield_name=self.ase_calculator_name, forcefield_version=_get_pkg_version(self.calculator_meta), - dir_name=str(Path.cwd()), + dir_name=os.getcwd(), ) diff --git a/src/atomate2/forcefields/utils.py b/src/atomate2/forcefields/utils.py index 19636fe628..9c516e4e26 100644 --- a/src/atomate2/forcefields/utils.py +++ b/src/atomate2/forcefields/utils.py @@ -40,7 +40,7 @@ class MLFF(Enum): # TODO inherit from StrEnum when 3.11+ MACE_MP_0 = "MACE-MP-0" MACE_MPA_0 = "MACE-MPA-0" MACE_MP_0B3 = "MACE-MP-0b3" - MACE_Field = "MACE-Field" + MACE_FIELD = "MACE-Field" GAP = "GAP" M3GNet = "M3GNet" CHGNet = "CHGNet" @@ -79,7 +79,7 @@ def _missing_(cls, value: Any) -> Any: MLFF.MACE_MP_0: {"model": "medium"}, MLFF.MACE_MP_0B3: {"model": "medium-0b3"}, MLFF.MACE_MPA_0: {"model": "medium-mpa-0"}, - MLFF.MACE_Field: {"head": "mp-dielectric", "default_dtype": "float64"}, + MLFF.MACE_FIELD: {"head": "mp-dielectric", "default_dtype": "float64"}, MLFF.MATPES_PBE: { "architecture": "TensorNet", "version": "2025.2", @@ -430,7 +430,7 @@ def ase_calculator( else: calculator = mace_mp(default_dtype=default_dtype or "", **kwargs) - case MLFF.MACE_Field: + case MLFF.MACE_FIELD: # needs the MACE-Field fork of mace and the path of a model file from mace.calculators import MACECalculator @@ -559,7 +559,7 @@ def _get_pkg_name(calculator_meta: MLFF | str | dict[str, Any]) -> str | None: | MLFF.MACE_MP_0 | MLFF.MACE_MPA_0 | MLFF.MACE_MP_0B3 - | MLFF.MACE_Field + | MLFF.MACE_FIELD ): ff_pkg = "mace-torch" case MLFF.MatterSim: diff --git a/src/atomate2/torchsim/flows/phonons.py b/src/atomate2/torchsim/flows/phonons.py index bb17c17288..4da39e5566 100644 --- a/src/atomate2/torchsim/flows/phonons.py +++ b/src/atomate2/torchsim/flows/phonons.py @@ -9,6 +9,7 @@ from atomate2.common.flows.phonons import BasePhononMaker if TYPE_CHECKING: + from atomate2.forcefields.jobs import ForceFieldDielectricMaker from atomate2.torchsim.core import TorchSimOptimizeMaker, TorchSimStaticMaker @@ -23,7 +24,8 @@ class PhononMaker(BasePhononMaker): forces are computed for these structures. With the help of phonopy, these forces are then converted into a dynamical matrix. To correct for polarization effects, a correction of the dynamical matrix based on BORN charges can - be performed. The BORN charges can be supplied manually. + be performed. The BORN charges can be supplied manually or computed + with ``born_maker``. Finally, phonon densities of states, phonon band structures and thermodynamic properties are computed. @@ -84,7 +86,7 @@ class PhononMaker(BasePhononMaker): A maker to perform the computation of the DFT energy on the bulk. Set to ``None`` to skip the static energy computation - born_maker: .TorchSimStaticMaker or None + born_maker: .ForceFieldDielectricMaker or None Maker to compute the BORN charges. phonon_displacement_maker : .TorchSimStaticMaker or None Maker used to compute the forces for a supercell. @@ -128,7 +130,7 @@ class PhononMaker(BasePhononMaker): kpath_scheme: str = "seekpath" code: str = "torchsim" store_force_constants: bool = True - born_maker: TorchSimStaticMaker | None = None + born_maker: ForceFieldDielectricMaker | None = None socket: bool = True @property diff --git a/tests/common/schemas/test_phonons.py b/tests/common/schemas/test_phonons.py index 38884f933d..681274a763 100644 --- a/tests/common/schemas/test_phonons.py +++ b/tests/common/schemas/test_phonons.py @@ -76,6 +76,8 @@ def get_nacl_phonon(): [ ("vasp", 1, True), ("forcefields", 1, True), + ("ase", 1, True), + ("torchsim", 1, True), ("aims", 1, False), ("vasp", 0, False), ], diff --git a/tests/forcefields/conftest.py b/tests/forcefields/conftest.py index 3a77b5bdaa..8e53e0a832 100644 --- a/tests/forcefields/conftest.py +++ b/tests/forcefields/conftest.py @@ -27,11 +27,11 @@ } # the MACE-Field fork installs as mace-torch, so only its model class tells them apart try: - _INSTALLED_MLFF["MACE_Field"] = hasattr( + _INSTALLED_MLFF["MACE_FIELD"] = hasattr( import_module("mace.modules.extensions"), "MACEField" ) except ImportError: - _INSTALLED_MLFF["MACE_Field"] = False + _INSTALLED_MLFF["MACE_FIELD"] = False def mlff_is_installed(mlff: str | MLFF) -> bool: diff --git a/tests/forcefields/flows/test_pheasy.py b/tests/forcefields/flows/test_pheasy.py index 3315963a1b..a627ff8c19 100644 --- a/tests/forcefields/flows/test_pheasy.py +++ b/tests/forcefields/flows/test_pheasy.py @@ -8,6 +8,7 @@ pytest.importorskip("pheasy") +import numpy as np from ase.build import bulk from emmet.core.phonon import ( PhononBS, @@ -16,12 +17,16 @@ ThermalDisplacementData, ) from jobflow import run_locally -from pymatgen.core import Structure +from pymatgen.core import Lattice, Structure from pymatgen.io.ase import AseAtomsAdaptor import atomate2.common.jobs.pheasy as pheasy_jobs from atomate2.forcefields.flows.pheasy import PhononMaker -from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker +from atomate2.forcefields.jobs import ( + ForceFieldDielectricMaker, + ForceFieldRelaxMaker, + ForceFieldStaticMaker, +) EMT = {"@module": "ase.calculators.emt", "@callable": "EMT"} @@ -76,3 +81,29 @@ def test_pheasy_wf_force_field(clean_dir): assert isinstance(ph_doc.structure, Structure) assert ph_doc.has_imaginary_modes is False assert isinstance(ph_doc.force_constants, list) + + +def test_pheasy_wf_force_field_born_charges(clean_dir, fake_dielectric_calculator): + structure = Structure.from_spacegroup( + "Fm-3m", Lattice.cubic(4.17), ["Ni", "O"], [[0, 0, 0], [0.5, 0.5, 0.5]] + ).get_primitive_structure() + maker = PhononMaker( + bulk_relax_maker=None, + static_energy_maker=None, + phonon_displacement_maker=ForceFieldStaticMaker(force_field_name=EMT), + born_maker=ForceFieldDielectricMaker(), + min_length=8, + create_thermal_displacements=False, + store_force_constants=False, + ) + flow = maker.make(structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + ph_doc = responses[flow.jobs[-1].uuid][1].output + + assert np.array(ph_doc.born) == pytest.approx( + np.array([2, -2])[:, None, None] * np.eye(3) + ) + # the LO-TO splitting raises the highest frequency + assert np.max(ph_doc.phonon_bandstructure.frequencies) == pytest.approx( + 17.974, abs=1e-2 + ) diff --git a/tests/forcefields/flows/test_phonon.py b/tests/forcefields/flows/test_phonon.py index 83c8fda584..4ff93c80dc 100644 --- a/tests/forcefields/flows/test_phonon.py +++ b/tests/forcefields/flows/test_phonon.py @@ -47,7 +47,7 @@ "MATPES_PBE", "Allegro", "FAIRChem", - "MACE_Field", + "MACE_FIELD", ], ) ) @@ -299,7 +299,6 @@ def test_ext_load_phonon_initialization(): def test_phonon_wf_force_field_born_charges( clean_dir, fake_dielectric_calculator, born_by_hand ): - """Born charges from a force field dielectric job or given by hand enter the NAC.""" structure = Structure.from_spacegroup( "Fm-3m", Lattice.cubic(4.17), ["Ni", "O"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() @@ -325,6 +324,5 @@ def test_phonon_wf_force_field_born_charges( assert np.array(doc.born) == pytest.approx(born) assert np.array(doc.epsilon_static) == pytest.approx(4 * np.eye(3)) - assert doc.phonon_bandstructure.has_nac # the LO-TO splitting raises the highest frequency from about 12.6 THz assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(17.976, abs=1e-2) diff --git a/tests/forcefields/test_jobs.py b/tests/forcefields/test_jobs.py index 386b88e73a..d39264c53f 100644 --- a/tests/forcefields/test_jobs.py +++ b/tests/forcefields/test_jobs.py @@ -916,7 +916,7 @@ def test_roundtrip_legacy(si_structure: Structure, import_str: str): assert isinstance(deser.maker.calculator, Calculator) -def test_dielectric_maker(fake_dielectric_calculator, clean_dir): +def test_dielectric_maker(fake_dielectric_calculator): structure = Structure.from_spacegroup( "Fm-3m", Lattice.cubic(5.6), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() @@ -926,6 +926,5 @@ def test_dielectric_maker(fake_dielectric_calculator, clean_dir): assert isinstance(output, ForceFieldDielectricDocument) assert output.structure == structure assert np.array(output.born) == approx(np.array([2, -2])[:, None, None] * np.eye(3)) - # eps_inf = 1 + chi assert np.array(output.epsilon_static) == approx(4 * np.eye(3)) - assert output.forcefield_name == "MLFF.MACE_Field" + assert output.forcefield_name == "MLFF.MACE_FIELD" diff --git a/tests/forcefields/test_mace_field.py b/tests/forcefields/test_mace_field.py index 48cca063fe..35ae441ba1 100644 --- a/tests/forcefields/test_mace_field.py +++ b/tests/forcefields/test_mace_field.py @@ -1,11 +1,8 @@ -"""Test the Born charges and the dielectric tensor of the MACE-Field model. - -The MACE-Field fork of mace installs as mace-torch, so these tests only run in -the mace-field CI group. -""" +"""Test the Born charges and the dielectric tensor of the MACE-Field model.""" import hashlib import urllib.request +from importlib.metadata import version as get_imported_version import numpy as np import pytest @@ -13,14 +10,11 @@ from jobflow import run_locally from pymatgen.core import Lattice, Structure +from atomate2.forcefields.flows.phonons import PhononMaker from atomate2.forcefields.jobs import ForceFieldDielectricMaker from .conftest import mlff_is_installed -pytestmark = pytest.mark.skipif( - not mlff_is_installed("MACE_Field"), reason="MACE-Field is not installed" -) - MODEL_URL = ( "https://github.com/mdi-group/mace-field/releases/download/1.0.2/" "MACEField-MH-0-omat-dielectric.model" @@ -36,21 +30,51 @@ def mace_field_model(tmp_path_factory): return path -def test_mace_field_dielectric_maker(mace_field_model, clean_dir): - structure = Structure.from_spacegroup( +@pytest.fixture +def nacl_structure(): + return Structure.from_spacegroup( "Fm-3m", Lattice.cubic(5.64), ["Na", "Cl"], [[0, 0, 0], [0.5, 0.5, 0.5]] ).get_primitive_structure() + + +@pytest.mark.skipif( + not mlff_is_installed("MACE_FIELD"), reason="MACE-Field is not installed" +) +def test_mace_field_dielectric_maker(mace_field_model, nacl_structure): job = ForceFieldDielectricMaker( calculator_kwargs={"model": str(mace_field_model)} - ).make(structure) + ).make(nacl_structure) output = run_locally(job, ensure_success=True)[job.uuid][1].output born = np.array(output.born) # the acoustic sum rule holds by construction assert born.sum(axis=0) == pytest.approx(np.zeros((3, 3)), abs=1e-6) - # cubic, so the tensors are isotropic. The Materials Project's Harmonic Phonon - # Database has 1.09 and 2.56 from DFPT. + # cubic, so the tensors are isotropic species = [str(site.specie) for site in output.structure] assert born[species.index("Na")] == pytest.approx(1.0898 * np.eye(3), abs=1e-3) epsilon = np.array(output.epsilon_static) assert epsilon == pytest.approx(2.5845 * np.eye(3), abs=1e-3) + assert output.forcefield_version == get_imported_version("mace-torch") + + +@pytest.mark.skipif( + not mlff_is_installed("MACE_FIELD"), reason="MACE-Field is not installed" +) +def test_mace_field_phonon_nac(mace_field_model, nacl_structure): + maker = PhononMaker.from_force_field_name( + "MACE_MP_0", + calculator_kwargs={"model": "medium-omat-0"}, + relax_initial_structure=False, + born_maker=ForceFieldDielectricMaker( + calculator_kwargs={"model": str(mace_field_model)} + ), + min_length=10, + create_thermal_displacements=False, + store_force_constants=False, + ) + flow = maker.make(nacl_structure) + responses = run_locally(flow, create_folders=True, ensure_success=True) + doc = responses[flow[-1].uuid][1].output + + # 6.486 THz without the MACE-Field Born charges + assert np.max(doc.phonon_bandstructure.bands) == pytest.approx(7.505, abs=1e-2) diff --git a/tests/forcefields/test_md.py b/tests/forcefields/test_md.py index 2aaef9f90f..09afaf3b68 100644 --- a/tests/forcefields/test_md.py +++ b/tests/forcefields/test_md.py @@ -47,7 +47,7 @@ def test_maker_initialization(mlff): # MACE-Field needs the path of its model file _mlffs_for_test = set(INSTALLED_MLFF).difference( - map(MLFF, ("Forcefield", "Allegro", "M3GNet", "MACE", "Nequip", "MACE_Field")) + map(MLFF, ("Forcefield", "Allegro", "M3GNet", "MACE", "Nequip", "MACE_FIELD")) ) _md_test_params = sorted(product(_mlffs_for_test, [True, False]), key=str) From 0b9ff919272bcec0615ca3d6bb5ca69933e3f311 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 13:27:18 -0700 Subject: [PATCH 28/43] Move the MACE-Field fork to a dependency group --- .github/workflows/testing.yml | 4 +++- docs/user/codes/forcefields.md | 2 +- pyproject.toml | 10 ++++++---- 3 files changed, 10 insertions(+), 6 deletions(-) diff --git a/.github/workflows/testing.yml b/.github/workflows/testing.yml index c2bf5e05f0..12670dcfab 100644 --- a/.github/workflows/testing.yml +++ b/.github/workflows/testing.yml @@ -68,7 +68,9 @@ jobs: python -m pip install --upgrade pip mkdir -p ~/.abinit/pseudos cp -r tests/test_data/abinit/pseudos/ONCVPSP-PBE-SR-PDv0.4 ~/.abinit/pseudos - uv pip install .[strict,strict-forcefields-${{ matrix.dep-group }},abinit,approxneb,aims] --group tests + # the MACE-Field fork is the mace-field dependency group, not an extra + uv pip install .[strict,abinit,approxneb,aims${{ matrix.dep-group != 'mace-field' && format(',strict-forcefields-{0}', matrix.dep-group) || '' }}] \ + --group tests ${{ matrix.dep-group == 'mace-field' && '--group mace-field' || '' }} # the thermal expansion tests use EMT, so one group is enough to run them - name: Install pheasy, ALM and phono3py for the thermal expansion tests diff --git a/docs/user/codes/forcefields.md b/docs/user/codes/forcefields.md index 0737695c1b..a8ddcedd9f 100644 --- a/docs/user/codes/forcefields.md +++ b/docs/user/codes/forcefields.md @@ -111,7 +111,7 @@ The default in `atomate2` is the OMat24 model with `uma-s-1p1`. The phonon workflows use them for the non-analytical correction when `ForceFieldDielectricMaker` is set as `born_maker`. MACE-Field is a fork of MACE that installs as `mace_torch`, so it replaces MACE. -Install it with `pip install 'atomate2[mace-field]'`. +Install it with `pip install git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64`, the commit atomate2 is tested with. The fork also runs the MACE foundation models, so the forces can come from MACE-OMAT in the same environment. The model file has to be downloaded from the [MACE-Field releases](https://github.com/mdi-group/mace-field/releases). There is no default model, so `model` must be set. diff --git a/pyproject.toml b/pyproject.toml index eff3fd4516..1ccc834dee 100644 --- a/pyproject.toml +++ b/pyproject.toml @@ -70,7 +70,6 @@ defects = [ ase = ["ase>=3.26.0"] ase-ext = ["tblite>=0.3.0; platform_system=='Linux'"] forcefields-demo = ["chgnet>=0.3.8","atomate2[ase]"] -mace-field = ["atomate2[ase]", "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64"] torchsim = [ "torch-sim-atomistic[symmetry]==0.6.1; python_version >= '3.12'" @@ -139,9 +138,6 @@ strict-forcefields-e3nn-limited = [ strict-forcefields-numpy-limited = [ "nequip-allegro==0.8.3", ] -# MACE-Field installs as mace-torch, so it cannot share a group with mace-torch. -# Remove this group once MACE-Field is in a mace-torch release (ACEsuit/mace#1177). -strict-forcefields-mace-field = ["atomate2[mace-field]"] strict = [ "atomate2[cclib, phonons, lobster, openmm, mp, defects, ase, ase-ext]", @@ -162,6 +158,12 @@ changelog = "https://github.com/materialsproject/atomate2/blob/main/CHANGELOG.md [dependency-groups] dev = ["pre-commit>=4.5.1"] +# MACE-Field installs as mace-torch, so it cannot share a group with mace-torch. +# It is a dependency group, since PyPI does not accept git URLs in extras. +# Remove it once MACE-Field is in a mace-torch release (ACEsuit/mace#1177). +mace-field = [ + "mace-torch @ git+https://github.com/mdi-group/mace-field.git@45d5c5fa7b40a155855b3d155df1760e36849e64", +] tests = [ "fireworks==2.1.4", "nbmake==1.5.5", From bb3218a98c9cb90960980d6a99fffeaab1aabadd Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 13:33:19 -0700 Subject: [PATCH 29/43] Use check_class_name for the Born charges in the finite-temperature flow --- .../common/flows/finite_temperature_phonons.py | 12 ++++-------- 1 file changed, 4 insertions(+), 8 deletions(-) diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 819ca1eb3d..362343e71e 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -21,6 +21,7 @@ ) from atomate2.common.jobs.pheasy import get_supercell_size from atomate2.common.jobs.phonons import run_phonon_displacements +from atomate2.common.utils import check_class_name if TYPE_CHECKING: from pathlib import Path @@ -377,17 +378,12 @@ def make( born_kwargs[self.prev_calc_dir_argname] = prev_dir born_job = self.born_maker.make(structure, **born_kwargs) jobs.append(born_job) - # As in the phonon workflow, a force field dielectric document has the - # Born charges as fields. A VASP task document has them in its last - # calculation. - schema = getattr(born_job, "output_schema", None) - if schema is not None and "born" in schema.model_fields: + if check_class_name(self.born_maker, "ForceFieldDielectricMaker"): born = born_job.output.born epsilon_static = born_job.output.epsilon_static else: - calc_output = born_job.output.calcs_reversed[0].output - born = calc_output.outcar["born"] - epsilon_static = calc_output.epsilon_static + born = born_job.output.calcs_reversed[0].output.outcar["born"] + epsilon_static = born_job.output.calcs_reversed[0].output.epsilon_static born_run_job_dir = born_job.output.dir_name born_run_uuid = born_job.output.uuid From 56b0668a637bef88cc285b21843ef624ce6e2b35 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 13:46:23 -0700 Subject: [PATCH 30/43] Mention MACE-Field Born charges in the finite-temperature tutorial --- tutorials/finite_temperature_phonons.ipynb | 8 +++++--- 1 file changed, 5 insertions(+), 3 deletions(-) diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 02876f9844..6f913b613b 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -784,7 +784,7 @@ " 100 K. Bi4S3N2 keeps imaginary modes down to -0.8 THz in 12 of 15 runs. Its\n", " AIMD reference has a small one as well, at -0.12 THz. Bi4S3N2 is polar, so\n", " these runs and the AIMD reference are compared without the non-analytical\n", - " correction. The force fields give no Born charges.\n", + " correction. The three MACE potentials give no Born charges.\n", "\n", "The trajectory check did not report \"stable\" for five runs:\n", "\n", @@ -1297,8 +1297,10 @@ "`run_npt=True` as in Section 2. The NPT cell is the average over one MD run, so\n", "it carries the noise of that run.\n", "\n", - "A machine-learned potential gives no Born charges, so the non-analytical\n", - "correction is not applied here. With VASP, the `born_maker` computes them.\n", + "The three MACE potentials give no Born charges, so the non-analytical\n", + "correction is not applied here. A `born_maker` can add them, either\n", + "`ForceFieldDielectricMaker` with MACE-Field (see the force field docs of\n", + "atomate2) or a VASP `DielectricMaker`.\n", "\n", "The trajectory check uses fixed limits. A Lindemann ratio above 0.15 is reported\n", "as melting. A displacement from the reference of more than 1.5 times the\n", From 14bfe9dda191fe3eba0f835d14f6423e122c2585 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 14:13:43 -0700 Subject: [PATCH 31/43] Point to the MACE-Field notes from the phonon docs --- docs/user/codes/vasp.md | 3 +++ 1 file changed, 3 insertions(+) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index f283cd436d..06e4372bc2 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -342,6 +342,9 @@ phonon_flow = PhononMaker(min_length=15.0, store_force_constants=False).make( ) ``` +The force field phonon, pheasy and hiPhive workflows can take the Born charges from MACE-Field, with `ForceFieldDielectricMaker` as `born_maker`. +See the [notes on MACE-Field](forcefields.md#mace-field-notes). + #### Pheasy Alternatively, users can accelerate the calculation of interatomic force constants using the machine-learning-based [Pheasy code](https://doi.org/10.48550/arXiv.2508.01020). From dccf688a84011229bd08cd8f89cbfd67f121c65f Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 14:55:45 -0700 Subject: [PATCH 32/43] Extract the consecutive MD jobs into ChainedMDMaker --- docs/user/codes/vasp.md | 1 + .../flows/finite_temperature_phonons.py | 118 +++++++++++------- .../flows/test_finite_temperature_phonons.py | 6 +- .../flows/test_finite_temperature_phonons.py | 14 ++- 4 files changed, 85 insertions(+), 54 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index 67d2dc9eaf..cb8ec37f99 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -456,6 +456,7 @@ Both set ISPIN from the relaxation directory with `auto_ispin`. `md_runs` splits the MD into consecutive jobs, for example to stay within the walltime of a queue. Each job continues from the positions and velocities of the previous one. The thermostat variables start again from zero in each job. +`ChainedMDMaker` in `atomate2.common.flows.finite_temperature_phonons` makes these jobs, for VASP and for force fields. The MD files are read by the job that picks the snapshots, so the MD run directories must be on a file system that this job can read. An NPT MD can be run first to include thermal expansion. diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 362343e71e..3553aff9a8 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -3,7 +3,7 @@ from __future__ import annotations from abc import ABC, abstractmethod -from dataclasses import dataclass +from dataclasses import dataclass, field from enum import Enum from typing import TYPE_CHECKING, Literal @@ -43,6 +43,69 @@ def _get_force_field(maker: Maker, code: str) -> tuple[str | None, dict | None]: ) +@dataclass +class ChainedMDMaker(Maker): + """ + Maker to run one MD as several consecutive MD jobs, with VASP or a force field. + + The first MD job starts from the input structure. Each later one starts from + the final positions and velocities of the previous one. The thermostat + variables are not carried over, so they start again from zero in each job. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + md_makers: list[Maker] + Makers of the MD jobs, in the order of the trajectory. + md_code: str + Code of the MD, 'vasp' or 'forcefields'. + """ + + name: str = "chained MD" + md_makers: list[Maker] = field(default_factory=list) + md_code: str = "vasp" + + def make(self, structure: Structure, prev_dir: str | Path | None = None) -> Flow: + """ + Make a flow of consecutive MD jobs. + + Parameters + ---------- + structure: Structure + The structure the first MD job starts from. Its magnetic moments, if + any, are also given to the later MD jobs. + prev_dir: str | Path | None + A previous calculation directory, passed to each MD job. + + Returns + ------- + Flow + Its output holds the directories and the uuids of the MD jobs, in + the order of the trajectory. + """ + jobs: list[Job] = [] + md_jobs: list[Job] = [] + md_structure = structure + for idx, maker in enumerate(self.md_makers, start=1): + md_job = maker.make(md_structure, prev_dir=prev_dir) + if len(self.md_makers) > 1: + md_job.append_name(f" {idx}/{len(self.md_makers)}") + jobs.append(md_job) + md_jobs.append(md_job) + if idx < len(self.md_makers): + restart = get_md_restart_structure( + md_job.output.dir_name, self.md_code, structure + ) + jobs.append(restart) + md_structure = restart.output + output = { + "dir_names": [md_job.output.dir_name for md_job in md_jobs], + "uuids": [md_job.uuid for md_job in md_jobs], + } + return Flow(jobs, output, name=self.name) + + @due.dcite( Doi("10.48550/arXiv.2508.01020"), description="Pheasy code for (an)harmonic force constants.", @@ -393,9 +456,12 @@ def make( jobs.append(reference_job) reference = reference_job.output - all_md_jobs, md_jobs = self.make_md(reference, prev_dir) - jobs.extend(all_md_jobs) - md_dirs = [md_job.output.dir_name for md_job in md_jobs] + md_flow = ChainedMDMaker( + md_makers=[self.get_md_maker(n_steps) for n_steps in self.get_md_steps()], + md_code=self.md_code, + ).make(reference, prev_dir=prev_dir) + jobs.append(md_flow) + md_dirs = md_flow.output["dir_names"] snapshot_job = select_md_snapshots( md_dirs, @@ -441,7 +507,7 @@ def make( force_field_kwargs=force_field_kwargs, md_force_field_name=md_force_field_name, md_force_field_kwargs=md_force_field_kwargs, - md_uuids=[md_job.uuid for md_job in md_jobs], + md_uuids=md_flow.output["uuids"], md_job_dirs=md_dirs, optimization_run_uuid=optimization_run_uuid, optimization_run_job_dir=optimization_run_job_dir, @@ -459,48 +525,6 @@ def make( jobs.append(fit_job) return Flow(jobs, fit_job.output, name=self.name) - def make_md( - self, - reference: Structure | OutputReference, - prev_dir: str | Path | None, - ) -> tuple[list[Job | Flow], list[Job]]: - """ - Make the MD jobs, starting from the undisplaced supercell. - - The first MD job starts from the undisplaced supercell. Each later one - continues from the final positions and velocities of the previous one. - - Parameters - ---------- - reference: Structure | OutputReference - The undisplaced supercell. - prev_dir: str | Path | None - A previous calculation directory, passed to each MD job. - - Returns - ------- - tuple[list[Job | Flow], list[Job]] - All jobs to add to the flow, and the MD jobs in the order of the - trajectory. - """ - jobs: list[Job | Flow] = [] - md_jobs: list[Job] = [] - structure = reference - md_steps = self.get_md_steps() - for idx, n_steps in enumerate(md_steps, start=1): - md_job = self.get_md_maker(n_steps).make(structure, prev_dir=prev_dir) - if len(md_steps) > 1: - md_job.append_name(f" {idx}/{len(md_steps)}") - jobs.append(md_job) - md_jobs.append(md_job) - if idx < len(md_steps): - restart = get_md_restart_structure( - md_job.output.dir_name, self.md_code, reference - ) - jobs.append(restart) - structure = restart.output - return jobs, md_jobs - @property @abstractmethod def prev_calc_dir_argname(self) -> str | None: diff --git a/tests/forcefields/flows/test_finite_temperature_phonons.py b/tests/forcefields/flows/test_finite_temperature_phonons.py index 0ae2877705..4708548806 100644 --- a/tests/forcefields/flows/test_finite_temperature_phonons.py +++ b/tests/forcefields/flows/test_finite_temperature_phonons.py @@ -112,11 +112,13 @@ def test_force_field_md_maker(cu3au): # the MD jobs have a number only when there are several flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) - md_names = [job.name for job in flow.jobs if "MD" in job.name] + md_flow = next(job for job in flow.jobs if job.name == "chained MD") + md_names = [job.name for job in md_flow.jobs if "MD" in job.name] assert md_names == ["ASE MD 1/3", "ASE MD 2/3", "ASE MD 3/3"] maker = ForceFieldFiniteTemperaturePhononMaker(md_time=2.0) flow = maker.make(cu3au, supercell_matrix=np.eye(3).tolist()) - assert [job.name for job in flow.jobs if "MD" in job.name] == ["ASE MD"] + md_flow = next(job for job in flow.jobs if job.name == "chained MD") + assert [job.name for job in md_flow.jobs] == ["ASE MD"] nose_hoover = ForceFieldFiniteTemperaturePhononMaker( thermostat="nose-hoover", md_time_step=2.0 diff --git a/tests/vasp/flows/test_finite_temperature_phonons.py b/tests/vasp/flows/test_finite_temperature_phonons.py index 8bc48c7c9e..4e6ac43c0e 100644 --- a/tests/vasp/flows/test_finite_temperature_phonons.py +++ b/tests/vasp/flows/test_finite_temperature_phonons.py @@ -45,15 +45,19 @@ def test_vasp_flows(si_structure, maker_cls, md_code, code): "get_supercell_size", *born_names, "get_md_supercell", - f"{md_names[0]} 1/2", - "get_md_restart_structure", - f"{md_names[1]} 2/2", + "chained MD", "select_md_snapshots", "run_phonon_displacements", "fit_finite_temperature_phonons", ] relax = flow.jobs[0] - reference, md_1, restart, md_2, snapshots, statics, fit = flow.jobs[-7:] + reference, md_flow, snapshots, statics, fit = flow.jobs[-5:] + md_1, restart, md_2 = md_flow.jobs + assert [job.name for job in md_flow.jobs] == [ + f"{md_names[0]} 1/2", + "get_md_restart_structure", + f"{md_names[1]} 2/2", + ] assert isinstance(relax, Flow) # a diagonal supercell @@ -115,7 +119,7 @@ def test_flow_from_output_reference(): structure = OutputReference("1234", attributes=(("a", "structure"),)) flow = FiniteTemperaturePhononMaker().make(structure) assert flow.jobs[0].name == "double relax" - assert [job.name for job in flow.jobs][4] == "molecular dynamics" + assert [job.name for job in flow.jobs][4] == "chained MD" def test_non_diagonal_supercell_matrix(si_structure): From fb9c90c16b3633875e2e6ca56a13c0a5a27bb8da Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 20:23:08 -0700 Subject: [PATCH 33/43] Move ChainedMDMaker and the MD restart job into common MD modules --- docs/user/codes/vasp.md | 2 +- .../flows/finite_temperature_phonons.py | 67 +--------------- src/atomate2/common/flows/md.py | 79 +++++++++++++++++++ .../common/jobs/finite_temperature_phonons.py | 57 +------------ src/atomate2/common/jobs/md.py | 68 ++++++++++++++++ .../flows/finite_temperature_phonons.py | 2 +- .../jobs/test_finite_temperature_phonons.py | 41 +--------- tests/common/jobs/test_md.py | 55 +++++++++++++ 8 files changed, 209 insertions(+), 162 deletions(-) create mode 100644 src/atomate2/common/flows/md.py create mode 100644 src/atomate2/common/jobs/md.py create mode 100644 tests/common/jobs/test_md.py diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index cb8ec37f99..ceb2c75b6c 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -456,7 +456,7 @@ Both set ISPIN from the relaxation directory with `auto_ispin`. `md_runs` splits the MD into consecutive jobs, for example to stay within the walltime of a queue. Each job continues from the positions and velocities of the previous one. The thermostat variables start again from zero in each job. -`ChainedMDMaker` in `atomate2.common.flows.finite_temperature_phonons` makes these jobs, for VASP and for force fields. +`ChainedMDMaker` in `atomate2.common.flows.md` makes these jobs, for VASP and for force fields. The MD files are read by the job that picks the snapshots, so the MD run directories must be on a file system that this job can read. An NPT MD can be run first to include thermal expansion. diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 3553aff9a8..808eebe431 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -3,7 +3,7 @@ from __future__ import annotations from abc import ABC, abstractmethod -from dataclasses import dataclass, field +from dataclasses import dataclass from enum import Enum from typing import TYPE_CHECKING, Literal @@ -12,9 +12,9 @@ from pymatgen.util.due import Doi, due from atomate2 import SETTINGS +from atomate2.common.flows.md import ChainedMDMaker from atomate2.common.jobs.finite_temperature_phonons import ( fit_finite_temperature_phonons, - get_md_restart_structure, get_md_supercell, get_npt_structure, select_md_snapshots, @@ -43,69 +43,6 @@ def _get_force_field(maker: Maker, code: str) -> tuple[str | None, dict | None]: ) -@dataclass -class ChainedMDMaker(Maker): - """ - Maker to run one MD as several consecutive MD jobs, with VASP or a force field. - - The first MD job starts from the input structure. Each later one starts from - the final positions and velocities of the previous one. The thermostat - variables are not carried over, so they start again from zero in each job. - - Parameters - ---------- - name: str - Name of the flows produced by this maker. - md_makers: list[Maker] - Makers of the MD jobs, in the order of the trajectory. - md_code: str - Code of the MD, 'vasp' or 'forcefields'. - """ - - name: str = "chained MD" - md_makers: list[Maker] = field(default_factory=list) - md_code: str = "vasp" - - def make(self, structure: Structure, prev_dir: str | Path | None = None) -> Flow: - """ - Make a flow of consecutive MD jobs. - - Parameters - ---------- - structure: Structure - The structure the first MD job starts from. Its magnetic moments, if - any, are also given to the later MD jobs. - prev_dir: str | Path | None - A previous calculation directory, passed to each MD job. - - Returns - ------- - Flow - Its output holds the directories and the uuids of the MD jobs, in - the order of the trajectory. - """ - jobs: list[Job] = [] - md_jobs: list[Job] = [] - md_structure = structure - for idx, maker in enumerate(self.md_makers, start=1): - md_job = maker.make(md_structure, prev_dir=prev_dir) - if len(self.md_makers) > 1: - md_job.append_name(f" {idx}/{len(self.md_makers)}") - jobs.append(md_job) - md_jobs.append(md_job) - if idx < len(self.md_makers): - restart = get_md_restart_structure( - md_job.output.dir_name, self.md_code, structure - ) - jobs.append(restart) - md_structure = restart.output - output = { - "dir_names": [md_job.output.dir_name for md_job in md_jobs], - "uuids": [md_job.uuid for md_job in md_jobs], - } - return Flow(jobs, output, name=self.name) - - @due.dcite( Doi("10.48550/arXiv.2508.01020"), description="Pheasy code for (an)harmonic force constants.", diff --git a/src/atomate2/common/flows/md.py b/src/atomate2/common/flows/md.py new file mode 100644 index 0000000000..4cbb651682 --- /dev/null +++ b/src/atomate2/common/flows/md.py @@ -0,0 +1,79 @@ +"""Flows for molecular dynamics that are shared between codes.""" + +from __future__ import annotations + +from dataclasses import dataclass, field +from typing import TYPE_CHECKING + +from jobflow import Flow, Maker + +from atomate2.common.jobs.md import get_md_restart_structure + +if TYPE_CHECKING: + from pathlib import Path + + from jobflow import Job + from pymatgen.core import Structure + + +@dataclass +class ChainedMDMaker(Maker): + """ + Maker to run one MD as several consecutive MD jobs, with VASP or a force field. + + The first MD job starts from the input structure. Each later one starts from + the final positions and velocities of the previous one. The thermostat + variables are not carried over, so they start again from zero in each job. + + Parameters + ---------- + name: str + Name of the flows produced by this maker. + md_makers: list[Maker] + Makers of the MD jobs, in the order of the trajectory. + md_code: str + Code of the MD, 'vasp' or 'forcefields'. + """ + + name: str = "chained MD" + md_makers: list[Maker] = field(default_factory=list) + md_code: str = "vasp" + + def make(self, structure: Structure, prev_dir: str | Path | None = None) -> Flow: + """ + Make a flow of consecutive MD jobs. + + Parameters + ---------- + structure: Structure + The structure the first MD job starts from. Its magnetic moments, if + any, are also given to the later MD jobs. + prev_dir: str | Path | None + A previous calculation directory, passed to each MD job. + + Returns + ------- + Flow + Its output holds the directories and the uuids of the MD jobs, in + the order of the trajectory. + """ + jobs: list[Job] = [] + md_jobs: list[Job] = [] + md_structure = structure + for idx, maker in enumerate(self.md_makers, start=1): + md_job = maker.make(md_structure, prev_dir=prev_dir) + if len(self.md_makers) > 1: + md_job.append_name(f" {idx}/{len(self.md_makers)}") + jobs.append(md_job) + md_jobs.append(md_job) + if idx < len(self.md_makers): + restart = get_md_restart_structure( + md_job.output.dir_name, self.md_code, structure + ) + jobs.append(restart) + md_structure = restart.output + output = { + "dir_names": [md_job.output.dir_name for md_job in md_jobs], + "uuids": [md_job.uuid for md_job in md_jobs], + } + return Flow(jobs, output, name=self.name) diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index 9fca439b4a..ee544f48b2 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -18,11 +18,12 @@ from phonopy.interface.vasp import write_vasp from pymatgen.core import Structure from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure -from pymatgen.io.vasp import Incar, Kpoints, Poscar, Xdatcar +from pymatgen.io.vasp import Incar, Kpoints, Xdatcar from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine from pymatgen.phonon.dos import PhononDos from pymatgen.symmetry.analyzer import SpacegroupAnalyzer +from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE, _get_site_properties from atomate2.common.jobs.pheasy import ( _DEFAULT_FILE_PATHS, _check_lasso_alpha, @@ -54,8 +55,6 @@ logger = logging.getLogger(__name__) -# file of the force field MD trajectory, written in the ASE format -ASE_TRAJECTORY_FILE = "md_trajectory.traj" _KPATH_SCHEME = "seekpath" # Limits of the trajectory check @@ -96,13 +95,6 @@ def _get_phonopy( ) -def _get_site_properties(reference: Structure) -> dict: - """Get the magnetic moments of the reference, the only site property kept.""" - if "magmom" in reference.site_properties: - return {"magmom": reference.site_properties["magmom"]} - return {} - - @job def get_md_supercell( structure: Structure, supercell_matrix: Matrix3D, symprec: float, code: str @@ -147,51 +139,6 @@ def get_md_supercell( ) -@job -def get_md_restart_structure( - md_dir: str, md_code: str, reference: Structure -) -> Structure: - """ - Get the final positions and velocities of an MD run. - - For VASP, they are read from CONTCAR, with the velocities in Angstrom/fs. - For force fields, they are read from the last frame of the ASE trajectory - file, with the velocities in ASE units. In both cases, the velocities are a - site property that the next MD run starts from. The thermostat variables - are not carried over, so they start again from zero in the next run. The - magnetic moments of the reference, if any, are added as a site property. - - Parameters - ---------- - md_dir: str - Directory of the MD run. - md_code: str - Code of the MD, "vasp" or "forcefields". - reference: Structure - The undisplaced supercell the MD started from. - - Returns - ------- - Structure - The final structure, with a "velocities" site property. - """ - directory = Path(strip_hostname(md_dir)) - if md_code == "vasp": - structure = Poscar.from_file(zpath(str(directory / "CONTCAR"))).structure - else: - atoms = ase_read(directory / ASE_TRAJECTORY_FILE, index=-1) - structure = Structure( - atoms.cell[:], - atoms.get_chemical_symbols(), - atoms.get_positions(), - coords_are_cartesian=True, - site_properties={"velocities": atoms.get_velocities().tolist()}, - ) - for key, values in _get_site_properties(reference).items(): - structure.add_site_property(key, values) - return structure - - def _read_vasp_md( directory: Path, ) -> tuple[np.ndarray, np.ndarray, np.ndarray, list[str], float]: diff --git a/src/atomate2/common/jobs/md.py b/src/atomate2/common/jobs/md.py new file mode 100644 index 0000000000..e1cca05131 --- /dev/null +++ b/src/atomate2/common/jobs/md.py @@ -0,0 +1,68 @@ +"""Jobs for molecular dynamics that are shared between codes.""" + +from __future__ import annotations + +from pathlib import Path + +from ase.io import read as ase_read +from jobflow import job +from monty.os.path import zpath +from pymatgen.core import Structure +from pymatgen.io.vasp import Poscar + +from atomate2.utils.path import strip_hostname + +# file of the force field MD trajectory, written in the ASE format +ASE_TRAJECTORY_FILE = "md_trajectory.traj" + + +def _get_site_properties(reference: Structure) -> dict: + """Get the magnetic moments of the reference, the only site property kept.""" + if "magmom" in reference.site_properties: + return {"magmom": reference.site_properties["magmom"]} + return {} + + +@job +def get_md_restart_structure( + md_dir: str, md_code: str, reference: Structure +) -> Structure: + """ + Get the final positions and velocities of an MD run. + + For VASP, they are read from CONTCAR, with the velocities in Angstrom/fs. + For force fields, they are read from the last frame of the ASE trajectory + file, with the velocities in ASE units. In both cases, the velocities are a + site property that the next MD run starts from. The thermostat variables + are not carried over, so they start again from zero in the next run. The + magnetic moments of the reference, if any, are added as a site property. + + Parameters + ---------- + md_dir: str + Directory of the MD run. + md_code: str + Code of the MD, "vasp" or "forcefields". + reference: Structure + The undisplaced supercell the MD started from. + + Returns + ------- + Structure + The final structure, with a "velocities" site property. + """ + directory = Path(strip_hostname(md_dir)) + if md_code == "vasp": + structure = Poscar.from_file(zpath(str(directory / "CONTCAR"))).structure + else: + atoms = ase_read(directory / ASE_TRAJECTORY_FILE, index=-1) + structure = Structure( + atoms.cell[:], + atoms.get_chemical_symbols(), + atoms.get_positions(), + coords_are_cartesian=True, + site_properties={"velocities": atoms.get_velocities().tolist()}, + ) + for key, values in _get_site_properties(reference).items(): + structure.add_site_property(key, values) + return structure diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index d36ca047a3..1b059187b5 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -12,7 +12,7 @@ from atomate2.common.flows.finite_temperature_phonons import ( BaseFiniteTemperaturePhononMaker, ) -from atomate2.common.jobs.finite_temperature_phonons import ASE_TRAJECTORY_FILE +from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker from atomate2.forcefields.md import ForceFieldMDMaker from atomate2.vasp.flows.finite_temperature_phonons import FiniteTemperaturePhononMaker diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index d241f28ee3..699f02ab62 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -19,17 +19,16 @@ from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure from atomate2.common.jobs.finite_temperature_phonons import ( - ASE_TRAJECTORY_FILE, _assess_trajectory, _get_rms_displacement, _remove_center_of_mass, average_npt_structure, fit_finite_temperature_phonons, - get_md_restart_structure, get_md_supercell, get_npt_structure, select_md_snapshots, ) +from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE TEMPERATURE = 300.0 # a long time step, so that the second half of the synthetic trajectories of 400 @@ -350,44 +349,6 @@ def test_get_md_supercell(): assert supercell.site_properties == {} -def test_get_md_restart_structure(cu_supercell): - rng = np.random.default_rng(4) - velocities = rng.normal(0, 0.01, size=(len(cu_supercell), 3)) - reference = cu_supercell.copy(site_properties={"magmom": [1.0] * 32}) - - # a CONTCAR of a VASP MD, with the predictor-corrector block after the - # velocities - md_dir = TEST_DIR / "vasp/Si_multi_md/molecular_dynamics_1/outputs" - si_reference = Structure( - np.eye(3) * 3.87, ["Si", "Si"], [[0, 0, 0], [0.25, 0.25, 0.25]] - ) - restart = get_md_restart_structure.original(str(md_dir), "vasp", si_reference) - assert restart.site_properties["velocities"][0] == pytest.approx( - [0.40252568e-03, -0.31480439e-02, -0.16045943e-02] - ) - assert "magmom" not in restart.site_properties - - Path("vasp").mkdir() - structure = cu_supercell.copy(site_properties={"velocities": velocities}) - structure.to(filename="vasp/CONTCAR", fmt="poscar") - restart = get_md_restart_structure.original( - str(Path("vasp").resolve()), "vasp", reference - ) - assert np.allclose(restart.site_properties["velocities"], velocities, atol=1e-8) - assert restart.site_properties["magmom"] == [1.0] * 32 - - Path("ase").mkdir() - atoms = AseAtomsAdaptor.get_atoms(cu_supercell) - atoms.set_velocities(velocities) - ase_write(Path("ase") / ASE_TRAJECTORY_FILE, [atoms.copy(), atoms]) - restart = get_md_restart_structure.original( - str(Path("ase").resolve()), "forcefields", reference - ) - assert np.allclose(restart.site_properties["velocities"], velocities) - assert np.allclose(restart.cart_coords, cu_supercell.cart_coords) - assert restart.site_properties["magmom"] == [1.0] * 32 - - def test_get_rms_displacement(): """An Einstein crystal has = 3 k_B T / k per atom.""" structure = AseAtomsAdaptor.get_structure(bulk("Cu", "fcc", a=3.61, cubic=True)) diff --git a/tests/common/jobs/test_md.py b/tests/common/jobs/test_md.py new file mode 100644 index 0000000000..06fdfd3f1d --- /dev/null +++ b/tests/common/jobs/test_md.py @@ -0,0 +1,55 @@ +"""Tests of the shared MD jobs.""" + +from pathlib import Path + +import numpy as np +import pytest +from ase.build import bulk +from ase.io import write as ase_write +from pymatgen.core import Structure +from pymatgen.io.ase import AseAtomsAdaptor + +from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE, get_md_restart_structure + +TEST_DIR = Path(__file__).resolve().parents[2] / "test_data" + + +def test_get_md_restart_structure(): + cu_supercell = AseAtomsAdaptor.get_structure( + bulk("Cu", "fcc", a=3.61, cubic=True) * (2, 2, 2) + ) + rng = np.random.default_rng(4) + velocities = rng.normal(0, 0.01, size=(len(cu_supercell), 3)) + reference = cu_supercell.copy(site_properties={"magmom": [1.0] * 32}) + + # a CONTCAR of a VASP MD, with the predictor-corrector block after the + # velocities + md_dir = TEST_DIR / "vasp/Si_multi_md/molecular_dynamics_1/outputs" + si_reference = Structure( + np.eye(3) * 3.87, ["Si", "Si"], [[0, 0, 0], [0.25, 0.25, 0.25]] + ) + restart = get_md_restart_structure.original(str(md_dir), "vasp", si_reference) + assert restart.site_properties["velocities"][0] == pytest.approx( + [0.40252568e-03, -0.31480439e-02, -0.16045943e-02] + ) + assert "magmom" not in restart.site_properties + + Path("vasp").mkdir() + structure = cu_supercell.copy(site_properties={"velocities": velocities}) + structure.to(filename="vasp/CONTCAR", fmt="poscar") + restart = get_md_restart_structure.original( + str(Path("vasp").resolve()), "vasp", reference + ) + assert np.allclose(restart.site_properties["velocities"], velocities, atol=1e-8) + assert restart.site_properties["magmom"] == [1.0] * 32 + + Path("ase").mkdir() + atoms = AseAtomsAdaptor.get_atoms(cu_supercell) + atoms.set_velocities(velocities) + ase_write(Path("ase") / ASE_TRAJECTORY_FILE, [atoms.copy(), atoms]) + restart = get_md_restart_structure.original( + str(Path("ase").resolve()), "forcefields", reference + ) + assert np.allclose(restart.site_properties["velocities"], velocities) + assert np.allclose(restart.cart_coords, cu_supercell.cart_coords) + assert restart.site_properties["magmom"] == [1.0] * 32 From f01795a6db77f8c7bdc933aadc3a0c9a9bae5374 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Mon, 5 Oct 2026 20:50:22 -0700 Subject: [PATCH 34/43] Get the MD code of ChainedMDMaker from its makers --- .../flows/finite_temperature_phonons.py | 1 - src/atomate2/common/flows/md.py | 19 +++++++++++---- .../common/jobs/finite_temperature_phonons.py | 4 +++- src/atomate2/common/jobs/md.py | 20 ++++++++-------- .../flows/finite_temperature_phonons.py | 2 +- .../jobs/test_finite_temperature_phonons.py | 2 +- tests/common/jobs/test_md.py | 23 ++++++++++++------- .../flows/test_finite_temperature_phonons.py | 4 +++- 8 files changed, 46 insertions(+), 29 deletions(-) diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index 808eebe431..a5f0377453 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -395,7 +395,6 @@ def make( md_flow = ChainedMDMaker( md_makers=[self.get_md_maker(n_steps) for n_steps in self.get_md_steps()], - md_code=self.md_code, ).make(reference, prev_dir=prev_dir) jobs.append(md_flow) md_dirs = md_flow.output["dir_names"] diff --git a/src/atomate2/common/flows/md.py b/src/atomate2/common/flows/md.py index 4cbb651682..1739cdebb4 100644 --- a/src/atomate2/common/flows/md.py +++ b/src/atomate2/common/flows/md.py @@ -7,6 +7,7 @@ from jobflow import Flow, Maker +from atomate2.ase.md import AseMDMaker from atomate2.common.jobs.md import get_md_restart_structure if TYPE_CHECKING: @@ -30,14 +31,14 @@ class ChainedMDMaker(Maker): name: str Name of the flows produced by this maker. md_makers: list[Maker] - Makers of the MD jobs, in the order of the trajectory. - md_code: str - Code of the MD, 'vasp' or 'forcefields'. + Makers of the MD jobs, in the order of the trajectory. VASP makers and + ASE makers, such as the force field ones, are supported. An ASE maker + that is followed by another job must write its trajectory in the ASE + format, with traj_file set. """ name: str = "chained MD" md_makers: list[Maker] = field(default_factory=list) - md_code: str = "vasp" def make(self, structure: Structure, prev_dir: str | Path | None = None) -> Flow: """ @@ -67,8 +68,16 @@ def make(self, structure: Structure, prev_dir: str | Path | None = None) -> Flow jobs.append(md_job) md_jobs.append(md_job) if idx < len(self.md_makers): + traj_file = None + if isinstance(maker, AseMDMaker): + if maker.traj_file is None or maker.traj_file_fmt != "ase": + raise ValueError( + f"{maker.name} must write its trajectory in the ASE " + "format, so that the next MD job can continue from it." + ) + traj_file = str(maker.traj_file) restart = get_md_restart_structure( - md_job.output.dir_name, self.md_code, structure + md_job.output.dir_name, structure, traj_file ) jobs.append(restart) md_structure = restart.output diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index ee544f48b2..e63d91190e 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -23,7 +23,7 @@ from pymatgen.phonon.dos import PhononDos from pymatgen.symmetry.analyzer import SpacegroupAnalyzer -from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE, _get_site_properties +from atomate2.common.jobs.md import _get_site_properties from atomate2.common.jobs.pheasy import ( _DEFAULT_FILE_PATHS, _check_lasso_alpha, @@ -55,6 +55,8 @@ logger = logging.getLogger(__name__) +# file of the force field MD trajectory, written in the ASE format +ASE_TRAJECTORY_FILE = "md_trajectory.traj" _KPATH_SCHEME = "seekpath" # Limits of the trajectory check diff --git a/src/atomate2/common/jobs/md.py b/src/atomate2/common/jobs/md.py index e1cca05131..dd8a520393 100644 --- a/src/atomate2/common/jobs/md.py +++ b/src/atomate2/common/jobs/md.py @@ -12,9 +12,6 @@ from atomate2.utils.path import strip_hostname -# file of the force field MD trajectory, written in the ASE format -ASE_TRAJECTORY_FILE = "md_trajectory.traj" - def _get_site_properties(reference: Structure) -> dict: """Get the magnetic moments of the reference, the only site property kept.""" @@ -25,14 +22,14 @@ def _get_site_properties(reference: Structure) -> dict: @job def get_md_restart_structure( - md_dir: str, md_code: str, reference: Structure + md_dir: str, reference: Structure, traj_file: str | None = None ) -> Structure: """ Get the final positions and velocities of an MD run. For VASP, they are read from CONTCAR, with the velocities in Angstrom/fs. - For force fields, they are read from the last frame of the ASE trajectory - file, with the velocities in ASE units. In both cases, the velocities are a + For an ASE MD, they are read from the last frame of its trajectory file, + with the velocities in ASE units. In both cases, the velocities are a site property that the next MD run starts from. The thermostat variables are not carried over, so they start again from zero in the next run. The magnetic moments of the reference, if any, are added as a site property. @@ -41,10 +38,11 @@ def get_md_restart_structure( ---------- md_dir: str Directory of the MD run. - md_code: str - Code of the MD, "vasp" or "forcefields". reference: Structure - The undisplaced supercell the MD started from. + The structure the MD started from. + traj_file: str | None + Name of the ASE trajectory file of an ASE MD, written in the ASE format. + None for a VASP MD. Returns ------- @@ -52,10 +50,10 @@ def get_md_restart_structure( The final structure, with a "velocities" site property. """ directory = Path(strip_hostname(md_dir)) - if md_code == "vasp": + if traj_file is None: structure = Poscar.from_file(zpath(str(directory / "CONTCAR"))).structure else: - atoms = ase_read(directory / ASE_TRAJECTORY_FILE, index=-1) + atoms = ase_read(directory / traj_file, index=-1) structure = Structure( atoms.cell[:], atoms.get_chemical_symbols(), diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index 1b059187b5..d36ca047a3 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -12,7 +12,7 @@ from atomate2.common.flows.finite_temperature_phonons import ( BaseFiniteTemperaturePhononMaker, ) -from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE +from atomate2.common.jobs.finite_temperature_phonons import ASE_TRAJECTORY_FILE from atomate2.forcefields.jobs import ForceFieldRelaxMaker, ForceFieldStaticMaker from atomate2.forcefields.md import ForceFieldMDMaker from atomate2.vasp.flows.finite_temperature_phonons import FiniteTemperaturePhononMaker diff --git a/tests/common/jobs/test_finite_temperature_phonons.py b/tests/common/jobs/test_finite_temperature_phonons.py index 699f02ab62..0991b229d8 100644 --- a/tests/common/jobs/test_finite_temperature_phonons.py +++ b/tests/common/jobs/test_finite_temperature_phonons.py @@ -19,6 +19,7 @@ from pymatgen.io.phonopy import get_phonopy_structure, get_pmg_structure from atomate2.common.jobs.finite_temperature_phonons import ( + ASE_TRAJECTORY_FILE, _assess_trajectory, _get_rms_displacement, _remove_center_of_mass, @@ -28,7 +29,6 @@ get_npt_structure, select_md_snapshots, ) -from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE TEMPERATURE = 300.0 # a long time step, so that the second half of the synthetic trajectories of 400 diff --git a/tests/common/jobs/test_md.py b/tests/common/jobs/test_md.py index 06fdfd3f1d..34629d3987 100644 --- a/tests/common/jobs/test_md.py +++ b/tests/common/jobs/test_md.py @@ -1,4 +1,4 @@ -"""Tests of the shared MD jobs.""" +"""Tests of the shared MD jobs and flows.""" from pathlib import Path @@ -9,7 +9,9 @@ from pymatgen.core import Structure from pymatgen.io.ase import AseAtomsAdaptor -from atomate2.common.jobs.md import ASE_TRAJECTORY_FILE, get_md_restart_structure +from atomate2.common.flows.md import ChainedMDMaker +from atomate2.common.jobs.md import get_md_restart_structure +from atomate2.forcefields.md import ForceFieldMDMaker TEST_DIR = Path(__file__).resolve().parents[2] / "test_data" @@ -28,7 +30,7 @@ def test_get_md_restart_structure(): si_reference = Structure( np.eye(3) * 3.87, ["Si", "Si"], [[0, 0, 0], [0.25, 0.25, 0.25]] ) - restart = get_md_restart_structure.original(str(md_dir), "vasp", si_reference) + restart = get_md_restart_structure.original(str(md_dir), si_reference) assert restart.site_properties["velocities"][0] == pytest.approx( [0.40252568e-03, -0.31480439e-02, -0.16045943e-02] ) @@ -37,19 +39,24 @@ def test_get_md_restart_structure(): Path("vasp").mkdir() structure = cu_supercell.copy(site_properties={"velocities": velocities}) structure.to(filename="vasp/CONTCAR", fmt="poscar") - restart = get_md_restart_structure.original( - str(Path("vasp").resolve()), "vasp", reference - ) + restart = get_md_restart_structure.original(str(Path("vasp").resolve()), reference) assert np.allclose(restart.site_properties["velocities"], velocities, atol=1e-8) assert restart.site_properties["magmom"] == [1.0] * 32 Path("ase").mkdir() atoms = AseAtomsAdaptor.get_atoms(cu_supercell) atoms.set_velocities(velocities) - ase_write(Path("ase") / ASE_TRAJECTORY_FILE, [atoms.copy(), atoms]) + ase_write(Path("ase") / "md.traj", [atoms.copy(), atoms]) restart = get_md_restart_structure.original( - str(Path("ase").resolve()), "forcefields", reference + str(Path("ase").resolve()), reference, "md.traj" ) assert np.allclose(restart.site_properties["velocities"], velocities) assert np.allclose(restart.cart_coords, cu_supercell.cart_coords) assert restart.site_properties["magmom"] == [1.0] * 32 + + +def test_chained_md_maker_needs_ase_trajectory(): + structure = Structure(np.eye(3) * 3.61, ["Cu"], [[0, 0, 0]]) + maker = ChainedMDMaker(md_makers=[ForceFieldMDMaker(), ForceFieldMDMaker()]) + with pytest.raises(ValueError, match="trajectory in the ASE format"): + maker.make(structure) diff --git a/tests/vasp/flows/test_finite_temperature_phonons.py b/tests/vasp/flows/test_finite_temperature_phonons.py index 4e6ac43c0e..87dcd5f959 100644 --- a/tests/vasp/flows/test_finite_temperature_phonons.py +++ b/tests/vasp/flows/test_finite_temperature_phonons.py @@ -2,6 +2,7 @@ from jobflow import Flow, OutputReference from pymatgen.core import Lattice, Structure +from atomate2.common.jobs.finite_temperature_phonons import ASE_TRAJECTORY_FILE from atomate2.forcefields.flows.finite_temperature_phonons import ( MLFFMDVaspStaticFiniteTemperaturePhononMaker, VaspMDMLFFStaticFiniteTemperaturePhononMaker, @@ -69,7 +70,8 @@ def test_vasp_flows(si_structure, maker_cls, md_code, code): # end of the first, and both get the relaxation directory assert md_1.function_args[0].uuid == reference.uuid assert md_2.function_args[0].uuid == restart.uuid - assert restart.function_args == (md_1.output.dir_name, md_code, reference.output) + traj_file = ASE_TRAJECTORY_FILE if md_code == "forcefields" else None + assert restart.function_args == (md_1.output.dir_name, reference.output, traj_file) for md_job in (md_1, md_2): assert md_job.function_kwargs["prev_dir"].uuid == relax.output.uuid assert maker.get_md_steps() == [4000, 4000] From dd198efa14781b6f99ec9e6abb9aeef73e8f8a25 Mon Sep 17 00:00:00 2001 From: Jiongzhi ZHENG Date: Tue, 6 Oct 2026 14:36:26 +0800 Subject: [PATCH 35/43] Update pheasy.py --- src/atomate2/common/jobs/pheasy.py | 5 ++++- 1 file changed, 4 insertions(+), 1 deletion(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index b6984f372b..8f522be503 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -360,7 +360,10 @@ def _run_anharmonic_fit( supercell_matrix: np.ndarray, symprec: float, anhar_max_order: int, - fcs_cutoff_radius: Sequence[float], + # set a defaut value for the cutoff radius of each order, I recommend the default values for third- and fourth order + # are 6.3 and 5.3 angstroms, respectively. Those values are large enough for accurate third- and fourth-order force constant fits. + # and they are more efficient than using larger cutoff radii. + fcs_cutoff_radius: Sequence[float], num_anhar: int, anhar_alpha_min: int, work_dir: Path, From 031a83a98845e2d58b1c22e24630f6cefff25a4d Mon Sep 17 00:00:00 2001 From: Jiongzhi ZHENG Date: Tue, 6 Oct 2026 14:44:47 +0800 Subject: [PATCH 36/43] Update pheasy.py --- src/atomate2/common/jobs/pheasy.py | 8 +++++++- 1 file changed, 7 insertions(+), 1 deletion(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 8f522be503..2be19befec 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -380,7 +380,9 @@ def _run_anharmonic_fit( pheasy writes FORCE_CONSTANTS_3RD and fc3.hdf5 to work_dir, and FORCE_CONSTANTS_4TH and fc4.hdf5 for fourth order. The one-shot fit also - writes its second-order force constants, fc2.hdf5. + writes its second-order force constants, fc2.hdf5. In order to make the FCs can + be read correctly by SHENGBTE and FourPhonon, we force pheasy to write FCs in the + text format. Parameters ---------- @@ -406,6 +408,10 @@ def _run_anharmonic_fit( it, the cross-validated penalty and the fitted force constants change from run to run on the same forces. """ + + # use the default cutoff radii if not provided by the users. In order to make the FCs fitting + # more effcient and accurate, oterwise, the users can not do the high-throughput calculations efficiently. + dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) base = ( f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR --dim {dim} -w {anhar_max_order} " From 35069da11841f3232beb41d8929f16bc3bd8792e Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 00:03:30 -0700 Subject: [PATCH 37/43] Revert the comments added to pheasy.py --- src/atomate2/common/jobs/pheasy.py | 13 ++----------- 1 file changed, 2 insertions(+), 11 deletions(-) diff --git a/src/atomate2/common/jobs/pheasy.py b/src/atomate2/common/jobs/pheasy.py index 2be19befec..b6984f372b 100644 --- a/src/atomate2/common/jobs/pheasy.py +++ b/src/atomate2/common/jobs/pheasy.py @@ -360,10 +360,7 @@ def _run_anharmonic_fit( supercell_matrix: np.ndarray, symprec: float, anhar_max_order: int, - # set a defaut value for the cutoff radius of each order, I recommend the default values for third- and fourth order - # are 6.3 and 5.3 angstroms, respectively. Those values are large enough for accurate third- and fourth-order force constant fits. - # and they are more efficient than using larger cutoff radii. - fcs_cutoff_radius: Sequence[float], + fcs_cutoff_radius: Sequence[float], num_anhar: int, anhar_alpha_min: int, work_dir: Path, @@ -380,9 +377,7 @@ def _run_anharmonic_fit( pheasy writes FORCE_CONSTANTS_3RD and fc3.hdf5 to work_dir, and FORCE_CONSTANTS_4TH and fc4.hdf5 for fourth order. The one-shot fit also - writes its second-order force constants, fc2.hdf5. In order to make the FCs can - be read correctly by SHENGBTE and FourPhonon, we force pheasy to write FCs in the - text format. + writes its second-order force constants, fc2.hdf5. Parameters ---------- @@ -408,10 +403,6 @@ def _run_anharmonic_fit( it, the cross-validated penalty and the fitted force constants change from run to run on the same forces. """ - - # use the default cutoff radii if not provided by the users. In order to make the FCs fitting - # more effcient and accurate, oterwise, the users can not do the high-throughput calculations efficiently. - dim = " ".join(str(int(supercell_matrix[i][i])) for i in range(3)) base = ( f"{SETTINGS.PHEASY_CMD} --scell SPOSCAR --dim {dim} -w {anhar_max_order} " From 7b4fab489182ad2ef8e546c04045192c3b3d10d1 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 00:06:56 -0700 Subject: [PATCH 38/43] Give the default pheasy cutoffs in Angstrom --- src/atomate2/common/flows/pheasy.py | 7 ++++--- src/atomate2/vasp/flows/pheasy.py | 7 ++++--- 2 files changed, 8 insertions(+), 6 deletions(-) diff --git a/src/atomate2/common/flows/pheasy.py b/src/atomate2/common/flows/pheasy.py index 910b606866..5e3b215254 100644 --- a/src/atomate2/common/flows/pheasy.py +++ b/src/atomate2/common/flows/pheasy.py @@ -142,9 +142,10 @@ class BasePhononMaker(PurePhonopyMaker, ABC): cutoff distance in Bohr for each FC order, starting at second order. The default value is [-1, 12, 10]. The first entry is not used, since pheasy fits the second-order FCs without a cutoff. The second and third entries - are the cutoffs for third- and fourth-order FCs. The cutoff of each fitted - order, up to anhar_max_order, must be positive. Longer cutoffs increase - the number of free FCs, and with it the number of displaced supercells. + are the cutoffs for third- and fourth-order FCs. The defaults of 12 and 10 + Bohr are 6.35 and 5.29 Å. The cutoff of each fitted order, up to + anhar_max_order, must be positive. Longer cutoffs increase the number of + free FCs, and with it the number of displaced supercells. min_length: float minimum length of lattice constants will be used to create the supercell, the default value is 8.0 A. It can be increased for larger supercells. diff --git a/src/atomate2/vasp/flows/pheasy.py b/src/atomate2/vasp/flows/pheasy.py index d934c538dd..1b7bd79a5b 100644 --- a/src/atomate2/vasp/flows/pheasy.py +++ b/src/atomate2/vasp/flows/pheasy.py @@ -105,9 +105,10 @@ class PhononMaker(BasePhononMaker): cutoff distance in Bohr for each FC order, starting at second order. The default value is [-1, 12, 10]. The first entry is not used, since pheasy fits the second-order FCs without a cutoff. The second and third entries - are the cutoffs for third- and fourth-order FCs. The cutoff of each fitted - order, up to anhar_max_order, must be positive. Longer cutoffs increase - the number of free FCs, and with it the number of displaced supercells. + are the cutoffs for third- and fourth-order FCs. The defaults of 12 and 10 + Bohr are 6.35 and 5.29 Å. The cutoff of each fitted order, up to + anhar_max_order, must be positive. Longer cutoffs increase the number of + free FCs, and with it the number of displaced supercells. min_length: float minimum length of lattice constants will be used to create the supercell, the default value is 8.0 A. It can be increased for larger supercells. From 3609f81fb8096ba8bb952b3ef69408618383d077 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 15:57:08 -0700 Subject: [PATCH 39/43] Seed the Langevin forces, reuse PhononBSDOSDoc and fix the docs --- docs/user/codes/vasp.md | 26 ++++-- src/atomate2/ase/md.py | 17 ++-- .../flows/finite_temperature_phonons.py | 52 +++++------ .../common/jobs/finite_temperature_phonons.py | 15 +++- .../schemas/finite_temperature_phonons.py | 79 ++++------------- .../flows/finite_temperature_phonons.py | 86 +++++++++++++------ .../vasp/flows/finite_temperature_phonons.py | 9 +- tests/ase/test_md.py | 18 ++++ .../flows/test_finite_temperature_phonons.py | 22 +---- tutorials/finite_temperature_phonons.ipynb | 63 +++++++------- 10 files changed, 204 insertions(+), 183 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index ceb2c75b6c..a01a78c9da 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -416,7 +416,8 @@ The cluster space grows faster there than the number of displacements the workfl #### Finite-temperature phonons `FiniteTemperaturePhononMaker` fits effective harmonic force constants at a finite temperature, as in the temperature-dependent effective potential ([TDEP](https://doi.org/10.1103/PhysRevB.84.180301)) method. -They include the anharmonic effects at that temperature. +They include the effect of the anharmonic forces on the frequencies at that temperature. +They give no phonon lifetimes. By default, the MD runs at the volume of the relaxed structure, so thermal expansion is not included. It can be switched on with an NPT MD before the NVT MD, see below. The structure is relaxed first. @@ -428,6 +429,7 @@ The displacements are measured from the undisplaced supercell. Pheasy then fits the second-order force constants to them with LASSO. As in the pheasy phonon workflow, a `DielectricMaker` computes the Born charges and the dielectric tensor for the non-analytical correction. It needs the `pheasy` extra, like the pheasy phonon workflow above. +The notebook `tutorials/finite_temperature_phonons.ipynb` runs it for six materials with three MACE potentials. ```{warning} This workflow is new and has not been tested widely. @@ -443,10 +445,11 @@ flow = FiniteTemperaturePhononMaker(temperature=300).make(structure) ``` The fit only uses the positions of the MD, not its dynamics. -What matters is that the MD samples the canonical ensemble. +The MD has to sample the canonical ensemble. A Langevin thermostat does this for every mode ([Bussi and Parrinello](https://doi.org/10.1103/PhysRevE.75.056707)). -A Nosé-Hoover thermostat can leave nearly harmonic modes out of equilibrium ([Legoll et al.](https://doi.org/10.1007/s00205-006-0029-1)), most of all at low temperature. -`thermostat="nose-hoover"` switches to it, but this is not recommended. +For a harmonic oscillator weakly coupled to a Nosé-Hoover thermostat, the dynamics is not ergodic ([Legoll et al.](https://doi.org/10.1007/s00205-006-0029-1)). +`thermostat="nose-hoover"` switches the NVT MD to a Nosé-Hoover thermostat with one thermostat variable. +In the KNaICl test of the notebook, 12 of 27 runs with it had imaginary modes, against 19 of 27 with Langevin. The MD uses looser settings than the statics, for example ENCUT = 500 eV instead of 600 eV. Only the forces of the statics enter the fit. @@ -470,9 +473,11 @@ The trajectory is also checked before the fit. The check looks for melting and for a move away from the reference structure. It also looks at the drift of the potential energy late in the run. The result is stored in `trajectory_health` of the output `FiniteTemperaturePhononDoc`, and a warning is raised when the check fails. -The limits of the check are rules of thumb, except for the Lindemann ratio of 0.15 at melting ([Saija et al.](https://doi.org/10.1063/1.2208357)). -Imaginary modes are counted at the q-points commensurate with the supercell. -They are reported and not removed. +The Lindemann ratio of 0.15 at melting is that of an fcc solid ([Saija et al.](https://doi.org/10.1063/1.2208357)). +The other limits of the check are rules of thumb. +`has_imaginary_modes` checks the band path. +`n_imaginary_modes` and `lowest_frequency` use the q-points commensurate with the supercell. +Imaginary modes are reported and not removed. The MD and the statics can also come from different codes. Three more makers are in `atomate2.forcefields.flows.finite_temperature_phonons`. @@ -482,7 +487,7 @@ Three more makers are in `atomate2.forcefields.flows.finite_temperature_phonons` Each has a `from_force_field_name` method to choose the force field. They need the package of the force field, for example `mace-torch` for MACE. All of them use the same fit. -A force field NPT MD uses ASE's `MTKNPT`, a Nosé-Hoover thermostat with the barostat of [Martyna et al.](https://doi.org/10.1063/1.467468). +A force field NPT MD uses ASE's `MTKNPT`, a Nosé-Hoover thermostat with one thermostat variable and the barostat of [Martyna et al.](https://doi.org/10.1063/1.467468). ```python from atomate2.forcefields.flows.finite_temperature_phonons import ( @@ -497,7 +502,9 @@ flow = maker.make(structure) `run_npt=True` sets the NPT MD and the relaxation of the atoms in its cell. -Most force fields give no Born charges, so the force field makers skip the non-analytical correction by default. +Most force fields give no Born charges. +`ForceFieldFiniteTemperaturePhononMaker` and `VaspMDMLFFStaticFiniteTemperaturePhononMaker` therefore skip the non-analytical correction by default. +`MLFFMDVaspStaticFiniteTemperaturePhononMaker` keeps the VASP `DielectricMaker`. The Born charges and the dielectric tensor can come from MACE-Field, see the [force field notes](forcefields.md#mace-field-notes), or from VASP. Either pass `born` and `epsilon_static` to `make`, or set a `born_maker`: @@ -518,6 +525,7 @@ Known limitations: - pheasy needs a diagonal supercell matrix. - The MD is classical, so there is no zero-point motion. - Each result comes from one MD trajectory, so it carries the noise of that trajectory. +- The Lindemann ratio is averaged over all atoms. It can pass 0.15 when only the light atoms move far, for example Li in a superionic conductor, while the rest of the crystal stays solid. - With a force field MD and VASP statics, the trajectory and the forces come from different potential energy surfaces. ### Grüneisen parameter workflow diff --git a/src/atomate2/ase/md.py b/src/atomate2/ase/md.py index d7a574b9cf..14ea89d751 100644 --- a/src/atomate2/ase/md.py +++ b/src/atomate2/ase/md.py @@ -3,6 +3,7 @@ from __future__ import annotations import contextlib +import inspect import io import logging import os @@ -156,7 +157,8 @@ class AseMDMaker(AseMaker, ABC): The step interval for saving the trajectories. mb_velocity_seed : int or None If an int, a random number seed for generating initial velocities - from a Maxwell-Boltzmann distribution. + from a Maxwell-Boltzmann distribution. It also seeds the random forces + of dynamics that take an rng argument, such as Langevin. zero_linear_momentum : bool = False Whether to initialize the atomic velocities with zero linear momentum zero_angular_momentum : bool = False @@ -381,13 +383,12 @@ def run_ase( # ASE NPT implementation requires upper triangular cell atoms.set_cell(atoms.cell.standard_form(form="upper")[0]) + rng = np.random.default_rng(seed=self.mb_velocity_seed) if initial_velocities: atoms.set_velocities(initial_velocities) elif not np.isnan(self.t_schedule).any(): MaxwellBoltzmannDistribution( - atoms=atoms, - temperature_K=self.t_schedule[0], - rng=np.random.default_rng(seed=self.mb_velocity_seed), + atoms=atoms, temperature_K=self.t_schedule[0], rng=rng ) if self.zero_linear_momentum: Stationary(atoms) @@ -398,8 +399,14 @@ def run_ase( md_observer = TrajectoryObserver(atoms, store_md_outputs=True) + md_kwargs = dict(self.ase_md_kwargs) + if ( + self.mb_velocity_seed is not None + and "rng" in inspect.signature(dynamics).parameters + ): + md_kwargs.setdefault("rng", rng) md_runner = dynamics( - atoms=atoms, timestep=self.time_step * units.fs, **self.ase_md_kwargs + atoms=atoms, timestep=self.time_step * units.fs, **md_kwargs ) md_runner.attach(md_observer, interval=self.traj_interval) diff --git a/src/atomate2/common/flows/finite_temperature_phonons.py b/src/atomate2/common/flows/finite_temperature_phonons.py index a5f0377453..f03a6442a1 100644 --- a/src/atomate2/common/flows/finite_temperature_phonons.py +++ b/src/atomate2/common/flows/finite_temperature_phonons.py @@ -74,12 +74,14 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): rest of the trajectory. The phonon displacement maker computes the forces on these snapshots and on the undisplaced supercell. The displacements of the snapshots are measured from the relaxed positions. pheasy fits one set of - second-order force constants to the displacements and forces with LASSO, as - in the temperature-dependent effective potential method. These force - constants contain the anharmonic effects at the temperature and at the - volume of the relaxed structure. Thermal expansion is not included. They - give the phonon band structure and density of states. Imaginary modes are - reported, not removed. + second-order force constants to the displacements and forces with LASSO. + Fitting effective harmonic force constants to MD is the idea of the + temperature-dependent effective potential method. The force constants + include the effect of the anharmonic forces on the frequencies, at the + temperature and at the volume of the relaxed structure. They give no + phonon lifetimes. The MD is classical. Thermal expansion is not included. + The force constants give the phonon band structure and density of states. + Imaginary modes are reported, not removed. If npt_maker is set, thermal expansion is included. An NPT MD run at the temperature and pressure first starts from the undisplaced supercell of the @@ -128,9 +130,10 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): thermostat: Literal["nose-hoover", "langevin"] Thermostat of the NVT MD. Langevin, the default, samples the canonical ensemble also for nearly harmonic modes (Bussi and Parrinello, Phys. Rev. - E 75, 056707 (2007)). A Nose-Hoover thermostat may leave such modes out - of equilibrium (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 - (2007)). The NPT MD does not use this setting. + E 75, 056707 (2007)). For a harmonic oscillator weakly coupled to a + Nose-Hoover thermostat, the dynamics is not ergodic (Legoll et al., + Arch. Ration. Mech. Anal. 184, 449 (2007)). The NPT MD does not use + this setting. md_runs: int Number of consecutive MD jobs that make up the trajectory. Each job continues from the positions and velocities of the previous one. The @@ -155,8 +158,9 @@ class BaseFiniteTemperaturePhononMaker(Maker, ABC): default. A warning is raised if the chosen penalty is on either bound of the search. random_seed: int | None - Seed of the LASSO fit, and of the initial velocities of a force field - MD. + Seed of the LASSO fit. It also seeds the initial velocities and the + Langevin random forces of a force field MD. MD job i, counted from 0, + uses random_seed + i and the NPT MD uses random_seed + md_runs. tol_imaginary_modes: float Frequencies below -tol_imaginary_modes in THz are imaginary. store_force_constants: bool @@ -227,10 +231,6 @@ def __post_init__(self) -> None: f"{key} must be one of {sorted(SUPPORTED_CODES)}, not " f"{getattr(self, key)!r}." ) - if self.socket and self.code == "vasp": - raise ValueError("socket is not supported by VASP.") - if min(self.md_runs, self.n_snapshots) < 1: - raise ValueError("md_runs and n_snapshots must be at least 1.") if self.alpha_min >= -2: raise ValueError(f"alpha_min must be below -2, not {self.alpha_min}.") if min(self.temperature, self.md_time, self.md_time_step) <= 0: @@ -242,10 +242,6 @@ def __post_init__(self) -> None: f"The MD has {n_steps} steps. After leaving out equilibration_time, " f"fewer than the {self.n_snapshots} snapshots are left." ) - if self.md_runs > n_steps: - raise ValueError( - f"md_runs ({self.md_runs}) is larger than the {n_steps} MD steps." - ) if self.npt_maker is not None and not ( 0 <= self.npt_equilibration_time < self.npt_time ): @@ -253,8 +249,6 @@ def __post_init__(self) -> None: "npt_equilibration_time must be at least zero and shorter than " "npt_time." ) - if self.fixed_cell_relax_maker is not None and self.npt_maker is None: - raise ValueError("fixed_cell_relax_maker is only used with npt_maker.") def get_md_steps(self) -> list[int]: """Get the number of MD steps of each MD job.""" @@ -302,8 +296,9 @@ def make( if not np.allclose(matrix, np.diag(np.diag(matrix))): raise ValueError("pheasy needs a diagonal supercell matrix.") - # VASP sorts the atoms by electronegativity. Sorting here as well keeps - # the Born charges of a force field born_maker in the order of the fit. + # The VASP input sets sort the atoms by electronegativity. Sorting here as + # well keeps the Born charges of a force field born_maker in the order of + # the fit. if not isinstance(structure, OutputReference): structure = structure.get_sorted_structure() @@ -327,7 +322,7 @@ def make( structure, self.min_length, None, - force_90_degrees=True, + force_90_degrees=False, force_diagonal=True, ) jobs.append(supercell_job) @@ -394,7 +389,10 @@ def make( reference = reference_job.output md_flow = ChainedMDMaker( - md_makers=[self.get_md_maker(n_steps) for n_steps in self.get_md_steps()], + md_makers=[ + self.get_md_maker(n_steps, idx) + for idx, n_steps in enumerate(self.get_md_steps()) + ], ).make(reference, prev_dir=prev_dir) jobs.append(md_flow) md_dirs = md_flow.output["dir_names"] @@ -485,7 +483,7 @@ def get_npt_maker(self, n_steps: int) -> Maker: """ @abstractmethod - def get_md_maker(self, n_steps: int) -> Maker: + def get_md_maker(self, n_steps: int, index: int = 0) -> Maker: """ Get the maker of one MD job, with the settings of this flow. @@ -493,6 +491,8 @@ def get_md_maker(self, n_steps: int) -> Maker: ---------- n_steps: int Number of MD steps of the job. + index: int + Position of the job in the MD, counted from 0. Returns ------- diff --git a/src/atomate2/common/jobs/finite_temperature_phonons.py b/src/atomate2/common/jobs/finite_temperature_phonons.py index e63d91190e..ad5483c948 100644 --- a/src/atomate2/common/jobs/finite_temperature_phonons.py +++ b/src/atomate2/common/jobs/finite_temperature_phonons.py @@ -41,6 +41,7 @@ ) from atomate2.common.schemas.phonons import ( ForceConstants, + PhononComputationalSettings, PhononJobDirs, PhononUUIDs, _set_nac_params, @@ -73,8 +74,7 @@ # Rule of thumb: the mean positions are only checked if the second half of the # trajectory lasts at least one period of a 1 THz vibration. _MIN_SHIFT_WINDOW = 1.0 # ps -# Three sigma rule: without a drift, a change this large has a probability below -# 5% for any unimodal distribution. Pukelsheim, Am. Stat. 48, 88 (1994) +# Rule of thumb: three standard deviations of the energy of single frames _DRIFT_SIGMA = 3.0 # Rule of thumb: a third of a typical nearest-neighbor distance of 3 Angstrom, # about twice the vibration at the Lindemann limit for that distance. @@ -246,14 +246,16 @@ def _assess_trajectory( - A root mean square displacement above 0.5 Angstrom in the first 10 frames means the atoms are not in the order of the reference. - A root mean square vibration u_vib above 0.15 of the nearest-neighbor - distance means the structure melted. + distance means the structure melted. u_vib and u_ref are measured in + the second half of the frames. - A total displacement u_ref above 1.5 times u_vib means the mean positions moved away from the reference. This check is skipped if the second half of the trajectory is shorter than 1 ps. - A change of the mean potential energy from the second to the last quarter of the frames above 3 times the standard deviation of the energy in the last fifth means the structure transformed (falling energy) - or is disordering (rising energy). + or is disordering (rising energy). This check is skipped below 20 + frames. - A root mean square displacement above 1 Angstrom in the last fifth of the frames points at diffusion or very soft motion. @@ -834,6 +836,11 @@ def fit_finite_temperature_phonons( lowest_frequency=float(frequencies.min()), phonon_bandstructure=bs_symm_line, phonon_dos=dos, + phonopy_settings=PhononComputationalSettings( + npoints_band=npoints_band, + kpath_scheme=_KPATH_SCHEME, + kpoint_density_dos=kpoint_density_dos, + ), force_constants=ForceConstants(phonon.force_constants.tolist()) if store_force_constants else None, diff --git a/src/atomate2/common/schemas/finite_temperature_phonons.py b/src/atomate2/common/schemas/finite_temperature_phonons.py index db1614a58c..85482155fc 100644 --- a/src/atomate2/common/schemas/finite_temperature_phonons.py +++ b/src/atomate2/common/schemas/finite_temperature_phonons.py @@ -2,14 +2,10 @@ from typing import Literal -from emmet.core.math import Matrix3D -from emmet.core.structure import StructureMetadata from pydantic import BaseModel, Field from pymatgen.core import Structure -from pymatgen.phonon.bandstructure import PhononBandStructureSymmLine -from pymatgen.phonon.dos import PhononDos -from atomate2.common.schemas.phonons import ForceConstants, PhononJobDirs, PhononUUIDs +from atomate2.common.schemas.phonons import PhononBSDOSDoc class TrajectoryHealth(BaseModel): @@ -38,7 +34,7 @@ class TrajectoryHealth(BaseModel): None, description="Result of the check. 'reference_mismatch' means the atoms of " "the MD are not in the order of the reference. Every other verdict except " - "'stable' means the trajectory left the reference structure.", + "'stable' means the trajectory may have left the reference structure.", ) n_frames: int | None = Field(None, description="Number of MD frames analysed.") rms_displacement_start: float | None = Field( @@ -89,21 +85,20 @@ class TrajectoryHealth(BaseModel): ) -class FiniteTemperaturePhononDoc(StructureMetadata): - """Effective harmonic phonons at a finite temperature.""" +class FiniteTemperaturePhononDoc(PhononBSDOSDoc): + """Effective harmonic phonons at a finite temperature. + + structure is the unit cell of the NVT MD and the fit, with its atoms sorted + by electronegativity. It is the relaxed unit cell, or the cell from the NPT + MD if there was one. code is the code of the phonon displacement + calculations. born and epsilon_static are the symmetrized values used for + the non-analytical correction. has_imaginary_modes is True if the band + structure has imaginary modes. The undisplaced supercell is the last + phonon displacement calculation in uuids and jobdirs. The thermodynamic + properties are not computed. + """ - structure: Structure | None = Field( - None, - description="Unit cell of the NVT MD and the fit, with its atoms sorted by " - "electronegativity. It is the relaxed unit cell, or the cell from the NPT MD " - "if there was one.", - ) temperature: float | None = Field(None, description="MD temperature in K.") - code: str | None = Field( - None, - description="Code of the phonon displacement calculations that give the " - "forces, 'vasp' or 'forcefields'.", - ) md_code: str | None = Field( None, description="Code of the MD, 'vasp' or 'forcefields'." ) @@ -141,12 +136,6 @@ class FiniteTemperaturePhononDoc(StructureMetadata): description="MD time of each snapshot in ps, its step number times the time " "step.", ) - supercell_matrix: Matrix3D | None = Field( - None, description="Supercell matrix of the MD and the statics." - ) - primitive_matrix: Matrix3D | None = Field( - None, description="Primitive matrix used by phonopy." - ) rotational_sum_rule: str | None = Field( None, description="Rotational sum rule passed to pheasy with --rasr." ) @@ -182,40 +171,17 @@ class FiniteTemperaturePhononDoc(StructureMetadata): tol_imaginary_modes: float | None = Field( None, description="Frequencies below -tol_imaginary_modes in THz are imaginary." ) - has_imaginary_modes: bool | None = Field( - None, description="True if the band structure has imaginary modes." - ) n_imaginary_modes: int | None = Field( None, - description="Number of imaginary modes at the q-points commensurate with the " - "supercell.", + description="Number of frequencies below -tol_imaginary_modes, summed over " + "all q-points commensurate with the supercell. q-points that are equivalent " + "by symmetry are each counted.", ) lowest_frequency: float | None = Field( None, description="Lowest frequency at the q-points commensurate with the " "supercell, in THz. Imaginary frequencies are negative.", ) - phonon_bandstructure: PhononBandStructureSymmLine | None = Field( - None, description="Phonon band structure of the effective force constants." - ) - phonon_dos: PhononDos | None = Field( - None, description="Phonon density of states of the effective force constants." - ) - force_constants: ForceConstants | None = Field( - None, - description="Effective second-order force constants of the supercell in " - "eV/Angstrom^2.", - ) - born: list[Matrix3D] | None = Field( - None, - description="Symmetrized Born effective charges. They are used for the " - "non-analytical correction unless they are all zero.", - ) - epsilon_static: Matrix3D | None = Field( - None, - description="Symmetrized high-frequency dielectric tensor, used for the " - "non-analytical correction together with born.", - ) md_uuids: list[str] | None = Field(None, description="UUIDs of the MD jobs.") md_job_dirs: list[str] | None = Field( None, description="Directories of the MD jobs." @@ -246,14 +212,3 @@ class FiniteTemperaturePhononDoc(StructureMetadata): description="Directory of the relaxation of the atoms in the cell from the " "NPT MD.", ) - uuids: PhononUUIDs | None = Field( - None, - description="UUIDs of the relaxation, the phonon displacement calculations " - "and the Born charge calculation. The undisplaced supercell is the last " - "phonon displacement calculation.", - ) - jobdirs: PhononJobDirs | None = Field( - None, - description="Directories of the relaxation, the phonon displacement " - "calculations, the Born charge calculation and the fit.", - ) diff --git a/src/atomate2/forcefields/flows/finite_temperature_phonons.py b/src/atomate2/forcefields/flows/finite_temperature_phonons.py index d36ca047a3..8709dc67af 100644 --- a/src/atomate2/forcefields/flows/finite_temperature_phonons.py +++ b/src/atomate2/forcefields/flows/finite_temperature_phonons.py @@ -46,7 +46,10 @@ def _get_md_maker( def _get_force_field_md_maker( - maker: BaseFiniteTemperaturePhononMaker, n_steps: int, npt: bool = False + maker: BaseFiniteTemperaturePhononMaker, + n_steps: int, + index: int = 0, + npt: bool = False, ) -> ForceFieldMDMaker: """ Get the force field MD maker of one MD job of a finite-temperature flow. @@ -59,6 +62,9 @@ def _get_force_field_md_maker( The finite-temperature phonon maker. n_steps: int Number of MD steps of the job. + index: int + Position of the job in the MD, counted from 0. It is added to + maker.random_seed. The NPT MD uses maker.md_runs instead. npt: bool If True, get the NPT MD maker from maker.npt_maker. If False, get the NVT MD maker from maker.md_maker. @@ -103,7 +109,11 @@ def _get_force_field_md_maker( traj_file_fmt="ase", traj_interval=1, store_trajectory="no", - mb_velocity_seed=maker.random_seed, + mb_velocity_seed=( + None + if maker.random_seed is None + else maker.random_seed + (maker.md_runs if npt else index) + ), zero_linear_momentum=True, ) @@ -118,21 +128,24 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): another one. The MD writes an ASE trajectory file with a frame at every time step. The snapshots are read from this file, and the trajectory is not stored in the output document of the MD job. The Langevin thermostat has - the default friction of :obj:`.AseMDMaker`, 10 ps^-1. Its random forces - come from numpy's global random number generator, so two runs give - different trajectories. The Nose-Hoover thermostat is ASE's - NoseHooverChainNVT with one thermostat variable, like MDALGO = 2 in VASP. - Its time constant gives a period of about 40 time steps, like SMASS = 0 in - VASP. The initial velocities of the first MD job follow the - Maxwell-Boltzmann distribution, seeded with random_seed, with zero total - momentum. The NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover - thermostat and barostat that change the whole cell, whatever the - thermostat setting (Martyna et al., J. Chem. Phys. 101, 4177 (1994)). Its - thermostat time constant is that of the Nose-Hoover thermostat above, and - its barostat time constant is 1000 time steps. + the default friction of :obj:`.AseMDMaker`, 10 ps^-1. The Nose-Hoover + thermostat is ASE's NoseHooverChainNVT with one thermostat variable, like + MDALGO = 2 in VASP. Its time constant gives a period of about 40 time + steps, like SMASS = 0 in VASP. The initial velocities of the first MD job + follow the Maxwell-Boltzmann distribution, with zero total momentum. The + NPT MD, if any, uses ASE's MTKNPT, a Nose-Hoover thermostat and barostat + that change the whole cell, whatever the thermostat setting (Martyna et + al., J. Chem. Phys. 101, 4177 (1994)). Its thermostat time constant is + that of the Nose-Hoover thermostat above, and its barostat time constant + is 1000 time steps. MD job i, counted from 0, seeds its initial velocities + and its Langevin random forces with random_seed + i. The NPT MD uses + random_seed + md_runs. See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. + This workflow is new and has not been tested widely. It might still change + in future versions. + Parameters ---------- name: str @@ -146,14 +159,17 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): DielectricMaker. It is None by default, as in the force field pheasy phonon workflow. npt_maker: .ForceFieldMDMaker | None - Maker for the NPT MD. It must not set dynamics or ase_md_kwargs. None - skips the NPT MD. + Maker for the NPT MD. The flow sets the same settings as for md_maker, + and the pressure. It must not set dynamics or ase_md_kwargs. None skips + the NPT MD. fixed_cell_relax_maker: .ForceFieldRelaxMaker | None Maker for the relaxation of the atoms in the cell from the NPT MD. It must keep the cell. md_maker: .ForceFieldMDMaker - Maker for the MD. It must not set dynamics or ase_md_kwargs, since the - flow sets the thermostat. + Maker for the MD. The flow sets its ensemble, temperature, n_steps, + time_step, dynamics, ase_md_kwargs, traj_file, traj_file_fmt, + traj_interval, store_trajectory, mb_velocity_seed and + zero_linear_momentum. It must not set dynamics or ase_md_kwargs. phonon_displacement_maker: .ForceFieldStaticMaker Maker for the static calculations on the snapshots and the undisplaced supercell. @@ -184,13 +200,14 @@ class ForceFieldFiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): @property def prev_calc_dir_argname(self) -> None: - """Name of the argument that passes prev_dir to the phonon displacement maker. + """Name of the prev_dir argument of the phonon displacement and Born makers. - Force field makers take no previous directory. + Force field makers take no previous directory, so it is None. A VASP + born_maker then runs without a previous directory. """ return - def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: + def get_md_maker(self, n_steps: int, index: int = 0) -> ForceFieldMDMaker: """ Get the force field MD maker of one MD job. @@ -198,12 +215,14 @@ def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: ---------- n_steps: int Number of MD steps of the job. + index: int + Position of the job in the MD, counted from 0. Returns ------- ForceFieldMDMaker """ - return _get_force_field_md_maker(self, n_steps) + return _get_force_field_md_maker(self, n_steps, index) def get_npt_maker(self, n_steps: int) -> ForceFieldMDMaker: """ @@ -305,6 +324,9 @@ class VaspMDMLFFStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) the undisplaced supercell come from a force field, MACE-MP-0 by default. Use :obj:`from_force_field_name` to use another one. + This workflow is new and has not been tested widely. It might still change + in future versions. + Parameters ---------- name: str @@ -335,9 +357,10 @@ class VaspMDMLFFStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) @property def prev_calc_dir_argname(self) -> None: - """Name of the argument that passes prev_dir to the phonon displacement maker. + """Name of the prev_dir argument of the phonon displacement and Born makers. - Force field makers take no previous directory. + Force field makers take no previous directory, so it is None. A VASP + born_maker then runs without a previous directory. """ return @@ -396,6 +419,9 @@ class MLFFMDVaspStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) force field. The MD settings are those of :obj:`ForceFieldFiniteTemperaturePhononMaker`. + This workflow is new and has not been tested widely. It might still change + in future versions. + Parameters ---------- name: str @@ -407,8 +433,10 @@ class MLFFMDVaspStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) for the non-analytical correction. It is a DielectricMaker by default, as in the VASP pheasy phonon workflow. None skips it. md_maker: .ForceFieldMDMaker - Maker for the MD. It must not set dynamics or ase_md_kwargs, since the - flow sets the thermostat. + Maker for the MD. The flow sets its ensemble, temperature, n_steps, + time_step, dynamics, ase_md_kwargs, traj_file, traj_file_fmt, + traj_interval, store_trajectory, mb_velocity_seed and + zero_linear_momentum. It must not set dynamics or ase_md_kwargs. npt_maker: .ForceFieldMDMaker | None Maker for the NPT MD, under the same conditions as md_maker. None skips the NPT MD. @@ -423,7 +451,7 @@ class MLFFMDVaspStaticFiniteTemperaturePhononMaker(FiniteTemperaturePhononMaker) md_maker: Maker = field(default_factory=lambda: _get_md_maker(_DEFAULT_FORCE_FIELD)) md_code: str = "forcefields" - def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: + def get_md_maker(self, n_steps: int, index: int = 0) -> ForceFieldMDMaker: """ Get the force field MD maker of one MD job. @@ -431,12 +459,14 @@ def get_md_maker(self, n_steps: int) -> ForceFieldMDMaker: ---------- n_steps: int Number of MD steps of the job. + index: int + Position of the job in the MD, counted from 0. Returns ------- ForceFieldMDMaker """ - return _get_force_field_md_maker(self, n_steps) + return _get_force_field_md_maker(self, n_steps, index) def get_npt_maker(self, n_steps: int) -> ForceFieldMDMaker: """ diff --git a/src/atomate2/vasp/flows/finite_temperature_phonons.py b/src/atomate2/vasp/flows/finite_temperature_phonons.py index 1c22f2fc98..8bf78746a8 100644 --- a/src/atomate2/vasp/flows/finite_temperature_phonons.py +++ b/src/atomate2/vasp/flows/finite_temperature_phonons.py @@ -71,6 +71,9 @@ class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): See :obj:`.BaseFiniteTemperaturePhononMaker` for the workflow. + This workflow is new and has not been tested widely. It might still change + in future versions. + Parameters ---------- name: str @@ -169,7 +172,7 @@ class FiniteTemperaturePhononMaker(BaseFiniteTemperaturePhononMaker): @property def prev_calc_dir_argname(self) -> str | None: - """Name of the argument that passes prev_dir to the phonon displacement maker. + """Name of the prev_dir argument of the phonon displacement and Born makers. Returns ------- @@ -177,7 +180,7 @@ def prev_calc_dir_argname(self) -> str | None: """ return "prev_dir" - def get_md_maker(self, n_steps: int) -> MDMaker: + def get_md_maker(self, n_steps: int, index: int = 0) -> MDMaker: """ Get the VASP MD maker of one MD job. @@ -185,6 +188,8 @@ def get_md_maker(self, n_steps: int) -> MDMaker: ---------- n_steps: int Number of MD steps of the job. + index: int + Position of the job in the MD, counted from 0. Unused. Returns ------- diff --git a/tests/ase/test_md.py b/tests/ase/test_md.py index 77178680a8..010e7415fc 100644 --- a/tests/ase/test_md.py +++ b/tests/ase/test_md.py @@ -97,6 +97,24 @@ def test_nvt_nose_hoover_chain(si_structure, clean_dir): maker.run_ase(si_structure) +def test_langevin_seed(si_structure, clean_dir): + """mb_velocity_seed also seeds the random forces of the Langevin thermostat.""" + si_structure.add_site_property("velocities", [[0.0, 0.0, 0.0]] * len(si_structure)) + + def positions(seed): + maker = LennardJonesMDMaker( + ensemble="nvt", + dynamics="langevin", + temperature=300, + n_steps=5, + mb_velocity_seed=seed, + ) + return maker.run_ase(si_structure).final_mol_or_struct.cart_coords + + assert positions(1) == pytest.approx(positions(1)) + assert positions(1) != pytest.approx(positions(2)) + + @pytest.mark.parametrize("calculator_name", list(name_to_maker)) def test_ase_nvt_maker(calculator_name, lj_fcc_ne_pars, fcc_ne_structure, clean_dir): # Langevin thermostat no longer works with single atom structures in ase>3.24.x diff --git a/tests/forcefields/flows/test_finite_temperature_phonons.py b/tests/forcefields/flows/test_finite_temperature_phonons.py index 4708548806..fa5f3841ec 100644 --- a/tests/forcefields/flows/test_finite_temperature_phonons.py +++ b/tests/forcefields/flows/test_finite_temperature_phonons.py @@ -20,11 +20,7 @@ ForceFieldFiniteTemperaturePhononMaker, _get_force_field_md_maker, ) -from atomate2.forcefields.jobs import ( - ForceFieldDielectricMaker, - ForceFieldRelaxMaker, - ForceFieldStaticMaker, -) +from atomate2.forcefields.jobs import ForceFieldDielectricMaker, ForceFieldStaticMaker from atomate2.forcefields.md import ForceFieldMDMaker from atomate2.vasp.jobs.core import DielectricMaker @@ -43,8 +39,6 @@ def cu3au(): def run_emt_flow(structure, **kwargs): """Run the force field workflow with EMT and return its output document.""" - # the Langevin thermostat of ASE draws from numpy's global generator - np.random.seed(103) # noqa: NPY002 maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( EMT, min_length=7.0, md_time_step=2.0, **kwargs ) @@ -56,27 +50,17 @@ def run_emt_flow(structure, **kwargs): @pytest.mark.parametrize( ("kwargs", "match"), [ - ({"md_runs": 0}, "md_runs and n_snapshots must be at least 1"), ({"alpha_min": -2}, "alpha_min must be below -2"), ({"md_time_step": 0}, "must be positive"), ({"equilibration_time": 8.0}, "fewer than the 50 snapshots"), ({"equilibration_time": -1.0}, "fewer than the 50 snapshots"), - ( - {"md_time": 0.01, "equilibration_time": 0, "n_snapshots": 5, "md_runs": 20}, - "larger than the 10", - ), ({"md_maker": None}, "md_maker and phonon_displacement_maker must be set"), ({"code": "aims"}, "code must be one of"), ({"md_code": None}, "md_code must be one of"), - ({"code": "vasp", "socket": True}, "socket is not supported by VASP"), ( {"npt_maker": ForceFieldMDMaker(), "npt_equilibration_time": 8.0}, "npt_equilibration_time must be", ), - ( - {"fixed_cell_relax_maker": ForceFieldRelaxMaker()}, - "only used with npt_maker", - ), ], ) def test_maker_checks(kwargs, match): @@ -99,6 +83,7 @@ def test_force_field_md_maker(cu3au): assert md_maker.time_step == 2.0 assert md_maker.temperature == 300 assert md_maker.mb_velocity_seed == 5 + assert maker.get_md_maker(166, 2).mb_velocity_seed == 7 assert md_maker.store_trajectory == "no" # Langevin by default, with the default friction of AseMDMaker assert md_maker.dynamics == "langevin" @@ -155,6 +140,8 @@ def test_force_field_npt_maker(cu3au): # a barostat time constant of 1000 steps assert npt_maker.ase_md_kwargs["pdamp"] / units.fs == pytest.approx(2000) assert maker.get_md_maker(100).ensemble == MDEnsemble.nvt + # the NPT MD has its own seed, after those of the md_runs NVT MD jobs + assert npt_maker.mb_velocity_seed == 104 # the atoms are relaxed in the cell from the NPT MD assert not maker.fixed_cell_relax_maker.relax_cell assert maker.fixed_cell_relax_maker.fix_symmetry @@ -258,7 +245,6 @@ def test_finite_temperature_phonon_maker_emt_born_charges( clean_dir, cu3au, fake_dielectric_calculator ): """Born charges from a force field dielectric job enter the NAC.""" - np.random.seed(103) # noqa: NPY002 maker = ForceFieldFiniteTemperaturePhononMaker.from_force_field_name( EMT, min_length=7.0, diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 6f913b613b..8330deedbd 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -32,8 +32,9 @@ "stabilize these modes at higher temperature. This workflow fits effective\n", "harmonic force constants to an MD trajectory at the temperature of interest, as\n", "in the temperature-dependent effective potential (TDEP) method of Hellman et\n", - "al., Phys. Rev. B 84, 180301 (2011). These force constants include the\n", - "anharmonic effects at that temperature.\n", + "al., Phys. Rev. B 84, 180301 (2011). These force constants include the effect\n", + "of the anharmonic forces on the frequencies at that temperature. They give no\n", + "phonon lifetimes.\n", "\n", "The flow has these steps:\n", "\n", @@ -58,8 +59,10 @@ "energy late in the run. The result is stored in the output. A warning is raised\n", "if the check fails, but the fit is still done.\n", "\n", - "Without the NPT step, the MD runs at constant volume (NVT), at the volume of\n", - "the starting structure, so thermal expansion is not included. The same workflow runs with VASP as\n", + "Without the NPT step, the MD runs at constant volume (NVT). The volume is that\n", + "of the relaxed structure, or of the input structure when the relaxation is\n", + "switched off, as in this notebook. Thermal expansion is not included. The same\n", + "workflow runs with VASP as\n", "`atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`.\n", "`atomate2.forcefields.flows.finite_temperature_phonons` also has two mixed\n", "versions. One runs the MD with VASP and the force calculations with a force\n", @@ -73,31 +76,29 @@ "source": [ "## Thermostats\n", "\n", - "The fit only uses the positions of the atoms in the MD, not how they move. What\n", - "matters is that the snapshots follow the canonical distribution, so that every\n", - "phonon mode holds its share of the thermal energy.\n", + "The fit only uses the positions of the atoms in the MD, not how they move. The\n", + "snapshots have to follow the canonical distribution, so that every phonon mode\n", + "holds its share of the thermal energy.\n", "\n", "The NVT MD uses a Langevin thermostat. It adds a friction and a random force to\n", "every atom, and it samples the canonical distribution (Bussi and Parrinello,\n", "Phys. Rev. E 75, 056707 (2007)). The friction is 10 ps^-1. A Nose-Hoover\n", "thermostat acts on the whole crystal through one extra variable. It changes the\n", "motion of the atoms less, which matters for vibrational spectra or diffusion.\n", - "But in a nearly harmonic crystal the modes barely exchange energy, and a\n", - "Nose-Hoover thermostat can leave them out of equilibrium. This is proven for a\n", - "harmonic oscillator (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 (2007)).\n", - "The problem is worst at low temperature, where the crystal is closest to\n", - "harmonic.\n", + "But in a nearly harmonic crystal the modes barely exchange energy. For a\n", + "harmonic oscillator weakly coupled to a Nose-Hoover thermostat, the dynamics is\n", + "not ergodic (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 (2007)). A\n", + "crystal is closest to harmonic at low temperature.\n", "\n", "The NPT MD of Section 2 uses ASE's `MTKNPT`. It combines a Nose-Hoover\n", - "thermostat with the barostat of Martyna, Tobias and Klein, which samples the\n", + "thermostat with one thermostat variable and the barostat of Martyna, Tobias and Klein, which samples the\n", "isothermal-isobaric ensemble (J. Chem. Phys. 101, 4177 (1994)). Only its\n", "average cell is used. With VASP, the NPT MD uses VASP's Langevin thermostat\n", "and Parrinello-Rahman barostat, since VASP only runs NPT MD with these.\n", "\n", - "`thermostat=\"nose-hoover\"` switches the NVT MD to a Nose-Hoover thermostat. We\n", - "do not recommend it. The random forces of the Langevin thermostat come from\n", - "numpy's random number generator, so two runs with the same settings give\n", - "different trajectories." + "`thermostat=\"nose-hoover\"` switches the NVT MD to a Nose-Hoover thermostat with\n", + "one thermostat variable. Section 3 compares the two for KNaICl. `random_seed`\n", + "seeds the initial velocities and the random forces of the Langevin thermostat." ] }, { @@ -132,8 +133,7 @@ "- **MACE-OMAT-0-medium.** `mace_mp(model=\"medium-omat-0\")` downloads it once and\n", " caches it under `~/.cache/mace`.\n", "- **MACE-MATPES-PBE-0** and **MACE-MATPES-r2SCAN-0.** These are MACE-OMAT-0\n", - " fine-tuned on the MatPES data set at the PBE and r2SCAN levels. They need\n", - " `mace-torch>=0.3.10`. Download the two files from the `mace_matpes_0` release of\n", + " fine-tuned on the MatPES data set at the PBE and r2SCAN levels. Download the two files from the `mace_matpes_0` release of\n", " [mace-foundations](https://github.com/ACEsuit/mace-foundations/releases/tag/mace_matpes_0):\n", " - [MACE-matpes-pbe-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-pbe-omat-ft.model)\n", " - [MACE-matpes-r2scan-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-r2scan-omat-ft.model)\n", @@ -159,7 +159,8 @@ "# macOS: conda's llvm-openmp and torch's bundled libomp both load and the\n", "# duplicate aborts the process. This must be set before torch is imported.\n", "os.environ.setdefault(\"KMP_DUPLICATE_LIB_OK\", \"TRUE\")\n", - "warnings.filterwarnings(\"ignore\")\n", + "# hide the warnings of torch, e3nn and MACE when the models are loaded\n", + "warnings.filterwarnings(\"ignore\", module=r\"(torch|e3nn|mace)(\\.|$)\")\n", "\n", "import torch # noqa: E402\n", "from mace.calculators import mace_mp # noqa: E402\n", @@ -191,8 +192,9 @@ "Every force field job builds its own calculator. `run_locally` runs all of\n", "them in this one Python process, and the workflow has a little over 50 jobs.\n", "Loading MACE for each of them grows the memory by about 150 MB per job. This\n", - "cell makes the jobs share one calculator. It is only needed when many jobs run\n", - "in one process, not with a workflow manager." + "cell makes the jobs share one calculator, as in the thermal expansion tutorial.\n", + "It is only needed when many jobs run in one process, not with a workflow\n", + "manager." ] }, { @@ -287,7 +289,8 @@ "`ForceFieldFiniteTemperaturePhononMaker.from_force_field_name` sets one force\n", "field for the relaxation, the MD and the force calculations. Any MACE model\n", "routes through `mace_mp`, and the model name in `calculator_kwargs` selects the\n", - "weights.\n", + "weights. The name \"MACE-MP-0\" only picks this calculator. The output keeps it as\n", + "`force_field_name`, and `force_field_kwargs` holds the model that was loaded.\n", "\n", "We skip the relaxation with `relax_initial_structure=False`. The cell is\n", "already relaxed with PBEsol, and our AIMD reference below uses the same cell. If\n", @@ -1270,8 +1273,8 @@ " supercell. They appear in 6 of 9 runs with 25 snapshots, 8 of 9 with 50 and\n", " 5 of 9 with 100. In an earlier round of the same grid with a Nose-Hoover\n", " thermostat, 12 of the 27 runs had them.\n", - "- The random forces of the Langevin thermostat are not seeded, so a second run\n", - " of the grid would not give the same numbers.\n", + "- Each run is one trajectory. Another `random_seed` gives another trajectory and\n", + " somewhat different numbers.\n", "- The MD takes most of the time. With MACE-OMAT-0-medium a run with 50\n", " snapshots took 3.5, 6.1 and 10.8 minutes for 4, 8 and 16 ps. Going from 50 to\n", " 100 snapshots added a few seconds of force calculations and fitting.\n", @@ -1305,14 +1308,16 @@ "The trajectory check uses fixed limits. A Lindemann ratio above 0.15 is reported\n", "as melting. A displacement from the reference of more than 1.5 times the\n", "vibration around the mean positions is reported as a shift. These are rules of\n", - "thumb, and the Lindemann ratio at melting differs between materials. We did not\n", + "thumb. The limit of 0.15 is the Lindemann ratio at melting of an fcc solid. The\n", + "ratio at melting differs between materials. We did not\n", "check whether any of the trajectories reported as melted is a liquid. A warning\n", - "is raised and the fit is still done.\n", + "is raised and the fit is still done. The ratio is averaged over all atoms. It\n", + "can pass 0.15 when only the light atoms move far, for example Li in a\n", + "superionic conductor, while the rest of the crystal stays solid.\n", "\n", "Every result above comes from one MD trajectory. Section 3 shows that runs with\n", "different settings differ by up to 0.1 THz on average and by up to 0.3 THz in\n", - "the highest frequency. The Langevin thermostat is not seeded, so a second run\n", - "gives somewhat different numbers." + "the highest frequency. Another `random_seed` gives somewhat different numbers." ] } ], From 4341cc30612a0796fbd8a4a7771e6fdf82eeb540 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 16:35:16 -0700 Subject: [PATCH 40/43] Add the Li3PS4 sections to the finite-temperature phonon tutorial --- docs/user/codes/vasp.md | 2 +- tutorials/finite_temperature_phonons.ipynb | 1159 +++++++++++++++++++- 2 files changed, 1157 insertions(+), 4 deletions(-) diff --git a/docs/user/codes/vasp.md b/docs/user/codes/vasp.md index a01a78c9da..1d8258cc6f 100644 --- a/docs/user/codes/vasp.md +++ b/docs/user/codes/vasp.md @@ -429,7 +429,7 @@ The displacements are measured from the undisplaced supercell. Pheasy then fits the second-order force constants to them with LASSO. As in the pheasy phonon workflow, a `DielectricMaker` computes the Born charges and the dielectric tensor for the non-analytical correction. It needs the `pheasy` extra, like the pheasy phonon workflow above. -The notebook `tutorials/finite_temperature_phonons.ipynb` runs it for six materials with three MACE potentials. +The notebook `tutorials/finite_temperature_phonons.ipynb` runs it for seven materials with three MACE potentials. ```{warning} This workflow is new and has not been tested widely. diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 8330deedbd..c3b02ade7e 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -16,6 +16,11 @@ "the cell at each temperature, found with an NPT MD. Section 3 tests the length\n", "of the MD and the number of snapshots for KNaICl.\n", "\n", + "Section 4 runs Li3PS4, a lithium conductor whose crystal is unstable at 0 K, from\n", + "100 to 1000 K. Section 5 shows what to do once its Li atoms start to hop. It\n", + "computes the vibrational DOS and the free energy from the MD, and compares the\n", + "free energies of two of its phases.\n", + "\n", "This workflow is new. It is less tested than the other phonon workflows in\n", "atomate2, and its defaults and output may still change." ] @@ -438,10 +443,18 @@ "\n", "\n", "def plot_bands(\n", - " ax: plt.Axes, bs: PhononBandStructureSymmLine, label: str | None = None, **style\n", + " ax: plt.Axes,\n", + " bs: PhononBandStructureSymmLine,\n", + " label: str | None = None,\n", + " distance: list[float] | None = None,\n", + " **style,\n", ") -> None:\n", - " \"\"\"Plot a phonon band structure, one segment of the path at a time.\"\"\"\n", - " distance = np.array(bs.distance)\n", + " \"\"\"Plot a phonon band structure, one segment of the path at a time.\n", + "\n", + " distance replaces the distances along the path of bs, for a band structure\n", + " computed on the same q-points as another one.\n", + " \"\"\"\n", + " distance = np.array(bs.distance if distance is None else distance)\n", " positions, names = [], []\n", " for idx, branch in enumerate(bs.branches):\n", " part = slice(branch[\"start_index\"], branch[\"end_index\"] + 1)\n", @@ -1291,6 +1304,1146 @@ "cell_type": "markdown", "id": "40", "metadata": {}, + "source": [ + "## 4. Li3PS4, a crystal that is unstable at 0 K\n", + "\n", + "Li3PS4 is a solid electrolyte for lithium batteries. In experiment it has three\n", + "phases at ambient pressure. γ (Pmn2₁) is stable up to 523 to 573 K. β (Pnma)\n", + "is stable up to 723 to 748 K. α (Cmcm) is stable above that (Homma et al.,\n", + "Solid State Ionics 182, 53 (2011); Kaup et al., J. Mater. Chem. A 8, 12446\n", + "(2020)). γ is ordered. In β and α the Li atoms sit on partly occupied sites.\n", + "\n", + "mp-985583 is a Pnma structure, so it is β. A DFT code needs every site fully\n", + "occupied, so it is one ordered choice of the Li sites. In the Materials\n", + "Project's Harmonic Phonon Database it has imaginary modes at 0 K. Here we run\n", + "it from 100 to 1000 K, in steps of 100 K, with the three potentials. Each\n", + "potential first relaxes the structure. We run every temperature twice. One run\n", + "uses the relaxed 0 K cell (NVT). The other uses the cell from an NPT MD at that\n", + "temperature (Section 2). The supercell has 128 atoms." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "41", + "metadata": {}, + "outputs": [], + "source": [ + "li3ps4 = get_pheasy_structure(\"mp-985583\")\n", + "LI3PS4_SUPERCELL = (2, 2, 1) # 128 atoms\n", + "LI3PS4_TEMPERATURES = tuple(range(100, 1001, 100))\n", + "li3ps4.composition, li3ps4.get_space_group_info()" + ] + }, + { + "cell_type": "markdown", + "id": "42", + "metadata": {}, + "source": [ + "## Phonons at 0 K\n", + "\n", + "For the 0 K reference we use the phonopy workflow of atomate2, not the pheasy\n", + "one. When imaginary modes appear, the pheasy workflow refits the force\n", + "constants to remove them. Here we want to see them. The relaxation keeps the\n", + "symmetry, as in the finite-temperature workflow." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "43", + "metadata": {}, + "outputs": [], + "source": [ + "from atomate2.common.schemas.phonons import PhononBSDOSDoc\n", + "from atomate2.forcefields.flows.phonons import PhononMaker\n", + "\n", + "\n", + "def li3ps4_harmonic(model: str) -> PhononBSDOSDoc:\n", + " \"\"\"Run the phonopy workflow at 0 K, in the cell relaxed by the potential.\"\"\"\n", + " maker = PhononMaker.from_force_field_name(\n", + " \"MACE-MP-0\", calculator_kwargs=calc_kwargs(model)\n", + " )\n", + " maker.bulk_relax_maker.fix_symmetry = True\n", + " flow = maker.make(li3ps4, supercell_matrix=np.diag(LI3PS4_SUPERCELL).tolist())\n", + " root_dir = f\"runs/Li3PS4_{model}_0K\"\n", + " os.makedirs(root_dir, exist_ok=True)\n", + " responses = run_locally(\n", + " flow,\n", + " store=JobStore(MemoryStore(), additional_stores={\"data\": MemoryStore()}),\n", + " create_folders=True,\n", + " root_dir=root_dir,\n", + " ensure_success=True,\n", + " )\n", + " return responses[flow.output.uuid][1].output\n", + "\n", + "\n", + "doc_0k = li3ps4_harmonic(\"OMAT-0-medium\")\n", + "float(np.min(doc_0k.phonon_bandstructure.bands))" + ] + }, + { + "cell_type": "markdown", + "id": "44", + "metadata": {}, + "source": [ + "Our run took 2 minutes. The lowest frequency is -2.59 THz. With\n", + "MACE-MATPES-PBE-0 it is -1.97 THz and with MACE-MATPES-r2SCAN-0 -3.48 THz." + ] + }, + { + "cell_type": "markdown", + "id": "45", + "metadata": {}, + "source": [ + "## One temperature\n", + "\n", + "We run 600 K with MACE-OMAT-0-medium and the NPT MD." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "46", + "metadata": {}, + "outputs": [], + "source": [ + "doc_li3ps4 = run_ft(\n", + " li3ps4,\n", + " LI3PS4_SUPERCELL,\n", + " \"OMAT-0-medium\",\n", + " \"runs/Li3PS4_OMAT-0-medium_600K_npt\",\n", + " 600,\n", + " relax=True,\n", + " run_npt=True,\n", + ")\n", + "{\n", + " \"volume at 0 K in A^3\": doc_li3ps4.npt_input_structure.volume,\n", + " \"volume at 600 K in A^3\": doc_li3ps4.structure.volume,\n", + " \"lowest frequency in THz\": float(np.min(doc_li3ps4.phonon_bandstructure.bands)),\n", + " \"trajectory check\": doc_li3ps4.trajectory_health.verdict,\n", + " \"Lindemann ratio\": doc_li3ps4.trajectory_health.lindemann_ratio,\n", + "}" + ] + }, + { + "cell_type": "markdown", + "id": "47", + "metadata": {}, + "source": [ + "Our run took 31 minutes. The volume grows from 664.8 to 698.5 ų. The lowest\n", + "frequency is -0.57 THz. The trajectory check reports \"melted\", with a Lindemann\n", + "ratio of 0.24. Section 5 shows that the crystal has not melted. The Li atoms\n", + "hop between sites while P and S stay in place." + ] + }, + { + "cell_type": "markdown", + "id": "48", + "metadata": {}, + "source": [ + "## The other temperatures and potentials\n", + "\n", + "The loop below runs all 60 settings and the three 0 K runs. It is off by\n", + "default. Each of our runs took 15 to 62 minutes on one A100 GPU." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "49", + "metadata": {}, + "outputs": [], + "source": [ + "RUN_LI3PS4 = False\n", + "li3ps4_docs = {}\n", + "if RUN_LI3PS4:\n", + " for model in MODEL_FILES:\n", + " li3ps4_docs[model, 0, \"harmonic\"] = li3ps4_harmonic(model)\n", + " for temperature in LI3PS4_TEMPERATURES:\n", + " for label, run_npt in ((\"nvt\", False), (\"npt\", True)):\n", + " li3ps4_docs[model, temperature, label] = run_ft(\n", + " li3ps4,\n", + " LI3PS4_SUPERCELL,\n", + " model,\n", + " f\"runs/Li3PS4_{model}_{temperature}K_{label}\",\n", + " temperature,\n", + " relax=True,\n", + " run_npt=run_npt,\n", + " )" + ] + }, + { + "cell_type": "markdown", + "id": "50", + "metadata": {}, + "source": [ + "The next cell plots the bands of one potential from 0 to 1000 K. Every run\n", + "keeps the Pnma symmetry, so all runs of a potential have the band path of its\n", + "0 K run. Their q-points are the same in reduced coordinates. The cells differ a\n", + "little, so we plot every run along the distances of the 0 K path." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "51", + "metadata": {}, + "outputs": [], + "source": [ + "def plot_li3ps4_bands(model: str, label: str) -> None:\n", + " \"\"\"Plot the bands of one potential from 0 to 1000 K on its 0 K band path.\"\"\"\n", + " reference = li3ps4_docs[model, 0, \"harmonic\"].phonon_bandstructure\n", + " _, ax = plt.subplots(figsize=(8, 4))\n", + " for temperature in LI3PS4_TEMPERATURES:\n", + " plot_bands(\n", + " ax,\n", + " li3ps4_docs[model, temperature, label].phonon_bandstructure,\n", + " label=f\"{temperature} K\",\n", + " distance=reference.distance,\n", + " color=plt.cm.viridis(temperature / 1000),\n", + " lw=0.4,\n", + " )\n", + " plot_bands(ax, reference, label=\"0 K\", color=\"black\", lw=0.6)\n", + " ax.set_ylabel(\"Frequency (THz)\")\n", + " ax.set_title(f\"{model}, {label.upper()}\")\n", + " ax.legend(fontsize=7, ncol=2)\n", + " plt.show()\n", + "\n", + "\n", + "if RUN_LI3PS4:\n", + " for model in MODEL_FILES:\n", + " for label in (\"nvt\", \"npt\"):\n", + " plot_li3ps4_bands(model, label)" + ] + }, + { + "cell_type": "markdown", + "id": "52", + "metadata": {}, + "source": [ + "## Our results\n", + "\n", + "The next cell holds the results of our runs. For each run it gives the lowest\n", + "frequency on the band path, the Lindemann ratio of the trajectory check and\n", + "the volume of the NPT cell." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "53", + "metadata": {}, + "outputs": [], + "source": [ + "# lowest frequency on the band path in THz and Lindemann ratio of the NVT MD,\n", + "# at 100 to 1000 K, in the relaxed 0 K cell (nvt) and in the NPT cell (npt)\n", + "LOWEST_FREQUENCY = {\n", + " \"nvt\": {\n", + " \"OMAT-0-medium\": (-0.8, -0.4, -0.9, -0.8, -0.4, -1.6, -1.1, -1.1, -1.5, -1.5),\n", + " \"MATPES-PBE-0\": (-0.2, -0.9, -1.0, -2.2, -1.4, -1.3, -1.7, -1.6, -1.5, -1.6),\n", + " \"MATPES-r2SCAN-0\": (-0.7, -0.3, -0.6, -0.3, -0.7, -1.1, -1.6, -1.5, -1.5, -1.4),\n", + " },\n", + " \"npt\": {\n", + " \"OMAT-0-medium\": (-0.7, -0.4, -0.7, -0.7, -0.5, -0.6, -1.4, -1.5, -1.3, -1.4),\n", + " \"MATPES-PBE-0\": (-0.4, -0.5, -1.4, -0.5, -1.3, -1.4, -1.3, -1.7, -1.6, -1.6),\n", + " \"MATPES-r2SCAN-0\": (-0.5, -0.6, -1.4, 0.0, -0.7, -1.0, -1.1, -1.3, -1.8, -1.6),\n", + " },\n", + "}\n", + "LINDEMANN = {\n", + " \"nvt\": {\n", + " \"OMAT-0-medium\": (0.06, 0.1, 0.12, 0.17, 0.18, 0.26, 0.28, 0.33, 0.51, 0.54),\n", + " \"MATPES-PBE-0\": (0.08, 0.13, 0.16, 0.2, 0.24, 0.36, 0.42, 0.41, 0.55, 0.84),\n", + " \"MATPES-r2SCAN-0\": (0.06, 0.1, 0.13, 0.17, 0.21, 0.26, 0.28, 0.36, 0.58, 0.45),\n", + " },\n", + " \"npt\": {\n", + " \"OMAT-0-medium\": (0.08, 0.11, 0.15, 0.17, 0.19, 0.24, 0.39, 0.36, 0.58, 0.77),\n", + " \"MATPES-PBE-0\": (0.08, 0.13, 0.18, 0.19, 0.23, 0.32, 0.33, 0.41, 0.61, 0.74),\n", + " \"MATPES-r2SCAN-0\": (0.07, 0.1, 0.13, 0.18, 0.21, 0.24, 0.27, 0.4, 0.52, 0.61),\n", + " },\n", + "}\n", + "# volume of the unit cell in A^3, relaxed at 0 K and from the NPT MD\n", + "VOLUME_0K = {\"OMAT-0-medium\": 664.7, \"MATPES-PBE-0\": 651.6, \"MATPES-r2SCAN-0\": 649.6}\n", + "NPT_VOLUME = {\n", + " \"OMAT-0-medium\": (670, 675, 680, 687, 693, 698, 702, 713, 776, 767),\n", + " \"MATPES-PBE-0\": (656, 658, 661, 660, 663, 662, 667, 672, 678, 692),\n", + " \"MATPES-r2SCAN-0\": (656, 661, 666, 669, 673, 673, 675, 683, 691, 699),\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 3, figsize=(14, 3.6))\n", + "for idx, model in enumerate(MODEL_FILES):\n", + " for label, style in ((\"nvt\", \"-o\"), (\"npt\", \"--s\")):\n", + " kwargs = {\"color\": f\"C{idx}\", \"ms\": 3, \"label\": f\"{model}, {label}\"}\n", + " axes[0].plot(\n", + " LI3PS4_TEMPERATURES, LOWEST_FREQUENCY[label][model], style, **kwargs\n", + " )\n", + " axes[1].plot(LI3PS4_TEMPERATURES, LINDEMANN[label][model], style, **kwargs)\n", + " ratio = np.array(NPT_VOLUME[model]) / VOLUME_0K[model]\n", + " axes[2].plot(LI3PS4_TEMPERATURES, ratio, \"--s\", color=f\"C{idx}\", ms=3)\n", + "axes[1].axhline(0.15, color=\"gray\", ls=\":\")\n", + "axes[0].set_ylabel(\"Lowest frequency (THz)\")\n", + "axes[1].set_ylabel(\"Lindemann ratio\")\n", + "axes[2].set_ylabel(\"V(NPT) / V(0 K)\")\n", + "for ax in axes:\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "axes[0].legend(fontsize=7)\n", + "fig.tight_layout()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "54", + "metadata": {}, + "source": [ + "- The imaginary modes of 0 K shrink at finite temperature, but they do not go\n", + " away. The lowest frequency lies between -0.2 and -2.2 THz in every run but\n", + " one. MACE-MATPES-r2SCAN-0 in the NPT cell at 400 K has no imaginary modes.\n", + "- At 100 K the trajectory check reports a shift in every run. The atoms move\n", + " away from the MP structure. At 200 K every run is stable.\n", + "- From 300 to 400 K the Lindemann ratio passes 0.15 and the check reports\n", + " melting. It then keeps rising, to 0.45 to 0.84 at 900 to 1000 K.\n", + "- From 0 to 800 K the NPT cell grows by 3 to 7% in volume. With\n", + " MACE-OMAT-0-medium it then jumps by 9% between 800 and 900 K.\n", + "- MACE-MATPES-PBE-0 gives the softest bands. Its highest frequency at 0 K is\n", + " 15.4 THz, against 17.8 and 17.9 THz for the other two.\n", + "\n", + "Li3PS4 does not melt at 400 K in experiment. Section 5 looks at what the atoms\n", + "do instead." + ] + }, + { + "cell_type": "markdown", + "id": "55", + "metadata": {}, + "source": [ + "## 5. When light atoms hop: Li3PS4 above 300 K\n", + "\n", + "In Section 4 the fitted phonons of Li3PS4 keep imaginary modes at every\n", + "temperature. At 0 K they come from the structure. This ordering of the Li\n", + "sites is not at a minimum of the energy. At high temperature a second cause\n", + "adds to this. The Li atoms start to hop from site to site, while the PS4\n", + "framework stays solid. A fit of force constants assumes that every atom\n", + "vibrates around one site. A Li atom that hops has no such site, so the fit\n", + "reads its motion as a very soft spring. The Lindemann ratio is an average over\n", + "all atoms, so the far moves of Li alone push it above 0.15.\n", + "\n", + "This section uses the MD itself, which needs no fixed sites. The mean-square\n", + "displacement of each element tells which atoms diffuse. The vibrational DOS\n", + "comes from the velocities in the MD. The free energy comes from thermodynamic\n", + "integration over the MD.\n", + "\n", + "The trajectories are the ones the workflow already saved, in\n", + "`md_trajectory.traj` in each run folder. They have one frame per time step and\n", + "include the momenta and the potential energies. The examples below use the\n", + "600 K run above." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "56", + "metadata": {}, + "outputs": [], + "source": [ + "from pathlib import Path\n", + "\n", + "from ase import Atoms\n", + "from ase.io import Trajectory\n", + "\n", + "SKIP = 1000 # frames left out at the start, as in the fit\n", + "TIME_STEP = 1e-3 # ps per frame\n", + "\n", + "\n", + "def nvt_trajectory(folder: str) -> list[Atoms]:\n", + " \"\"\"Get the frames of the NVT MD in a run folder, after the first SKIP.\"\"\"\n", + " for path in Path(folder).rglob(\"md_trajectory.traj\"):\n", + " traj = Trajectory(str(path))\n", + " if np.allclose(traj[0].cell.array, traj[-1].cell.array):\n", + " return [traj[i] for i in range(SKIP, len(traj))]\n", + " raise FileNotFoundError(f\"no NVT trajectory in {folder}\")\n", + "\n", + "\n", + "def unwrapped_positions(frames: list[Atoms]) -> np.ndarray:\n", + " \"\"\"Get the Cartesian positions of every frame, without jumps across the cell.\"\"\"\n", + " cell = frames[0].cell.array\n", + " frac = np.array([atoms.get_scaled_positions(wrap=False) for atoms in frames])\n", + " steps = np.diff(frac, axis=0)\n", + " steps -= np.round(steps)\n", + " frac = np.concatenate([frac[:1], frac[:1] + np.cumsum(steps, axis=0)])\n", + " return frac @ cell\n", + "\n", + "\n", + "frames_600k = nvt_trajectory(\"runs/Li3PS4_OMAT-0-medium_600K_npt\")" + ] + }, + { + "cell_type": "markdown", + "id": "57", + "metadata": {}, + "source": [ + "## Which atoms move\n", + "\n", + "The mean-square displacement (MSD) of an atom grows linearly in time if it\n", + "diffuses. It levels off if the atom only vibrates. Its slope gives the\n", + "diffusion coefficient, $D = \\mathrm{slope}/6$. We fit the slope from 1 to 3 ps." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "58", + "metadata": {}, + "outputs": [], + "source": [ + "def diffusion(\n", + " frames: list[Atoms], max_lag: int = 3000, fit: tuple[int, int] = (1000, 3000)\n", + ") -> dict[str, tuple[np.ndarray, np.ndarray, float]]:\n", + " \"\"\"Get the MSD (A^2) against time (ps) and D (cm^2/s) of each element.\n", + "\n", + " The motion of the center of mass is removed. fit gives the range of lags in\n", + " frames where the slope of the MSD is fitted.\n", + " \"\"\"\n", + " masses = frames[0].get_masses()\n", + " symbols = np.array(frames[0].get_chemical_symbols())\n", + " pos = unwrapped_positions(frames)\n", + " pos -= ((pos * masses[None, :, None]).sum(1) / masses.sum())[:, None]\n", + " lags = np.arange(0, max_lag + 1, 10)\n", + " origins = np.arange(0, len(pos) - max_lag, 100)\n", + " msd = np.array(\n", + " [((pos[origins + lag] - pos[origins]) ** 2).sum(2).mean(0) for lag in lags]\n", + " )\n", + " keep = (lags >= fit[0]) & (lags <= fit[1])\n", + " out = {}\n", + " for element in (\"Li\", \"P\", \"S\"):\n", + " curve = msd[:, symbols == element].mean(1)\n", + " slope = np.polyfit(lags[keep] * TIME_STEP, curve[keep], 1)[0]\n", + " out[element] = (lags * TIME_STEP, curve, slope / 6 * 1e-4)\n", + " return out\n", + "\n", + "\n", + "{element: f\"{d:.1e}\" for element, (_, _, d) in diffusion(frames_600k).items()}" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "59", + "metadata": {}, + "outputs": [], + "source": [ + "# diffusion coefficient in cm^2/s of each element in the NVT MD in the relaxed\n", + "# 0 K cell, at 300 to 1000 K\n", + "D_TEMPERATURES = (300, 400, 500, 600, 700, 800, 900, 1000)\n", + "DIFFUSION = {\n", + " \"OMAT-0-medium\": {\n", + " \"Li\": (-4.4e-07, 2e-06, -4.9e-08, 7.6e-06, 8e-06, 5e-06, 3.1e-05, 4.7e-05),\n", + " \"P\": (-1.3e-08, -3.3e-08, 1.2e-08, 1.4e-07, 1.3e-07, 6.9e-08, 9.6e-07, 2.6e-07),\n", + " \"S\": (-3.3e-08, -1.9e-08, 2.1e-08, 2.4e-07, 2.1e-07, 4.7e-07, 1.9e-06, 1.3e-06),\n", + " },\n", + " \"MATPES-PBE-0\": {\n", + " \"Li\": (1.9e-06, 3e-06, 6.3e-06, 1.5e-05, 2.6e-05, 2.9e-05, 4.6e-05, 6.4e-05),\n", + " \"P\": (4.6e-08, 2e-08, -1.9e-08, 1.4e-07, -2.6e-07, 2.9e-07, 1.2e-07, 3.5e-07),\n", + " \"S\": (1.2e-07, 1.8e-08, 3.9e-08, 2.7e-07, -3.7e-07, 5.4e-07, -2.7e-07, 8.1e-07),\n", + " },\n", + " \"MATPES-r2SCAN-0\": {\n", + " \"Li\": (1.6e-06, 7.9e-07, 2.6e-06, 4.8e-06, 6.8e-06, 2.6e-05, 3.8e-05, 3.4e-05),\n", + " \"P\": (\n", + " 3.2e-09,\n", + " -4.1e-09,\n", + " -6.6e-08,\n", + " 8.4e-08,\n", + " 1.5e-07,\n", + " 1.4e-07,\n", + " 4.2e-07,\n", + " -2.2e-07,\n", + " ),\n", + " \"S\": (1e-07, 9.1e-09, 7e-08, 1.8e-07, 7e-08, 3e-07, 9.3e-07, -3.7e-09),\n", + " },\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 3, figsize=(14, 3.6), sharey=True)\n", + "inverse_t = 1000 / np.array(D_TEMPERATURES)\n", + "for ax, model in zip(axes, MODEL_FILES, strict=True):\n", + " ax.axvspan(1000 / 748, 1000 / 523, color=\"0.9\")\n", + " for element, color in ((\"Li\", \"C0\"), (\"P\", \"C2\"), (\"S\", \"C3\")):\n", + " d = np.array(DIFFUSION[model][element])\n", + " keep = d > 1e-8\n", + " ax.semilogy(inverse_t[keep], d[keep], \"-o\", color=color, ms=3, label=element)\n", + " ax.axhline(3e-7, color=\"gray\", ls=\":\")\n", + " ax.set_title(model)\n", + " ax.set_xlabel(\"1000 / T (1/K)\")\n", + "axes[0].set_ylabel(\"D (cm$^2$/s)\")\n", + "axes[0].legend()\n", + "fig.tight_layout()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "60", + "metadata": {}, + "source": [ + "A D below about 3×10⁻⁷ cm²/s is noise in these 7 ps runs. P and S stay near\n", + "that level up to 700 K.\n", + "\n", + "- Li diffuses clearly from about 600 K with MACE-OMAT-0-medium and\n", + " MACE-MATPES-r2SCAN-0, and from about 500 K with MACE-MATPES-PBE-0. D_Li is\n", + " 5×10⁻⁶ to 3×10⁻⁵ cm²/s at 600 to 800 K.\n", + "- Below that, a D_Li of 10⁻⁶ cm²/s means a few single hops in the run. One hop\n", + " of 2.5 Å by one of the 48 Li atoms already gives 0.13 Ų. A converged D below\n", + " 600 K needs MD of nanoseconds.\n", + "- At 900 K the D of P and S passes 10⁻⁶ cm²/s with MACE-OMAT-0-medium. With\n", + " the other two it stays below that in the 0 K cell, and passes it in the NPT\n", + " cell at 1000 K. The framework starts to flow.\n", + "\n", + "So from about 600 K to about 800 K, Li3PS4 is a solid framework with mobile\n", + "Li. This is the range where the fitted phonons fail.\n", + "\n", + "The MD uses the Langevin thermostat, and D depends on its friction. For a D to\n", + "compare with experiment, run an MD without a thermostat (NVE) from the end of\n", + "the NVT MD." + ] + }, + { + "cell_type": "markdown", + "id": "61", + "metadata": {}, + "source": [ + "## The vibrational DOS from the velocities\n", + "\n", + "The vibrational DOS is the Fourier transform of the velocity autocorrelation\n", + "function, weighted by mass. By the Wiener-Khinchin theorem this is the squared\n", + "Fourier transform of each velocity:\n", + "\n", + "$$g(\\nu) \\propto \\sum_i m_i \\left| \\int v_i(t)\\, e^{2\\pi i \\nu t}\\, dt \\right|^2$$\n", + "\n", + "It holds all the anharmonicity at that temperature and has no imaginary\n", + "frequencies. An atom that diffuses adds to the DOS at $\\nu = 0$, in proportion\n", + "to its D. The friction of the Langevin thermostat, $\\gamma$ = 10 ps⁻¹, gives\n", + "every peak a width of $\\gamma/2\\pi$ = 1.6 THz (full width at half maximum)." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "62", + "metadata": {}, + "outputs": [], + "source": [ + "def md_dos(\n", + " frames: list[Atoms], smearing: float = 0.15, max_frequency: float = 25.0\n", + ") -> tuple[np.ndarray, dict[str, np.ndarray]]:\n", + " \"\"\"Get the DOS of each element from the velocities, in states/THz per Li3PS4.\n", + "\n", + " The DOS is smeared with a Gaussian of width smearing in THz, mirrored at 0.\n", + " It integrates to 3 states per atom.\n", + " \"\"\"\n", + " velocities = np.array([atoms.get_velocities() for atoms in frames])\n", + " masses = frames[0].get_masses()\n", + " symbols = np.array(frames[0].get_chemical_symbols())\n", + " nu = np.fft.rfftfreq(len(velocities), TIME_STEP)\n", + " keep = nu <= max_frequency\n", + " power = (np.abs(np.fft.rfft(velocities, axis=0)) ** 2).sum(2)[keep] * masses\n", + " step = nu[1]\n", + " half = int(4 * smearing / step)\n", + " kernel = np.exp(-0.5 * (np.arange(-half, half + 1) * step / smearing) ** 2)\n", + " n_formula_units = len(symbols) / 8\n", + " out = {}\n", + " for element in (\"Li\", \"P\", \"S\"):\n", + " g = power[:, symbols == element].sum(1)\n", + " g = np.convolve(np.concatenate([g[half:0:-1], g]), kernel, \"same\")[half:]\n", + " n_states = 3 * (symbols == element).sum() / n_formula_units\n", + " out[element] = g * n_states / (g.sum() * step)\n", + " return nu[keep], out\n", + "\n", + "\n", + "nu_600k, dos_600k = md_dos(frames_600k)" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "63", + "metadata": {}, + "outputs": [], + "source": [ + "# vibrational DOS of the NVT MD in the relaxed 0 K cell, against the DOS of\n", + "# the force constants fitted to the same MD, at 300, 500 and 700 K: the fraction\n", + "# of the Li DOS below 5 THz, and the frequency in THz of the P-S stretch, the\n", + "# highest peak of the P DOS\n", + "VDOS_TEMPERATURES = (300, 500, 700)\n", + "LI_BELOW_5_THZ = {\n", + " \"OMAT-0-medium\": {\"MD\": (0.15, 0.18, 0.23), \"fit\": (0.18, 0.27, 0.9)},\n", + " \"MATPES-PBE-0\": {\"MD\": (0.21, 0.23, 0.25), \"fit\": (0.53, 0.98, 1.0)},\n", + " \"MATPES-r2SCAN-0\": {\"MD\": (0.14, 0.17, 0.21), \"fit\": (0.19, 0.41, 0.99)},\n", + "}\n", + "PS_STRETCH = {\n", + " \"OMAT-0-medium\": {\"MD\": (16.4, 16.0, 16.4), \"fit\": (15.9, 15.2, 12.9)},\n", + " \"MATPES-PBE-0\": {\"MD\": (14.6, 15.0, 15.0), \"fit\": (13.8, 12.4, 12.0)},\n", + " \"MATPES-r2SCAN-0\": {\"MD\": (16.3, 16.3, 16.3), \"fit\": (16.1, 15.2, 13.2)},\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 2, figsize=(12, 3.6))\n", + "for idx, model in enumerate(MODEL_FILES):\n", + " for source, style in ((\"MD\", \"-o\"), (\"fit\", \"--s\")):\n", + " kwargs = {\"color\": f\"C{idx}\", \"ms\": 3, \"label\": f\"{model}, {source}\"}\n", + " axes[0].plot(VDOS_TEMPERATURES, LI_BELOW_5_THZ[model][source], style, **kwargs)\n", + " axes[1].plot(VDOS_TEMPERATURES, PS_STRETCH[model][source], style, **kwargs)\n", + "axes[0].set_ylabel(\"Fraction of the Li DOS below 5 THz\")\n", + "axes[1].set_ylabel(\"P-S stretch (THz)\")\n", + "for ax in axes:\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "axes[0].legend(fontsize=7)\n", + "fig.tight_layout()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "64", + "metadata": {}, + "source": [ + "The fitted DOS is smeared with the same 0.15 THz as the MD DOS.\n", + "\n", + "- At 300 K, with MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0, 14 to 19% of the\n", + " Li DOS lies below 5 THz, in the MD and in the fit. With MACE-MATPES-PBE-0 the\n", + " fit already puts 53% of it there, against 21% in the MD.\n", + "- At 700 K the fit puts 90 to 100% of the Li DOS below 5 THz, and 6 to 18% of\n", + " it at imaginary frequencies. In the MD it is 21 to 25%. The Li DOS of the MD\n", + " stays a broad band, with a small value at zero from the diffusion.\n", + "- In the MD the P-S stretch stays at 16.0 to 16.4 THz with MACE-OMAT-0-medium\n", + " and MACE-MATPES-r2SCAN-0, and at 14.6 to 15.0 THz with MACE-MATPES-PBE-0. In\n", + " the fit it drops to 12.0 to 13.2 THz at 700 K. The framework does not soften.\n", + " The fit around fixed sites makes it look soft." + ] + }, + { + "cell_type": "markdown", + "id": "65", + "metadata": {}, + "source": [ + "## The free energy from the MD\n", + "\n", + "The fitted phonons give a free energy only through their frequencies, so they\n", + "carry the same errors. The MD gives it without a fit, in two steps.\n", + "\n", + "**1. F at one temperature, $T_0$ = 100 K, by Frenkel-Ladd.** An Einstein\n", + "crystal, with every atom tied by a spring to a site, has a free energy known in\n", + "closed form. We switch the potential from the Einstein crystal to the MACE\n", + "potential, $U(\\lambda) = \\lambda U_\\mathrm{MLIP} + (1 - \\lambda) U_E$, and run\n", + "an MD at 8 values of $\\lambda$. Then\n", + "\n", + "$$F_\\mathrm{MLIP} = F_E + \\int_0^1 \\langle U_\\mathrm{MLIP} - U_E \\rangle_\\lambda\\, d\\lambda$$\n", + "\n", + "The springs sit at the mean positions of the 100 K MD. Their constants are\n", + "$3k_BT$ over the mean-square displacement of each element. The center of mass\n", + "is fixed in the MD, and $F_E$ has a term for that. We choose 100 K because no\n", + "Li hops there in any run.\n", + "\n", + "**2. F at every other temperature, by Gibbs-Helmholtz.**\n", + "\n", + "$$\\frac{d(F/T)}{dT} = -\\frac{U}{T^2}$$\n", + "\n", + "U is the mean energy of the MD at each temperature, the potential energy plus\n", + "$3k_BT/2$ per atom. For the NPT runs it is the mean enthalpy at zero pressure,\n", + "and the result is the Gibbs free energy. Then $S = (U - F)/T$. We stop at\n", + "800 K. Above it the P and S atoms start to diffuse.\n", + "\n", + "The MD treats the nuclei as classical. We add the difference between the\n", + "quantum and the classical free energy of the MD DOS at each temperature. It\n", + "matters most at low temperature." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "66", + "metadata": {}, + "outputs": [], + "source": [ + "from ase import units\n", + "from ase.calculators.calculator import Calculator, all_changes\n", + "from ase.constraints import FixCom\n", + "from ase.md.langevin import Langevin\n", + "from ase.md.velocitydistribution import MaxwellBoltzmannDistribution, Stationary\n", + "from scipy import constants\n", + "\n", + "\n", + "class Switched(Calculator):\n", + " \"\"\"Energy and forces of lam U_MLIP + (1 - lam) U_E.\n", + "\n", + " delta holds U_MLIP - U_E of the last call.\n", + " \"\"\"\n", + "\n", + " implemented_properties = (\"energy\", \"forces\")\n", + "\n", + " def __init__(\n", + " self,\n", + " mlip: Calculator,\n", + " positions: np.ndarray,\n", + " springs: np.ndarray,\n", + " lam: float,\n", + " ) -> None:\n", + " super().__init__()\n", + " self.mlip, self.r0, self.k, self.lam = mlip, positions, springs, lam\n", + "\n", + " def calculate(\n", + " self,\n", + " atoms: Atoms | None = None,\n", + " properties: tuple[str, ...] = (\"energy\",),\n", + " system_changes: list[str] = all_changes,\n", + " ) -> None:\n", + " \"\"\"Compute the switched energy and forces.\"\"\"\n", + " super().calculate(atoms, properties, system_changes)\n", + " self.mlip.calculate(self.atoms, [\"energy\", \"forces\"], system_changes)\n", + " d = self.atoms.positions - self.r0\n", + " e_einstein = 0.5 * (self.k * (d**2).sum(1)).sum()\n", + " self.delta = self.mlip.results[\"energy\"] - e_einstein\n", + " self.results = {\n", + " \"energy\": self.lam * self.mlip.results[\"energy\"]\n", + " + (1 - self.lam) * e_einstein,\n", + " \"forces\": self.lam * self.mlip.results[\"forces\"]\n", + " - (1 - self.lam) * self.k[:, None] * d,\n", + " }\n", + "\n", + "\n", + "def einstein_free_energy(\n", + " masses: np.ndarray, springs: np.ndarray, volume: float, temperature: float\n", + ") -> float:\n", + " \"\"\"Get the classical F (eV) of the Einstein crystal with a fixed center of mass.\n", + "\n", + " It includes the term for a center of mass that is free in the volume of the\n", + " cell.\n", + " \"\"\"\n", + " kt = units.kB * temperature\n", + " hbar = constants.hbar / constants.e * units.second # eV in ASE time units\n", + " free = 3 * kt * np.log(hbar * np.sqrt(springs / masses) / kt).sum()\n", + " variance = ((masses / masses.sum()) ** 2 * kt / springs).sum()\n", + " return free + kt * np.log((2 * np.pi * variance) ** 1.5 / volume)\n", + "\n", + "\n", + "def frenkel_ladd(\n", + " frames: list[Atoms],\n", + " mlip: Calculator,\n", + " temperature: float = 100.0,\n", + " n_lambda: int = 8,\n", + " steps: tuple[int, int] = (2000, 8000),\n", + " seed: int = 103,\n", + ") -> float:\n", + " \"\"\"Get F (eV per atom) of the potential at the temperature of the frames.\n", + "\n", + " steps gives the equilibration and production steps of the MD at each\n", + " lambda.\n", + " \"\"\"\n", + " rng = np.random.default_rng(seed)\n", + " atoms = frames[0].copy()\n", + " masses = atoms.get_masses()\n", + " pos = unwrapped_positions(frames)\n", + " com = (pos * masses[None, :, None]).sum(1) / masses.sum()\n", + " pos = pos - com[:, None] + com[0]\n", + " atoms.positions = pos.mean(0)\n", + " msd = ((pos - atoms.positions) ** 2).sum(2).mean(0)\n", + " symbols = np.array(atoms.get_chemical_symbols())\n", + " springs = np.empty(len(atoms))\n", + " for element in set(symbols):\n", + " springs[symbols == element] = (\n", + " 3 * units.kB * temperature / msd[symbols == element].mean()\n", + " )\n", + " nodes, weights = np.polynomial.legendre.leggauss(n_lambda)\n", + " integral = 0.0\n", + " for node, weight in zip(nodes, weights, strict=True):\n", + " run = atoms.copy()\n", + " run.set_constraint(FixCom())\n", + " run.calc = Switched(mlip, atoms.positions.copy(), springs, (node + 1) / 2)\n", + " MaxwellBoltzmannDistribution(run, temperature_K=temperature, rng=rng)\n", + " Stationary(run)\n", + " dyn = Langevin(\n", + " run,\n", + " units.fs,\n", + " temperature_K=temperature,\n", + " friction=0.01 / units.fs,\n", + " fixcm=False,\n", + " rng=rng,\n", + " )\n", + " dyn.run(steps[0])\n", + " deltas = []\n", + " for _ in range(steps[1] // 10):\n", + " dyn.run(10)\n", + " deltas.append(run.calc.delta)\n", + " integral += weight / 2 * np.mean(deltas)\n", + " f_e = einstein_free_energy(masses, springs, atoms.get_volume(), temperature)\n", + " return (f_e + integral) / len(atoms)" + ] + }, + { + "cell_type": "markdown", + "id": "67", + "metadata": {}, + "source": [ + "We tested these functions on a periodic Cu-Ag crystal with an EMT potential at\n", + "10 K, where the harmonic free energy is exact. Frenkel-Ladd gave 0.247542 ±\n", + "0.000087 eV and the exact value is 0.247599 eV.\n", + "\n", + "The next cell runs Frenkel-Ladd on the 100 K NVT run of the loop in Section 4.\n", + "It is off by default." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "68", + "metadata": {}, + "outputs": [], + "source": [ + "RUN_FL = False\n", + "if RUN_FL:\n", + " mlip = mace_mp(**calc_kwargs(\"OMAT-0-medium\"))\n", + " frames = nvt_trajectory(\"runs/Li3PS4_OMAT-0-medium_100K_nvt\")\n", + " f_100 = frenkel_ladd(frames, mlip) # eV per atom" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "69", + "metadata": {}, + "outputs": [], + "source": [ + "PLANCK = constants.h / constants.e * 1e12 # eV/THz\n", + "\n", + "\n", + "def gibbs_helmholtz(\n", + " t0: float, f0: float, temperatures: list[float], energies: list[float]\n", + ") -> np.ndarray:\n", + " \"\"\"Get F at each temperature from F at t0 and the mean energy U.\n", + "\n", + " F and U are in eV per atom. temperatures starts at t0, and U is linear in T\n", + " between the temperatures.\n", + " \"\"\"\n", + " f_over_t = [f0 / t0]\n", + " for i in range(1, len(temperatures)):\n", + " t1, t2 = temperatures[i - 1], temperatures[i]\n", + " b = (energies[i] - energies[i - 1]) / (t2 - t1)\n", + " a = energies[i - 1] - b * t1\n", + " f_over_t.append(f_over_t[-1] - (a * (1 / t1 - 1 / t2) + b * np.log(t2 / t1)))\n", + " return np.array(f_over_t) * np.array(temperatures)\n", + "\n", + "\n", + "def quantum_correction(\n", + " nu: np.ndarray, dos: np.ndarray, temperature: float\n", + ") -> tuple[float, float]:\n", + " \"\"\"Get the quantum minus the classical harmonic F (eV) and S (eV/K) of a DOS.\n", + "\n", + " nu is in THz. The result is per formula unit for a DOS per formula unit, as\n", + " md_dos gives it. Divide by 8 for a value per atom.\n", + " \"\"\"\n", + " keep = nu > 0\n", + " nu, g, step = nu[keep], dos[keep], nu[1] - nu[0]\n", + " kt = units.kB * temperature\n", + " x = PLANCK * nu / kt\n", + " df = PLANCK * nu / 2 + kt * (np.log1p(-np.exp(-x)) - np.log(x))\n", + " ds = units.kB * (x / np.expm1(x) - np.log1p(-np.exp(-x)) - 1 + np.log(x))\n", + " return (df * g).sum() * step, (ds * g).sum() * step" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "70", + "metadata": {}, + "outputs": [], + "source": [ + "# per formula unit, at 100 to 800 K: F in kJ/mol relative to the relaxed 0 K\n", + "# energy and S in J/(K mol). From the MD in the relaxed 0 K cell (nvt) and in the\n", + "# NPT cell (npt), from the force constants fitted in the 0 K cell with U0 added,\n", + "# and from the 0 K force constants.\n", + "THERMO_T = (100, 200, 300, 400, 500, 600, 700, 800)\n", + "MD_F = {\n", + " \"nvt\": {\n", + " \"OMAT-0-medium\": (31.5, 21.2, 2.7, -22.9, -52.3, -87.4, -125.5, -167.4),\n", + " \"MATPES-PBE-0\": (27.2, 13.7, -7.6, -34.6, -67.0, -103.4, -143.5, -186.4),\n", + " \"MATPES-r2SCAN-0\": (31.2, 19.2, 0.3, -25.0, -55.6, -90.5, -129.0, -170.8),\n", + " },\n", + " \"npt\": {\n", + " \"OMAT-0-medium\": (31.1, 19.6, -0.4, -26.5, -58.7, -94.0, -134.6, -178.8),\n", + " \"MATPES-PBE-0\": (27.6, 13.6, -9.0, -36.5, -69.8, -106.9, -148.2, -192.3),\n", + " \"MATPES-r2SCAN-0\": (30.9, 18.5, -1.4, -27.5, -58.6, -94.8, -134.6, -178.4),\n", + " },\n", + "}\n", + "MD_S = {\n", + " \"nvt\": {\n", + " \"OMAT-0-medium\": (63, 150, 218, 273, 317, 363, 401, 435),\n", + " \"MATPES-PBE-0\": (79, 169, 242, 296, 343, 384, 415, 441),\n", + " \"MATPES-r2SCAN-0\": (68, 154, 221, 278, 326, 361, 400, 433),\n", + " },\n", + " \"npt\": {\n", + " \"OMAT-0-medium\": (68, 158, 230, 286, 334, 380, 419, 461),\n", + " \"MATPES-PBE-0\": (87, 178, 246, 306, 351, 392, 426, 456),\n", + " \"MATPES-r2SCAN-0\": (76, 159, 229, 284, 334, 379, 417, 449),\n", + " },\n", + "}\n", + "FIT_F = {\n", + " \"OMAT-0-medium\": (32.2, 19.7, 0.3, -36.5, -60.3, -118.8, -166.6, -219.7),\n", + " \"MATPES-PBE-0\": (27.1, 12.4, -17.5, -49.0, -95.1, -139.5, -184.4, -240.1),\n", + " \"MATPES-r2SCAN-0\": (31.3, 18.9, -0.7, -29.4, -68.5, -115.1, -168.9, -225.2),\n", + "}\n", + "FIT_S = {\n", + " \"OMAT-0-medium\": (68, 155, 223, 305, 333, 410, 452, 493),\n", + " \"MATPES-PBE-0\": (82, 179, 273, 326, 391, 433, 457, 495),\n", + " \"MATPES-r2SCAN-0\": (65, 155, 224, 288, 350, 401, 449, 489),\n", + "}\n", + "HARMONIC_F = {\n", + " \"OMAT-0-medium\": (35.4, 25.5, 8.8, -13.4, -40.1, -70.3, -103.7, -139.7),\n", + " \"MATPES-PBE-0\": (30.0, 18.0, -1.4, -26.7, -56.5, -90.1, -126.8, -166.2),\n", + " \"MATPES-r2SCAN-0\": (35.6, 26.0, 9.6, -12.3, -38.4, -68.2, -101.0, -136.5),\n", + "}\n", + "HARMONIC_S = {\n", + " \"OMAT-0-medium\": (59, 135, 197, 246, 286, 319, 348, 373),\n", + " \"MATPES-PBE-0\": (75, 160, 226, 277, 318, 352, 381, 407),\n", + " \"MATPES-r2SCAN-0\": (58, 132, 193, 241, 281, 314, 342, 367),\n", + "}\n", + "\n", + "fig, axes = plt.subplots(2, 3, figsize=(14, 7), sharex=True)\n", + "for col, model in enumerate(MODEL_FILES):\n", + " for row, (md, fit, harmonic) in enumerate(\n", + " ((MD_F, FIT_F, HARMONIC_F), (MD_S, FIT_S, HARMONIC_S))\n", + " ):\n", + " ax = axes[row, col]\n", + " ax.plot(THERMO_T, md[\"nvt\"][model], \"-o\", ms=3, label=\"MD, 0 K cell\")\n", + " ax.plot(THERMO_T, md[\"npt\"][model], \"-s\", ms=3, label=\"MD, NPT cell\")\n", + " ax.plot(THERMO_T, fit[model], \"--\", label=\"fit\")\n", + " ax.plot(\n", + " THERMO_T, harmonic[model], \":\", color=\"gray\", label=\"0 K force constants\"\n", + " )\n", + " axes[0, col].set_title(model)\n", + " axes[1, col].set_xlabel(\"Temperature (K)\")\n", + "axes[0, 0].set_ylabel(\"F (kJ/mol)\")\n", + "axes[1, 0].set_ylabel(\"S (J/(K mol))\")\n", + "axes[1, 0].legend(fontsize=8)\n", + "fig.tight_layout()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "71", + "metadata": {}, + "source": [ + "The fitted F includes U₀, the mean potential energy of its MD minus 3kT/2 per\n", + "atom. All values are per formula unit.\n", + "\n", + "- Up to 300 K the fitted F and the MD F agree to within 1 kJ/mol with\n", + " MACE-MATPES-r2SCAN-0, and to within 2.5 kJ/mol with MACE-OMAT-0-medium. Both\n", + " start from the same MD, but they get F in different ways, so the agreement\n", + " checks both. With MACE-MATPES-PBE-0 they start to differ at 300 K.\n", + "- Where Li diffuses, the fit gives too high an entropy. At 700 K the MD gives\n", + " S = 400 to 415 J/(K mol) in the 0 K cell, and the fit 449 to 457 J/(K mol).\n", + " The fit puts the Li modes at too low a frequency.\n", + "- The 0 K force constants give too low an entropy, 342 to 381 J/(K mol) at\n", + " 700 K. They miss the softening, and they leave out the imaginary modes. So\n", + " does the entropy in the Materials Project's Harmonic Phonon Database.\n", + "- The NPT cell adds 10 to 20 J/(K mol) at 700 K." + ] + }, + { + "cell_type": "markdown", + "id": "72", + "metadata": {}, + "source": [ + "## γ against β\n", + "\n", + "The free energy from the MD includes the anharmonicity, the hopping of Li and\n", + "the thermal expansion. So the phase with the lowest Gibbs free energy should be\n", + "the stable one. The temperature where two curves cross should be a transition.\n", + "\n", + "The Materials Project has no entry for γ. Its two Pnma entries, mp-985583 and\n", + "mp-1097036, are orderings of β. No entry has the framework of α. We take γ from\n", + "Kaup et al., Table S1 of the supporting information. It agrees with Homma et\n", + "al., COD 1570309. γ is ordered and needs no choice of Li sites." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "73", + "metadata": {}, + "outputs": [], + "source": [ + "from pymatgen.core import Lattice\n", + "\n", + "gamma = Structure.from_spacegroup(\n", + " \"Pmn2_1\",\n", + " Lattice.orthorhombic(7.7557, 6.5627, 6.1362),\n", + " [\"Li\", \"Li\", \"P\", \"S\", \"S\", \"S\"],\n", + " [\n", + " [0.2441, 0.3122, -0.0029],\n", + " [0, 0.1493, 0.475],\n", + " [0, 0.8174, 0.9955],\n", + " [0.2177, 0.6717, 0.8864],\n", + " [0, 0.1115, 0.8935],\n", + " [0, 0.8094, 0.3274],\n", + " ],\n", + ")\n", + "GAMMA_SUPERCELL = (2, 2, 2) # 128 atoms\n", + "gamma.composition, gamma.get_space_group_info()" + ] + }, + { + "cell_type": "markdown", + "id": "74", + "metadata": {}, + "source": [ + "At 0 K all three potentials put γ below β. β lies 11.9 meV/atom higher with\n", + "MACE-MATPES-PBE-0, 10.5 with MACE-MATPES-r2SCAN-0 and 4.7 with\n", + "MACE-OMAT-0-medium. For β to become stable, its entropy has to make up\n", + "this difference.\n", + "\n", + "We run γ with the NPT MD at the same temperatures and with Frenkel-Ladd at\n", + "100 K, as for β. The loop is off by default." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "75", + "metadata": {}, + "outputs": [], + "source": [ + "RUN_GAMMA = False\n", + "gamma_docs = {}\n", + "if RUN_GAMMA:\n", + " for model in MODEL_FILES:\n", + " for temperature in LI3PS4_TEMPERATURES:\n", + " gamma_docs[model, temperature] = run_ft(\n", + " gamma,\n", + " GAMMA_SUPERCELL,\n", + " model,\n", + " f\"runs/gamma_{model}_{temperature}K_npt\",\n", + " temperature,\n", + " relax=True,\n", + " run_npt=True,\n", + " )" + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "76", + "metadata": {}, + "outputs": [], + "source": [ + "# G(beta) - G(gamma) in meV/atom and S of each phase in J/(K mol) per formula\n", + "# unit, at 100 to 800 K and zero pressure, with the quantum correction\n", + "PHASE_T = (100, 200, 300, 400, 500, 600, 700, 800)\n", + "DELTA_G = {\n", + " \"OMAT-0-medium\": (-0.3, -1.8, -3.6, -5.1, -6.6, -7.3, -6.9, -4.9),\n", + " \"MATPES-PBE-0\": (7.1, 5.5, 3.4, 1.1, -1.1, -2.2, -1.9, -0.4),\n", + " \"MATPES-r2SCAN-0\": (3.0, 1.6, -0.5, -2.4, -4.6, -7.2, -9.5, -10.5),\n", + "}\n", + "PHASE_S = {\n", + " \"gamma\": {\n", + " \"OMAT-0-medium\": (80, 156, 222, 278, 327, 380, 430, 484),\n", + " \"MATPES-PBE-0\": (92, 172, 238, 292, 340, 391, 436, 474),\n", + " \"MATPES-r2SCAN-0\": (79, 154, 219, 273, 319, 360, 403, 450),\n", + " },\n", + " \"beta\": {\n", + " \"OMAT-0-medium\": (90, 168, 235, 290, 338, 383, 422, 463),\n", + " \"MATPES-PBE-0\": (103, 188, 255, 311, 355, 395, 429, 458),\n", + " \"MATPES-r2SCAN-0\": (91, 169, 235, 288, 337, 382, 419, 451),\n", + " },\n", + "}\n", + "\n", + "fig, axes = plt.subplots(1, 2, figsize=(12, 3.8))\n", + "for ax in axes:\n", + " ax.axvspan(523, 573, color=\"0.9\")\n", + "axes[0].axhline(0, color=\"gray\", lw=0.5)\n", + "for idx, model in enumerate(MODEL_FILES):\n", + " axes[0].plot(PHASE_T, DELTA_G[model], \"-o\", color=f\"C{idx}\", ms=3, label=model)\n", + " for phase, style in ((\"gamma\", \"--\"), (\"beta\", \"-\")):\n", + " axes[1].plot(PHASE_T, PHASE_S[phase][model], style, color=f\"C{idx}\")\n", + "axes[0].set_ylabel(\"G(beta) - G(gamma) (meV/atom)\")\n", + "axes[1].set_ylabel(\"S (J/(K mol)), beta solid, gamma dashed\")\n", + "for ax in axes:\n", + " ax.set_xlabel(\"Temperature (K)\")\n", + "axes[0].legend(fontsize=8)\n", + "fig.tight_layout()\n", + "plt.show()" + ] + }, + { + "cell_type": "markdown", + "id": "77", + "metadata": {}, + "source": [ + "G(β) crosses G(γ) at 278 K with MACE-MATPES-r2SCAN-0 and at 450 K with\n", + "MACE-MATPES-PBE-0. In experiment γ turns into β at 523 to 573 K. With\n", + "MACE-OMAT-0-medium, G(β) is already 0.3 meV/atom below G(γ) at 100 K, so there\n", + "is no crossing in our range. MACE-MATPES-PBE-0 gives a second crossing at\n", + "822 K. The framework of γ already flows there, so it does not count.\n", + "\n", + "- At 100 K the classical F of β lies above that of γ by 0.2 meV/atom with\n", + " MACE-OMAT-0-medium, 7.9 with MACE-MATPES-PBE-0 and 4.1 with\n", + " MACE-MATPES-r2SCAN-0. This is much less than the gap at 0 K. β has softer\n", + " modes, so its vibrations lower its free energy more.\n", + "- At 300 K the entropy of β is 13 to 17 J/(K mol) higher than that of γ.\n", + "- The quantum correction is 17 to 21 meV/atom for each phase at 100 K and\n", + " about 5 meV/atom at 500 K. Most of it cancels in G(β) - G(γ). It lowers the\n", + " difference by 0.5 to 1.1 meV/atom at 100 K and by 0.1 to 0.2 meV/atom at\n", + " 500 K.\n", + "- Each Frenkel-Ladd F has an error of about 0.1 meV/atom, from the spread of\n", + " ⟨U_MLIP - U_E⟩ at each λ. The center-of-mass term of F_E is -1.3 meV/atom.\n", + " Both supercells have 128 atoms and nearly the same springs, so this term\n", + " changes G(β) - G(γ) by only 0.02 meV/atom." + ] + }, + { + "cell_type": "markdown", + "id": "78", + "metadata": {}, + "source": [ + "## What this approach cannot do\n", + "\n", + "- **The free energy of α, and so the β to α transition.** Frenkel-Ladd needs a\n", + " structure that is stable at its starting temperature. α exists only with its\n", + " Li disorder. We relaxed 100 orderings of its Li sites with each potential.\n", + " In about 90 of them the PS4 units rotate into a distorted structure that\n", + " matches none of the known phases. The lowest lie 18 to 22 meV/atom above γ.\n", + " So ordered α is not a sound start at 100 K. α needs another method, for\n", + " example a cluster expansion for the Li disorder together with the vibrations.\n", + "- **Melting.** Its free energy needs a reference for the liquid, which\n", + " Frenkel-Ladd does not give.\n", + "- **Hysteresis.** In experiment the transitions happen at different\n", + " temperatures on heating and on cooling. The free energies only give the\n", + " temperature where two phases have the same G. Which phase forms depends also\n", + " on how fast the atoms rearrange.\n", + "\n", + "## Limits of the γ to β temperature\n", + "\n", + "- **The potentials.** γ and β differ by 5 to 12 meV/atom at 0 K, about the\n", + " size of the errors of these potentials. The transition temperature depends on\n", + " this difference, so it can shift by hundreds of kelvin between potentials.\n", + " Kam et al. computed the transitions with DFT, with the vibrational and the\n", + " configurational entropy (arXiv:2307.00878). With r²SCAN they found them 200\n", + " to 300 K below experiment. MACE-MATPES-r2SCAN-0 gives 250 to 300 K below\n", + " experiment. With PBE they found γ never stable. MACE-MATPES-PBE-0 instead\n", + " puts γ below β up to 450 K.\n", + "- **The Li disorder of β.** The MD only samples the disorder that the Li atoms\n", + " reach in 8 ps. Below about 500 K only a few Li hop, so the MD misses part of\n", + " the configurational entropy of β. Its free energy is then too high, which\n", + " moves the transition up.\n", + "- **One ordering of β.** We start from mp-985583. Other orderings start from a\n", + " different energy.\n", + "- **Classical nuclei.** The quantum correction uses a harmonic formula on the\n", + " MD DOS. It is exact only for harmonic vibrations. Its effect on G(β) - G(γ)\n", + " is 1.1 meV/atom or less, and 0.2 meV/atom or less from 500 K.\n", + "- **Size and length.** 128 atoms and 8 ps of MD." + ] + }, + { + "cell_type": "markdown", + "id": "79", + "metadata": {}, "source": [ "## Known limitations\n", "\n", From 24574391b8dafd870f48e2d8f3d5f32cdfc7687f Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 17:23:17 -0700 Subject: [PATCH 41/43] Show the tutorial figures and tables without running the notebook --- tutorials/finite_temperature_phonons.ipynb | 263 +++++++++++++----- .../s1_bands_AlAsPt5.png | Bin 0 -> 106556 bytes .../s1_bands_Bi4S3N2.png | Bin 0 -> 98076 bytes .../s1_bands_Ca3Ir4Sn13.png | Bin 0 -> 114542 bytes .../s1_bands_Er5Tl3.png | Bin 0 -> 117950 bytes .../s1_bands_Zn3P2.png | Bin 0 -> 105143 bytes .../s1_ca3ir4sn13_300k.png | Bin 0 -> 81866 bytes .../s1_max_frequency.png | Bin 0 -> 32359 bytes .../s2_max_frequency.png | Bin 0 -> 71198 bytes .../s2_volume.png | Bin 0 -> 32016 bytes .../s3_knaicl_grid.png | Bin 0 -> 18283 bytes .../s4_bands_MATPES-PBE-0.png | Bin 0 -> 102289 bytes .../s4_bands_MATPES-r2SCAN-0.png | Bin 0 -> 95989 bytes .../s4_bands_OMAT-0-medium.png | Bin 0 -> 101828 bytes .../s4_runs.png | Bin 0 -> 35203 bytes .../s5_diffusion.png | Bin 0 -> 19781 bytes .../s5_phases.png | Bin 0 -> 23973 bytes .../s5_thermo.png | Bin 0 -> 45142 bytes .../s5_vdos.png | Bin 0 -> 23891 bytes 19 files changed, 187 insertions(+), 76 deletions(-) create mode 100644 tutorials/finite_temperature_phonons_figures/s1_bands_AlAsPt5.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_bands_Bi4S3N2.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_bands_Ca3Ir4Sn13.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_bands_Er5Tl3.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_bands_Zn3P2.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_ca3ir4sn13_300k.png create mode 100644 tutorials/finite_temperature_phonons_figures/s1_max_frequency.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_max_frequency.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_volume.png create mode 100644 tutorials/finite_temperature_phonons_figures/s3_knaicl_grid.png create mode 100644 tutorials/finite_temperature_phonons_figures/s4_bands_MATPES-PBE-0.png create mode 100644 tutorials/finite_temperature_phonons_figures/s4_bands_MATPES-r2SCAN-0.png create mode 100644 tutorials/finite_temperature_phonons_figures/s4_bands_OMAT-0-medium.png create mode 100644 tutorials/finite_temperature_phonons_figures/s4_runs.png create mode 100644 tutorials/finite_temperature_phonons_figures/s5_diffusion.png create mode 100644 tutorials/finite_temperature_phonons_figures/s5_phases.png create mode 100644 tutorials/finite_temperature_phonons_figures/s5_thermo.png create mode 100644 tutorials/finite_temperature_phonons_figures/s5_vdos.png diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index c3b02ade7e..093171a338 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -510,6 +510,8 @@ "id": "20", "metadata": {}, "source": [ + "![Band structure and DOS of Ca3Ir4Sn13 at 0 K and at 300 K](finite_temperature_phonons_figures/s1_ca3ir4sn13_300k.png)\n", + "\n", "At 0 K, Ca3Ir4Sn13 has imaginary modes down to about -0.75 THz. At 300 K they\n", "are gone. The motion of the atoms at 300 K stabilizes them.\n", "\n", @@ -678,6 +680,24 @@ "cell_type": "markdown", "id": "25", "metadata": {}, + "source": [ + "The figures below show our runs.\n", + "\n", + "![Band structures of Ca3Ir4Sn13 at 100, 500 and 900 K](finite_temperature_phonons_figures/s1_bands_Ca3Ir4Sn13.png)\n", + "\n", + "![Band structures of AlAsPt5 at 100, 500 and 900 K](finite_temperature_phonons_figures/s1_bands_AlAsPt5.png)\n", + "\n", + "![Band structures of Zn3P2 at 100, 500 and 900 K](finite_temperature_phonons_figures/s1_bands_Zn3P2.png)\n", + "\n", + "![Band structures of Bi4S3N2 at 100, 500 and 900 K](finite_temperature_phonons_figures/s1_bands_Bi4S3N2.png)\n", + "\n", + "![Band structures of Er5Tl3 at 100, 500 and 900 K](finite_temperature_phonons_figures/s1_bands_Er5Tl3.png)" + ] + }, + { + "cell_type": "markdown", + "id": "26", + "metadata": {}, "source": [ "## Our results\n", "\n", @@ -689,7 +709,7 @@ { "cell_type": "code", "execution_count": null, - "id": "26", + "id": "27", "metadata": {}, "outputs": [], "source": [ @@ -781,9 +801,19 @@ }, { "cell_type": "markdown", - "id": "27", + "id": "28", "metadata": {}, "source": [ + "![Highest frequency against temperature](finite_temperature_phonons_figures/s1_max_frequency.png)\n", + "\n", + "| Material | OMAT-0-medium | MATPES-PBE-0 | MATPES-r2SCAN-0 | AIMD highest frequency (THz) |\n", + "|---|---|---|---|---|\n", + "| Ca3Ir4Sn13 | 0.07 | 0.17 | 0.10 | 6.03 |\n", + "| AlAsPt5 | 0.11 | 0.19 | 0.17 | 7.79 |\n", + "| Zn3P2 | 0.21 | 0.10 | 0.44 | 10.09 |\n", + "| Bi4S3N2 | 0.15 | 0.46 | 0.16 | 17.03 |\n", + "| Er5Tl3 | 0.18 | 0.17 | 0.13 | 3.97 |\n", + "\n", "The table gives the mean absolute difference from the AIMD reference at 300 K\n", "in THz, over all branches and q-points of the band path.\n", "\n", @@ -824,7 +854,7 @@ }, { "cell_type": "markdown", - "id": "28", + "id": "29", "metadata": {}, "source": [ "## 2. Thermal expansion with an NPT MD\n", @@ -858,7 +888,7 @@ { "cell_type": "code", "execution_count": null, - "id": "29", + "id": "30", "metadata": {}, "outputs": [], "source": [ @@ -889,7 +919,7 @@ }, { "cell_type": "markdown", - "id": "30", + "id": "31", "metadata": {}, "source": [ "Our run took 19 minutes. The NPT MD and the NVT MD took about 8 minutes each\n", @@ -902,7 +932,7 @@ }, { "cell_type": "markdown", - "id": "31", + "id": "32", "metadata": {}, "source": [ "## The other temperatures, potentials and materials\n", @@ -917,7 +947,7 @@ { "cell_type": "code", "execution_count": null, - "id": "32", + "id": "33", "metadata": {}, "outputs": [], "source": [ @@ -942,7 +972,7 @@ }, { "cell_type": "markdown", - "id": "33", + "id": "34", "metadata": {}, "source": [ "## Our results\n", @@ -957,7 +987,7 @@ { "cell_type": "code", "execution_count": null, - "id": "34", + "id": "35", "metadata": {}, "outputs": [], "source": [ @@ -1093,9 +1123,13 @@ }, { "cell_type": "markdown", - "id": "35", + "id": "36", "metadata": {}, "source": [ + "![Volume against temperature](finite_temperature_phonons_figures/s2_volume.png)\n", + "\n", + "![Highest frequency in three cells](finite_temperature_phonons_figures/s2_max_frequency.png)\n", + "\n", "We do not compare these runs with the AIMD reference. It used the PBEsol cell\n", "at every temperature.\n", "\n", @@ -1155,7 +1189,7 @@ }, { "cell_type": "markdown", - "id": "36", + "id": "37", "metadata": {}, "source": [ "## 3. MD length and number of snapshots for KNaICl\n", @@ -1178,7 +1212,7 @@ { "cell_type": "code", "execution_count": null, - "id": "37", + "id": "38", "metadata": {}, "outputs": [], "source": [ @@ -1203,7 +1237,7 @@ { "cell_type": "code", "execution_count": null, - "id": "38", + "id": "39", "metadata": {}, "outputs": [], "source": [ @@ -1268,9 +1302,23 @@ }, { "cell_type": "markdown", - "id": "39", + "id": "40", "metadata": {}, "source": [ + "![Difference from AIMD against MD length and snapshots](finite_temperature_phonons_figures/s3_knaicl_grid.png)\n", + "\n", + "| Potential | MD length | 25 snapshots | 50 snapshots | 100 snapshots |\n", + "|---|---|---|---|---|\n", + "| OMAT-0-medium | 4 ps | 5.48 | 5.52 | 5.66 |\n", + "| OMAT-0-medium | 8 ps | 5.35 | 5.56 | 5.63 |\n", + "| OMAT-0-medium | 16 ps | 5.57 | 5.62 | 5.61 |\n", + "| MATPES-PBE-0 | 4 ps | 5.20 | 5.18 | 5.13 |\n", + "| MATPES-PBE-0 | 8 ps | 5.07 | 5.22 | 5.33 |\n", + "| MATPES-PBE-0 | 16 ps | 5.05 | 5.31 | 5.24 |\n", + "| MATPES-r2SCAN-0 | 4 ps | 5.64 | 5.51 | 5.57 |\n", + "| MATPES-r2SCAN-0 | 8 ps | 5.32 | 5.58 | 5.42 |\n", + "| MATPES-r2SCAN-0 | 16 ps | 5.42 | 5.53 | 5.53 |\n", + "\n", "In the plot, a star marks a run with imaginary modes on the band path. The\n", "table gives the highest frequency in THz.\n", "\n", @@ -1302,7 +1350,7 @@ }, { "cell_type": "markdown", - "id": "40", + "id": "41", "metadata": {}, "source": [ "## 4. Li3PS4, a crystal that is unstable at 0 K\n", @@ -1325,7 +1373,7 @@ { "cell_type": "code", "execution_count": null, - "id": "41", + "id": "42", "metadata": {}, "outputs": [], "source": [ @@ -1337,7 +1385,7 @@ }, { "cell_type": "markdown", - "id": "42", + "id": "43", "metadata": {}, "source": [ "## Phonons at 0 K\n", @@ -1351,7 +1399,7 @@ { "cell_type": "code", "execution_count": null, - "id": "43", + "id": "44", "metadata": {}, "outputs": [], "source": [ @@ -1384,7 +1432,7 @@ }, { "cell_type": "markdown", - "id": "44", + "id": "45", "metadata": {}, "source": [ "Our run took 2 minutes. The lowest frequency is -2.59 THz. With\n", @@ -1393,7 +1441,7 @@ }, { "cell_type": "markdown", - "id": "45", + "id": "46", "metadata": {}, "source": [ "## One temperature\n", @@ -1404,7 +1452,7 @@ { "cell_type": "code", "execution_count": null, - "id": "46", + "id": "47", "metadata": {}, "outputs": [], "source": [ @@ -1428,7 +1476,7 @@ }, { "cell_type": "markdown", - "id": "47", + "id": "48", "metadata": {}, "source": [ "Our run took 31 minutes. The volume grows from 664.8 to 698.5 ų. The lowest\n", @@ -1439,7 +1487,7 @@ }, { "cell_type": "markdown", - "id": "48", + "id": "49", "metadata": {}, "source": [ "## The other temperatures and potentials\n", @@ -1451,7 +1499,7 @@ { "cell_type": "code", "execution_count": null, - "id": "49", + "id": "50", "metadata": {}, "outputs": [], "source": [ @@ -1475,51 +1523,66 @@ }, { "cell_type": "markdown", - "id": "50", + "id": "51", "metadata": {}, "source": [ - "The next cell plots the bands of one potential from 0 to 1000 K. Every run\n", - "keeps the Pnma symmetry, so all runs of a potential have the band path of its\n", - "0 K run. Their q-points are the same in reduced coordinates. The cells differ a\n", - "little, so we plot every run along the distances of the 0 K path." + "The next cell plots the bands of one potential at 0, 300 and 700 K, in the\n", + "relaxed 0 K cell (NVT) and in the NPT cell. Every run keeps the Pnma symmetry,\n", + "so all runs of a potential have the band path of its 0 K run. Their q-points\n", + "are the same in reduced coordinates. The cells differ a little, so we plot\n", + "every run along the distances of the 0 K path." ] }, { "cell_type": "code", "execution_count": null, - "id": "51", + "id": "52", "metadata": {}, "outputs": [], "source": [ - "def plot_li3ps4_bands(model: str, label: str) -> None:\n", - " \"\"\"Plot the bands of one potential from 0 to 1000 K on its 0 K band path.\"\"\"\n", + "def plot_li3ps4_bands(model: str) -> None:\n", + " \"\"\"Plot the bands of one potential at 0, 300 and 700 K, in both cells.\"\"\"\n", " reference = li3ps4_docs[model, 0, \"harmonic\"].phonon_bandstructure\n", - " _, ax = plt.subplots(figsize=(8, 4))\n", - " for temperature in LI3PS4_TEMPERATURES:\n", - " plot_bands(\n", - " ax,\n", - " li3ps4_docs[model, temperature, label].phonon_bandstructure,\n", - " label=f\"{temperature} K\",\n", - " distance=reference.distance,\n", - " color=plt.cm.viridis(temperature / 1000),\n", - " lw=0.4,\n", - " )\n", - " plot_bands(ax, reference, label=\"0 K\", color=\"black\", lw=0.6)\n", - " ax.set_ylabel(\"Frequency (THz)\")\n", - " ax.set_title(f\"{model}, {label.upper()}\")\n", - " ax.legend(fontsize=7, ncol=2)\n", + " _, axes = plt.subplots(1, 2, figsize=(14, 4), sharey=True)\n", + " for ax, label in zip(axes, (\"nvt\", \"npt\"), strict=True):\n", + " plot_bands(ax, reference, label=\"0 K\", color=\"gray\", lw=0.5)\n", + " for temperature, color in ((300, \"C0\"), (700, \"C3\")):\n", + " plot_bands(\n", + " ax,\n", + " li3ps4_docs[model, temperature, label].phonon_bandstructure,\n", + " label=f\"{temperature} K\",\n", + " distance=reference.distance,\n", + " color=color,\n", + " lw=0.5,\n", + " )\n", + " ax.set_title(f\"{model}, {label.upper()}\")\n", + " axes[0].set_ylabel(\"Frequency (THz)\")\n", + " axes[1].legend(fontsize=8)\n", " plt.show()\n", "\n", "\n", "if RUN_LI3PS4:\n", " for model in MODEL_FILES:\n", - " for label in (\"nvt\", \"npt\"):\n", - " plot_li3ps4_bands(model, label)" + " plot_li3ps4_bands(model)" ] }, { "cell_type": "markdown", - "id": "52", + "id": "53", + "metadata": {}, + "source": [ + "The figures below show our runs.\n", + "\n", + "![Band structures of Li3PS4 with OMAT-0-medium at 0, 300 and 700 K](finite_temperature_phonons_figures/s4_bands_OMAT-0-medium.png)\n", + "\n", + "![Band structures of Li3PS4 with MATPES-PBE-0 at 0, 300 and 700 K](finite_temperature_phonons_figures/s4_bands_MATPES-PBE-0.png)\n", + "\n", + "![Band structures of Li3PS4 with MATPES-r2SCAN-0 at 0, 300 and 700 K](finite_temperature_phonons_figures/s4_bands_MATPES-r2SCAN-0.png)" + ] + }, + { + "cell_type": "markdown", + "id": "54", "metadata": {}, "source": [ "## Our results\n", @@ -1532,7 +1595,7 @@ { "cell_type": "code", "execution_count": null, - "id": "53", + "id": "55", "metadata": {}, "outputs": [], "source": [ @@ -1593,9 +1656,11 @@ }, { "cell_type": "markdown", - "id": "54", + "id": "56", "metadata": {}, "source": [ + "![Lowest frequency, Lindemann ratio and volume of Li3PS4](finite_temperature_phonons_figures/s4_runs.png)\n", + "\n", "- The imaginary modes of 0 K shrink at finite temperature, but they do not go\n", " away. The lowest frequency lies between -0.2 and -2.2 THz in every run but\n", " one. MACE-MATPES-r2SCAN-0 in the NPT cell at 400 K has no imaginary modes.\n", @@ -1614,7 +1679,7 @@ }, { "cell_type": "markdown", - "id": "55", + "id": "57", "metadata": {}, "source": [ "## 5. When light atoms hop: Li3PS4 above 300 K\n", @@ -1642,7 +1707,7 @@ { "cell_type": "code", "execution_count": null, - "id": "56", + "id": "58", "metadata": {}, "outputs": [], "source": [ @@ -1679,7 +1744,7 @@ }, { "cell_type": "markdown", - "id": "57", + "id": "59", "metadata": {}, "source": [ "## Which atoms move\n", @@ -1692,7 +1757,7 @@ { "cell_type": "code", "execution_count": null, - "id": "58", + "id": "60", "metadata": {}, "outputs": [], "source": [ @@ -1728,7 +1793,7 @@ { "cell_type": "code", "execution_count": null, - "id": "59", + "id": "61", "metadata": {}, "outputs": [], "source": [ @@ -1781,9 +1846,19 @@ }, { "cell_type": "markdown", - "id": "60", + "id": "62", "metadata": {}, "source": [ + "![Diffusion coefficients of Li3PS4](finite_temperature_phonons_figures/s5_diffusion.png)\n", + "\n", + "D of Li in 10⁻⁶ cm²/s, in the relaxed 0 K cell:\n", + "\n", + "| Potential | 300 K | 400 K | 500 K | 600 K | 700 K | 800 K | 900 K | 1000 K |\n", + "|---|---|---|---|---|---|---|---|---|\n", + "| OMAT-0-medium | -0.4 | 2.0 | 0.0 | 7.6 | 8.0 | 5.0 | 31.0 | 47.0 |\n", + "| MATPES-PBE-0 | 1.9 | 3.0 | 6.3 | 15.0 | 26.0 | 29.0 | 46.0 | 64.0 |\n", + "| MATPES-r2SCAN-0 | 1.6 | 0.8 | 2.6 | 4.8 | 6.8 | 26.0 | 38.0 | 34.0 |\n", + "\n", "A D below about 3×10⁻⁷ cm²/s is noise in these 7 ps runs. P and S stay near\n", "that level up to 700 K.\n", "\n", @@ -1807,7 +1882,7 @@ }, { "cell_type": "markdown", - "id": "61", + "id": "63", "metadata": {}, "source": [ "## The vibrational DOS from the velocities\n", @@ -1827,7 +1902,7 @@ { "cell_type": "code", "execution_count": null, - "id": "62", + "id": "64", "metadata": {}, "outputs": [], "source": [ @@ -1864,7 +1939,7 @@ { "cell_type": "code", "execution_count": null, - "id": "63", + "id": "65", "metadata": {}, "outputs": [], "source": [ @@ -1901,9 +1976,25 @@ }, { "cell_type": "markdown", - "id": "64", + "id": "66", "metadata": {}, "source": [ + "![Li DOS below 5 THz and P-S stretch, MD against fit](finite_temperature_phonons_figures/s5_vdos.png)\n", + "\n", + "Li DOS below 5 THz and P-S stretch, in the relaxed 0 K cell:\n", + "\n", + "| Potential | T (K) | Li DOS below 5 THz, MD | fit | P-S stretch (THz), MD | fit |\n", + "|---|---|---|---|---|---|\n", + "| OMAT-0-medium | 300 | 15% | 18% | 16.4 | 15.9 |\n", + "| OMAT-0-medium | 500 | 18% | 27% | 16.0 | 15.2 |\n", + "| OMAT-0-medium | 700 | 23% | 90% | 16.4 | 12.9 |\n", + "| MATPES-PBE-0 | 300 | 21% | 53% | 14.6 | 13.8 |\n", + "| MATPES-PBE-0 | 500 | 23% | 98% | 15.0 | 12.4 |\n", + "| MATPES-PBE-0 | 700 | 25% | 100% | 15.0 | 12.0 |\n", + "| MATPES-r2SCAN-0 | 300 | 14% | 19% | 16.3 | 16.1 |\n", + "| MATPES-r2SCAN-0 | 500 | 17% | 41% | 16.3 | 15.2 |\n", + "| MATPES-r2SCAN-0 | 700 | 21% | 99% | 16.3 | 13.2 |\n", + "\n", "The fitted DOS is smeared with the same 0.15 THz as the MD DOS.\n", "\n", "- At 300 K, with MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0, 14 to 19% of the\n", @@ -1920,7 +2011,7 @@ }, { "cell_type": "markdown", - "id": "65", + "id": "67", "metadata": {}, "source": [ "## The free energy from the MD\n", @@ -1958,7 +2049,7 @@ { "cell_type": "code", "execution_count": null, - "id": "66", + "id": "68", "metadata": {}, "outputs": [], "source": [ @@ -2078,7 +2169,7 @@ }, { "cell_type": "markdown", - "id": "67", + "id": "69", "metadata": {}, "source": [ "We tested these functions on a periodic Cu-Ag crystal with an EMT potential at\n", @@ -2092,7 +2183,7 @@ { "cell_type": "code", "execution_count": null, - "id": "68", + "id": "70", "metadata": {}, "outputs": [], "source": [ @@ -2106,7 +2197,7 @@ { "cell_type": "code", "execution_count": null, - "id": "69", + "id": "71", "metadata": {}, "outputs": [], "source": [ @@ -2150,7 +2241,7 @@ { "cell_type": "code", "execution_count": null, - "id": "70", + "id": "72", "metadata": {}, "outputs": [], "source": [ @@ -2227,9 +2318,19 @@ }, { "cell_type": "markdown", - "id": "71", + "id": "73", "metadata": {}, "source": [ + "![Free energy and entropy of Li3PS4](finite_temperature_phonons_figures/s5_thermo.png)\n", + "\n", + "S at 700 K in J/(K mol) per formula unit:\n", + "\n", + "| Potential | MD, 0 K cell | MD, NPT cell | fit | 0 K force constants |\n", + "|---|---|---|---|---|\n", + "| OMAT-0-medium | 401 | 419 | 452 | 348 |\n", + "| MATPES-PBE-0 | 415 | 426 | 457 | 381 |\n", + "| MATPES-r2SCAN-0 | 400 | 417 | 449 | 342 |\n", + "\n", "The fitted F includes U₀, the mean potential energy of its MD minus 3kT/2 per\n", "atom. All values are per formula unit.\n", "\n", @@ -2248,7 +2349,7 @@ }, { "cell_type": "markdown", - "id": "72", + "id": "74", "metadata": {}, "source": [ "## γ against β\n", @@ -2266,7 +2367,7 @@ { "cell_type": "code", "execution_count": null, - "id": "73", + "id": "75", "metadata": {}, "outputs": [], "source": [ @@ -2291,7 +2392,7 @@ }, { "cell_type": "markdown", - "id": "74", + "id": "76", "metadata": {}, "source": [ "At 0 K all three potentials put γ below β. β lies 11.9 meV/atom higher with\n", @@ -2306,7 +2407,7 @@ { "cell_type": "code", "execution_count": null, - "id": "75", + "id": "77", "metadata": {}, "outputs": [], "source": [ @@ -2329,7 +2430,7 @@ { "cell_type": "code", "execution_count": null, - "id": "76", + "id": "78", "metadata": {}, "outputs": [], "source": [ @@ -2373,9 +2474,19 @@ }, { "cell_type": "markdown", - "id": "77", + "id": "79", "metadata": {}, "source": [ + "![G(beta) - G(gamma) and entropies](finite_temperature_phonons_figures/s5_phases.png)\n", + "\n", + "G(β) - G(γ) in meV/atom:\n", + "\n", + "| Potential | 100 K | 200 K | 300 K | 400 K | 500 K | 600 K | 700 K | 800 K |\n", + "|---|---|---|---|---|---|---|---|---|\n", + "| OMAT-0-medium | -0.3 | -1.8 | -3.6 | -5.1 | -6.6 | -7.3 | -6.9 | -4.9 |\n", + "| MATPES-PBE-0 | 7.1 | 5.5 | 3.4 | 1.1 | -1.1 | -2.2 | -1.9 | -0.4 |\n", + "| MATPES-r2SCAN-0 | 3.0 | 1.6 | -0.5 | -2.4 | -4.6 | -7.2 | -9.5 | -10.5 |\n", + "\n", "G(β) crosses G(γ) at 278 K with MACE-MATPES-r2SCAN-0 and at 450 K with\n", "MACE-MATPES-PBE-0. In experiment γ turns into β at 523 to 573 K. With\n", "MACE-OMAT-0-medium, G(β) is already 0.3 meV/atom below G(γ) at 100 K, so there\n", @@ -2399,7 +2510,7 @@ }, { "cell_type": "markdown", - "id": "78", + "id": "80", "metadata": {}, "source": [ "## What this approach cannot do\n", @@ -2442,7 +2553,7 @@ }, { "cell_type": "markdown", - "id": "79", + "id": "81", "metadata": {}, "source": [ "## Known limitations\n", diff --git a/tutorials/finite_temperature_phonons_figures/s1_bands_AlAsPt5.png b/tutorials/finite_temperature_phonons_figures/s1_bands_AlAsPt5.png new file mode 100644 index 0000000000000000000000000000000000000000..c8ad751da72f6f319d74549ba81f5e7a15572e54 GIT binary patch literal 106556 zcmb4qbx<5YvuChiAvgqgx1d26cMTrgA-Fp%?(Xic!QEwXC%DVv?y_9I_wMSd?yq-K zT{BZtzv=3+>h9^8a3uvv6eN74PoF-aNK1(+fBFOi{`3jT4guz03yF>l#=nM7N^+{= zA0Ho(|D<;a74eSdj-d3k$&{zuPm zPcKi8uaK8($nyo{=@jyK^z!uZdjE8P{|tFJfZXpw?zZ0Uk6v%??r$ERFK(aCZXQmr zudg33FYnLK?oLl`A-C(0n`Ow=0_1WAaxw9KJ^?u!hMe?2fUoa%FYfnu-oU-bN7sjk 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z^{C+6rYOPqA?LDW;#&SX@rOvYtMNj(ScPbVyS&z}k;cz*v0d?-amr{4g~lM4uAn6a-8!+t9&@r;qHq)iDuY*5=5KN=xr%?g7Vr#CO01d4Sb zdVHrKc)?KJ_m(7&3K)JdP09F)FrIh3Me#;;jB2{j_g3oDxxNB4U`3%*2y#uYT%5dd zBXrw#Z0-QHS#7c3b%bh=WvlBao@*2rSF)*U`Cvw^MsM+@n#HxE@CiR*NZ#>5z!^FJjtNQRNEz3Z71MOmy0f7r z6mh&)^1Gib-Vzuv-( z4Fb}!BWH)2D&8PMwtqCX(rluTlZ|;T0@>3yHrf}nx8>O2)IwKj%6t2#A6ilZpz%M; zT<;he(GQ!IL{=>wKVo!6F|9k#2nQ}PzcZN-F=z4VFutt)Ql{7zWyxg84#Y&!i~Otq lx&HT};s1I{!rgwvN{z1SZf4l!L=i*-RFyOpE9IeK{{@PdwX^^L literal 0 HcmV?d00001 From 8f48c987d1b451acfa0039bd220af84002f4931a Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 17:42:27 -0700 Subject: [PATCH 42/43] Shorten the text of the finite-temperature phonon tutorial --- tutorials/finite_temperature_phonons.ipynb | 992 +++++++-------------- 1 file changed, 313 insertions(+), 679 deletions(-) diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 093171a338..419290f044 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -7,22 +7,21 @@ "source": [ "# Finite-temperature phonons with pheasy and machine-learned potentials\n", "\n", - "This notebook computes phonons at a finite temperature with the\n", - "`ForceFieldFiniteTemperaturePhononMaker` workflow. The forces come from three\n", - "MACE potentials, so no DFT is needed.\n", + "This notebook runs `ForceFieldFiniteTemperaturePhononMaker` with three MACE\n", + "potentials. The workflow fits effective harmonic force constants to MD\n", + "snapshots at a given temperature. The workflow is new and less tested than the\n", + "other phonon workflows, so its defaults may still change.\n", "\n", - "Section 1 runs five materials at 100, 300, 500, 700 and 900 K, in the 0 K cell.\n", - "Ca3Ir4Sn13 is worked through step by step. Section 2 runs the same materials in\n", - "the cell at each temperature, found with an NPT MD. Section 3 tests the length\n", - "of the MD and the number of snapshots for KNaICl.\n", + "## Contents\n", "\n", - "Section 4 runs Li3PS4, a lithium conductor whose crystal is unstable at 0 K, from\n", - "100 to 1000 K. Section 5 shows what to do once its Li atoms start to hop. It\n", - "computes the vibrational DOS and the free energy from the MD, and compares the\n", - "free energies of two of its phases.\n", + "1. Five materials from 100 to 900 K\n", + "2. Thermal expansion with an NPT MD\n", + "3. MD length and number of snapshots\n", + "4. Li3PS4, a crystal that is unstable at 0 K\n", + "5. Li3PS4 with hopping Li: diffusion, DOS and free energies from the MD\n", + "6. Known limitations\n", "\n", - "This workflow is new. It is less tested than the other phonon workflows in\n", - "atomate2, and its defaults and output may still change." + "The long runs are switched off. Our results are shown as figures and tables." ] }, { @@ -30,48 +29,25 @@ "id": "1", "metadata": {}, "source": [ - "## Background\n", - "\n", - "Harmonic phonons from finite displacements describe the crystal at 0 K. Many\n", - "materials have imaginary modes at 0 K. The anharmonic motion of the atoms can\n", - "stabilize these modes at higher temperature. This workflow fits effective\n", - "harmonic force constants to an MD trajectory at the temperature of interest, as\n", - "in the temperature-dependent effective potential (TDEP) method of Hellman et\n", - "al., Phys. Rev. B 84, 180301 (2011). These force constants include the effect\n", - "of the anharmonic forces on the frequencies at that temperature. They give no\n", - "phonon lifetimes.\n", - "\n", - "The flow has these steps:\n", - "\n", - "1. The structure is relaxed. The relaxation can be switched off, as done below.\n", - "2. A diagonal supercell is built. Its lattice vectors are at least `min_length`\n", - " long, 12 Å by default. A supercell matrix can also be given.\n", - "3. Optional, off by default: an NPT MD gives the cell at the temperature.\n", - " Section 2 explains this step.\n", - "4. An NVT MD run of the supercell at the temperature. The defaults are 8 ps with\n", - " a 1 fs time step and a Langevin thermostat.\n", - "5. The first 1 ps of the MD is left out. 50 snapshots are picked, evenly spread\n", - " over the rest of the trajectory.\n", - "6. The forces on the snapshots and on the undisplaced supercell are computed.\n", - "7. pheasy fits the second-order force constants with LASSO. The displacements\n", - " are measured from the undisplaced supercell. The forces of the undisplaced\n", - " supercell are subtracted from the forces of each snapshot.\n", - "8. The band structure and the density of states (DOS) follow from the force\n", - " constants. Imaginary modes are reported. They are not removed.\n", - "\n", - "The MD trajectory is also checked. The check looks for melting and for a move\n", - "away from the starting structure. It also looks at the drift of the potential\n", - "energy late in the run. The result is stored in the output. A warning is raised\n", - "if the check fails, but the fit is still done.\n", - "\n", - "Without the NPT step, the MD runs at constant volume (NVT). The volume is that\n", - "of the relaxed structure, or of the input structure when the relaxation is\n", - "switched off, as in this notebook. Thermal expansion is not included. The same\n", - "workflow runs with VASP as\n", - "`atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`.\n", - "`atomate2.forcefields.flows.finite_temperature_phonons` also has two mixed\n", - "versions. One runs the MD with VASP and the force calculations with a force\n", - "field. The other one does the reverse." + "## How the workflow works\n", + "\n", + "1. Relax the structure (optional).\n", + "2. Build a diagonal supercell with lattice vectors of at least `min_length`,\n", + " 12 Å by default.\n", + "3. Optional: run an NPT MD to get the cell at the temperature (Section 2).\n", + "4. Run an NVT MD, 8 ps with a 1 fs time step by default.\n", + "5. Leave out the first 1 ps and pick 50 evenly spaced snapshots.\n", + "6. Compute the forces on the snapshots and on the undisplaced supercell.\n", + "7. Fit the second-order force constants with pheasy (LASSO).\n", + "8. Compute the band structure and the DOS. Imaginary modes are reported, not\n", + " removed.\n", + "\n", + "A check of the trajectory flags melting, a shift away from the starting\n", + "structure and a drift of the energy. It raises a warning, and the fit is still\n", + "done. The idea is that of TDEP (Hellman et al., Phys. Rev. B 84, 180301\n", + "(2011)). The force constants include the effect of the anharmonic forces on the\n", + "frequencies. They give no lifetimes, and the MD is classical. The VASP version\n", + "is `atomate2.vasp.flows.finite_temperature_phonons.FiniteTemperaturePhononMaker`." ] }, { @@ -79,31 +55,14 @@ "id": "2", "metadata": {}, "source": [ - "## Thermostats\n", - "\n", - "The fit only uses the positions of the atoms in the MD, not how they move. The\n", - "snapshots have to follow the canonical distribution, so that every phonon mode\n", - "holds its share of the thermal energy.\n", - "\n", - "The NVT MD uses a Langevin thermostat. It adds a friction and a random force to\n", - "every atom, and it samples the canonical distribution (Bussi and Parrinello,\n", - "Phys. Rev. E 75, 056707 (2007)). The friction is 10 ps^-1. A Nose-Hoover\n", - "thermostat acts on the whole crystal through one extra variable. It changes the\n", - "motion of the atoms less, which matters for vibrational spectra or diffusion.\n", - "But in a nearly harmonic crystal the modes barely exchange energy. For a\n", - "harmonic oscillator weakly coupled to a Nose-Hoover thermostat, the dynamics is\n", - "not ergodic (Legoll et al., Arch. Ration. Mech. Anal. 184, 449 (2007)). A\n", - "crystal is closest to harmonic at low temperature.\n", + "## Thermostat\n", "\n", - "The NPT MD of Section 2 uses ASE's `MTKNPT`. It combines a Nose-Hoover\n", - "thermostat with one thermostat variable and the barostat of Martyna, Tobias and Klein, which samples the\n", - "isothermal-isobaric ensemble (J. Chem. Phys. 101, 4177 (1994)). Only its\n", - "average cell is used. With VASP, the NPT MD uses VASP's Langevin thermostat\n", - "and Parrinello-Rahman barostat, since VASP only runs NPT MD with these.\n", - "\n", - "`thermostat=\"nose-hoover\"` switches the NVT MD to a Nose-Hoover thermostat with\n", - "one thermostat variable. Section 3 compares the two for KNaICl. `random_seed`\n", - "seeds the initial velocities and the random forces of the Langevin thermostat." + "The NVT MD uses a Langevin thermostat with a friction of 10 ps⁻¹. It samples\n", + "the canonical ensemble for every mode (Bussi and Parrinello, Phys. Rev. E 75,\n", + "056707 (2007)). `thermostat=\"nose-hoover\"` is also available, but a weakly\n", + "coupled Nose-Hoover thermostat is not ergodic for a harmonic oscillator (Legoll\n", + "et al., Arch. Ration. Mech. Anal. 184, 449 (2007)). The NPT MD uses ASE's\n", + "`MTKNPT`. `random_seed` seeds the initial velocities and the Langevin forces." ] }, { @@ -113,16 +72,13 @@ "source": [ "## Installation\n", "\n", - "The `pheasy` and `ase` extras are needed, plus MACE and the Materials Project\n", - "client:\n", - "\n", "```\n", "pip install 'atomate2[pheasy,ase]'\n", "pip install 'mace-torch>=0.3.16' mp-api\n", "```\n", "\n", - "The `pheasy` extra pulls in pheasy and ALM. ALM is compiled from source. The\n", - "hiPhive tutorial and the atomate2 VASP documentation list what the build needs." + "The `pheasy` extra builds ALM from source. The hiPhive tutorial lists what the\n", + "build needs." ] }, { @@ -130,25 +86,17 @@ "id": "4", "metadata": {}, "source": [ - "## The potentials\n", - "\n", - "The notebook uses three MACE foundation models. All three are released under the\n", - "Academic Software License.\n", + "## Potentials\n", "\n", - "- **MACE-OMAT-0-medium.** `mace_mp(model=\"medium-omat-0\")` downloads it once and\n", - " caches it under `~/.cache/mace`.\n", - "- **MACE-MATPES-PBE-0** and **MACE-MATPES-r2SCAN-0.** These are MACE-OMAT-0\n", - " fine-tuned on the MatPES data set at the PBE and r2SCAN levels. Download the two files from the `mace_matpes_0` release of\n", - " [mace-foundations](https://github.com/ACEsuit/mace-foundations/releases/tag/mace_matpes_0):\n", - " - [MACE-matpes-pbe-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-pbe-omat-ft.model)\n", - " - [MACE-matpes-r2scan-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-r2scan-omat-ft.model)\n", + "- MACE-OMAT-0-medium. `mace_mp(model=\"medium-omat-0\")` downloads it.\n", + "- MACE-MATPES-PBE-0 and MACE-MATPES-r2SCAN-0. Download\n", + " [MACE-matpes-pbe-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-pbe-omat-ft.model)\n", + " and\n", + " [MACE-matpes-r2scan-omat-ft.model](https://github.com/ACEsuit/mace-foundations/releases/download/mace_matpes_0/MACE-matpes-r2scan-omat-ft.model)\n", + " and set their paths in the next cell.\n", "\n", - "Set the paths to the two downloaded files in the next cell. The Ca3Ir4Sn13\n", - "example below only needs MACE-OMAT-0-medium.\n", - "\n", - "The MD takes most of the time, so a GPU helps a lot. The next cell uses one if\n", - "PyTorch finds it. All our runs used `float64` on one NVIDIA A100 GPU of a\n", - "Perlmutter node." + "All three use the Academic Software License. Section 1 only needs\n", + "MACE-OMAT-0-medium. We ran in `float64` on one NVIDIA A100 GPU." ] }, { @@ -194,12 +142,9 @@ "source": [ "## One calculator for all jobs\n", "\n", - "Every force field job builds its own calculator. `run_locally` runs all of\n", - "them in this one Python process, and the workflow has a little over 50 jobs.\n", - "Loading MACE for each of them grows the memory by about 150 MB per job. This\n", - "cell makes the jobs share one calculator, as in the thermal expansion tutorial.\n", - "It is only needed when many jobs run in one process, not with a workflow\n", - "manager." + "`run_locally` runs all jobs in one process, and each force field job loads its\n", + "own calculator. The next cell makes them share one, as in the thermal expansion\n", + "tutorial. A workflow manager does not need this." ] }, { @@ -234,29 +179,18 @@ "id": "8", "metadata": {}, "source": [ - "## 1. Five materials from 100 K to 900 K\n", + "## 1. Five materials from 100 to 900 K\n", "\n", - "The first part runs Ca3Ir4Sn13 at 300 K with MACE-OMAT-0-medium step by step.\n", - "The other temperatures, potentials and materials follow with the same code." - ] - }, - { - "cell_type": "markdown", - "id": "9", - "metadata": {}, - "source": [ - "## The structure\n", - "\n", - "Ca3Ir4Sn13 (mp-1200211) is cubic, with 40 atoms in the primitive cell. We start\n", - "from its PBEsol cell in the Materials Project's Harmonic Phonon Database. The\n", - "phonon documents of the Materials Project hold this cell. Set your key first with\n", - "`export MP_API_KEY=...`." + "We first run Ca3Ir4Sn13 (mp-1200211) at 300 K with MACE-OMAT-0-medium. It has\n", + "40 atoms in the primitive cell and imaginary modes at 0 K. We take its PBEsol\n", + "cell from the Materials Project's Harmonic Phonon Database. Set\n", + "`MP_API_KEY` first." ] }, { "cell_type": "code", "execution_count": null, - "id": "10", + "id": "9", "metadata": {}, "outputs": [], "source": [ @@ -286,31 +220,21 @@ }, { "cell_type": "markdown", - "id": "11", + "id": "10", "metadata": {}, "source": [ "## Building the workflow\n", "\n", - "`ForceFieldFiniteTemperaturePhononMaker.from_force_field_name` sets one force\n", - "field for the relaxation, the MD and the force calculations. Any MACE model\n", - "routes through `mace_mp`, and the model name in `calculator_kwargs` selects the\n", - "weights. The name \"MACE-MP-0\" only picks this calculator. The output keeps it as\n", - "`force_field_name`, and `force_field_kwargs` holds the model that was loaded.\n", - "\n", - "We skip the relaxation with `relax_initial_structure=False`. The cell is\n", - "already relaxed with PBEsol, and our AIMD reference below uses the same cell. If\n", - "your input cell is not properly relaxed, keep the default\n", - "`relax_initial_structure=True`. The force field then relaxes the cell before\n", - "the MD.\n", - "\n", - "We give the supercell matrix of our AIMD reference, 2x2x2 with 320 atoms.\n", - "Everything else stays at the workflow defaults." + "`from_force_field_name` uses one force field for every job. \"MACE-MP-0\" picks\n", + "the MACE calculator, and `calculator_kwargs` picks the model. The cell is\n", + "already relaxed with PBEsol, so we skip the relaxation. We use the 2x2x2\n", + "supercell (320 atoms) of our AIMD reference." ] }, { "cell_type": "code", "execution_count": null, - "id": "12", + "id": "11", "metadata": {}, "outputs": [], "source": [ @@ -330,23 +254,20 @@ }, { "cell_type": "markdown", - "id": "13", + "id": "12", "metadata": {}, "source": [ "## Running the workflow\n", "\n", - "The flow has one MD job and 51 force calculations, 50 snapshots and the\n", - "undisplaced supercell. On one A100 GPU the whole run took 12 minutes. The MD\n", - "took 9 minutes, the force calculations 12 seconds and the fit 2 minutes.\n", - "\n", - "`create_folders=True` is needed, because the snapshots are read from the\n", - "trajectory file in the folder of the MD job." + "The flow has one MD job and 51 force calculations. It took 12 minutes on one\n", + "A100 GPU. `create_folders=True` is needed, since the snapshots are read from the\n", + "trajectory file of the MD job." ] }, { "cell_type": "code", "execution_count": null, - "id": "14", + "id": "13", "metadata": {}, "outputs": [], "source": [ @@ -360,19 +281,16 @@ }, { "cell_type": "markdown", - "id": "15", + "id": "14", "metadata": {}, "source": [ - "## Results\n", - "\n", - "The output is a `FiniteTemperaturePhononDoc`. It holds the band structure, the\n", - "DOS, the force constants, the fit and the trajectory check." + "The output is a `FiniteTemperaturePhononDoc`." ] }, { "cell_type": "code", "execution_count": null, - "id": "16", + "id": "15", "metadata": {}, "outputs": [], "source": [ @@ -392,46 +310,33 @@ }, { "cell_type": "markdown", - "id": "17", + "id": "16", "metadata": {}, "source": [ "Our run gave a highest frequency of 5.97 THz, no imaginary modes and a stable\n", - "trajectory.\n", - "\n", - "- `has_imaginary_modes` checks the whole band path. `lowest_frequency` only covers\n", - " the q-points commensurate with the supercell. The fit sets the frequencies at\n", - " these points directly. Everywhere else they are interpolated. Section 3 shows\n", - " why the difference matters.\n", - "- The force RMSE is the part of the forces that the force constants do not\n", - " describe. It grows with temperature, from 0.05 eV/Å at 100 K to 0.29 eV/Å at\n", - " 900 K for Ca3Ir4Sn13.\n", - "- The Lindemann ratio is the root mean square vibration of the atoms around\n", - " their mean positions, divided by the nearest-neighbor distance. By the\n", - " Lindemann criterion, a solid melts when this ratio reaches a fixed value\n", - " (Lindemann, Phys. Z. 11, 609 (1910); Gilvarry, Phys. Rev. 102, 308 (1956)).\n", - " The check reports the trajectory as melted above 0.15. This is the ratio at\n", - " melting of fcc solids, defined the same way (Saija et al., J. Chem. Phys. 124,\n", - " 244504 (2006))." + "trajectory. `has_imaginary_modes` checks the band path. `lowest_frequency` uses\n", + "only the q-points of the supercell, where the fit sets the frequencies directly\n", + "(Section 3). The check reports melting above a Lindemann ratio of 0.15, the\n", + "value at melting of fcc solids (Saija et al., J. Chem. Phys. 124, 244504\n", + "(2006))." ] }, { "cell_type": "markdown", - "id": "18", + "id": "17", "metadata": {}, "source": [ "## Comparing with 0 K\n", "\n", - "The Materials Project's Harmonic Phonon Database has the 0 K phonons of the same\n", - "cell, computed with PBEsol (Sahasrabuddhe et al., ChemRxiv (2026),\n", - "doi:10.26434/chemrxiv.15004632/v1). The next cell plots them next to ours. The\n", - "two band structures use different paths through the Brillouin zone, so they are\n", - "drawn side by side." + "The next cell plots our 300 K bands next to the 0 K PBEsol bands of the\n", + "Materials Project's Harmonic Phonon Database (Sahasrabuddhe et al., ChemRxiv\n", + "(2026), doi:10.26434/chemrxiv.15004632/v1)." ] }, { "cell_type": "code", "execution_count": null, - "id": "19", + "id": "18", "metadata": {}, "outputs": [], "source": [ @@ -507,44 +412,32 @@ }, { "cell_type": "markdown", - "id": "20", + "id": "19", "metadata": {}, "source": [ "![Band structure and DOS of Ca3Ir4Sn13 at 0 K and at 300 K](finite_temperature_phonons_figures/s1_ca3ir4sn13_300k.png)\n", "\n", - "At 0 K, Ca3Ir4Sn13 has imaginary modes down to about -0.75 THz. At 300 K they\n", - "are gone. The motion of the atoms at 300 K stabilizes them.\n", - "\n", - "To check the force field, we compare with effective harmonic force constants\n", - "fitted to ab initio MD at 300 K. These were computed with PBEsol in the same\n", - "cell and supercell. Their highest frequency is 6.03 THz, against 5.97 THz from\n", - "MACE-OMAT-0-medium. Over the whole band path the frequencies differ by 0.07 THz\n", - "on average." + "The imaginary modes of 0 K, down to -0.75 THz, are gone at 300 K. AIMD with\n", + "PBEsol in the same supercell gives a highest frequency of 6.03 THz. Over the\n", + "band path, MACE-OMAT-0-medium differs from it by 0.07 THz on average." ] }, { "cell_type": "markdown", - "id": "21", + "id": "20", "metadata": {}, "source": [ - "## The other temperatures, potentials and materials\n", + "## All temperatures, potentials and materials\n", "\n", - "The same workflow runs at five temperatures, with all three potentials and for\n", - "four more materials. AlAsPt5, Zn3P2 and Er5Tl3 also have imaginary modes at 0 K.\n", - "Bi4S3N2 is polar. The Materials Project lists AlAsPt5 and Bi4S3N2 as\n", - "theoretical. They are predicted compounds with no known experimental structure.\n", - "\n", - "The function below builds and runs one workflow in its own folder. Sections 2\n", - "and 3 use it as well.\n", - "\n", - "The loop runs 75 workflows, so it is off by default. Set `RUN_ALL = True` to\n", - "run it. Each of our runs took 6 to 22 minutes on one A100 GPU." + "The loop runs five materials with three potentials at five temperatures. AlAsPt5,\n", + "Zn3P2 and Er5Tl3 also have imaginary modes at 0 K, and Bi4S3N2 is polar. The\n", + "loop is off by default. Each run took 6 to 22 minutes." ] }, { "cell_type": "code", "execution_count": null, - "id": "22", + "id": "21", "metadata": {}, "outputs": [], "source": [ @@ -616,19 +509,17 @@ }, { "cell_type": "markdown", - "id": "23", + "id": "22", "metadata": {}, "source": [ - "The next cell plots the results of the loop. For each potential it shows the\n", - "band structure at 100, 500 and 900 K. Ca3Ir4Sn13 and Zn3P2 have 40 atoms in the\n", - "primitive cell, so their 120 branches are hard to follow. For these two the DOS\n", - "at all five temperatures is shown as well." + "The next cell plots the bands at 100, 500 and 900 K. For the two materials with\n", + "40 atoms in the primitive cell it also plots the DOS." ] }, { "cell_type": "code", "execution_count": null, - "id": "24", + "id": "23", "metadata": {}, "outputs": [], "source": [ @@ -678,7 +569,7 @@ }, { "cell_type": "markdown", - "id": "25", + "id": "24", "metadata": {}, "source": [ "The figures below show our runs.\n", @@ -696,20 +587,18 @@ }, { "cell_type": "markdown", - "id": "26", + "id": "25", "metadata": {}, "source": [ "## Our results\n", "\n", - "The next cell holds the results of our runs. For each material it gives the\n", - "highest frequency on the band path at each temperature. The dashed line is the\n", - "highest frequency of the AIMD reference at 300 K." + "The dashed line is the highest frequency of AIMD at 300 K." ] }, { "cell_type": "code", "execution_count": null, - "id": "27", + "id": "26", "metadata": {}, "outputs": [], "source": [ @@ -801,7 +690,7 @@ }, { "cell_type": "markdown", - "id": "28", + "id": "27", "metadata": {}, "source": [ "![Highest frequency against temperature](finite_temperature_phonons_figures/s1_max_frequency.png)\n", @@ -814,81 +703,38 @@ "| Bi4S3N2 | 0.15 | 0.46 | 0.16 | 17.03 |\n", "| Er5Tl3 | 0.18 | 0.17 | 0.13 | 3.97 |\n", "\n", - "The table gives the mean absolute difference from the AIMD reference at 300 K\n", - "in THz, over all branches and q-points of the band path.\n", + "The table gives the mean absolute difference from AIMD at 300 K over the band\n", + "path, in THz.\n", "\n", - "- No potential is closest to AIMD for all five materials. MACE-OMAT-0-medium is\n", - " closest for Ca3Ir4Sn13, AlAsPt5 and Bi4S3N2, within 0.07 to 0.15 THz.\n", - " MACE-MATPES-r2SCAN-0 is closest for Er5Tl3 and MACE-MATPES-PBE-0 for Zn3P2.\n", - "- MACE-MATPES-PBE-0 gives the lowest frequencies for most materials. For\n", - " Bi4S3N2 its highest branches lie about 1.8 THz below AIMD.\n", + "- No potential is best for all materials. MACE-OMAT-0-medium is closest for\n", + " three of the five.\n", "- Most frequencies soften with temperature. The highest frequency of Bi4S3N2\n", - " drops by 2.2 THz from 100 K to 900 K with MACE-OMAT-0-medium. AlAsPt5 barely\n", - " changes.\n", - "- The imaginary modes at 0 K are gone at every temperature for Ca3Ir4Sn13, Zn3P2\n", - " and Er5Tl3. AlAsPt5 keeps a small one, -0.12 THz, with MACE-MATPES-PBE-0 at\n", - " 100 K. Bi4S3N2 keeps imaginary modes down to -0.8 THz in 12 of 15 runs. Its\n", - " AIMD reference has a small one as well, at -0.12 THz. Bi4S3N2 is polar, so\n", - " these runs and the AIMD reference are compared without the non-analytical\n", - " correction. The three MACE potentials give no Born charges.\n", - "\n", - "The trajectory check did not report \"stable\" for five runs:\n", - "\n", - "- By the Lindemann criterion, Zn3P2 melts at 900 K with MACE-OMAT-0-medium and\n", - " MACE-MATPES-PBE-0. Its Lindemann ratio there is 0.161 and 0.157. With\n", - " MACE-MATPES-r2SCAN-0 it reaches 0.144 at 900 K, below the limit of 0.15. No\n", - " other material reaches the limit up to 900 K. The highest ratio among them is\n", - " 0.127, for Bi4S3N2. Every run keeps the volume of the 0 K cell. Section 2 adds\n", - " thermal expansion.\n", - "- At 100 K three runs are reported as shifted or diffusing: Ca3Ir4Sn13 with\n", - " MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0, and Er5Tl3 with\n", - " MACE-MATPES-r2SCAN-0. The mean positions of the atoms moved away from the\n", - " starting structure by more than they vibrate. Both materials have imaginary\n", - " modes at 0 K. Section 2 shows the same at 100 K in the force field's own cell,\n", - " for Ca3Ir4Sn13 and AlAsPt5. From 300 K on, their NVT runs are stable.\n", - " Most likely the atoms stay in a slightly distorted structure at 100 K and\n", - " move between such structures at higher temperature. We did not check which\n", - " distortion it is. The force constants of these runs describe vibrations\n", - " around the symmetric structure, so use them with care." + " drops by 2.2 THz from 100 to 900 K. AlAsPt5 barely changes.\n", + "- The imaginary modes of 0 K are gone for Ca3Ir4Sn13, Zn3P2 and Er5Tl3. Bi4S3N2\n", + " keeps some in 12 of 15 runs, and so does its AIMD reference.\n", + "- Zn3P2 melts at 900 K with two of the potentials. At 100 K three runs are\n", + " reported as shifted. Their atoms likely sit in a slightly distorted\n", + " structure." ] }, { "cell_type": "markdown", - "id": "29", + "id": "28", "metadata": {}, "source": [ "## 2. Thermal expansion with an NPT MD\n", "\n", - "In Section 1 every MD ran in the PBEsol cell at 0 K. Two things change this\n", - "cell. Each force field has its own 0 K cell, a little different from the PBEsol\n", - "one. And the crystal expands as it heats up. With `run_npt=True` the workflow\n", - "includes both:\n", - "\n", - "1. The force field relaxes the structure. Keep the default\n", - " `relax_initial_structure=True`, so that the NPT MD starts from the force\n", - " field's own 0 K cell.\n", - "2. An NPT MD of the supercell runs at the temperature and at `pressure`, 0 kbar\n", - " by default. It runs for `npt_time`, 8 ps by default, with a Nose-Hoover\n", - " thermostat and a Martyna-Tobias-Klein barostat.\n", - "3. The cell is averaged over the NPT MD after `npt_equilibration_time`, 2 ps by\n", - " default. The average keeps the symmetry of the structure. The atoms keep\n", - " their fractional coordinates and are then relaxed in the new cell, with the\n", - " cell fixed.\n", - "4. The NVT MD, the snapshots, the fit and the trajectory check follow as in\n", - " Section 1, in the new cell. The relaxed structure in the new cell is the\n", - " undisplaced supercell of the fit.\n", - "\n", - "The NPT trajectory is checked like the NVT one, and the result is stored as\n", - "`npt_trajectory_health`. `structure` holds the cell of the NVT MD and\n", - "`npt_input_structure` the cell that the NPT MD started from.\n", - "\n", - "We run Ca3Ir4Sn13 at 900 K with MACE-OMAT-0-medium." + "Each force field has its own 0 K cell, and the crystal expands as it heats up.\n", + "With `run_npt=True`, the workflow relaxes the structure and runs an NPT MD at\n", + "the temperature, 8 ps by default. It averages the cell after the first 2 ps,\n", + "keeping the symmetry, and relaxes the atoms in that cell. The NVT MD and the fit\n", + "then use this cell. We run Ca3Ir4Sn13 at 900 K." ] }, { "cell_type": "code", "execution_count": null, - "id": "30", + "id": "29", "metadata": {}, "outputs": [], "source": [ @@ -919,35 +765,30 @@ }, { "cell_type": "markdown", - "id": "31", + "id": "30", "metadata": {}, "source": [ - "Our run took 19 minutes. The NPT MD and the NVT MD took about 8 minutes each\n", - "and the fit 2 minutes. The 0 K cell of MACE-OMAT-0-medium has a lattice\n", - "parameter of 9.825 Å, and its volume is 3.8% larger than that of the PBEsol\n", - "cell. At 900 K the lattice parameter is 9.964 Å, 4.3% more volume. Both\n", - "trajectories were stable. The highest frequency is 4.91 THz, against 5.78 THz\n", - "in the PBEsol cell in Section 1." + "Our run took about 20 minutes. The 0 K cell of MACE-OMAT-0-medium is 3.8% larger\n", + "than the PBEsol cell, and the 900 K cell 4.3% larger again. Both trajectories\n", + "were stable. The highest frequency is 4.91 THz, against 5.78 THz in the PBEsol\n", + "cell." ] }, { "cell_type": "markdown", - "id": "32", + "id": "31", "metadata": {}, "source": [ - "## The other temperatures, potentials and materials\n", + "## All runs\n", "\n", - "We ran all 75 settings of Section 1 again with `run_npt=True`. To tell the two\n", - "effects apart, we also ran them with the relaxation but without the NPT MD,\n", - "that is in the force field's own 0 K cell. `run_ft` takes both options. The two\n", - "loops run 150 workflows, so they are off by default. Each of our runs took 6 to\n", - "29 minutes on one A100 GPU." + "The loop runs the 75 settings of Section 1 again, in the force field's 0 K cell\n", + "and with the NPT MD. It is off by default." ] }, { "cell_type": "code", "execution_count": null, - "id": "33", + "id": "32", "metadata": {}, "outputs": [], "source": [ @@ -972,22 +813,19 @@ }, { "cell_type": "markdown", - "id": "34", + "id": "33", "metadata": {}, "source": [ "## Our results\n", "\n", - "The next cell holds the results of our runs. The first plot gives the volume\n", - "relative to the PBEsol cell. The point at 0 K is the force field's relaxed cell.\n", - "The second plot gives the highest frequency for each potential in three cells:\n", - "the PBEsol cell of Section 1, the force field's 0 K cell, and the cell from the\n", - "NPT MD." + "The plots give the volume relative to the PBEsol cell, and the highest frequency\n", + "in three cells: the PBEsol cell, the force field's 0 K cell and the NPT cell." ] }, { "cell_type": "code", "execution_count": null, - "id": "35", + "id": "34", "metadata": {}, "outputs": [], "source": [ @@ -1123,96 +961,46 @@ }, { "cell_type": "markdown", - "id": "36", + "id": "35", "metadata": {}, "source": [ "![Volume against temperature](finite_temperature_phonons_figures/s2_volume.png)\n", "\n", "![Highest frequency in three cells](finite_temperature_phonons_figures/s2_max_frequency.png)\n", "\n", - "We do not compare these runs with the AIMD reference. It used the PBEsol cell\n", - "at every temperature.\n", - "\n", - "- The 0 K cells of the force fields are larger than the PBEsol cell, by up to\n", - " 12% in volume. MACE-OMAT-0-medium and MACE-MATPES-PBE-0 are trained on PBE\n", - " data, and PBE gives larger cells than PBEsol. MACE-MATPES-r2SCAN-0 gives the\n", - " cell closest to PBEsol for four of the five materials. For AlAsPt5 the two\n", - " differ by 0.2%.\n", - "- From 0 K to 900 K the volume grows by 3 to 6.5%. Bi4S3N2 with\n", - " MACE-MATPES-PBE-0 is the exception, with 11%.\n", - "- The larger 0 K cell alone lowers the frequencies. At 300 K the highest\n", - " frequency of Ca3Ir4Sn13 drops from 5.97 THz in the PBEsol cell to 5.58 THz\n", - " in the cell of MACE-OMAT-0-medium. With MACE-MATPES-PBE-0 the 0 K cell of\n", - " Er5Tl3 is 12% larger, and its highest frequency at 300 K drops from 4.12 to\n", - " 3.62 THz. With MACE-MATPES-r2SCAN-0 the cell of Zn3P2 grows by less than 1%,\n", - " and its highest frequency at 300 K stays at 10.9 THz.\n", - "- Thermal expansion lowers the frequencies further. At 100 K the NPT cell\n", - " changes the highest frequency by 0.15 THz or less, except for Bi4S3N2. At\n", - " 900 K it lowers it by 0.15 to 0.8 THz. For Bi4S3N2 with MACE-MATPES-PBE-0,\n", - " whose cell grows by 11%, it lowers it by 2.1 THz.\n", - "- At constant volume a frequency can also rise with temperature. In the PBEsol\n", - " cell, the highest frequency of AlAsPt5 with MACE-MATPES-PBE-0 rises from\n", - " 7.58 THz at 100 K to 7.80 THz at 900 K. In the NPT cell it falls from 7.15 to\n", - " 6.64 THz.\n", - "\n", - "The trajectory check did not report \"stable\" for these runs:\n", - "\n", - "- Zn3P2 at 900 K melts with all three potentials in the NPT MD and in the NVT MD\n", - " that follows. With MACE-MATPES-r2SCAN-0, its Lindemann ratio in Section 1\n", - " stayed below the limit, at 0.144. In the NVT MD in the NPT cell it is 0.150,\n", - " just above the limit. In the 0 K cell it melts at 900 K with MACE-OMAT-0-medium and\n", + "- The 0 K cells of the force fields are up to 12% larger than the PBEsol cell.\n", + " MACE-MATPES-r2SCAN-0 is closest to PBEsol for four of the five materials.\n", + "- From 0 to 900 K the volume grows by 3 to 6.5%, and by 11% for Bi4S3N2 with\n", " MACE-MATPES-PBE-0.\n", - "- Bi4S3N2 melts at 900 K in the NPT cell. The NPT MD is reported as melted with\n", - " all three potentials, and the NVT MD that follows with MACE-OMAT-0-medium and\n", - " MACE-MATPES-PBE-0. With MACE-MATPES-PBE-0 the NPT MD is also reported as\n", - " melted at 500 K and as shifted at 700 K, and the volume jumps by 5% between\n", - " these two temperatures. In the PBEsol cell and in the 0 K cell none of its\n", - " runs melted.\n", - "- AlAsPt5 at 900 K with MACE-MATPES-PBE-0: the NPT MD is reported as shifted,\n", - " and its volume does not grow from 700 to 900 K. The cell of this run is not\n", - " reliable, even though the NVT MD that follows is stable.\n", - "- At 100 K, the shift check fires for Ca3Ir4Sn13 and AlAsPt5. In the 0 K cell\n", - " this happens with MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0 for both. In the\n", - " NPT cell it happens for Ca3Ir4Sn13 with MACE-MATPES-r2SCAN-0 and for AlAsPt5\n", - " with all three potentials. Section 1 discusses this.\n", - "\n", - "Bi4S3N2 has imaginary modes on the band path in all 30 runs. A few runs at\n", - "100 K have small ones too: Ca3Ir4Sn13 with MACE-MATPES-r2SCAN-0 in both cells,\n", - "and AlAsPt5 in the NPT cell with MACE-OMAT-0-medium and MACE-MATPES-PBE-0. The\n", - "check reports all of these runs as shifted.\n", - "\n", - "A run with the NPT MD took 12 to 29 minutes, against 6 to 21 minutes in the\n", - "0 K cell. To compare a force field with DFT phonons in a given cell, run in\n", - "that cell, as in Section 1. To predict the phonons at a temperature with the\n", - "force field alone, use `run_npt=True`." + "- The larger 0 K cell alone lowers the frequencies, by up to 0.5 THz at 300 K.\n", + "- Thermal expansion lowers them by 0.15 to 0.8 THz at 900 K, and by 2.1 THz for\n", + " Bi4S3N2 with MACE-MATPES-PBE-0.\n", + "- Zn3P2 and Bi4S3N2 melt at 900 K in the NPT runs. AlAsPt5 with\n", + " MACE-MATPES-PBE-0 is reported as shifted at 900 K, and its cell does not grow\n", + " from 700 to 900 K.\n", + "\n", + "To compare with DFT in a given cell, run in that cell as in Section 1. To\n", + "predict the phonons at a temperature with the force field alone, use\n", + "`run_npt=True`." ] }, { "cell_type": "markdown", - "id": "37", + "id": "36", "metadata": {}, "source": [ - "## 3. MD length and number of snapshots for KNaICl\n", - "\n", - "Two settings control how well the MD samples the temperature:\n", + "## 3. MD length and number of snapshots\n", "\n", - "- `md_time` sets the length of the MD in ps. The default is 8 ps, of which the\n", - " first 1 ps is left out.\n", - "- `n_snapshots` sets the number of snapshots used in the fit. The default is 50.\n", - "\n", - "We tested 4, 8 and 16 ps with 25, 50 and 100 snapshots at 300 K for KNaICl\n", - "(mp-1002081). It has 4 atoms in the primitive cell and 72 in the 3x3x2\n", - "supercell. Like AlAsPt5 and Bi4S3N2, KNaICl is a predicted compound. KNaICl is polar, so it is compared with the AIMD reference without\n", - "the non-analytical correction. The highest frequency of that reference is\n", - "5.51 THz.\n", - "\n", - "The grid runs 27 workflows, so it is off by default." + "We run KNaICl (mp-1002081, 72 atoms in the supercell) at 300 K with 4, 8 and 16 ps\n", + "of MD and 25, 50 and 100 snapshots, and compare with AIMD. KNaICl is polar, so\n", + "the comparison is without the non-analytical correction. The grid is off by\n", + "default." ] }, { "cell_type": "code", "execution_count": null, - "id": "38", + "id": "37", "metadata": {}, "outputs": [], "source": [ @@ -1237,7 +1025,7 @@ { "cell_type": "code", "execution_count": null, - "id": "39", + "id": "38", "metadata": {}, "outputs": [], "source": [ @@ -1302,7 +1090,7 @@ }, { "cell_type": "markdown", - "id": "40", + "id": "39", "metadata": {}, "source": [ "![Difference from AIMD against MD length and snapshots](finite_temperature_phonons_figures/s3_knaicl_grid.png)\n", @@ -1319,61 +1107,38 @@ "| MATPES-r2SCAN-0 | 8 ps | 5.32 | 5.58 | 5.42 |\n", "| MATPES-r2SCAN-0 | 16 ps | 5.42 | 5.53 | 5.53 |\n", "\n", - "In the plot, a star marks a run with imaginary modes on the band path. The\n", - "table gives the highest frequency in THz.\n", - "\n", - "- The mean absolute difference from AIMD lies between 0.09 and 0.19 THz. It\n", - " shows no trend with the MD length or the number of snapshots. Each run is one\n", - " MD trajectory, so these differences are the noise of a single run.\n", - "- The highest frequency changes by up to 0.3 THz between runs, also without a\n", - " trend.\n", - "- 19 of the 27 runs have imaginary modes on the band path, down to -1.5 THz. In\n", - " all but two of them they only appear at q-points that are not commensurate\n", - " with the supercell, where the frequencies are interpolated from the fitted\n", - " force constants. The AIMD reference has no imaginary modes in the same\n", - " supercell. They appear in 6 of 9 runs with 25 snapshots, 8 of 9 with 50 and\n", - " 5 of 9 with 100. In an earlier round of the same grid with a Nose-Hoover\n", - " thermostat, 12 of the 27 runs had them.\n", - "- Each run is one trajectory. Another `random_seed` gives another trajectory and\n", - " somewhat different numbers.\n", - "- The MD takes most of the time. With MACE-OMAT-0-medium a run with 50\n", - " snapshots took 3.5, 6.1 and 10.8 minutes for 4, 8 and 16 ps. Going from 50 to\n", - " 100 snapshots added a few seconds of force calculations and fitting.\n", - "\n", - "With a force field the force calculations cost little next to the MD, so more\n", - "snapshots are cheap. In this test they did not remove the imaginary modes,\n", - "though. The default stays at 50, because with VASP each snapshot is a DFT\n", - "calculation of the whole supercell. For the MD length, 4 ps gave about the same\n", - "agreement with AIMD as 8 and 16 ps for KNaICl. We kept the default of 8 ps for\n", - "the other materials." + "A star marks a run with imaginary modes on the band path. The table gives the\n", + "highest frequency in THz.\n", + "\n", + "- The difference from AIMD is 0.09 to 0.19 THz, with no trend. It is the noise\n", + " of a single trajectory.\n", + "- 19 of the 27 runs have imaginary modes, mostly at q-points between those of\n", + " the supercell, where the frequencies are interpolated. AIMD has none. An\n", + " earlier round with a Nose-Hoover thermostat gave 12 of 27.\n", + "- More snapshots cost little with a force field, but they did not remove these\n", + " modes. The defaults stay at 8 ps and 50 snapshots, since with VASP each\n", + " snapshot is a DFT calculation." ] }, { "cell_type": "markdown", - "id": "41", + "id": "40", "metadata": {}, "source": [ "## 4. Li3PS4, a crystal that is unstable at 0 K\n", "\n", - "Li3PS4 is a solid electrolyte for lithium batteries. In experiment it has three\n", - "phases at ambient pressure. γ (Pmn2₁) is stable up to 523 to 573 K. β (Pnma)\n", - "is stable up to 723 to 748 K. α (Cmcm) is stable above that (Homma et al.,\n", - "Solid State Ionics 182, 53 (2011); Kaup et al., J. Mater. Chem. A 8, 12446\n", - "(2020)). γ is ordered. In β and α the Li atoms sit on partly occupied sites.\n", - "\n", - "mp-985583 is a Pnma structure, so it is β. A DFT code needs every site fully\n", - "occupied, so it is one ordered choice of the Li sites. In the Materials\n", - "Project's Harmonic Phonon Database it has imaginary modes at 0 K. Here we run\n", - "it from 100 to 1000 K, in steps of 100 K, with the three potentials. Each\n", - "potential first relaxes the structure. We run every temperature twice. One run\n", - "uses the relaxed 0 K cell (NVT). The other uses the cell from an NPT MD at that\n", - "temperature (Section 2). The supercell has 128 atoms." + "In experiment Li3PS4 is γ up to 523 to 573 K, β up to 723 to 748 K and α above\n", + "(Homma et al., Solid State Ionics 182, 53 (2011); Kaup et al., J. Mater. Chem. A\n", + "8, 12446 (2020)). mp-985583 is one ordering of the partly occupied Li sites of\n", + "β, and it has imaginary modes at 0 K. We run it from 100 to 1000 K with each\n", + "potential, in the relaxed 0 K cell (NVT) and in the NPT cell. The supercell has\n", + "128 atoms." ] }, { "cell_type": "code", "execution_count": null, - "id": "42", + "id": "41", "metadata": {}, "outputs": [], "source": [ @@ -1385,21 +1150,19 @@ }, { "cell_type": "markdown", - "id": "43", + "id": "42", "metadata": {}, "source": [ "## Phonons at 0 K\n", "\n", - "For the 0 K reference we use the phonopy workflow of atomate2, not the pheasy\n", - "one. When imaginary modes appear, the pheasy workflow refits the force\n", - "constants to remove them. Here we want to see them. The relaxation keeps the\n", - "symmetry, as in the finite-temperature workflow." + "We use the phonopy workflow here, since the pheasy workflow refits the force\n", + "constants to remove imaginary modes. The relaxation keeps the symmetry." ] }, { "cell_type": "code", "execution_count": null, - "id": "44", + "id": "43", "metadata": {}, "outputs": [], "source": [ @@ -1432,7 +1195,7 @@ }, { "cell_type": "markdown", - "id": "45", + "id": "44", "metadata": {}, "source": [ "Our run took 2 minutes. The lowest frequency is -2.59 THz. With\n", @@ -1441,7 +1204,7 @@ }, { "cell_type": "markdown", - "id": "46", + "id": "45", "metadata": {}, "source": [ "## One temperature\n", @@ -1452,7 +1215,7 @@ { "cell_type": "code", "execution_count": null, - "id": "47", + "id": "46", "metadata": {}, "outputs": [], "source": [ @@ -1476,30 +1239,29 @@ }, { "cell_type": "markdown", - "id": "48", + "id": "47", "metadata": {}, "source": [ "Our run took 31 minutes. The volume grows from 664.8 to 698.5 ų. The lowest\n", - "frequency is -0.57 THz. The trajectory check reports \"melted\", with a Lindemann\n", - "ratio of 0.24. Section 5 shows that the crystal has not melted. The Li atoms\n", - "hop between sites while P and S stay in place." + "frequency is -0.57 THz, and the check reports \"melted\" with a Lindemann ratio of\n", + "0.24. Section 5 shows that only the Li atoms move." ] }, { "cell_type": "markdown", - "id": "49", + "id": "48", "metadata": {}, "source": [ - "## The other temperatures and potentials\n", + "## All runs\n", "\n", - "The loop below runs all 60 settings and the three 0 K runs. It is off by\n", - "default. Each of our runs took 15 to 62 minutes on one A100 GPU." + "The loop runs the 60 settings and the three 0 K runs. It is off by default. Each\n", + "run took 15 to 62 minutes." ] }, { "cell_type": "code", "execution_count": null, - "id": "50", + "id": "49", "metadata": {}, "outputs": [], "source": [ @@ -1523,20 +1285,17 @@ }, { "cell_type": "markdown", - "id": "51", + "id": "50", "metadata": {}, "source": [ - "The next cell plots the bands of one potential at 0, 300 and 700 K, in the\n", - "relaxed 0 K cell (NVT) and in the NPT cell. Every run keeps the Pnma symmetry,\n", - "so all runs of a potential have the band path of its 0 K run. Their q-points\n", - "are the same in reduced coordinates. The cells differ a little, so we plot\n", - "every run along the distances of the 0 K path." + "The next cell plots the bands at 0, 300 and 700 K. Every run keeps the Pnma\n", + "symmetry, so all runs of a potential share the band path of its 0 K run." ] }, { "cell_type": "code", "execution_count": null, - "id": "52", + "id": "51", "metadata": {}, "outputs": [], "source": [ @@ -1568,7 +1327,7 @@ }, { "cell_type": "markdown", - "id": "53", + "id": "52", "metadata": {}, "source": [ "The figures below show our runs.\n", @@ -1582,20 +1341,18 @@ }, { "cell_type": "markdown", - "id": "54", + "id": "53", "metadata": {}, "source": [ "## Our results\n", "\n", - "The next cell holds the results of our runs. For each run it gives the lowest\n", - "frequency on the band path, the Lindemann ratio of the trajectory check and\n", - "the volume of the NPT cell." + "The lowest frequency, the Lindemann ratio and the NPT volume of each run." ] }, { "cell_type": "code", "execution_count": null, - "id": "55", + "id": "54", "metadata": {}, "outputs": [], "source": [ @@ -1656,58 +1413,39 @@ }, { "cell_type": "markdown", - "id": "56", + "id": "55", "metadata": {}, "source": [ "![Lowest frequency, Lindemann ratio and volume of Li3PS4](finite_temperature_phonons_figures/s4_runs.png)\n", "\n", - "- The imaginary modes of 0 K shrink at finite temperature, but they do not go\n", - " away. The lowest frequency lies between -0.2 and -2.2 THz in every run but\n", - " one. MACE-MATPES-r2SCAN-0 in the NPT cell at 400 K has no imaginary modes.\n", - "- At 100 K the trajectory check reports a shift in every run. The atoms move\n", - " away from the MP structure. At 200 K every run is stable.\n", - "- From 300 to 400 K the Lindemann ratio passes 0.15 and the check reports\n", - " melting. It then keeps rising, to 0.45 to 0.84 at 900 to 1000 K.\n", - "- From 0 to 800 K the NPT cell grows by 3 to 7% in volume. With\n", - " MACE-OMAT-0-medium it then jumps by 9% between 800 and 900 K.\n", - "- MACE-MATPES-PBE-0 gives the softest bands. Its highest frequency at 0 K is\n", - " 15.4 THz, against 17.8 and 17.9 THz for the other two.\n", - "\n", - "Li3PS4 does not melt at 400 K in experiment. Section 5 looks at what the atoms\n", - "do instead." + "- The imaginary modes shrink with temperature but do not go away. The one\n", + " exception is MACE-MATPES-r2SCAN-0 at 400 K in the NPT cell.\n", + "- The Lindemann ratio passes 0.15 at 300 to 400 K, and the check reports\n", + " melting. Li3PS4 does not melt there in experiment.\n", + "- The NPT cell grows by 3 to 7% up to 800 K.\n", + "- MACE-MATPES-PBE-0 gives the softest bands, with 15.4 THz at 0 K against 17.8\n", + " and 17.9 THz." ] }, { "cell_type": "markdown", - "id": "57", + "id": "56", "metadata": {}, "source": [ - "## 5. When light atoms hop: Li3PS4 above 300 K\n", + "## 5. Li3PS4 with hopping Li\n", "\n", - "In Section 4 the fitted phonons of Li3PS4 keep imaginary modes at every\n", - "temperature. At 0 K they come from the structure. This ordering of the Li\n", - "sites is not at a minimum of the energy. At high temperature a second cause\n", - "adds to this. The Li atoms start to hop from site to site, while the PS4\n", - "framework stays solid. A fit of force constants assumes that every atom\n", - "vibrates around one site. A Li atom that hops has no such site, so the fit\n", - "reads its motion as a very soft spring. The Lindemann ratio is an average over\n", - "all atoms, so the far moves of Li alone push it above 0.15.\n", - "\n", - "This section uses the MD itself, which needs no fixed sites. The mean-square\n", - "displacement of each element tells which atoms diffuse. The vibrational DOS\n", - "comes from the velocities in the MD. The free energy comes from thermodynamic\n", - "integration over the MD.\n", - "\n", - "The trajectories are the ones the workflow already saved, in\n", - "`md_trajectory.traj` in each run folder. They have one frame per time step and\n", - "include the momenta and the potential energies. The examples below use the\n", - "600 K run above." + "At 0 K the imaginary modes come from the structure, since this ordering is not\n", + "at an energy minimum. Above about 500 K the Li atoms also start to hop, while\n", + "the PS4 framework stays solid. A fit around fixed sites reads this as very soft\n", + "springs. The MD itself needs no fixed sites. We get the diffusion, the\n", + "vibrational DOS and the free energy from the saved trajectories,\n", + "`md_trajectory.traj`, starting with the 600 K run above." ] }, { "cell_type": "code", "execution_count": null, - "id": "58", + "id": "57", "metadata": {}, "outputs": [], "source": [ @@ -1744,20 +1482,19 @@ }, { "cell_type": "markdown", - "id": "59", + "id": "58", "metadata": {}, "source": [ - "## Which atoms move\n", + "## Diffusion\n", "\n", - "The mean-square displacement (MSD) of an atom grows linearly in time if it\n", - "diffuses. It levels off if the atom only vibrates. Its slope gives the\n", - "diffusion coefficient, $D = \\mathrm{slope}/6$. We fit the slope from 1 to 3 ps." + "$D$ is the slope of the mean-square displacement divided by 6, fitted from 1 to\n", + "3 ps." ] }, { "cell_type": "code", "execution_count": null, - "id": "60", + "id": "59", "metadata": {}, "outputs": [], "source": [ @@ -1793,7 +1530,7 @@ { "cell_type": "code", "execution_count": null, - "id": "61", + "id": "60", "metadata": {}, "outputs": [], "source": [ @@ -1846,7 +1583,7 @@ }, { "cell_type": "markdown", - "id": "62", + "id": "61", "metadata": {}, "source": [ "![Diffusion coefficients of Li3PS4](finite_temperature_phonons_figures/s5_diffusion.png)\n", @@ -1859,50 +1596,32 @@ "| MATPES-PBE-0 | 1.9 | 3.0 | 6.3 | 15.0 | 26.0 | 29.0 | 46.0 | 64.0 |\n", "| MATPES-r2SCAN-0 | 1.6 | 0.8 | 2.6 | 4.8 | 6.8 | 26.0 | 38.0 | 34.0 |\n", "\n", - "A D below about 3×10⁻⁷ cm²/s is noise in these 7 ps runs. P and S stay near\n", - "that level up to 700 K.\n", + "A $D$ below 3×10⁻⁷ cm²/s is noise in these 7 ps runs.\n", "\n", - "- Li diffuses clearly from about 600 K with MACE-OMAT-0-medium and\n", - " MACE-MATPES-r2SCAN-0, and from about 500 K with MACE-MATPES-PBE-0. D_Li is\n", - " 5×10⁻⁶ to 3×10⁻⁵ cm²/s at 600 to 800 K.\n", - "- Below that, a D_Li of 10⁻⁶ cm²/s means a few single hops in the run. One hop\n", - " of 2.5 Å by one of the 48 Li atoms already gives 0.13 Ų. A converged D below\n", - " 600 K needs MD of nanoseconds.\n", - "- At 900 K the D of P and S passes 10⁻⁶ cm²/s with MACE-OMAT-0-medium. With\n", - " the other two it stays below that in the 0 K cell, and passes it in the NPT\n", - " cell at 1000 K. The framework starts to flow.\n", - "\n", - "So from about 600 K to about 800 K, Li3PS4 is a solid framework with mobile\n", - "Li. This is the range where the fitted phonons fail.\n", - "\n", - "The MD uses the Langevin thermostat, and D depends on its friction. For a D to\n", - "compare with experiment, run an MD without a thermostat (NVE) from the end of\n", - "the NVT MD." + "- Li diffuses from about 600 K, and from about 500 K with MACE-MATPES-PBE-0.\n", + "- P and S start to diffuse at 900 to 1000 K.\n", + "- $D$ depends on the Langevin friction. For transport, run an NVE MD." ] }, { "cell_type": "markdown", - "id": "63", + "id": "62", "metadata": {}, "source": [ - "## The vibrational DOS from the velocities\n", + "## Vibrational DOS\n", "\n", - "The vibrational DOS is the Fourier transform of the velocity autocorrelation\n", - "function, weighted by mass. By the Wiener-Khinchin theorem this is the squared\n", - "Fourier transform of each velocity:\n", + "The DOS is the mass-weighted power spectrum of the velocities,\n", "\n", "$$g(\\nu) \\propto \\sum_i m_i \\left| \\int v_i(t)\\, e^{2\\pi i \\nu t}\\, dt \\right|^2$$\n", "\n", - "It holds all the anharmonicity at that temperature and has no imaginary\n", - "frequencies. An atom that diffuses adds to the DOS at $\\nu = 0$, in proportion\n", - "to its D. The friction of the Langevin thermostat, $\\gamma$ = 10 ps⁻¹, gives\n", - "every peak a width of $\\gamma/2\\pi$ = 1.6 THz (full width at half maximum)." + "It includes all the anharmonicity and has no imaginary frequencies. The\n", + "Langevin friction $\\gamma$ broadens every peak by $\\gamma/2\\pi$ = 1.6 THz." ] }, { "cell_type": "code", "execution_count": null, - "id": "64", + "id": "63", "metadata": {}, "outputs": [], "source": [ @@ -1939,7 +1658,7 @@ { "cell_type": "code", "execution_count": null, - "id": "65", + "id": "64", "metadata": {}, "outputs": [], "source": [ @@ -1976,7 +1695,7 @@ }, { "cell_type": "markdown", - "id": "66", + "id": "65", "metadata": {}, "source": [ "![Li DOS below 5 THz and P-S stretch, MD against fit](finite_temperature_phonons_figures/s5_vdos.png)\n", @@ -1995,61 +1714,36 @@ "| MATPES-r2SCAN-0 | 500 | 17% | 41% | 16.3 | 15.2 |\n", "| MATPES-r2SCAN-0 | 700 | 21% | 99% | 16.3 | 13.2 |\n", "\n", - "The fitted DOS is smeared with the same 0.15 THz as the MD DOS.\n", - "\n", - "- At 300 K, with MACE-OMAT-0-medium and MACE-MATPES-r2SCAN-0, 14 to 19% of the\n", - " Li DOS lies below 5 THz, in the MD and in the fit. With MACE-MATPES-PBE-0 the\n", - " fit already puts 53% of it there, against 21% in the MD.\n", - "- At 700 K the fit puts 90 to 100% of the Li DOS below 5 THz, and 6 to 18% of\n", - " it at imaginary frequencies. In the MD it is 21 to 25%. The Li DOS of the MD\n", - " stays a broad band, with a small value at zero from the diffusion.\n", - "- In the MD the P-S stretch stays at 16.0 to 16.4 THz with MACE-OMAT-0-medium\n", - " and MACE-MATPES-r2SCAN-0, and at 14.6 to 15.0 THz with MACE-MATPES-PBE-0. In\n", - " the fit it drops to 12.0 to 13.2 THz at 700 K. The framework does not soften.\n", - " The fit around fixed sites makes it look soft." + "- At 300 K the MD and the fit agree, except with MACE-MATPES-PBE-0.\n", + "- At 700 K the fit puts 90 to 100% of the Li DOS below 5 THz. The MD puts 21 to\n", + " 25% there.\n", + "- The P-S stretch stays at 15 to 16.4 THz in the MD, but drops to 12 to 13 THz in\n", + " the fit. The framework does not soften. The fit around fixed sites makes it\n", + " look soft." ] }, { "cell_type": "markdown", - "id": "67", + "id": "66", "metadata": {}, "source": [ - "## The free energy from the MD\n", - "\n", - "The fitted phonons give a free energy only through their frequencies, so they\n", - "carry the same errors. The MD gives it without a fit, in two steps.\n", - "\n", - "**1. F at one temperature, $T_0$ = 100 K, by Frenkel-Ladd.** An Einstein\n", - "crystal, with every atom tied by a spring to a site, has a free energy known in\n", - "closed form. We switch the potential from the Einstein crystal to the MACE\n", - "potential, $U(\\lambda) = \\lambda U_\\mathrm{MLIP} + (1 - \\lambda) U_E$, and run\n", - "an MD at 8 values of $\\lambda$. Then\n", + "## Free energy from the MD\n", "\n", - "$$F_\\mathrm{MLIP} = F_E + \\int_0^1 \\langle U_\\mathrm{MLIP} - U_E \\rangle_\\lambda\\, d\\lambda$$\n", - "\n", - "The springs sit at the mean positions of the 100 K MD. Their constants are\n", - "$3k_BT$ over the mean-square displacement of each element. The center of mass\n", - "is fixed in the MD, and $F_E$ has a term for that. We choose 100 K because no\n", - "Li hops there in any run.\n", - "\n", - "**2. F at every other temperature, by Gibbs-Helmholtz.**\n", - "\n", - "$$\\frac{d(F/T)}{dT} = -\\frac{U}{T^2}$$\n", - "\n", - "U is the mean energy of the MD at each temperature, the potential energy plus\n", - "$3k_BT/2$ per atom. For the NPT runs it is the mean enthalpy at zero pressure,\n", - "and the result is the Gibbs free energy. Then $S = (U - F)/T$. We stop at\n", - "800 K. Above it the P and S atoms start to diffuse.\n", - "\n", - "The MD treats the nuclei as classical. We add the difference between the\n", - "quantum and the classical free energy of the MD DOS at each temperature. It\n", - "matters most at low temperature." + "1. **F at 100 K by Frenkel-Ladd.** We switch from an Einstein crystal, with\n", + " springs at the mean positions of the 100 K MD, to the MACE potential at 8\n", + " values of $\\lambda$. No Li hops at 100 K.\n", + " $$F = F_E + \\int_0^1 \\langle U_\\mathrm{MLIP} - U_E \\rangle_\\lambda\\, d\\lambda$$\n", + "2. **F at higher temperatures by Gibbs-Helmholtz,** with $U$ the mean energy of\n", + " the MD, or the mean enthalpy for NPT. We stop at 800 K, where P and S start to\n", + " diffuse.\n", + " $$\\frac{d(F/T)}{dT} = -\\frac{U}{T^2}$$\n", + "3. **A quantum correction** from the MD DOS, since the MD is classical." ] }, { "cell_type": "code", "execution_count": null, - "id": "68", + "id": "67", "metadata": {}, "outputs": [], "source": [ @@ -2169,21 +1863,18 @@ }, { "cell_type": "markdown", - "id": "69", + "id": "68", "metadata": {}, "source": [ - "We tested these functions on a periodic Cu-Ag crystal with an EMT potential at\n", - "10 K, where the harmonic free energy is exact. Frenkel-Ladd gave 0.247542 ±\n", - "0.000087 eV and the exact value is 0.247599 eV.\n", - "\n", - "The next cell runs Frenkel-Ladd on the 100 K NVT run of the loop in Section 4.\n", - "It is off by default." + "On a Cu-Ag crystal with EMT at 10 K, these functions gave 0.247542 ± 0.000087 eV\n", + "against the exact 0.247599 eV. The next cell runs them on the 100 K run of\n", + "Section 4. It is off by default." ] }, { "cell_type": "code", "execution_count": null, - "id": "70", + "id": "69", "metadata": {}, "outputs": [], "source": [ @@ -2197,7 +1888,7 @@ { "cell_type": "code", "execution_count": null, - "id": "71", + "id": "70", "metadata": {}, "outputs": [], "source": [ @@ -2241,7 +1932,7 @@ { "cell_type": "code", "execution_count": null, - "id": "72", + "id": "71", "metadata": {}, "outputs": [], "source": [ @@ -2318,7 +2009,7 @@ }, { "cell_type": "markdown", - "id": "73", + "id": "72", "metadata": {}, "source": [ "![Free energy and entropy of Li3PS4](finite_temperature_phonons_figures/s5_thermo.png)\n", @@ -2332,42 +2023,31 @@ "| MATPES-r2SCAN-0 | 400 | 417 | 449 | 342 |\n", "\n", "The fitted F includes U₀, the mean potential energy of its MD minus 3kT/2 per\n", - "atom. All values are per formula unit.\n", + "atom.\n", "\n", - "- Up to 300 K the fitted F and the MD F agree to within 1 kJ/mol with\n", - " MACE-MATPES-r2SCAN-0, and to within 2.5 kJ/mol with MACE-OMAT-0-medium. Both\n", - " start from the same MD, but they get F in different ways, so the agreement\n", - " checks both. With MACE-MATPES-PBE-0 they start to differ at 300 K.\n", - "- Where Li diffuses, the fit gives too high an entropy. At 700 K the MD gives\n", - " S = 400 to 415 J/(K mol) in the 0 K cell, and the fit 449 to 457 J/(K mol).\n", - " The fit puts the Li modes at too low a frequency.\n", - "- The 0 K force constants give too low an entropy, 342 to 381 J/(K mol) at\n", - " 700 K. They miss the softening, and they leave out the imaginary modes. So\n", - " does the entropy in the Materials Project's Harmonic Phonon Database.\n", - "- The NPT cell adds 10 to 20 J/(K mol) at 700 K." + "- Up to 300 K the fit and the MD agree within 1 to 2.5 kJ/mol, except with\n", + " MACE-MATPES-PBE-0.\n", + "- Where Li hops, the fit overestimates S at 700 K by 40 to 50 J/(K mol).\n", + "- The 0 K force constants underestimate it by 35 to 60 J/(K mol). So does the\n", + " entropy in the Materials Project's Harmonic Phonon Database." ] }, { "cell_type": "markdown", - "id": "74", + "id": "73", "metadata": {}, "source": [ "## γ against β\n", "\n", - "The free energy from the MD includes the anharmonicity, the hopping of Li and\n", - "the thermal expansion. So the phase with the lowest Gibbs free energy should be\n", - "the stable one. The temperature where two curves cross should be a transition.\n", - "\n", - "The Materials Project has no entry for γ. Its two Pnma entries, mp-985583 and\n", - "mp-1097036, are orderings of β. No entry has the framework of α. We take γ from\n", - "Kaup et al., Table S1 of the supporting information. It agrees with Homma et\n", - "al., COD 1570309. γ is ordered and needs no choice of Li sites." + "The phase with the lowest G is stable, so a crossing of G(β) and G(γ) is a\n", + "transition. The Materials Project has no γ entry and no α framework. We take γ\n", + "from Kaup et al. (Table S1), which matches Homma et al. (COD 1570309)." ] }, { "cell_type": "code", "execution_count": null, - "id": "75", + "id": "74", "metadata": {}, "outputs": [], "source": [ @@ -2392,22 +2072,18 @@ }, { "cell_type": "markdown", - "id": "76", + "id": "75", "metadata": {}, "source": [ - "At 0 K all three potentials put γ below β. β lies 11.9 meV/atom higher with\n", - "MACE-MATPES-PBE-0, 10.5 with MACE-MATPES-r2SCAN-0 and 4.7 with\n", - "MACE-OMAT-0-medium. For β to become stable, its entropy has to make up\n", - "this difference.\n", - "\n", - "We run γ with the NPT MD at the same temperatures and with Frenkel-Ladd at\n", - "100 K, as for β. The loop is off by default." + "At 0 K β lies above γ by 4.7 meV/atom with MACE-OMAT-0-medium, 11.9 with\n", + "MACE-MATPES-PBE-0 and 10.5 with MACE-MATPES-r2SCAN-0. We run γ like β, with the\n", + "NPT MD and Frenkel-Ladd. The loop is off by default." ] }, { "cell_type": "code", "execution_count": null, - "id": "77", + "id": "76", "metadata": {}, "outputs": [], "source": [ @@ -2430,7 +2106,7 @@ { "cell_type": "code", "execution_count": null, - "id": "78", + "id": "77", "metadata": {}, "outputs": [], "source": [ @@ -2474,7 +2150,7 @@ }, { "cell_type": "markdown", - "id": "79", + "id": "78", "metadata": {}, "source": [ "![G(beta) - G(gamma) and entropies](finite_temperature_phonons_figures/s5_phases.png)\n", @@ -2487,101 +2163,59 @@ "| MATPES-PBE-0 | 7.1 | 5.5 | 3.4 | 1.1 | -1.1 | -2.2 | -1.9 | -0.4 |\n", "| MATPES-r2SCAN-0 | 3.0 | 1.6 | -0.5 | -2.4 | -4.6 | -7.2 | -9.5 | -10.5 |\n", "\n", - "G(β) crosses G(γ) at 278 K with MACE-MATPES-r2SCAN-0 and at 450 K with\n", - "MACE-MATPES-PBE-0. In experiment γ turns into β at 523 to 573 K. With\n", - "MACE-OMAT-0-medium, G(β) is already 0.3 meV/atom below G(γ) at 100 K, so there\n", - "is no crossing in our range. MACE-MATPES-PBE-0 gives a second crossing at\n", - "822 K. The framework of γ already flows there, so it does not count.\n", + "β becomes stable above 278 K with MACE-MATPES-r2SCAN-0 and above 450 K with\n", + "MACE-MATPES-PBE-0, against 523 to 573 K in experiment. With MACE-OMAT-0-medium β\n", + "is already lower at 100 K. The second crossing of MACE-MATPES-PBE-0 at 822 K\n", + "does not count, since γ flows there.\n", "\n", - "- At 100 K the classical F of β lies above that of γ by 0.2 meV/atom with\n", - " MACE-OMAT-0-medium, 7.9 with MACE-MATPES-PBE-0 and 4.1 with\n", - " MACE-MATPES-r2SCAN-0. This is much less than the gap at 0 K. β has softer\n", - " modes, so its vibrations lower its free energy more.\n", - "- At 300 K the entropy of β is 13 to 17 J/(K mol) higher than that of γ.\n", - "- The quantum correction is 17 to 21 meV/atom for each phase at 100 K and\n", - " about 5 meV/atom at 500 K. Most of it cancels in G(β) - G(γ). It lowers the\n", - " difference by 0.5 to 1.1 meV/atom at 100 K and by 0.1 to 0.2 meV/atom at\n", - " 500 K.\n", - "- Each Frenkel-Ladd F has an error of about 0.1 meV/atom, from the spread of\n", - " ⟨U_MLIP - U_E⟩ at each λ. The center-of-mass term of F_E is -1.3 meV/atom.\n", - " Both supercells have 128 atoms and nearly the same springs, so this term\n", - " changes G(β) - G(γ) by only 0.02 meV/atom." + "- β is softer. At 100 K its classical F lies only 0.2 to 7.9 meV/atom above γ,\n", + " much less than the gap at 0 K.\n", + "- The quantum correction is about 5 meV/atom for each phase at 500 K, but it\n", + " changes G(β) - G(γ) by 1.1 meV/atom or less.\n", + "- The error of each Frenkel-Ladd F is about 0.1 meV/atom." ] }, { "cell_type": "markdown", - "id": "80", + "id": "79", "metadata": {}, "source": [ "## What this approach cannot do\n", "\n", - "- **The free energy of α, and so the β to α transition.** Frenkel-Ladd needs a\n", - " structure that is stable at its starting temperature. α exists only with its\n", - " Li disorder. We relaxed 100 orderings of its Li sites with each potential.\n", - " In about 90 of them the PS4 units rotate into a distorted structure that\n", - " matches none of the known phases. The lowest lie 18 to 22 meV/atom above γ.\n", - " So ordered α is not a sound start at 100 K. α needs another method, for\n", - " example a cluster expansion for the Li disorder together with the vibrations.\n", - "- **Melting.** Its free energy needs a reference for the liquid, which\n", - " Frenkel-Ladd does not give.\n", - "- **Hysteresis.** In experiment the transitions happen at different\n", - " temperatures on heating and on cooling. The free energies only give the\n", - " temperature where two phases have the same G. Which phase forms depends also\n", - " on how fast the atoms rearrange.\n", - "\n", - "## Limits of the γ to β temperature\n", - "\n", - "- **The potentials.** γ and β differ by 5 to 12 meV/atom at 0 K, about the\n", - " size of the errors of these potentials. The transition temperature depends on\n", - " this difference, so it can shift by hundreds of kelvin between potentials.\n", - " Kam et al. computed the transitions with DFT, with the vibrational and the\n", - " configurational entropy (arXiv:2307.00878). With r²SCAN they found them 200\n", - " to 300 K below experiment. MACE-MATPES-r2SCAN-0 gives 250 to 300 K below\n", - " experiment. With PBE they found γ never stable. MACE-MATPES-PBE-0 instead\n", - " puts γ below β up to 450 K.\n", - "- **The Li disorder of β.** The MD only samples the disorder that the Li atoms\n", - " reach in 8 ps. Below about 500 K only a few Li hop, so the MD misses part of\n", - " the configurational entropy of β. Its free energy is then too high, which\n", - " moves the transition up.\n", - "- **One ordering of β.** We start from mp-985583. Other orderings start from a\n", - " different energy.\n", - "- **Classical nuclei.** The quantum correction uses a harmonic formula on the\n", - " MD DOS. It is exact only for harmonic vibrations. Its effect on G(β) - G(γ)\n", - " is 1.1 meV/atom or less, and 0.2 meV/atom or less from 500 K.\n", + "- **α.** Its ordered versions relax into distorted structures 18 to 22 meV/atom\n", + " above γ, so Frenkel-Ladd has no stable start. α needs a treatment of its Li\n", + " disorder, for example a cluster expansion.\n", + "- **Melting.** It needs a reference for the liquid.\n", + "- **Kinetics.** The free energies give the equilibrium temperature only, not the\n", + " hysteresis seen in experiment.\n", + "\n", + "## Why the γ to β temperature is off\n", + "\n", + "- **The potentials.** 1 meV/atom in G(β) - G(γ) moves the crossing by about\n", + " 50 K, and the 0 K gaps differ by 7 meV/atom between the potentials. Kam et al.\n", + " found r²SCAN DFT 200 to 300 K too low (arXiv:2307.00878), and\n", + " MACE-MATPES-r2SCAN-0 falls in the same range.\n", + "- **One ordering of β.** Below about 500 K the MD misses part of the Li disorder\n", + " of β.\n", "- **Size and length.** 128 atoms and 8 ps of MD." ] }, { "cell_type": "markdown", - "id": "81", + "id": "80", "metadata": {}, "source": [ "## Known limitations\n", "\n", - "By default the MD runs at constant volume (NVT). At every temperature it keeps\n", - "the volume of the starting structure, as in Section 1. A real crystal expands as\n", - "it heats up, and the expansion changes the phonons. At high temperature, use\n", - "`run_npt=True` as in Section 2. The NPT cell is the average over one MD run, so\n", - "it carries the noise of that run.\n", - "\n", - "The three MACE potentials give no Born charges, so the non-analytical\n", - "correction is not applied here. A `born_maker` can add them, either\n", - "`ForceFieldDielectricMaker` with MACE-Field (see the force field docs of\n", - "atomate2) or a VASP `DielectricMaker`.\n", - "\n", - "The trajectory check uses fixed limits. A Lindemann ratio above 0.15 is reported\n", - "as melting. A displacement from the reference of more than 1.5 times the\n", - "vibration around the mean positions is reported as a shift. These are rules of\n", - "thumb. The limit of 0.15 is the Lindemann ratio at melting of an fcc solid. The\n", - "ratio at melting differs between materials. We did not\n", - "check whether any of the trajectories reported as melted is a liquid. A warning\n", - "is raised and the fit is still done. The ratio is averaged over all atoms. It\n", - "can pass 0.15 when only the light atoms move far, for example Li in a\n", - "superionic conductor, while the rest of the crystal stays solid.\n", - "\n", - "Every result above comes from one MD trajectory. Section 3 shows that runs with\n", - "different settings differ by up to 0.1 THz on average and by up to 0.3 THz in\n", - "the highest frequency. Another `random_seed` gives somewhat different numbers." + "- Without `run_npt=True` the MD keeps the volume of the starting structure. The\n", + " NPT cell comes from one MD run and carries its noise.\n", + "- MACE gives no Born charges, so no non-analytical correction is applied. A\n", + " `born_maker` adds it, either `ForceFieldDielectricMaker` with MACE-Field or a\n", + " VASP `DielectricMaker`.\n", + "- The trajectory check uses fixed limits. The Lindemann limit of 0.15 is that of\n", + " fcc solids, and light atoms that hop can pass it while the crystal stays solid.\n", + "- Each result comes from one trajectory. Runs differ by up to 0.1 THz on average\n", + " and 0.3 THz in the highest frequency (Section 3)." ] } ], From ef3339bcfa336d9990c09f465f3ab73b72bac808 Mon Sep 17 00:00:00 2001 From: Hrushikesh Sahasrabuddhe <111614145+hrushikesh-s@users.noreply.github.com> Date: Tue, 6 Oct 2026 18:04:14 -0700 Subject: [PATCH 43/43] Plot the NPT band structures in the finite-temperature tutorial --- tutorials/finite_temperature_phonons.ipynb | 152 ++++++++++++------ .../s2_bands_AlAsPt5.png | Bin 0 -> 117486 bytes .../s2_bands_Bi4S3N2.png | Bin 0 -> 104042 bytes .../s2_bands_Ca3Ir4Sn13.png | Bin 0 -> 113426 bytes .../s2_bands_Er5Tl3.png | Bin 0 -> 119333 bytes .../s2_bands_Zn3P2.png | Bin 0 -> 106753 bytes 6 files changed, 100 insertions(+), 52 deletions(-) create mode 100644 tutorials/finite_temperature_phonons_figures/s2_bands_AlAsPt5.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_bands_Bi4S3N2.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_bands_Ca3Ir4Sn13.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_bands_Er5Tl3.png create mode 100644 tutorials/finite_temperature_phonons_figures/s2_bands_Zn3P2.png diff --git a/tutorials/finite_temperature_phonons.ipynb b/tutorials/finite_temperature_phonons.ipynb index 419290f044..5726ffe022 100644 --- a/tutorials/finite_temperature_phonons.ipynb +++ b/tutorials/finite_temperature_phonons.ipynb @@ -523,8 +523,12 @@ "metadata": {}, "outputs": [], "source": [ - "def plot_temperatures(name: str, with_dos: bool) -> None:\n", - " \"\"\"Plot the band structures of one material at 100, 500 and 900 K.\"\"\"\n", + "def plot_temperatures(name: str, with_dos: bool, label: str | None = None) -> None:\n", + " \"\"\"Plot the band structures of one material at 100, 500 and 900 K.\n", + "\n", + " label picks the runs of Section 2, \"relaxed\" or \"npt\". None picks Section 1.\n", + " \"\"\"\n", + " suffix = () if label is None else (label,)\n", " ratios = [3, 1] * len(MODEL_FILES) if with_dos else [3] * len(MODEL_FILES)\n", " fig, axes = plt.subplots(\n", " 1,\n", @@ -542,7 +546,7 @@ " for temperature in (100, 500, 900):\n", " plot_bands(\n", " ax,\n", - " docs[name, model, temperature].phonon_bandstructure,\n", + " docs[(name, model, temperature, *suffix)].phonon_bandstructure,\n", " label=f\"{temperature} K\",\n", " color=colors[temperature],\n", " lw=0.6,\n", @@ -552,13 +556,13 @@ " for temperature in TEMPERATURES:\n", " plot_dos(\n", " axes[step * idx + 1],\n", - " docs[name, model, temperature].phonon_dos,\n", + " docs[(name, model, temperature, *suffix)].phonon_dos,\n", " label=f\"{temperature} K\",\n", " color=colors[temperature],\n", " )\n", " axes[0].set_ylabel(\"Frequency (THz)\")\n", " axes[-1].legend(fontsize=8)\n", - " fig.suptitle(name, y=1.02)\n", + " fig.suptitle(name if label is None else f\"{name}, {label} cell\", y=1.02)\n", " plt.show()\n", "\n", "\n", @@ -815,6 +819,50 @@ "cell_type": "markdown", "id": "33", "metadata": {}, + "source": [ + "The next cell plots the bands in the NPT cell at 100, 500 and 900 K, as in\n", + "Section 1." + ] + }, + { + "cell_type": "code", + "execution_count": null, + "id": "34", + "metadata": {}, + "outputs": [], + "source": [ + "if RUN_NPT:\n", + " for name in (\"Ca3Ir4Sn13\", \"AlAsPt5\", \"Zn3P2\", \"Bi4S3N2\", \"Er5Tl3\"):\n", + " plot_temperatures(name, with_dos=name in (\"Ca3Ir4Sn13\", \"Zn3P2\"), label=\"npt\")" + ] + }, + { + "cell_type": "markdown", + "id": "35", + "metadata": {}, + "source": [ + "The figures below show our runs.\n", + "\n", + "![Band structures of Ca3Ir4Sn13 in the NPT cell at 100, 500 and 900 K](finite_temperature_phonons_figures/s2_bands_Ca3Ir4Sn13.png)\n", + "\n", + "![Band structures of AlAsPt5 in the NPT cell at 100, 500 and 900 K](finite_temperature_phonons_figures/s2_bands_AlAsPt5.png)\n", + "\n", + "![Band structures of Zn3P2 in the NPT cell at 100, 500 and 900 K](finite_temperature_phonons_figures/s2_bands_Zn3P2.png)\n", + "\n", + "![Band structures of Bi4S3N2 in the NPT cell at 100, 500 and 900 K](finite_temperature_phonons_figures/s2_bands_Bi4S3N2.png)\n", + "\n", + "![Band structures of Er5Tl3 in the NPT cell at 100, 500 and 900 K](finite_temperature_phonons_figures/s2_bands_Er5Tl3.png)\n", + "\n", + "- From 100 to 900 K the highest frequency drops by 0.3 to 3.2 THz in the NPT\n", + " cell, against at most 2.3 THz in the PBEsol cell of Section 1.\n", + "- AlAsPt5 barely changes in the PBEsol cell, but softens by 0.3 to 0.6 THz in\n", + " the NPT cell." + ] + }, + { + "cell_type": "markdown", + "id": "36", + "metadata": {}, "source": [ "## Our results\n", "\n", @@ -825,7 +873,7 @@ { "cell_type": "code", "execution_count": null, - "id": "34", + "id": "37", "metadata": {}, "outputs": [], "source": [ @@ -961,7 +1009,7 @@ }, { "cell_type": "markdown", - "id": "35", + "id": "38", "metadata": {}, "source": [ "![Volume against temperature](finite_temperature_phonons_figures/s2_volume.png)\n", @@ -986,7 +1034,7 @@ }, { "cell_type": "markdown", - "id": "36", + "id": "39", "metadata": {}, "source": [ "## 3. MD length and number of snapshots\n", @@ -1000,7 +1048,7 @@ { "cell_type": "code", "execution_count": null, - "id": "37", + "id": "40", "metadata": {}, "outputs": [], "source": [ @@ -1025,7 +1073,7 @@ { "cell_type": "code", "execution_count": null, - "id": "38", + "id": "41", "metadata": {}, "outputs": [], "source": [ @@ -1090,7 +1138,7 @@ }, { "cell_type": "markdown", - "id": "39", + "id": "42", "metadata": {}, "source": [ "![Difference from AIMD against MD length and snapshots](finite_temperature_phonons_figures/s3_knaicl_grid.png)\n", @@ -1122,7 +1170,7 @@ }, { "cell_type": "markdown", - "id": "40", + "id": "43", "metadata": {}, "source": [ "## 4. Li3PS4, a crystal that is unstable at 0 K\n", @@ -1138,7 +1186,7 @@ { "cell_type": "code", "execution_count": null, - "id": "41", + "id": "44", "metadata": {}, "outputs": [], "source": [ @@ -1150,7 +1198,7 @@ }, { "cell_type": "markdown", - "id": "42", + "id": "45", "metadata": {}, "source": [ "## Phonons at 0 K\n", @@ -1162,7 +1210,7 @@ { "cell_type": "code", "execution_count": null, - "id": "43", + "id": "46", "metadata": {}, "outputs": [], "source": [ @@ -1195,7 +1243,7 @@ }, { "cell_type": "markdown", - "id": "44", + "id": "47", "metadata": {}, "source": [ "Our run took 2 minutes. The lowest frequency is -2.59 THz. With\n", @@ -1204,7 +1252,7 @@ }, { "cell_type": "markdown", - "id": "45", + "id": "48", "metadata": {}, "source": [ "## One temperature\n", @@ -1215,7 +1263,7 @@ { "cell_type": "code", "execution_count": null, - "id": "46", + "id": "49", "metadata": {}, "outputs": [], "source": [ @@ -1239,7 +1287,7 @@ }, { "cell_type": "markdown", - "id": "47", + "id": "50", "metadata": {}, "source": [ "Our run took 31 minutes. The volume grows from 664.8 to 698.5 ų. The lowest\n", @@ -1249,7 +1297,7 @@ }, { "cell_type": "markdown", - "id": "48", + "id": "51", "metadata": {}, "source": [ "## All runs\n", @@ -1261,7 +1309,7 @@ { "cell_type": "code", "execution_count": null, - "id": "49", + "id": "52", "metadata": {}, "outputs": [], "source": [ @@ -1285,7 +1333,7 @@ }, { "cell_type": "markdown", - "id": "50", + "id": "53", "metadata": {}, "source": [ "The next cell plots the bands at 0, 300 and 700 K. Every run keeps the Pnma\n", @@ -1295,7 +1343,7 @@ { "cell_type": "code", "execution_count": null, - "id": "51", + "id": "54", "metadata": {}, "outputs": [], "source": [ @@ -1327,7 +1375,7 @@ }, { "cell_type": "markdown", - "id": "52", + "id": "55", "metadata": {}, "source": [ "The figures below show our runs.\n", @@ -1341,7 +1389,7 @@ }, { "cell_type": "markdown", - "id": "53", + "id": "56", "metadata": {}, "source": [ "## Our results\n", @@ -1352,7 +1400,7 @@ { "cell_type": "code", "execution_count": null, - "id": "54", + "id": "57", "metadata": {}, "outputs": [], "source": [ @@ -1413,7 +1461,7 @@ }, { "cell_type": "markdown", - "id": "55", + "id": "58", "metadata": {}, "source": [ "![Lowest frequency, Lindemann ratio and volume of Li3PS4](finite_temperature_phonons_figures/s4_runs.png)\n", @@ -1429,7 +1477,7 @@ }, { "cell_type": "markdown", - "id": "56", + "id": "59", "metadata": {}, "source": [ "## 5. Li3PS4 with hopping Li\n", @@ -1445,7 +1493,7 @@ { "cell_type": "code", "execution_count": null, - "id": "57", + "id": "60", "metadata": {}, "outputs": [], "source": [ @@ -1482,7 +1530,7 @@ }, { "cell_type": "markdown", - "id": "58", + "id": "61", "metadata": {}, "source": [ "## Diffusion\n", @@ -1494,7 +1542,7 @@ { "cell_type": "code", "execution_count": null, - "id": "59", + "id": "62", "metadata": {}, "outputs": [], "source": [ @@ -1530,7 +1578,7 @@ { "cell_type": "code", "execution_count": null, - "id": "60", + "id": "63", "metadata": {}, "outputs": [], "source": [ @@ -1583,7 +1631,7 @@ }, { "cell_type": "markdown", - "id": "61", + "id": "64", "metadata": {}, "source": [ "![Diffusion coefficients of Li3PS4](finite_temperature_phonons_figures/s5_diffusion.png)\n", @@ -1605,7 +1653,7 @@ }, { "cell_type": "markdown", - "id": "62", + "id": "65", "metadata": {}, "source": [ "## Vibrational DOS\n", @@ -1621,7 +1669,7 @@ { "cell_type": "code", "execution_count": null, - "id": "63", + "id": "66", "metadata": {}, "outputs": [], "source": [ @@ -1658,7 +1706,7 @@ { "cell_type": "code", "execution_count": null, - "id": "64", + "id": "67", "metadata": {}, "outputs": [], "source": [ @@ -1695,7 +1743,7 @@ }, { "cell_type": "markdown", - "id": "65", + "id": "68", "metadata": {}, "source": [ "![Li DOS below 5 THz and P-S stretch, MD against fit](finite_temperature_phonons_figures/s5_vdos.png)\n", @@ -1724,7 +1772,7 @@ }, { "cell_type": "markdown", - "id": "66", + "id": "69", "metadata": {}, "source": [ "## Free energy from the MD\n", @@ -1743,7 +1791,7 @@ { "cell_type": "code", "execution_count": null, - "id": "67", + "id": "70", "metadata": {}, "outputs": [], "source": [ @@ -1863,7 +1911,7 @@ }, { "cell_type": "markdown", - "id": "68", + "id": "71", "metadata": {}, "source": [ "On a Cu-Ag crystal with EMT at 10 K, these functions gave 0.247542 ± 0.000087 eV\n", @@ -1874,7 +1922,7 @@ { "cell_type": "code", "execution_count": null, - "id": "69", + "id": "72", "metadata": {}, "outputs": [], "source": [ @@ -1888,7 +1936,7 @@ { "cell_type": "code", "execution_count": null, - "id": "70", + "id": "73", "metadata": {}, "outputs": [], "source": [ @@ -1932,7 +1980,7 @@ { "cell_type": "code", "execution_count": null, - "id": "71", + "id": "74", "metadata": {}, "outputs": [], "source": [ @@ -2009,7 +2057,7 @@ }, { "cell_type": "markdown", - "id": "72", + "id": "75", "metadata": {}, "source": [ "![Free energy and entropy of Li3PS4](finite_temperature_phonons_figures/s5_thermo.png)\n", @@ -2034,7 +2082,7 @@ }, { "cell_type": "markdown", - "id": "73", + "id": "76", "metadata": {}, "source": [ "## γ against β\n", @@ -2047,7 +2095,7 @@ { "cell_type": "code", "execution_count": null, - "id": "74", + "id": "77", "metadata": {}, "outputs": [], "source": [ @@ -2072,7 +2120,7 @@ }, { "cell_type": "markdown", - "id": "75", + "id": "78", "metadata": {}, "source": [ "At 0 K β lies above γ by 4.7 meV/atom with MACE-OMAT-0-medium, 11.9 with\n", @@ -2083,7 +2131,7 @@ { "cell_type": "code", "execution_count": null, - "id": "76", + "id": "79", "metadata": {}, "outputs": [], "source": [ @@ -2106,7 +2154,7 @@ { "cell_type": "code", "execution_count": null, - "id": "77", + "id": "80", "metadata": {}, "outputs": [], "source": [ @@ -2150,7 +2198,7 @@ }, { "cell_type": "markdown", - "id": "78", + "id": "81", "metadata": {}, "source": [ "![G(beta) - G(gamma) and entropies](finite_temperature_phonons_figures/s5_phases.png)\n", @@ -2177,7 +2225,7 @@ }, { "cell_type": "markdown", - "id": "79", + "id": "82", "metadata": {}, "source": [ "## What this approach cannot do\n", @@ -2202,7 +2250,7 @@ }, { "cell_type": "markdown", - "id": "80", + "id": "83", "metadata": {}, "source": [ "## Known limitations\n", diff --git a/tutorials/finite_temperature_phonons_figures/s2_bands_AlAsPt5.png b/tutorials/finite_temperature_phonons_figures/s2_bands_AlAsPt5.png new file mode 100644 index 0000000000000000000000000000000000000000..52408670dee877eb1878ebc43f18e38d61761293 GIT binary patch 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