From 2fb353f4b50c8d829c6a3501b347ba940af39824 Mon Sep 17 00:00:00 2001 From: Atsushi Togo Date: Thu, 19 Sep 2024 16:14:53 +0900 Subject: [PATCH] Add document for pypolymlp interface --- doc/index.md | 1 + doc/pypolymlp.md | 327 +++++++++++++++++++ example/NaCl-pypolymlp/BORN | 4 + example/NaCl-pypolymlp/POSCAR-unitcell | 16 + example/NaCl-pypolymlp/phono3py_disp.yaml.xz | Bin 0 -> 144596 bytes phono3py/cui/create_force_sets.py | 7 +- 6 files changed, 352 insertions(+), 3 deletions(-) create mode 100644 doc/pypolymlp.md create mode 100644 example/NaCl-pypolymlp/BORN create mode 100644 example/NaCl-pypolymlp/POSCAR-unitcell create mode 100644 example/NaCl-pypolymlp/phono3py_disp.yaml.xz diff --git a/doc/index.md b/doc/index.md index d7272258..8b3bf4d3 100644 --- a/doc/index.md +++ b/doc/index.md @@ -44,6 +44,7 @@ direct-solution wigner-solution workload-distribution random-displacements +pypolymlp cutoff-pair external-tools phono3py-api diff --git a/doc/pypolymlp.md b/doc/pypolymlp.md new file mode 100644 index 00000000..bd15f858 --- /dev/null +++ b/doc/pypolymlp.md @@ -0,0 +1,327 @@ +(pypolymlp-interface)= + +# Force constants calculation using pypolymlp (machine learning potential) + +With the `--pypolymlp` option, phono3py can interface with the polynomial +machine learning potential (MLP) code, +[pypolymlp](https://github.com/sekocha/pypolymlp), to perform training and +evaluation tasks of MLPs. This feature aims to reduce the computational cost of +anharmonic force constant calculations by using MLPs as an intermediary layer, +efficiently representing atomic interactions. + +The training process involves using a dataset consisting of supercell +displacements, forces, and energies. The trained MLPs are then employed to +compute forces for supercells with specific displacements. + +For more details on the methodology, refer to A. Togo and A. Seko, J. Chem. Phys. +**160**, 211001 (2024) [[doi](https://doi.org/10.1063/5.0211296)]. + +An example of its usage can be found in the `example/NaCl-pypolymlp` directory +in the distribution from GitHub or PyPI. + +## Requirement + +- [pypolymlp](https://github.com/sekocha/pypolymlp) +- [symfc](https://github.com/symfc/symfc) + +## Workflow + +1. Generate random displacements in supercells. Use {ref}`--rd + ` option. +2. Calculate corresponding forces and energies in supercells. Use of VASP + interface is recommended for {ref}`--sp ` option is supported. +3. Prepare dataset composed of displacements, forces, and energies in + supercells. The dataset must be stored in a phono3py-yaml-like file, e.g., + `phono3py_params.yaml`. Use {ref}`--cf3 ` and {ref}`--sp + ` option simultaneously. +4. Develop MLPs. At this step `phono3py.pmlp` is saved. +5. Generate displacements in supercells either systematic or random displacements. +6. Evaluate MLPs for forces of the supercells generated in step 5. +7. Calculate force constants from displacement-force dataset from steps 5 and 6. + +The steps 4-7 are executed in running phono3py with `--pypolymlp` +option. + +### Steps 1-3: Dataset preparation + +For the training, the following supercell data are required in the phono3py +setting to use pypolymlp: + +- Displacements +- Forces +- Total energies + +These data must be stored in phono3py.yaml-like file. + +The supercells with displacements are generated by + +``` +% phono3py --pa auto --rd 100 -c POSCAR-unitcell --dim 2 2 2 + _ _____ + _ __ | |__ ___ _ __ ___|___ / _ __ _ _ + | '_ \| '_ \ / _ \| '_ \ / _ \ |_ \| '_ \| | | | + | |_) | | | | (_) | | | | (_) |__) | |_) | |_| | + | .__/|_| |_|\___/|_| |_|\___/____/| .__/ \__, | + |_| |_| |___/ + 3.5.0 + +-------------------------[time 2024-09-19 14:40:00]------------------------- +Compiled with OpenMP support (max 10 threads). +Python version 3.12.4 +Spglib version 2.5.0 + +Unit cell was read from "POSCAR-unitcell". +-------------------------------- unit cell --------------------------------- +Lattice vectors: + a 5.603287477054753 0.000000000000000 0.000000000000000 + b 0.000000000000000 5.603287477054753 0.000000000000000 + c 0.000000000000000 0.000000000000000 5.603287477054753 +Atomic positions (fractional): + 1 Na 0.00000000000000 0.00000000000000 0.00000000000000 22.990 + 2 Na 0.00000000000000 0.50000000000000 0.50000000000000 22.990 + 3 Na 0.50000000000000 0.00000000000000 0.50000000000000 22.990 + 4 Na 0.50000000000000 0.50000000000000 0.00000000000000 22.990 + 5 Cl 0.50000000000000 0.50000000000000 0.50000000000000 35.453 + 6 Cl 0.50000000000000 0.00000000000000 0.00000000000000 35.453 + 7 Cl 0.00000000000000 0.50000000000000 0.00000000000000 35.453 + 8 Cl 0.00000000000000 0.00000000000000 0.50000000000000 35.453 +---------------------------------------------------------------------------- +Supercell (dim): [2 2 2] +Primitive matrix: + [0. 0.5 0.5] + [0.5 0. 0.5] + [0.5 0.5 0. ] +Displacement distance: 0.03 +Number of displacements: 100 +NAC parameters were read from "BORN". +Spacegroup: Fm-3m (225) +Displacement dataset was written in "phono3py_disp.yaml". +-------------------------[time 2024-09-19 14:40:00]------------------------- + _ + ___ _ __ __| | + / _ \ '_ \ / _` | + | __/ | | | (_| | + \___|_| |_|\__,_| +``` + +For the generated supercells, forces and energies are calculated. Here it is +assumed to use the VASP code. Once the calculations are complete, the data +(forces and energies) can be extracted using the following command: + +```bash +% phono3py --sp --cf3 vasprun_xmls/vasprun-{00001..00100}.xml +``` + +This command extracts the necessary data and stores it in the +`phono3py_params.yaml` file. For more details, refer to the description of the +{ref}`--sp ` option. Currently, supercell energy extraction from +calculator outputs is only supported when using the VASP interface. + +``````{note} +A set of the VASP calculation results is placed in `example/NaCl-rd`. It is +obtained by + +```bash +% tar xvfa ../NaCl-rd/vasprun_xmls.tar.xz +``` +`````` + + +### Steps 4-7: Force constants calculation (systematic displacements in step 5) + +After developing MLPs, displacements are generated systematically considering +crystal symmetry. + +Having `phono3py_params.yaml`, phono3py is executed with `--pypolymlp` option, + +``` +% phono3py-load --pypolymlp phono3py_params.yaml + _ _____ + _ __ | |__ ___ _ __ ___|___ / _ __ _ _ + | '_ \| '_ \ / _ \| '_ \ / _ \ |_ \| '_ \| | | | + | |_) | | | | (_) | | | | (_) |__) | |_) | |_| | + | .__/|_| |_|\___/|_| |_|\___/____/| .__/ \__, | + |_| |_| |___/ + 3.5.0 + +-------------------------[time 2024-09-19 15:20:27]------------------------- +Compiled with OpenMP support (max 10 threads). +Running in phono3py.load mode. +Python version 3.12.6 +Spglib version 2.5.0 +----------------------------- General settings ----------------------------- +HDF5 data compression filter: gzip +Crystal structure was read from "phono3py_params.yaml". +Supercell (dim): [2 2 2] +Primitive matrix: + [0. 0.5 0.5] + [0.5 0. 0.5] + [0.5 0.5 0. ] +Spacegroup: Fm-3m (225) +Use -v option to watch primitive cell, unit cell, and supercell structures. +NAC parameters were read from "phono3py_params.yaml". +----------------------------- Force constants ------------------------------ +Displacement dataset for fc3 was read from "phono3py_params.yaml". +----------------------------- pypolymlp start ------------------------------ +Pypolymlp is a generator of polynomial machine learning potentials. +Please cite the paper: A. Seko, J. Appl. Phys. 133, 011101 (2023). +Pypolymlp is developed at https://github.com/sekocha/pypolymlp. +Developing MLPs by pypolymlp... +Regression: cholesky decomposition ... +- alpha: 0.001 +- alpha: 0.01 +- alpha: 0.1 +- alpha: 1.0 +- alpha: 10.0 +Clear training X.T @ X +Calculate X.T @ X for test data +Clear test X.T @ X +Regression: model selection ... +- alpha = 1.000e-03 : rmse (train, test) = 9.39542e+14 9.39543e+14 +- alpha = 1.000e-02 : rmse (train, test) = 9.39542e+14 9.39543e+14 +- alpha = 1.000e-01 : rmse (train, test) = 0.03738 0.04961 +- alpha = 1.000e+00 : rmse (train, test) = 0.03900 0.04742 +- alpha = 1.000e+01 : rmse (train, test) = 0.04058 0.04584 +MLPs were written into "phono3py.pmlp" +------------------------------ pypolymlp end ------------------------------- +Generate displacements + Displacement distance: 0.001 +Evaluate forces in 292 supercells by pypolymlp +Computing fc3[ 1, x, x ] using numpy.linalg.pinv. +Displacements (in Angstrom): + [ 0.0010 0.0000 0.0000] + [-0.0010 0.0000 0.0000] +Computing fc3[ 33, x, x ] using numpy.linalg.pinv. +Displacements (in Angstrom): + [ 0.0010 0.0000 0.0000] + [-0.0010 0.0000 0.0000] +Expanding fc3. +fc3 was symmetrized. +fc2 was symmetrized. +Max drift of fc3: -0.000000 (zzz) -0.000000 (zzz) -0.000000 (zzz) +Max drift of fc2: -0.000000 (zz) -0.000000 (zz) +fc3 was written into "fc3.hdf5". +fc2 was written into "fc2.hdf5". +----------- None of ph-ph interaction calculation was performed. ----------- +Dataset generated using MMLPs was written in "phono3py_mlp_eval_dataset.yaml". +Summary of calculation was written in "phono3py.yaml". +-------------------------[time 2024-09-19 15:21:41]------------------------- + _ + ___ _ __ __| | + / _ \ '_ \ / _` | + | __/ | | | (_| | + \___|_| |_|\__,_| +``` + +Information about the development of MLPs using pypolymlp is provided between +the `pypolymlp start` and `pypolymlp end` sections. The polynomial MLPs are +saved in the `phono3py.pmlp` file, which can be reused in subsequent phono3py +executions with the `--pypolymlp` option when only displacements (and no forces) +are provided. + +After the MLPs are developed, systematic displacements, such as those involving +the displacement of one or two atoms in supercells, are generated with a +displacement distance of 0.001 Angstrom. The forces for these supercells are +then evaluated using pypolymlp. Both the generated displacements and the +corresponding forces are stored in the `phono3py_mlp_eval_dataset` file. + +### Steps 4-6: Force constants calculation (random displacements in step 5) + +After developing MLPs, random displacements are generated by specifying +{ref}`--rd ` option. To compute force constants +with random displacements, an external force constants calculator is necessary. +For this, symfc is used which is invoked by `--symfc` option. + +Having `phono3py_params.yaml`, phono3py is executed with `--pypolymlp` option, + +``` +% phono3py-load --pypolymlp --rd 200 --symfc phono3py_params.yaml + _ _____ + _ __ | |__ ___ _ __ ___|___ / _ __ _ _ + | '_ \| '_ \ / _ \| '_ \ / _ \ |_ \| '_ \| | | | + | |_) | | | | (_) | | | | (_) |__) | |_) | |_| | + | .__/|_| |_|\___/|_| |_|\___/____/| .__/ \__, | + |_| |_| |___/ + 3.5.0-dev22+g575c4107 + +-------------------------[time 2024-09-19 15:33:23]------------------------- +Compiled with OpenMP support (max 10 threads). +Running in phono3py.load mode. +Python version 3.12.6 +Spglib version 2.5.0 +----------------------------- General settings ----------------------------- +HDF5 data compression filter: gzip +Crystal structure was read from "phono3py_params.yaml". +Supercell (dim): [2 2 2] +Primitive matrix: + [0. 0.5 0.5] + [0.5 0. 0.5] + [0.5 0.5 0. ] +Spacegroup: Fm-3m (225) +Use -v option to watch primitive cell, unit cell, and supercell structures. +NAC parameters were read from "phono3py_params.yaml". +----------------------------- Force constants ------------------------------ +Displacement dataset for fc3 was read from "phono3py_params.yaml". +----------------------------- pypolymlp start ------------------------------ +Pypolymlp is a generator of polynomial machine learning potentials. +Please cite the paper: A. Seko, J. Appl. Phys. 133, 011101 (2023). +Pypolymlp is developed at https://github.com/sekocha/pypolymlp. +Developing MLPs by pypolymlp... +Regression: cholesky decomposition ... +- alpha: 0.001 +- alpha: 0.01 +- alpha: 0.1 +- alpha: 1.0 +- alpha: 10.0 +Clear training X.T @ X +Calculate X.T @ X for test data +Clear test X.T @ X +Regression: model selection ... +- alpha = 1.000e-03 : rmse (train, test) = 9.39542e+14 9.39543e+14 +- alpha = 1.000e-02 : rmse (train, test) = 9.39542e+14 9.39543e+14 +- alpha = 1.000e-01 : rmse (train, test) = 0.03738 0.04961 +- alpha = 1.000e+00 : rmse (train, test) = 0.03900 0.04742 +- alpha = 1.000e+01 : rmse (train, test) = 0.04058 0.04584 +MLPs were written into "phono3py.pmlp" +------------------------------ pypolymlp end ------------------------------- +Generate random displacements + Twice of number of snapshots will be generated for plus-minus displacements. + Displacement distance: 0.001 +Evaluate forces in 400 supercells by pypolymlp +-------------------------------- Symfc start ------------------------------- +Symfc is a non-trivial force constants calculator. Please cite the paper: +A. Seko and A. Togo, arXiv:2403.03588. +Symfc is developed at https://github.com/symfc/symfc. +Computing [2, 3] order force constants. +Increase log-level to watch detailed symfc log. +--------------------------------- Symfc end -------------------------------- +-------------------------------- Symfc start ------------------------------- +Symfc is a non-trivial force constants calculator. Please cite the paper: +A. Seko and A. Togo, arXiv:2403.03588. +Symfc is developed at https://github.com/symfc/symfc. +Computing [2] order force constants. +Increase log-level to watch detailed symfc log. +--------------------------------- Symfc end -------------------------------- +Max drift of fc3: -0.000000 (xyx) 0.000000 (zyy) -0.000000 (xyx) +Max drift of fc2: 0.000000 (xx) 0.000000 (xx) +fc3 was written into "fc3.hdf5". +fc2 was written into "fc2.hdf5". +----------- None of ph-ph interaction calculation was performed. ----------- +Dataset generated using MMLPs was written in "phono3py_mlp_eval_dataset.yaml". +Summary of calculation was written in "phono3py.yaml". +-------------------------[time 2024-09-19 15:34:41]------------------------- + _ + ___ _ __ __| | + / _ \ '_ \ / _` | + | __/ | | | (_| | + \___|_| |_|\__,_| +``` + +The development of MLPs follows the same procedure as described for the +systematic displacements (in step 5) above. + +After the MLPs are developed, 200 supercells with random directional +displacements are generated. These displacements are then inverted, resulting in +an additional 200 supercells. In total, 400 supercells are created. The forces +for these supercells are then evaluated. Finally, the force constants are +calculated using symfc. diff --git a/example/NaCl-pypolymlp/BORN b/example/NaCl-pypolymlp/BORN new file mode 100644 index 00000000..c6199d2a --- /dev/null +++ b/example/NaCl-pypolymlp/BORN @@ -0,0 +1,4 @@ +# epsilon and Z* of atoms 1 2 + 2.56345522 0.00000000 -0.00000000 0.00000000 2.56345522 -0.00000000 0.00000000 -0.00000000 2.56345522 + 1.09044426 0.00000000 -0.00000000 0.00000000 1.09044426 -0.00000000 0.00000000 -0.00000000 1.09044426 + -1.09044426 -0.00000000 0.00000000 -0.00000000 -1.09044426 0.00000000 -0.00000000 0.00000000 -1.09044426 diff --git a/example/NaCl-pypolymlp/POSCAR-unitcell b/example/NaCl-pypolymlp/POSCAR-unitcell new file mode 100644 index 00000000..8fc4f52a --- /dev/null +++ b/example/NaCl-pypolymlp/POSCAR-unitcell @@ -0,0 +1,16 @@ +generated by phonopy + 1.0 + 5.6032874770547529 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 5.6032874770547529 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 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84bec1ff..ed5b654f 100644 --- a/phono3py/cui/create_force_sets.py +++ b/phono3py/cui/create_force_sets.py @@ -417,6 +417,7 @@ def _set_forces_and_nac_params( calc_dataset_fc2["supercell_energies"], dtype="double" ) - nac_params = get_nac_params(primitive=ph3py_yaml.primitive) - if nac_params: - ph3py_yaml.nac_params = nac_params + if ph3py_yaml.nac_params is None: + nac_params = get_nac_params(primitive=ph3py_yaml.primitive) + if nac_params: + ph3py_yaml.nac_params = nac_params