From a44b909977bef7e275afba5cafd5d90dfe144a6d Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 9 Dec 2024 11:48:22 -0500 Subject: [PATCH 01/35] Added vscf functionality --- pennylane/qchem/vibrational/vscf.py | 370 ++++++++++++++++++ .../qchem/vibrational/test_ref_files/H2S.hdf5 | Bin 662512 -> 905600 bytes tests/qchem/vibrational/test_vscf.py | 77 ++++ 3 files changed, 447 insertions(+) create mode 100644 pennylane/qchem/vibrational/vscf.py create mode 100644 tests/qchem/vibrational/test_vscf.py diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py new file mode 100644 index 00000000000..3191f82055e --- /dev/null +++ b/pennylane/qchem/vibrational/vscf.py @@ -0,0 +1,370 @@ +# Copyright 2018-2024 Xanadu Quantum Technologies Inc. + +# Licensed under the Apache License, Version 2.0 (the "License"); +# you may not use this file except in compliance with the License. +# You may obtain a copy of the License at + +# http://www.apache.org/licenses/LICENSE-2.0 + +# Unless required by applicable law or agreed to in writing, software +# distributed under the License is distributed on an "AS IS" BASIS, +# WITHOUT WARRANTIES OR CONDITIONS OF ANY KIND, either express or implied. +# See the License for the specific language governing permissions and +# limitations under the License. +"""This module contains functions to perform VSCF calculation.""" + +import numpy as np + +# pylint: disable=too-many-arguments + + +def _build_Fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): + r"""Builds the fock matrix for each vibrational mode. + + Args: + mode (int): index of the active mode for which the Fock matrix is being calculated + active_ham_terms (dict): A dictionary containing the active Hamiltonian terms. + active_terms (list): A list containing the active Hamiltonian terms for the given mode. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + h_mat (Array[Array[float]]): the Hamiltonian matrix + mode_rot (TensorLike[float]): rotation matrix for the given vibrational mode + Returns: + Array[Array[float]]: fock matrix for the given mode + """ + + fock_matrix = np.zeros((modals[mode], modals[mode])) + for term in active_terms: + ham_term = active_ham_terms[term] + h_val = ham_term[0] + modal_indices = [*ham_term[1]] + excitation_indices = [*ham_term[2]] + + if mode in modal_indices: + modal_idx = modal_indices.index(mode) + + im = excitation_indices[modal_idx] + jm = excitation_indices[modal_idx + len(modal_indices)] + if im < modals[mode] and jm < modals[mode]: + h_val = h_val * np.prod( + [h_mat[term, modal] for modal in modal_indices if modal != mode] + ) + fock_matrix[im, jm] += h_val + + fock_matrix = mode_rot.T @ fock_matrix @ mode_rot + return fock_matrix + + +def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): + r"""Updates value of h matrix for a mode after other modes have been rotated. + + Args: + h_mat (Array[Array[float]]): the hamiltonian matrix + mode (int): index of the active mode for which the h matrix is being updated. + active_ham_terms (dict): A dictionary containing the active Hamiltonian terms. + mode_rot (array[array[float]]): rotation matrix for a given mode + active_terms (list): A list containing active Hamiltonian terms for the given mode. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + Array[Array[float]]: the updated hamiltonian matrix + + """ + u_coeffs = mode_rot[:, 0] + + for t in ts_act: + ham_term = active_ham_terms[t] + modal_indices = ham_term[1] + excitation_indices = ham_term[2] + + if mode in modal_indices: + modal_idx = modal_indices.index(mode) + + im = excitation_indices[modal_idx] + jm = excitation_indices[modal_idx + len(modal_indices)] + + if im < modals[mode] and jm < modals[mode]: + h_mat[t, mode] = u_coeffs[im] * u_coeffs[jm] + + return h_mat + + +def _find_active_terms(ham_integrals, modals, cutoff): + r"""Identifies the active terms in the Hamiltonian + + Args: + ham_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + cutoff (float): threshold value for including matrix elements into operator. + + Returns: + tuple: A tuple containing the following: + - dict: A dictionary containing the active Hamiltonian terms. + - dict: A dictionary containing the active Hamiltonian terms for all vibrational modes. + - int: total number of active terms in the Hamiltonian + + """ + active_ham_terms = {} + active_num = 0 + nmodes = np.shape(ham_integrals[0])[0] + + for n, ham_n in enumerate(ham_integrals): + ham_n = ham_integrals[n] + for idx, h_val in np.ndenumerate(ham_n): + if np.abs(h_val) < cutoff: + continue + + M_arr = idx[: n + 1] + + right_order = True + for i in range(n): + if M_arr[i] <= M_arr[i + 1]: + right_order = False + break + + if right_order: + exc_arr = idx[n + 1 :] + exc_in_modals = True + for m_idx, m in enumerate(M_arr): + im = exc_arr[m_idx] + jm = exc_arr[m_idx + len(M_arr)] + if im >= modals[m] or jm >= modals[m]: + exc_in_modals = False + break + if exc_in_modals: + active_ham_terms[active_num] = [h_val, M_arr, exc_arr] + active_num += 1 + + active_mode_terms = {} + for m in range(nmodes): + ts_for_m_arr = [] + for t in range(active_num): + if m in active_ham_terms[t][1]: + ts_for_m_arr.append(t) + active_mode_terms[m] = ts_for_m_arr + return active_ham_terms, active_mode_terms, active_num + + +def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): + r"""Calculates vibrational energy + + Args: + h_mat (Array[Array[float]]): the Hamiltonian matrix + active_ham_terms (dict): A dictionary containing the active Hamiltonian terms + active_mode_terms (dict): A list containing the active Hamiltonian terms for all vibrational modes. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + mode_rots (List[TensorLike[float]]): A list of rotation matrices for each vibrational mode. + + Returns: + float: vibrational energy + + """ + nmodes = h_mat.shape[1] + e0s = np.zeros(nmodes) + for mode in range(nmodes): + fock_mat = _build_Fock( + mode, active_ham_terms, active_mode_terms[mode], modals, h_mat, mode_rots[mode] + ) + e0s[mode] = fock_mat[0, 0] + + return np.sum(e0s) + + +def _vscf(ham_integrals, modals, cutoff, tol=1e-8, max_iters=10000): + r"""Performs the VSCF calculation. + + Args: + ham_integrals (list(TensorLike[float])): a list containing Hamiltonian integral matrices + modals (list(int)): A list containing the maximum number of modals to consider for each mode. + cutoff (float): threshold value for including matrix elements into operator. + tol (float): convergence tolerance for vscf calculation + max_iters (int): Maximum number of iterations for vscf to converge. + + Returns: + tuple : A tuple of the following: + - float: vscf energy + - List[TensorLike[float]]: A list of rotation matrices for all vibrational modes. + + """ + + nmodes = np.shape(ham_integrals[0])[0] + + active_ham_terms, active_mode_terms, active_num = _find_active_terms( + ham_integrals, modals, cutoff + ) + mode_rots = [np.eye(modals[mode]) for mode in range(nmodes)] + h_mat = np.zeros((active_num, nmodes)) + for mode in range(nmodes): + h_mat = _update_h( + h_mat, mode, active_ham_terms, mode_rots[mode], active_mode_terms[mode], modals + ) + + e0 = _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots) + + enew = e0 + 2 * tol + curr_iter = 0 + while curr_iter <= max_iters and np.abs(enew - e0) > tol: + if curr_iter != 0: + e0 = enew + + curr_iter += 1 + + for mode in range(nmodes): + fock = _build_Fock( + mode, active_ham_terms, active_mode_terms[mode], modals, h_mat, mode_rots[mode] + ) + _, eigvec = np.linalg.eigh(fock) + mode_rots[mode] = mode_rots[mode] @ eigvec + h_mat = _update_h( + h_mat, mode, active_ham_terms, mode_rots[mode], active_mode_terms[mode], modals + ) + fock = np.transpose(eigvec) @ fock @ eigvec + + enew = _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots) + e0 = enew + return e0, mode_rots + + +def _rotate_one_body(h1, nmodes, mode_rots, modals): + r"""Rotates one body integrals. + + Args: + h1 (TensorLike[float]): one-body integrals + nmodes (int): number of vibrational modes + mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + TensorLike[float]: rotated one-body integrals. + + """ + imax = np.max(modals) + if imax > np.shape(h1)[1]: + raise ValueError( + "Number of maximum modals cannot be greater than the modals for unrotated integrals." + ) + + h1_rot = np.zeros((nmodes, imax, imax)) + for m in range(nmodes): + h1_rot[m, : modals[m], : modals[m]] = np.einsum( + "ij,ia,jb->ab", h1[m, :, :], mode_rots[m][:, : modals[m]], mode_rots[m][:, : modals[m]] + ) + + return h1_rot + + +def _rotate_two_body(h2, nmodes, mode_rots, modals): + r"""Rotates two body integrals. + + Args: + h2 (TensorLike[float]): two-body integrals + nmodes (int): number of vibrational modes + mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + TensorLike[float]: rotated two-body integrals. + + """ + imax = np.max(modals) + + U_mats = [mode_rots[m] for m in range(nmodes)] + h2_rot = np.zeros((nmodes, nmodes, imax, imax, imax, imax)) + for m1 in range(nmodes): + for m2 in range(nmodes): + h2_rot[m1, m2, : modals[m1], : modals[m2], : modals[m1], : modals[m2]] = np.einsum( + "ijkl,ia,jb,kc,ld->abcd", + h2[m1, m2, :, :, :, :], + U_mats[m1][:, : modals[m1]], + U_mats[m2][:, : modals[m2]], + U_mats[m1][:, : modals[m1]], + U_mats[m2][:, : modals[m2]], + ) + + return h2_rot + + +def _rotate_three_body(h3, nmodes, mode_rots, modals): + r"""Rotates three body integrals. + + Args: + h3 (TensorLike[float]): three-body integrals + nmodes (int): number of vibrational modes + mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + TensorLike[float]: rotated three-body integrals. + + """ + imax = np.max(modals) + + h3_rot = np.zeros((nmodes, nmodes, nmodes, imax, imax, imax, imax, imax, imax)) + for m1 in range(nmodes): + for m2 in range(nmodes): + for m3 in range(nmodes): + h3_rot[ + m1, + m2, + m3, + : modals[m1], + : modals[m2], + : modals[m3], + : modals[m1], + : modals[m2], + : modals[m3], + ] = np.einsum( + "ijklmn,ia,jb,kc,ld,me,nf->abcdef", + h3[m1, m2, m3, :, :, :, :, :, :], + mode_rots[m1][:, : modals[m1]], + mode_rots[m2][:, : modals[m2]], + mode_rots[m3][:, : modals[m3]], + mode_rots[m1][:, : modals[m1]], + mode_rots[m2][:, : modals[m2]], + mode_rots[m3][:, : modals[m3]], + ) + + return h3_rot + + +def vscf_hamiltonian(ham_integrals, modals=None, cutoff=None, cutoff_ratio=1e-6): + r"""Generates VSCF rotated integrals for vibrational Hamiltonian. + + Args: + ham_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. Defaults to maximum value if none is provided + cutoff (float): threshold value for including matrix elements into operator. + cutoff_ratio (float): default ratio for zeroing elements which are smaller than this ratio with respect to biggest element in all H1,H2,...'s + + Returns: + List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. + + """ + n = len(ham_integrals) + + if n > 3: + raise ValueError(f"Building n-mode Hamiltonian not implemented for {n}=>3!") + + nmodes = np.shape(ham_integrals[0])[0] + + imax = np.shape(ham_integrals[0])[1] + max_modals = nmodes * [imax] + if modals is None: + modals = max_modals + else: + imax = np.max(modals) + + if cutoff is None: + max_val = np.max([np.max(np.abs(H)) for H in ham_integrals]) + cutoff = max_val * cutoff_ratio + + _, mode_rots = _vscf(ham_integrals, modals=max_modals, cutoff=cutoff) + h1_rot = _rotate_one_body(ham_integrals[0], nmodes, mode_rots, modals) + if n == 1: + return [h1_rot] + + h2_rot = 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Version 2.0 (the "License"); +# you may not use this file except in compliance with the License. +# You may obtain a copy of the License at + +# http://www.apache.org/licenses/LICENSE-2.0 + +# Unless required by applicable law or agreed to in writing, software +# distributed under the License is distributed on an "AS IS" BASIS, +# WITHOUT WARRANTIES OR CONDITIONS OF ANY KIND, either express or implied. +# See the License for the specific language governing permissions and +# limitations under the License. +""" +This module contains tests for functions needed to do vscf calculations. +""" +from pathlib import Path + +import numpy as np +import pytest + +from pennylane.qchem.vibrational import vscf + +# pylint: disable=protected-access + +h5py = pytest.importorskip("h5py") + +cform_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S.hdf5" + +with h5py.File(cform_file, "r+") as f: + h1_h2s = f["H1"][()] + h2_h2s = f["H2"][()] + h3_h2s = f["H3"][()] +h_data_h2s = [h1_h2s, h2_h2s, h3_h2s] + + +result_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S_vscf_result.hdf5" + +with h5py.File(result_file, "r+") as f: + h1_h2s = f["H1_rot"][()] + h2_h2s = f["H2_rot"][()] + h3_h2s = f["H3_rot"][()] + energy = f["energy"][()] + u_mat = f["u_mat"][()] + +h2s_exp_result = {"h_data": [h1_h2s, h2_h2s, h3_h2s], "energy": energy, "u_mat": u_mat} + + +@pytest.mark.parametrize( + ("h_data", "h2s_result"), + [ + (h_data_h2s, h2s_exp_result), + ], +) +def test_vscf_calculation(h_data, h2s_result): + r"""Test that vscf calculation produces correct energy and rotation matrices""" + + vib_energy, rot_matrix = vscf._vscf(h_data, modals=[8, 8, 8], cutoff=1e-8) + assert np.isclose(vib_energy, h2s_result["energy"]) + assert np.allclose(rot_matrix, h2s_result["u_mat"]) + + +@pytest.mark.parametrize( + ("h_data", "h2s_result"), + [ + (h_data_h2s, h2s_exp_result), + ], +) +def test_vscf_hamiltonian(h_data, h2s_result): + r"""Test that correct rotated Hamiltonian is produced.""" + + result_h = vscf.vscf_hamiltonian(h_data, modals=[3, 3, 3], cutoff=1e-8) + + expected_h = h2s_result["h_data"] + assert np.allclose(result_h[0], expected_h[0]) + assert np.allclose(result_h[1], expected_h[1]) + assert np.allclose(result_h[2], expected_h[2]) From 6bbdbb71de5bd3b1feefa9ade34b47bfbea82f6c Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 9 Dec 2024 11:50:20 -0500 Subject: [PATCH 02/35] Added reference file --- .../test_ref_files/H2S_vscf_result.hdf5 | Bin 0 -> 169440 bytes tests/qchem/vibrational/test_vscf.py | 2 +- 2 files changed, 1 insertion(+), 1 deletion(-) create mode 100644 tests/qchem/vibrational/test_ref_files/H2S_vscf_result.hdf5 diff --git a/tests/qchem/vibrational/test_ref_files/H2S_vscf_result.hdf5 b/tests/qchem/vibrational/test_ref_files/H2S_vscf_result.hdf5 new file mode 100644 index 0000000000000000000000000000000000000000..58fb2c26c837922fba523c7c056981c4626c98d3 GIT binary patch literal 169440 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z0SZun0u-PC1t>rP3Q&Lo6rcbFC_n)UP=Epypa2CZKmiI+fC3bt00k&O0SZun0u-PC b1t>rP3Q&Lo6rcbFC_n)UP=EseuLb@KSuLe3 literal 0 HcmV?d00001 diff --git a/tests/qchem/vibrational/test_vscf.py b/tests/qchem/vibrational/test_vscf.py index 398db6011f7..cec93ed4048 100644 --- a/tests/qchem/vibrational/test_vscf.py +++ b/tests/qchem/vibrational/test_vscf.py @@ -55,7 +55,7 @@ def test_vscf_calculation(h_data, h2s_result): r"""Test that vscf calculation produces correct energy and rotation matrices""" - vib_energy, rot_matrix = vscf._vscf(h_data, modals=[8, 8, 8], cutoff=1e-8) + vib_energy, rot_matrix = vscf._vscf(h_data, modals=[4,4,4], cutoff=1e-8) assert np.isclose(vib_energy, h2s_result["energy"]) assert np.allclose(rot_matrix, h2s_result["u_mat"]) From 2f327fc9c7b7ddddcc571d4346451fc5be378abb Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 9 Dec 2024 14:39:42 -0500 Subject: [PATCH 03/35] Added dipole --- pennylane/qchem/__init__.py | 2 +- pennylane/qchem/vibrational/__init__.py | 1 + pennylane/qchem/vibrational/pes_generator.py | 10 +- pennylane/qchem/vibrational/vscf.py | 149 ++++++++++++++---- .../qchem/vibrational/test_ref_files/H2S.hdf5 | Bin 905600 -> 3618304 bytes .../test_ref_files/H2S_vscf_result.hdf5 | Bin 169440 -> 659328 bytes tests/qchem/vibrational/test_vscf.py | 80 +++++++++- 7 files changed, 192 insertions(+), 50 deletions(-) diff --git a/pennylane/qchem/__init__.py b/pennylane/qchem/__init__.py index 0af1c7a23dc..d2bd29a658b 100644 --- a/pennylane/qchem/__init__.py +++ b/pennylane/qchem/__init__.py @@ -82,4 +82,4 @@ taper_hf, taper_operation, ) -from .vibrational import optimize_geometry, localize_normal_modes, vibrational_pes +from .vibrational import optimize_geometry, localize_normal_modes, vscf_hamiltonian diff --git a/pennylane/qchem/vibrational/__init__.py b/pennylane/qchem/vibrational/__init__.py index e3de1dbbd18..7beffbedae1 100644 --- a/pennylane/qchem/vibrational/__init__.py +++ b/pennylane/qchem/vibrational/__init__.py @@ -5,3 +5,4 @@ from .localize_modes import localize_normal_modes from .pes_generator import vibrational_pes from .vibrational_class import optimize_geometry +from .vscf import vscf_hamiltonian diff --git a/pennylane/qchem/vibrational/pes_generator.py b/pennylane/qchem/vibrational/pes_generator.py index c474cb40818..dc99fb48b4b 100644 --- a/pennylane/qchem/vibrational/pes_generator.py +++ b/pennylane/qchem/vibrational/pes_generator.py @@ -23,13 +23,9 @@ from pennylane.data.base._lazy_modules import h5py from .localize_modes import localize_normal_modes -from .vibrational_class import ( - VibrationalPES, - _get_dipole, - _harmonic_analysis, - _single_point, - optimize_geometry, -) +from .vibrational_class import (VibrationalPES, _get_dipole, + _harmonic_analysis, _single_point, + optimize_geometry) # pylint: disable=too-many-arguments, too-many-function-args, c-extension-no-member # pylint: disable= import-outside-toplevel, too-many-positional-arguments, dangerous-default-value diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3191f82055e..ab94b67106d 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -88,11 +88,11 @@ def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): return h_mat -def _find_active_terms(ham_integrals, modals, cutoff): +def _find_active_terms(ham_data, modals, cutoff): r"""Identifies the active terms in the Hamiltonian Args: - ham_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. modals (list[int]): A list containing the maximum number of modals to consider for each mode. cutoff (float): threshold value for including matrix elements into operator. @@ -105,10 +105,10 @@ def _find_active_terms(ham_integrals, modals, cutoff): """ active_ham_terms = {} active_num = 0 - nmodes = np.shape(ham_integrals[0])[0] + nmodes = np.shape(ham_data[0])[0] - for n, ham_n in enumerate(ham_integrals): - ham_n = ham_integrals[n] + for n, ham_n in enumerate(ham_data): + ham_n = ham_data[n] for idx, h_val in np.ndenumerate(ham_n): if np.abs(h_val) < cutoff: continue @@ -169,11 +169,11 @@ def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): return np.sum(e0s) -def _vscf(ham_integrals, modals, cutoff, tol=1e-8, max_iters=10000): +def _vscf(ham_data, modals, cutoff, tol=1e-8, max_iters=10000): r"""Performs the VSCF calculation. Args: - ham_integrals (list(TensorLike[float])): a list containing Hamiltonian integral matrices + ham_data (list(TensorLike[float])): a list containing Hamiltonian integral matrices modals (list(int)): A list containing the maximum number of modals to consider for each mode. cutoff (float): threshold value for including matrix elements into operator. tol (float): convergence tolerance for vscf calculation @@ -186,11 +186,9 @@ def _vscf(ham_integrals, modals, cutoff, tol=1e-8, max_iters=10000): """ - nmodes = np.shape(ham_integrals[0])[0] + nmodes = np.shape(ham_data[0])[0] - active_ham_terms, active_mode_terms, active_num = _find_active_terms( - ham_integrals, modals, cutoff - ) + active_ham_terms, active_mode_terms, active_num = _find_active_terms(ham_data, modals, cutoff) mode_rots = [np.eye(modals[mode]) for mode in range(nmodes)] h_mat = np.zeros((active_num, nmodes)) for mode in range(nmodes): @@ -238,11 +236,6 @@ def _rotate_one_body(h1, nmodes, mode_rots, modals): """ imax = np.max(modals) - if imax > np.shape(h1)[1]: - raise ValueError( - "Number of maximum modals cannot be greater than the modals for unrotated integrals." - ) - h1_rot = np.zeros((nmodes, imax, imax)) for m in range(nmodes): h1_rot[m, : modals[m], : modals[m]] = np.einsum( @@ -326,45 +319,131 @@ def _rotate_three_body(h3, nmodes, mode_rots, modals): return h3_rot -def vscf_hamiltonian(ham_integrals, modals=None, cutoff=None, cutoff_ratio=1e-6): +def _rotate_dipole(dipole_data, mode_rots, modals): + r"""Generates VSCF rotated dipole. + + Args: + dipole_data (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. + mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + tuple(TensorLike[float]): a tuple of rotated dipole integrals + + """ + n = len(dipole_data) + + if n > 3: + raise ValueError(f"Building n-mode dipole not implemented for {n}=>3!") + + nmodes = np.shape(dipole_data[0])[0] + imax = np.max(modals) + d1_rot = np.zeros((3, nmodes, imax, imax)) + + for alpha in range(3): + d1_rot[alpha, ::] = _rotate_one_body( + dipole_data[0][alpha, ::], nmodes, mode_rots, modals=modals + ) + dip_data = [d1_rot] + + if n > 1: + d2_rot = np.zeros((3, nmodes, nmodes, imax, imax, imax, imax)) + for alpha in range(3): + d2_rot[alpha, ::] = _rotate_two_body( + dipole_data[1][alpha, ::], nmodes, mode_rots, modals=modals + ) + dip_data = [d1_rot, d2_rot] + + if n > 2: + d3_rot = np.zeros((3, nmodes, nmodes, nmodes, imax, imax, imax, imax, imax, imax)) + for alpha in range(3): + d3_rot[alpha, ::] = _rotate_three_body( + dipole_data[2][alpha, ::], nmodes, mode_rots, modals=modals + ) + dip_data = [d1_rot, d2_rot, d3_rot] + + return dip_data + + +def _rotate_hamiltonian(ham_data, mode_rots, modals): + r"""Generates VSCF rotated Hamiltonian. + + Args: + ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes + modals (list[int]): A list containing the maximum number of modals to consider for each mode. + + Returns: + tuple(TensorLike[float]): a tuple of rotated Hamiltonian integrals + + """ + + n = len(ham_data) + nmodes = np.shape(ham_data[0])[0] + + h1_rot = _rotate_one_body(ham_data[0], nmodes, mode_rots, modals) + h_data = [h1_rot] + + if n > 1: + h2_rot = _rotate_two_body(ham_data[1], nmodes, mode_rots, modals) + h_data = [h1_rot, h2_rot] + + if n > 2: + h3_rot = _rotate_three_body(ham_data[2], nmodes, mode_rots, modals) + h_data = [h1_rot, h2_rot, h3_rot] + + return h_data + + +def vscf_hamiltonian(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates VSCF rotated integrals for vibrational Hamiltonian. Args: - ham_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. Defaults to maximum value if none is provided + ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + dipole_data (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. Default is ``None``. + modals (list[int]): A list containing the maximum number of modals to consider for each mode. Defalt to maximum number of modals. cutoff (float): threshold value for including matrix elements into operator. - cutoff_ratio (float): default ratio for zeroing elements which are smaller than this ratio with respect to biggest element in all H1,H2,...'s + cutoff_ratio (float): Default ratio for zeroing elements which are smaller than this ratio with respect to biggest element in all integrals. Default value is ``1e-6``. Returns: List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. """ - n = len(ham_integrals) - if n > 3: - raise ValueError(f"Building n-mode Hamiltonian not implemented for {n}=>3!") + if len(ham_data) > 3: + raise ValueError( + f"Building n-mode Hamiltonian is not implemented for n equal to {len(ham_data)}." + ) + + if dipole_data is not None: + if len(dipole_data) > 3: + raise ValueError( + f"Building n-mode dipole is not implemented for n equal to {len(dipole_data)}." + ) - nmodes = np.shape(ham_integrals[0])[0] + nmodes = np.shape(ham_data[0])[0] - imax = np.shape(ham_integrals[0])[1] + imax = np.shape(ham_data[0])[1] max_modals = nmodes * [imax] if modals is None: modals = max_modals else: + if np.max(modals) > imax: + raise ValueError( + "Number of maximum modals cannot be greater than the modals for unrotated integrals." + ) imax = np.max(modals) if cutoff is None: - max_val = np.max([np.max(np.abs(H)) for H in ham_integrals]) + max_val = np.max([np.max(np.abs(H)) for H in ham_data]) cutoff = max_val * cutoff_ratio - _, mode_rots = _vscf(ham_integrals, modals=max_modals, cutoff=cutoff) - h1_rot = _rotate_one_body(ham_integrals[0], nmodes, mode_rots, modals) - if n == 1: - return [h1_rot] + _, mode_rots = _vscf(ham_data, modals=max_modals, cutoff=cutoff) + + h_data = _rotate_hamiltonian(ham_data, mode_rots, modals) - h2_rot = _rotate_two_body(ham_integrals[1], nmodes, mode_rots, modals) - if n == 2: - return [h1_rot, h2_rot] + if dipole_data is not None: + dip_data = _rotate_dipole(dipole_data, mode_rots, modals) + return h_data, dip_data - h3_rot = _rotate_three_body(ham_integrals[2], nmodes, mode_rots, modals) - return [h1_rot, h2_rot, h3_rot] + return h_data, None diff --git a/tests/qchem/vibrational/test_ref_files/H2S.hdf5 b/tests/qchem/vibrational/test_ref_files/H2S.hdf5 index a63de1867275116db90e7a491d1c4cf25ae6ebb9..4161e01aab817570f308e75315763f0c87bc4f48 100644 GIT binary patch literal 3618304 zcmeF(1z1(x+BbT_?(RlKMJx=gu@nnT$}U9g#CimL?C!u03`DW9Fvqexun+^pZWL57 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Improvements 🛠

From 92a1ea0c6e562aca1680d5d828df2b087ad5c92a Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Sat, 14 Dec 2024 01:24:34 -0500 Subject: [PATCH 26/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 7a01850774a..7cded4863fc 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -18,7 +18,7 @@ # pylint: disable=too-many-arguments -def _build_Fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): +def _build_fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): r"""Builds the fock matrix for each vibrational mode. Args: From 84de7e26b0af6a97f4d54ac852d18b33aca93a29 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Sat, 14 Dec 2024 01:24:47 -0500 Subject: [PATCH 27/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 4 +--- 1 file changed, 1 insertion(+), 3 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 7cded4863fc..3b052f45385 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -35,9 +35,7 @@ def _build_fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): fock_matrix = np.zeros((modals[mode], modals[mode])) for term in active_terms: ham_term = active_ham_terms[term] - h_val = ham_term[0] - modal_indices = [*ham_term[1]] - excitation_indices = [*ham_term[2]] + h_val, modal_indices, excitation_indices = ham_term[0], list(ham_term[1]), list(ham_term[2]) modal_idx = modal_indices.index(mode) im = excitation_indices[modal_idx] From 99b750694360b9d0bff79fece8b683197c3c15a6 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Sat, 14 Dec 2024 01:25:01 -0500 Subject: [PATCH 28/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3b052f45385..3ec39c83b71 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -166,7 +166,7 @@ def _vscf(h_integrals, modals, cutoff, tol=1e-8, max_iters=10000): max_iters (int): Maximum number of iterations for vscf to converge. Returns: - tuple : A tuple of the following: + tuple: A tuple of the following: - float: vscf energy - List[TensorLike[float]]: A list of rotation matrices for all vibrational modes. From 8e5a7ec72559e4d0da058b58fd090fa3a94f9da5 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 16 Dec 2024 03:21:32 -0500 Subject: [PATCH 29/35] Addressed comments --- pennylane/qchem/vibrational/vscf.py | 133 +++++++++--------- .../qchem/vibrational/test_ref_files/H2S.hdf5 | Bin 3618304 -> 0 bytes .../test_ref_files/H2S_dipole.hdf5 | Bin 2712704 -> 0 bytes tests/qchem/vibrational/test_vscf.py | 2 +- 4 files changed, 68 insertions(+), 67 deletions(-) delete mode 100644 tests/qchem/vibrational/test_ref_files/H2S.hdf5 delete mode 100644 tests/qchem/vibrational/test_ref_files/H2S_dipole.hdf5 diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3ec39c83b71..40edd9fca52 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -23,61 +23,61 @@ def _build_fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): Args: mode (int): index of the active mode for which the Fock matrix is being calculated - active_ham_terms (dict): A dictionary containing the active Hamiltonian terms. - active_terms (list): A list containing the active Hamiltonian terms for the given mode. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. - h_mat (Array[Array[float]]): the Hamiltonian matrix + active_ham_terms (dict): dictionary containing the active Hamiltonian terms + active_terms (list): list containing the active Hamiltonian terms for the given mode + modals (list[int]): list containing the maximum number of modals to consider for each mode + h_mat (array[array[float]]): the Hamiltonian matrix mode_rot (TensorLike[float]): rotation matrix for the given vibrational mode + Returns: - Array[Array[float]]: fock matrix for the given mode + array[array[float]]: fock matrix for the given mode """ fock_matrix = np.zeros((modals[mode], modals[mode])) for term in active_terms: ham_term = active_ham_terms[term] - h_val, modal_indices, excitation_indices = ham_term[0], list(ham_term[1]), list(ham_term[2]) + h_val, modal_indices, excitation_indices = ham_term[0], list(ham_term[1]), list(ham_term[2]) modal_idx = modal_indices.index(mode) - im = excitation_indices[modal_idx] - jm = excitation_indices[modal_idx + len(modal_indices)] - if im < modals[mode] and jm < modals[mode]: + i = excitation_indices[modal_idx] + j = excitation_indices[modal_idx + len(modal_indices)] + if i < modals[mode] and j < modals[mode]: h_val = h_val * np.prod( [h_mat[term, modal] for modal in modal_indices if modal != mode] ) - fock_matrix[im, jm] += h_val + fock_matrix[i, j] += h_val fock_matrix = mode_rot.T @ fock_matrix @ mode_rot return fock_matrix -def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): +def _update_h(h_mat, mode, active_ham_terms, mode_rot, active_terms, modals): r"""Updates value of Hamiltonian matrix for a mode after other modes have been rotated. Args: - h_mat (Array[Array[float]]): the hamiltonian matrix - mode (int): index of the active mode for which the h matrix is being updated. - active_ham_terms (dict): A dictionary containing the active Hamiltonian terms. + h_mat (array[array[float]]): the Hamiltonian matrix + mode (int): index of the active mode for which the Hamiltonian matrix is being updated + active_ham_terms (dict): dictionary containing the active Hamiltonian terms mode_rot (array[array[float]]): rotation matrix for a given mode - active_terms (list): A list containing active Hamiltonian terms for the given mode. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + active_terms (list): list containing active Hamiltonian terms for the given mode + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: - Array[Array[float]]: the updated hamiltonian matrix + array[array[float]]: the updated Hamiltonian matrix """ u_coeffs = mode_rot[:, 0] - for t in ts_act: + for t in active_terms: ham_term = active_ham_terms[t] - modal_indices = ham_term[1] - excitation_indices = ham_term[2] + modal_indices, excitation_indices = ham_term[1], ham_term[2] modal_idx = modal_indices.index(mode) - im = excitation_indices[modal_idx] - jm = excitation_indices[modal_idx + len(modal_indices)] + i = excitation_indices[modal_idx] + j = excitation_indices[modal_idx + len(modal_indices)] - if im < modals[mode] and jm < modals[mode]: - h_mat[t, mode] = u_coeffs[im] * u_coeffs[jm] + if i < modals[mode] and j < modals[mode]: + h_mat[t, mode] = u_coeffs[i] * u_coeffs[j] return h_mat @@ -88,15 +88,15 @@ def _find_active_terms(h_integrals, modals, cutoff): The equation suggests that if mode m is not contained in a Hamiltonian term, it evaluates to zero. Args: - h_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. - cutoff (float): threshold value for including matrix elements into operator. + h_integrals (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals + modals (list[int]): list containing the maximum number of modals to consider for each mode + cutoff (float): threshold value for including matrix elements into operator Returns: tuple: A tuple containing the following: - - dict: A dictionary containing the active Hamiltonian terms. - - dict: A dictionary containing the active Hamiltonian terms for all vibrational modes. - - int: total number of active terms in the Hamiltonian + - dict: dictionary containing the active Hamiltonian terms + - dict: dictionary containing the active Hamiltonian terms for all vibrational modes + - int: total number of active terms in the Hamiltonian """ active_ham_terms = {} @@ -114,9 +114,9 @@ def _find_active_terms(h_integrals, modals, cutoff): excitation_indices = idx[n + 1 :] exc_in_modals = True for m_idx, m in enumerate(modal_indices): - im = excitation_indices[m_idx] - jm = excitation_indices[m_idx + len(modal_indices)] - if im >= modals[m] or jm >= modals[m]: + i = excitation_indices[m_idx] + j = excitation_indices[m_idx + len(modal_indices)] + if i >= modals[m] or j >= modals[m]: exc_in_modals = False break if exc_in_modals: @@ -134,11 +134,11 @@ def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): r"""Calculates vibrational energy. Args: - h_mat (Array[Array[float]]): the Hamiltonian matrix - active_ham_terms (dict): A dictionary containing the active Hamiltonian terms - active_mode_terms (dict): A list containing the active Hamiltonian terms for all vibrational modes. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. - mode_rots (List[TensorLike[float]]): A list of rotation matrices for each vibrational mode. + h_mat (array[array[float]]): the Hamiltonian matrix + active_ham_terms (dict): dictionary containing the active Hamiltonian terms + active_mode_terms (dict): list containing the active Hamiltonian terms for all vibrational modes + modals (list[int]): list containing the maximum number of modals to consider for each mode + mode_rots (List[TensorLike[float]]): list of rotation matrices for each vibrational mode Returns: float: vibrational energy @@ -147,7 +147,7 @@ def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): nmodes = h_mat.shape[1] e0s = np.zeros(nmodes) for mode in range(nmodes): - fock_mat = _build_Fock( + fock_mat = _build_fock( mode, active_ham_terms, active_mode_terms[mode], modals, h_mat, mode_rots[mode] ) e0s[mode] = fock_mat[0, 0] @@ -159,16 +159,16 @@ def _vscf(h_integrals, modals, cutoff, tol=1e-8, max_iters=10000): r"""Performs the VSCF calculation. Args: - h_integrals (list(TensorLike[float])): a list containing Hamiltonian integral matrices - modals (list(int)): A list containing the maximum number of modals to consider for each mode. + h_integrals (list(TensorLike[float])): list containing Hamiltonian integral matrices + modals (list(int)): list containing the maximum number of modals to consider for each mode cutoff (float): threshold value for including matrix elements into operator. tol (float): convergence tolerance for vscf calculation - max_iters (int): Maximum number of iterations for vscf to converge. + max_iters (int): maximum number of iterations for vscf to converge Returns: tuple: A tuple of the following: - - float: vscf energy - - List[TensorLike[float]]: A list of rotation matrices for all vibrational modes. + - float: vscf energy + - list[TensorLike[float]]: list of rotation matrices for all vibrational modes """ @@ -187,15 +187,12 @@ def _vscf(h_integrals, modals, cutoff, tol=1e-8, max_iters=10000): e0 = _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots) enew = e0 + 2 * tol - curr_iter = 0 - while curr_iter <= max_iters and np.abs(enew - e0) > tol: + for curr_iter in range(max_iters): if curr_iter != 0: e0 = enew - curr_iter += 1 - for mode in range(nmodes): - fock = _build_Fock( + fock = _build_fock( mode, active_ham_terms, active_mode_terms[mode], modals, h_mat, mode_rots[mode] ) _, eigvec = np.linalg.eigh(fock) @@ -206,8 +203,11 @@ def _vscf(h_integrals, modals, cutoff, tol=1e-8, max_iters=10000): fock = np.transpose(eigvec) @ fock @ eigvec enew = _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots) - e0 = enew - return e0, mode_rots + + if np.abs(enew - e0) <= tol: + break + + return enew, mode_rots def _rotate_one_body(h1, nmodes, mode_rots, modals): @@ -217,10 +217,10 @@ def _rotate_one_body(h1, nmodes, mode_rots, modals): h1 (TensorLike[float]): one-body integrals nmodes (int): number of vibrational modes mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: - TensorLike[float]: rotated one-body integrals. + TensorLike[float]: rotated one-body integrals """ imax = np.max(modals) @@ -240,10 +240,10 @@ def _rotate_two_body(h2, nmodes, mode_rots, modals): h2 (TensorLike[float]): two-body integrals nmodes (int): number of vibrational modes mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: - TensorLike[float]: rotated two-body integrals. + TensorLike[float]: rotated two-body integrals """ imax = np.max(modals) @@ -271,10 +271,10 @@ def _rotate_three_body(h3, nmodes, mode_rots, modals): h3 (TensorLike[float]): three-body integrals nmodes (int): number of vibrational modes mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: - TensorLike[float]: rotated three-body integrals. + TensorLike[float]: rotated three-body integrals """ imax = np.max(modals) @@ -311,9 +311,9 @@ def _rotate_dipole(d_integrals, mode_rots, modals): r"""Generates VSCF rotated dipole. Args: - d_integrals (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. + d_integrals (list[TensorLike[float]]): list of n-mode expansion of dipole integrals mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: tuple(TensorLike[float]): a tuple of rotated dipole integrals @@ -354,12 +354,12 @@ def _rotate_hamiltonian(h_integrals, mode_rots, modals): r"""Generates VSCF rotated Hamiltonian. Args: - h_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + h_integrals (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes - modals (list[int]): A list containing the maximum number of modals to consider for each mode. + modals (list[int]): list containing the maximum number of modals to consider for each mode Returns: - tuple(TensorLike[float]): a tuple of rotated Hamiltonian integrals + tuple(TensorLike[float]): tuple of rotated Hamiltonian integrals """ @@ -389,9 +389,9 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: - h_integrals (list[TensorLike[float]]): list of Hamiltonian integrals for up to 3 coupled vibrational modes. + h_integrals (list[TensorLike[float]]): List of Hamiltonian integrals for up to 3 coupled vibrational modes. Look at the Usage Details for more information. - d_integrals (list[TensorLike[float]]): list of dipole integrals for up to 3 coupled vibrational modes. + d_integrals (list[TensorLike[float]]): List of dipole integrals for up to 3 coupled vibrational modes. Look at the Usage Details for more information. modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. @@ -401,8 +401,9 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto Returns: tuple: a tuple containing: - - List[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3 coupled vibrational modes. - - List[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3 coupled vibrational modes. 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pytest.importorskip("h5py") -cform_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S.hdf5" +cform_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S_cform_ham.hdf5" # Data was generated for H2S molecule with geometry (in Angstrom) # [['H', [0.0,-1.0,-1.0]], ['H', [0.0,1.0,-1.0]], ['S', [0.0,0.0,0.0]]], # basis=6-31g, quad_order=9 and nbos=4 for localized modes. 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zi~u9R2rvSS03*N%FanGKBftnS0*nA7zz8q`i~u9R2rvSS03*N%FanGKBftnS0*nA7 zzz8q`i~u9R2rvSS03*N%FanGKBftnS0*nA7zz8q`i~u9R2rvSS03*N%FanGKBftnS z0*nA7zz8q`i~u9R2rvSS03*N%FanGKBftnS0*nA7zz8q`i~u9R2rvSS03*N%FanGK zBftnS0*nA7zz8q`i~u9R2rvSS03*N%FanGKBftnS0*nA7zz8q`i~u9R2rvSS03*N% XFanGKBftnS0*nA7zz8q`e-ZdUmd15x literal 0 HcmV?d00001 From f37c8d1f5aa01a72fd317138ae54b08f2e86681e Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 16 Dec 2024 03:54:15 -0500 Subject: [PATCH 31/35] Black --- pennylane/qchem/__init__.py | 4 ++-- 1 file changed, 2 insertions(+), 2 deletions(-) diff --git a/pennylane/qchem/__init__.py b/pennylane/qchem/__init__.py index 5cac9e3230f..c74ae2aa949 100644 --- a/pennylane/qchem/__init__.py +++ b/pennylane/qchem/__init__.py @@ -90,5 +90,5 @@ taylor_coeffs, taylor_dipole_coeffs, taylor_hamiltonian, - vscf_integrals -) \ No newline at end of file + vscf_integrals, +) From d3a7c30f0bb575f01a204a4fd126201016534148 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Tue, 17 Dec 2024 03:50:23 -0500 Subject: [PATCH 32/35] Update doc/releases/changelog-dev.md Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- doc/releases/changelog-dev.md | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/doc/releases/changelog-dev.md b/doc/releases/changelog-dev.md index 8997017dc44..2b55a58abb8 100644 --- a/doc/releases/changelog-dev.md +++ b/doc/releases/changelog-dev.md @@ -203,7 +203,7 @@ such as `shots`, `rng` and `prng_key`. * Implemented wrapper function for vibrational Hamiltonian calculation and dataclass for storing the data. [(#6652)](https://github.com/PennyLaneAI/pennylane/pull/6652) - * Implemented functions for generating the vibrational Hamiltonian in vscf basis + * Implemented functions for generating the vibrational Hamiltonian in VSCF basis [(#6688)](https://github.com/PennyLaneAI/pennylane/pull/6688)

Improvements 🛠

From 0e29449ae6065142785c29cadf9bace537079ca7 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Tue, 17 Dec 2024 03:50:40 -0500 Subject: [PATCH 33/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 4 ++-- 1 file changed, 2 insertions(+), 2 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 40edd9fca52..18fafbf75f8 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -401,8 +401,8 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto Returns: tuple: a tuple containing: - - List[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3 coupled vibrational modes. - - List[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3 coupled vibrational modes. + - list[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3 coupled vibrational modes. + - list[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3 coupled vibrational modes. Returns ``None`` if d_integrals are not provided. **Example** From dcc84e84bd4b60d1ed038ad16197527a180ed07f Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Tue, 17 Dec 2024 03:50:50 -0500 Subject: [PATCH 34/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Austin Huang <65315367+austingmhuang@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 18fafbf75f8..eadcc2d77fa 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -403,7 +403,7 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto tuple: a tuple containing: - list[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3 coupled vibrational modes. - list[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3 coupled vibrational modes. - Returns ``None`` if d_integrals are not provided. + Returns ``None`` if ``d_integrals`` are ``None``. **Example** From d1490614cc19e0a44efc1dda2938ea478248430a Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Tue, 17 Dec 2024 03:52:44 -0500 Subject: [PATCH 35/35] Addressed codefactor warning --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index eadcc2d77fa..e08e0d15580 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -15,7 +15,7 @@ import numpy as np -# pylint: disable=too-many-arguments +# pylint: disable=too-many-arguments, too-many-positional-arguments def _build_fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot):

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b/tests/qchem/vibrational/test_vscf.py index cec93ed4048..d6c62561a01 100644 --- a/tests/qchem/vibrational/test_vscf.py +++ b/tests/qchem/vibrational/test_vscf.py @@ -19,6 +19,7 @@ import numpy as np import pytest +from pennylane.qchem import vibrational from pennylane.qchem.vibrational import vscf # pylint: disable=protected-access @@ -27,23 +28,66 @@ cform_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S.hdf5" -with h5py.File(cform_file, "r+") as f: +with h5py.File(cform_file, "r") as f: h1_h2s = f["H1"][()] h2_h2s = f["H2"][()] h3_h2s = f["H3"][()] + d1_h2s = f["D1"][()] + d2_h2s = f["D2"][()] + d3_h2s = f["D3"][()] h_data_h2s = [h1_h2s, h2_h2s, h3_h2s] - +dip_data_h2s = [d1_h2s, d2_h2s, d3_h2s] result_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S_vscf_result.hdf5" -with h5py.File(result_file, "r+") as f: +with h5py.File(result_file, "r") as f: h1_h2s = f["H1_rot"][()] h2_h2s = f["H2_rot"][()] h3_h2s = f["H3_rot"][()] + d1_h2s = f["D1_rot"][()] + d2_h2s = f["D2_rot"][()] + d3_h2s = f["D3_rot"][()] energy = f["energy"][()] u_mat = f["u_mat"][()] -h2s_exp_result = {"h_data": [h1_h2s, h2_h2s, h3_h2s], "energy": energy, "u_mat": u_mat} +h2s_exp_result = { + "h_data": [h1_h2s, h2_h2s, h3_h2s], + "dip_data": [d1_h2s, d2_h2s, d3_h2s], + "energy": energy, + "u_mat": u_mat, +} + + +def test_error_vscf_hamiltonian(): + r"""Test that an error is raised if wrong shape is provided for Hamiltonian""" + with pytest.raises( + ValueError, match="Building n-mode Hamiltonian is not implemented for n equal to 4" + ): + vibrational.vscf_hamiltonian(ham_data=[1, 2, 3, 4]) + + +def test_error_vscf_dipole(): + r"""Test that an error is raised if wrong shape is provided for dipole.""" + with pytest.raises( + ValueError, match="Building n-mode dipole is not implemented for n equal to 4" + ): + vibrational.vscf_hamiltonian(ham_data=[1, 2, 3], dipole_data=[1, 2, 3, 4]) + + +@pytest.mark.parametrize( + ("h_data"), + [ + (h_data_h2s), + ], +) +def test_modal_error(h_data): + r"""Test that an error is raised if number of modals provided is incorrect""" + + with pytest.raises( + ValueError, + match="Number of maximum modals cannot be greater than the modals for unrotated integrals.", + ): + vibrational.vscf_hamiltonian(ham_data=h_data, modals=[5, 5, 5]) @pytest.mark.parametrize( @@ -55,11 +99,31 @@ def test_vscf_calculation(h_data, h2s_result): r"""Test that vscf calculation produces correct energy and rotation matrices""" - vib_energy, rot_matrix = vscf._vscf(h_data, modals=[4,4,4], cutoff=1e-8) + vib_energy, rot_matrix = vscf._vscf(h_data, modals=[4, 4, 4], cutoff=1e-8) assert np.isclose(vib_energy, h2s_result["energy"]) assert np.allclose(rot_matrix, h2s_result["u_mat"]) +@pytest.mark.parametrize( + ("h_data", "dip_data", "h2s_result"), + [ + (h_data_h2s, dip_data_h2s, h2s_exp_result), + ], +) +def test_vscf_hamiltonian_dipole(h_data, dip_data, h2s_result): + r"""Test that correct rotated Hamiltonian and dipole is produced.""" + result_h, result_dip = vscf.vscf_hamiltonian(h_data, dip_data, modals=[3, 3, 3], cutoff=1e-8) + + expected_h = h2s_result["h_data"] + expected_dip = h2s_result["dip_data"] + assert np.allclose(result_h[0], expected_h[0]) + assert np.allclose(result_h[1], expected_h[1]) + assert np.allclose(result_h[2], expected_h[2]) + assert np.allclose(result_dip[0], expected_dip[0]) + assert np.allclose(result_dip[1], expected_dip[1]) + assert np.allclose(result_dip[2], expected_dip[2]) + + @pytest.mark.parametrize( ("h_data", "h2s_result"), [ @@ -68,10 +132,12 @@ def test_vscf_calculation(h_data, h2s_result): ) def test_vscf_hamiltonian(h_data, h2s_result): r"""Test that correct rotated Hamiltonian is produced.""" - - result_h = vscf.vscf_hamiltonian(h_data, modals=[3, 3, 3], cutoff=1e-8) + result_h, result_dip = vscf.vscf_hamiltonian(h_data, modals=[3, 3, 3], cutoff=1e-8) expected_h = h2s_result["h_data"] + assert np.allclose(result_h[0], expected_h[0]) assert np.allclose(result_h[1], expected_h[1]) assert np.allclose(result_h[2], expected_h[2]) + + assert result_dip is None From b6283599dfbe5372a9c6f51056f00e0afba62546 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 9 Dec 2024 14:51:06 -0500 Subject: [PATCH 04/35] Fixed errors --- pennylane/qchem/vibrational/__init__.py | 1 - pennylane/qchem/vibrational/vscf.py | 6 ++++-- 2 files changed, 4 insertions(+), 3 deletions(-) diff --git a/pennylane/qchem/vibrational/__init__.py b/pennylane/qchem/vibrational/__init__.py index 2c68f853b7e..5c088e890a3 100644 --- a/pennylane/qchem/vibrational/__init__.py +++ b/pennylane/qchem/vibrational/__init__.py @@ -5,4 +5,3 @@ from .localize_modes import localize_normal_modes from .vibrational_class import VibrationalPES, optimize_geometry from .vscf import vscf_hamiltonian - diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index ab94b67106d..4baa59cad16 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -41,7 +41,8 @@ def _build_Fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): if mode in modal_indices: modal_idx = modal_indices.index(mode) - + else: + continue im = excitation_indices[modal_idx] jm = excitation_indices[modal_idx + len(modal_indices)] if im < modals[mode] and jm < modals[mode]: @@ -78,7 +79,8 @@ def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): if mode in modal_indices: modal_idx = modal_indices.index(mode) - + else: + continue im = excitation_indices[modal_idx] jm = excitation_indices[modal_idx + len(modal_indices)] From e9a7050cfdbf1abe60e15672463c7e11091229aa Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Mon, 9 Dec 2024 14:58:48 -0500 Subject: [PATCH 05/35] Updated reference files --- .../qchem/vibrational/test_ref_files/H2S.hdf5 | Bin 0 -> 3618304 bytes .../test_ref_files/H2S_dipole.hdf5 | Bin 0 -> 2712704 bytes 2 files changed, 0 insertions(+), 0 deletions(-) create mode 100644 tests/qchem/vibrational/test_ref_files/H2S.hdf5 create mode 100644 tests/qchem/vibrational/test_ref_files/H2S_dipole.hdf5 diff --git a/tests/qchem/vibrational/test_ref_files/H2S.hdf5 b/tests/qchem/vibrational/test_ref_files/H2S.hdf5 new file mode 100644 index 0000000000000000000000000000000000000000..4161e01aab817570f308e75315763f0c87bc4f48 GIT binary patch literal 3618304 zcmeF(1z1(x+BbT_?(RlKMJx=gu@nnT$}U9g#CimL?C!u03`DW9Fvqexun+^pZWL57 z;mqm$kLO(PdOzRiJ?DJixxVY1|K8WN*_+L?#+tu--DAvg-*c>4u1%X~&r&3dmHw|x znXJ-T<@)_!)qkYnUskp2{QlKH{~LecgP+#;ITJs(+8F=E+DiYol~p19J~v+9^6$Jo zn>Dl2{!+cZ`iXzcs#-eZzp2+zzvs{Ye+alXYwWIHX(wE+Gk#vc=M4YT%C)-j-&||p zr<3usDSqD+zi*1)tIusInBsHophRgv`-~GydFaqI%01sXu=Hzw^VZ zZM&w{RvD~HVYrDmvj3L@SHSu>$ne+LAsQVRGFqpMkLZ2CX^0e-FK zlbIR*>%aS-{r~>w&y^8J>kLMC)#a(5>T~s{pX%?_&p-X0`n|38xzb1azy3L#m>CwX z|ItKccsj2n)_s^>eUk z>%LK+CY=Z{P3U#}?y}GA&DFY1uiGY|j_KC^b(vPI@HDI6&krv>J#5JmQ_V|FUzgu7 z%-sKI*EUWSJxuEF>)`kAdW7__Tfg4qG34BV$>D#S)$6FgSHJHTu=4o2<6BHMt9JN3 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z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 z6JP>NfC(@GCcp%k025#WOn?b60Vco%m;e)C0!)AjFaajO1egF5U;<2l2`~XBzyz28 K6JP>41pW{BMF>Lx literal 0 HcmV?d00001 From 353b8b1e93d2466c757c89c0a8a7af430ec89964 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Tue, 10 Dec 2024 12:07:51 -0500 Subject: [PATCH 06/35] Fixed some codecov --- pennylane/qchem/vibrational/vscf.py | 13 ++----------- 1 file changed, 2 insertions(+), 11 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 4baa59cad16..a3cdeebb102 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -39,10 +39,7 @@ def _build_Fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): modal_indices = [*ham_term[1]] excitation_indices = [*ham_term[2]] - if mode in modal_indices: - modal_idx = modal_indices.index(mode) - else: - continue + modal_idx = modal_indices.index(mode) im = excitation_indices[modal_idx] jm = excitation_indices[modal_idx + len(modal_indices)] if im < modals[mode] and jm < modals[mode]: @@ -77,10 +74,7 @@ def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): modal_indices = ham_term[1] excitation_indices = ham_term[2] - if mode in modal_indices: - modal_idx = modal_indices.index(mode) - else: - continue + modal_idx = modal_indices.index(mode) im = excitation_indices[modal_idx] jm = excitation_indices[modal_idx + len(modal_indices)] @@ -335,9 +329,6 @@ def _rotate_dipole(dipole_data, mode_rots, modals): """ n = len(dipole_data) - if n > 3: - raise ValueError(f"Building n-mode dipole not implemented for {n}=>3!") - nmodes = np.shape(dipole_data[0])[0] imax = np.max(modals) d1_rot = np.zeros((3, nmodes, imax, imax)) From 8f16c8a7b947f1f17ff21ee9fb7c769b0b42e931 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 02:13:24 -0500 Subject: [PATCH 07/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index a3cdeebb102..a13978bb95c 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -141,7 +141,7 @@ def _find_active_terms(ham_data, modals, cutoff): def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): - r"""Calculates vibrational energy + r"""Calculates vibrational energy. Args: h_mat (Array[Array[float]]): the Hamiltonian matrix From 4bd9c271345f00743eda4f6e77247a8a6ba57c8c Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 02:13:45 -0500 Subject: [PATCH 08/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 10 +++++----- 1 file changed, 5 insertions(+), 5 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index a13978bb95c..a04349b76e9 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -392,11 +392,11 @@ def vscf_hamiltonian(ham_data, dipole_data=None, modals=None, cutoff=None, cutof r"""Generates VSCF rotated integrals for vibrational Hamiltonian. Args: - ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. - dipole_data (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. Default is ``None``. - modals (list[int]): A list containing the maximum number of modals to consider for each mode. Defalt to maximum number of modals. - cutoff (float): threshold value for including matrix elements into operator. - cutoff_ratio (float): Default ratio for zeroing elements which are smaller than this ratio with respect to biggest element in all integrals. Default value is ``1e-6``. + ham_data (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals + dipole_data (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. + modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default to maximum number of modals. + cutoff (float): threshold value for including matrix elements into operator + cutoff_ratio (float): ratio for discarding elements with respect to biggest element in the integrals. Default value is ``1e-6``. Returns: List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. From 26cf957338625a6ab4c8611de7c7225eee0c1384 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 02:14:10 -0500 Subject: [PATCH 09/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index a04349b76e9..6ab1ea840d3 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -388,7 +388,7 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): return h_data -def vscf_hamiltonian(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): +def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates VSCF rotated integrals for vibrational Hamiltonian. Args: From b2fc51220613f6920b22d11c3822d0b57c1ad57f Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Thu, 12 Dec 2024 07:39:05 -0500 Subject: [PATCH 10/35] Increased test coverage and addressed comments --- pennylane/qchem/__init__.py | 2 +- pennylane/qchem/vibrational/__init__.py | 15 ++++++- pennylane/qchem/vibrational/vscf.py | 41 ++++++++---------- .../test_ref_files/H2S_vscf_result.hdf5 | Bin 659328 -> 679808 bytes tests/qchem/vibrational/test_vscf.py | 33 +++++++------- 5 files changed, 49 insertions(+), 42 deletions(-) diff --git a/pennylane/qchem/__init__.py b/pennylane/qchem/__init__.py index b84bf541b5f..6db74e9e2d5 100644 --- a/pennylane/qchem/__init__.py +++ b/pennylane/qchem/__init__.py @@ -82,4 +82,4 @@ taper_hf, taper_operation, ) -from .vibrational import optimize_geometry, localize_normal_modes, VibrationalPES, vscf_hamiltonian +from .vibrational import optimize_geometry, localize_normal_modes, VibrationalPES, vscf_integrals diff --git a/pennylane/qchem/vibrational/__init__.py b/pennylane/qchem/vibrational/__init__.py index 5c088e890a3..f6a2ec75739 100644 --- a/pennylane/qchem/vibrational/__init__.py +++ b/pennylane/qchem/vibrational/__init__.py @@ -1,7 +1,20 @@ +# Copyright 2018-2024 Xanadu Quantum Technologies Inc. + +# Licensed under the Apache License, Version 2.0 (the "License"); +# you may not use this file except in compliance with the License. +# You may obtain a copy of the License at + +# http://www.apache.org/licenses/LICENSE-2.0 + +# Unless required by applicable law or agreed to in writing, software +# distributed under the License is distributed on an "AS IS" BASIS, +# WITHOUT WARRANTIES OR CONDITIONS OF ANY KIND, either express or implied. +# See the License for the specific language governing permissions and +# limitations under the License. """ This submodule provides the functionality to calculate vibrational Hamiltonians. """ from .localize_modes import localize_normal_modes from .vibrational_class import VibrationalPES, optimize_geometry -from .vscf import vscf_hamiltonian +from .vscf import vscf_integrals diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 6ab1ea840d3..3f3a16c2947 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -53,7 +53,7 @@ def _build_Fock(mode, active_ham_terms, active_terms, modals, h_mat, mode_rot): def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): - r"""Updates value of h matrix for a mode after other modes have been rotated. + r"""Updates value of Hamiltonian matrix for a mode after other modes have been rotated. Args: h_mat (Array[Array[float]]): the hamiltonian matrix @@ -85,7 +85,9 @@ def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): def _find_active_terms(ham_data, modals, cutoff): - r"""Identifies the active terms in the Hamiltonian + r"""Identifies the active terms in the Hamiltonian, following the equations 20-22 + in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. + The equation suggests that if mode m is not contained in a Hamiltonian term, it evaluates to zero. Args: ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. @@ -104,39 +106,29 @@ def _find_active_terms(ham_data, modals, cutoff): nmodes = np.shape(ham_data[0])[0] for n, ham_n in enumerate(ham_data): - ham_n = ham_data[n] for idx, h_val in np.ndenumerate(ham_n): if np.abs(h_val) < cutoff: continue - M_arr = idx[: n + 1] + modal_indices = idx[: n + 1] - right_order = True - for i in range(n): - if M_arr[i] <= M_arr[i + 1]: - right_order = False - break - - if right_order: - exc_arr = idx[n + 1 :] + if all(modal_indices[i] > modal_indices[i + 1] for i in range(n)): + excitation_indices = idx[n + 1 :] exc_in_modals = True - for m_idx, m in enumerate(M_arr): - im = exc_arr[m_idx] - jm = exc_arr[m_idx + len(M_arr)] + for m_idx, m in enumerate(modal_indices): + im = excitation_indices[m_idx] + jm = excitation_indices[m_idx + len(modal_indices)] if im >= modals[m] or jm >= modals[m]: exc_in_modals = False break if exc_in_modals: - active_ham_terms[active_num] = [h_val, M_arr, exc_arr] + active_ham_terms[active_num] = [h_val, modal_indices, excitation_indices] active_num += 1 - active_mode_terms = {} - for m in range(nmodes): - ts_for_m_arr = [] - for t in range(active_num): - if m in active_ham_terms[t][1]: - ts_for_m_arr.append(t) - active_mode_terms[m] = ts_for_m_arr + active_mode_terms = { + m: [t for t in range(active_num) if m in active_ham_terms[t][1]] for m in range(nmodes) + } + return active_ham_terms, active_mode_terms, active_num @@ -389,7 +381,8 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): - r"""Generates VSCF rotated integrals for vibrational Hamiltonian. + r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. + This implementation is based on `J. Chem. Theory Comput. 2010, 6, 235–248 `_. 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vibrational.vscf_hamiltonian(ham_data=[1, 2, 3, 4]) + vibrational.vscf_integrals(ham_data=[1, 2, 3, 4]) def test_error_vscf_dipole(): @@ -71,7 +74,7 @@ def test_error_vscf_dipole(): with pytest.raises( ValueError, match="Building n-mode dipole is not implemented for n equal to 4" ): - vibrational.vscf_hamiltonian(ham_data=[1, 2, 3], dipole_data=[1, 2, 3, 4]) + vibrational.vscf_integrals(ham_data=[1, 2, 3], dipole_data=[1, 2, 3, 4]) @pytest.mark.parametrize( @@ -87,7 +90,7 @@ def test_modal_error(h_data): ValueError, match="Number of maximum modals cannot be greater than the modals for unrotated integrals.", ): - vibrational.vscf_hamiltonian(ham_data=h_data, modals=[5, 5, 5]) + vibrational.vscf_integrals(ham_data=h_data, modals=[5, 5, 5]) @pytest.mark.parametrize( @@ -99,7 +102,7 @@ def test_modal_error(h_data): def test_vscf_calculation(h_data, h2s_result): r"""Test that vscf calculation produces correct energy and rotation matrices""" - vib_energy, rot_matrix = vscf._vscf(h_data, modals=[4, 4, 4], cutoff=1e-8) + vib_energy, rot_matrix = vscf._vscf(h_data, modals=[3, 3, 3], cutoff=1e-8) assert np.isclose(vib_energy, h2s_result["energy"]) assert np.allclose(rot_matrix, h2s_result["u_mat"]) @@ -110,9 +113,9 @@ def test_vscf_calculation(h_data, h2s_result): (h_data_h2s, dip_data_h2s, h2s_exp_result), ], ) -def test_vscf_hamiltonian_dipole(h_data, dip_data, h2s_result): +def test_vscf_integrals_dipole(h_data, dip_data, h2s_result): r"""Test that correct rotated Hamiltonian and dipole is produced.""" - result_h, result_dip = vscf.vscf_hamiltonian(h_data, dip_data, modals=[3, 3, 3], cutoff=1e-8) + result_h, result_dip = vscf.vscf_integrals(h_data, dip_data, modals=[3, 3, 3], cutoff=1e-8) expected_h = h2s_result["h_data"] expected_dip = h2s_result["dip_data"] @@ -125,19 +128,17 @@ def test_vscf_hamiltonian_dipole(h_data, dip_data, h2s_result): @pytest.mark.parametrize( - ("h_data", "h2s_result"), + ("h_data", "h2s_result", "modals", "cutoff"), [ - (h_data_h2s, h2s_exp_result), + (h_data_h2s, h2s_exp_result["h_data"], [3, 3, 3], 1e-8), + (h_data_h2s[0:2], h2s_exp_result["h_full"], None, None), ], ) -def test_vscf_hamiltonian(h_data, h2s_result): +def test_vscf_integrals(h_data, h2s_result, modals, cutoff): r"""Test that correct rotated Hamiltonian is produced.""" - result_h, result_dip = vscf.vscf_hamiltonian(h_data, modals=[3, 3, 3], cutoff=1e-8) - - expected_h = h2s_result["h_data"] + result_h, result_dip = vscf.vscf_integrals(h_data, modals=modals, cutoff=cutoff) - assert np.allclose(result_h[0], expected_h[0]) - assert np.allclose(result_h[1], expected_h[1]) - assert np.allclose(result_h[2], expected_h[2]) + for idx, h in enumerate(result_h): + assert np.allclose(h, h2s_result[idx]) assert result_dip is None From 149eb478f1ca9d47b0bb748cd52bca8925afe9f0 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Thu, 12 Dec 2024 07:48:22 -0500 Subject: [PATCH 11/35] Minor docstring change --- pennylane/qchem/vibrational/vscf.py | 3 ++- 1 file changed, 2 insertions(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3f3a16c2947..299c886fc8c 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -382,7 +382,8 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. - This implementation is based on `J. Chem. Theory Comput. 2010, 6, 235–248 `_. + This implementation is based on the method described in + `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: ham_data (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals From 8009e7b65fa64118411cdd4ed4c1a42c4fc24b25 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 09:06:00 -0500 Subject: [PATCH 12/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 1 + 1 file changed, 1 insertion(+) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 299c886fc8c..35b91c11fbe 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -382,6 +382,7 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. + This implementation is based on the method described in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. From f9fa41f17c18ed258b82ffc590cbddf28f30cefc Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 09:06:08 -0500 Subject: [PATCH 13/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 35b91c11fbe..3abec995c5a 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -389,7 +389,7 @@ def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ Args: ham_data (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals dipole_data (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. - modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default to maximum number of modals. + modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. cutoff (float): threshold value for including matrix elements into operator cutoff_ratio (float): ratio for discarding elements with respect to biggest element in the integrals. Default value is ``1e-6``. From c1d0859309b23dd7eaba80f8cf62c7fe777c5683 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 09:06:14 -0500 Subject: [PATCH 14/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3abec995c5a..f84b81c1d3b 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -380,7 +380,7 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): return h_data -def vscf_integrals(ham_data, dipole_data=None, modals=None, cutoff=None, cutoff_ratio=1e-6): +def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. This implementation is based on the method described in From dbf7215c1f74574fca1f22aa7f8a78bb2c8bdff9 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Thu, 12 Dec 2024 09:06:23 -0500 Subject: [PATCH 15/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 4 ++-- 1 file changed, 2 insertions(+), 2 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index f84b81c1d3b..69144709cc5 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -387,8 +387,8 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: - ham_data (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals - dipole_data (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. + h_integrals (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals + d_integrals (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. cutoff (float): threshold value for including matrix elements into operator cutoff_ratio (float): ratio for discarding elements with respect to biggest element in the integrals. Default value is ``1e-6``. From 11dfcf7968f6bb800b28368d837338a04408aa11 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Thu, 12 Dec 2024 09:49:07 -0500 Subject: [PATCH 16/35] Added example --- pennylane/qchem/vibrational/vscf.py | 97 +++++++++++++++++----------- tests/qchem/vibrational/test_vscf.py | 9 ++- 2 files changed, 64 insertions(+), 42 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 69144709cc5..3ac47202727 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -84,13 +84,13 @@ def _update_h(h_mat, mode, active_ham_terms, mode_rot, ts_act, modals): return h_mat -def _find_active_terms(ham_data, modals, cutoff): +def _find_active_terms(h_integrals, modals, cutoff): r"""Identifies the active terms in the Hamiltonian, following the equations 20-22 in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. The equation suggests that if mode m is not contained in a Hamiltonian term, it evaluates to zero. Args: - ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + h_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. modals (list[int]): A list containing the maximum number of modals to consider for each mode. cutoff (float): threshold value for including matrix elements into operator. @@ -103,9 +103,9 @@ def _find_active_terms(ham_data, modals, cutoff): """ active_ham_terms = {} active_num = 0 - nmodes = np.shape(ham_data[0])[0] + nmodes = np.shape(h_integrals[0])[0] - for n, ham_n in enumerate(ham_data): + for n, ham_n in enumerate(h_integrals): for idx, h_val in np.ndenumerate(ham_n): if np.abs(h_val) < cutoff: continue @@ -157,11 +157,11 @@ def _fock_energy(h_mat, active_ham_terms, active_mode_terms, modals, mode_rots): return np.sum(e0s) -def _vscf(ham_data, modals, cutoff, tol=1e-8, max_iters=10000): +def _vscf(h_integrals, modals, cutoff, tol=1e-8, max_iters=10000): r"""Performs the VSCF calculation. Args: - ham_data (list(TensorLike[float])): a list containing Hamiltonian integral matrices + h_integrals (list(TensorLike[float])): a list containing Hamiltonian integral matrices modals (list(int)): A list containing the maximum number of modals to consider for each mode. cutoff (float): threshold value for including matrix elements into operator. tol (float): convergence tolerance for vscf calculation @@ -174,9 +174,11 @@ def _vscf(ham_data, modals, cutoff, tol=1e-8, max_iters=10000): """ - nmodes = np.shape(ham_data[0])[0] + nmodes = np.shape(h_integrals[0])[0] - active_ham_terms, active_mode_terms, active_num = _find_active_terms(ham_data, modals, cutoff) + active_ham_terms, active_mode_terms, active_num = _find_active_terms( + h_integrals, modals, cutoff + ) mode_rots = [np.eye(modals[mode]) for mode in range(nmodes)] h_mat = np.zeros((active_num, nmodes)) for mode in range(nmodes): @@ -307,11 +309,11 @@ def _rotate_three_body(h3, nmodes, mode_rots, modals): return h3_rot -def _rotate_dipole(dipole_data, mode_rots, modals): +def _rotate_dipole(d_integrals, mode_rots, modals): r"""Generates VSCF rotated dipole. Args: - dipole_data (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. + d_integrals (list[TensorLike[float]]): A list of n-mode expansion of dipole integrals. mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes modals (list[int]): A list containing the maximum number of modals to consider for each mode. @@ -319,15 +321,15 @@ def _rotate_dipole(dipole_data, mode_rots, modals): tuple(TensorLike[float]): a tuple of rotated dipole integrals """ - n = len(dipole_data) + n = len(d_integrals) - nmodes = np.shape(dipole_data[0])[0] + nmodes = np.shape(d_integrals[0])[0] imax = np.max(modals) d1_rot = np.zeros((3, nmodes, imax, imax)) for alpha in range(3): d1_rot[alpha, ::] = _rotate_one_body( - dipole_data[0][alpha, ::], nmodes, mode_rots, modals=modals + d_integrals[0][alpha, ::], nmodes, mode_rots, modals=modals ) dip_data = [d1_rot] @@ -335,7 +337,7 @@ def _rotate_dipole(dipole_data, mode_rots, modals): d2_rot = np.zeros((3, nmodes, nmodes, imax, imax, imax, imax)) for alpha in range(3): d2_rot[alpha, ::] = _rotate_two_body( - dipole_data[1][alpha, ::], nmodes, mode_rots, modals=modals + d_integrals[1][alpha, ::], nmodes, mode_rots, modals=modals ) dip_data = [d1_rot, d2_rot] @@ -343,18 +345,18 @@ def _rotate_dipole(dipole_data, mode_rots, modals): d3_rot = np.zeros((3, nmodes, nmodes, nmodes, imax, imax, imax, imax, imax, imax)) for alpha in range(3): d3_rot[alpha, ::] = _rotate_three_body( - dipole_data[2][alpha, ::], nmodes, mode_rots, modals=modals + d_integrals[2][alpha, ::], nmodes, mode_rots, modals=modals ) dip_data = [d1_rot, d2_rot, d3_rot] return dip_data -def _rotate_hamiltonian(ham_data, mode_rots, modals): +def _rotate_hamiltonian(h_integrals, mode_rots, modals): r"""Generates VSCF rotated Hamiltonian. Args: - ham_data (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. + h_integrals (list[TensorLike[float]]): A list of n-mode expansion of Hamiltonian integrals. mode_rots (list[TensorLike[float]]): list of rotation matrices for all vibrational modes modals (list[int]): A list containing the maximum number of modals to consider for each mode. @@ -363,18 +365,18 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): """ - n = len(ham_data) - nmodes = np.shape(ham_data[0])[0] + n = len(h_integrals) + nmodes = np.shape(h_integrals[0])[0] - h1_rot = _rotate_one_body(ham_data[0], nmodes, mode_rots, modals) + h1_rot = _rotate_one_body(h_integrals[0], nmodes, mode_rots, modals) h_data = [h1_rot] if n > 1: - h2_rot = _rotate_two_body(ham_data[1], nmodes, mode_rots, modals) + h2_rot = _rotate_two_body(h_integrals[1], nmodes, mode_rots, modals) h_data = [h1_rot, h2_rot] if n > 2: - h3_rot = _rotate_three_body(ham_data[2], nmodes, mode_rots, modals) + h3_rot = _rotate_three_body(h_integrals[2], nmodes, mode_rots, modals) h_data = [h1_rot, h2_rot, h3_rot] return h_data @@ -382,36 +384,53 @@ def _rotate_hamiltonian(ham_data, mode_rots, modals): def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. - + This implementation is based on the method described in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: h_integrals (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals d_integrals (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. - modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. + modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. + Default value is the maximum number of modals. cutoff (float): threshold value for including matrix elements into operator - cutoff_ratio (float): ratio for discarding elements with respect to biggest element in the integrals. Default value is ``1e-6``. + cutoff_ratio (float): ratio for discarding elements with respect to biggest element in the integrals. + Default value is ``1e-6``. Returns: - List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. - + tuple: A tuple of the following: + - List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. + - List[TensorLike[float]]: List of n-mode expansion of dipole integrals in VSCF basis, + returns ``None`` if d_integrals are not provided. + + **Example** + + >>> h1 = np.array([[[0.00968289, 0.00233724, 0.0007408, 0.00199125], + ... [0.00233724, 0.02958449, 0.00675431, 0.0021936], + ... [0.0007408, 0.00675431, 0.0506012, 0.01280986], + ... [0.00199125, 0.0021936, 0.01280986, 0.07282307]]]) + >>> qml.qchem.vcf_integrals(h_integrals=[h1], modals=[4,4,4]) + ([[[ 9.36124041e-03, 3.63798208e-19, -3.42019607e-19, -3.83743044e-19], + [ 9.59982270e-19, 2.77803512e-02, 5.18290259e-18, -4.82000376e-18], + [-2.73826508e-19, 4.88583546e-18, 4.63297357e-02, -2.87022759e-18], + [-1.94549340e-19, -5.48544743e-18, -1.41379640e-18, 7.92203227e-02]]], + None) """ - if len(ham_data) > 3: + if len(h_integrals) > 3: raise ValueError( - f"Building n-mode Hamiltonian is not implemented for n equal to {len(ham_data)}." + f"Building n-mode Hamiltonian is not implemented for n equal to {len(h_integrals)}." ) - if dipole_data is not None: - if len(dipole_data) > 3: + if d_integrals is not None: + if len(d_integrals) > 3: raise ValueError( - f"Building n-mode dipole is not implemented for n equal to {len(dipole_data)}." + f"Building n-mode dipole is not implemented for n equal to {len(d_integrals)}." ) - nmodes = np.shape(ham_data[0])[0] + nmodes = np.shape(h_integrals[0])[0] - imax = np.shape(ham_data[0])[1] + imax = np.shape(h_integrals[0])[1] max_modals = nmodes * [imax] if modals is None: modals = max_modals @@ -423,15 +442,15 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto imax = np.max(modals) if cutoff is None: - max_val = np.max([np.max(np.abs(H)) for H in ham_data]) + max_val = np.max([np.max(np.abs(H)) for H in h_integrals]) cutoff = max_val * cutoff_ratio - _, mode_rots = _vscf(ham_data, modals=max_modals, cutoff=cutoff) + _, mode_rots = _vscf(h_integrals, modals=max_modals, cutoff=cutoff) - h_data = _rotate_hamiltonian(ham_data, mode_rots, modals) + h_data = _rotate_hamiltonian(h_integrals, mode_rots, modals) - if dipole_data is not None: - dip_data = _rotate_dipole(dipole_data, mode_rots, modals) + if d_integrals is not None: + dip_data = _rotate_dipole(d_integrals, mode_rots, modals) return h_data, dip_data return h_data, None diff --git a/tests/qchem/vibrational/test_vscf.py b/tests/qchem/vibrational/test_vscf.py index 9e8a11dfc78..b2effbf185b 100644 --- a/tests/qchem/vibrational/test_vscf.py +++ b/tests/qchem/vibrational/test_vscf.py @@ -27,6 +27,9 @@ h5py = pytest.importorskip("h5py") cform_file = Path(__file__).resolve().parent / "test_ref_files" / "H2S.hdf5" +# Data was generated for H2S molecule with geometry (in Angstrom) +# [['H', [0.0,-1.0,-1.0]], ['H', [0.0,1.0,-1.0]], ['S', [0.0,0.0,0.0]]], +# basis=6-31g, quad_order=9 and nbos=4 for localized modes. with h5py.File(cform_file, "r") as f: h1_h2s = f["H1"][()] @@ -66,7 +69,7 @@ def test_error_vscf_integrals(): with pytest.raises( ValueError, match="Building n-mode Hamiltonian is not implemented for n equal to 4" ): - vibrational.vscf_integrals(ham_data=[1, 2, 3, 4]) + vibrational.vscf_integrals(h_integrals=[1, 2, 3, 4]) def test_error_vscf_dipole(): @@ -74,7 +77,7 @@ def test_error_vscf_dipole(): with pytest.raises( ValueError, match="Building n-mode dipole is not implemented for n equal to 4" ): - vibrational.vscf_integrals(ham_data=[1, 2, 3], dipole_data=[1, 2, 3, 4]) + vibrational.vscf_integrals(h_integrals=[1, 2, 3], d_integrals=[1, 2, 3, 4]) @pytest.mark.parametrize( @@ -90,7 +93,7 @@ def test_modal_error(h_data): ValueError, match="Number of maximum modals cannot be greater than the modals for unrotated integrals.", ): - vibrational.vscf_integrals(ham_data=h_data, modals=[5, 5, 5]) + vibrational.vscf_integrals(h_integrals=h_data, modals=[5, 5, 5]) @pytest.mark.parametrize( From aaf0703c625ee928b64ef3a603165dc598dd9716 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 02:06:44 -0500 Subject: [PATCH 17/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3ac47202727..5ff6c9c4e00 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -385,7 +385,7 @@ def _rotate_hamiltonian(h_integrals, mode_rots, modals): def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. - This implementation is based on the method described in + This function converts the Christiansen vibrational Hamiltonian integrals obtained in the harmonic oscillator basis to integrals in the vibrational self-consistent field (VSCF) basis. The implementation is based on the method described in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: From d5e93dfe9ec581aca201fbdd01a65df43a847ace Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Fri, 13 Dec 2024 10:19:56 -0500 Subject: [PATCH 18/35] Improved docstring --- pennylane/qchem/vibrational/vscf.py | 56 ++++++++++++++++++++++------- 1 file changed, 44 insertions(+), 12 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 5ff6c9c4e00..3412741678a 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -385,12 +385,16 @@ def _rotate_hamiltonian(h_integrals, mode_rots, modals): def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cutoff_ratio=1e-6): r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. - This function converts the Christiansen vibrational Hamiltonian integrals obtained in the harmonic oscillator basis to integrals in the vibrational self-consistent field (VSCF) basis. The implementation is based on the method described in + This function converts the Christiansen vibrational Hamiltonian integrals obtained in the harmonic + oscillator basis to integrals in the vibrational self-consistent field (VSCF) basis. + The implementation is based on the method described in `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: - h_integrals (list[TensorLike[float]]): list of n-mode expansion of Hamiltonian integrals - d_integrals (list[TensorLike[float]]): list of n-mode expansion of dipole integrals. Default is ``None``. + h_integrals (list[TensorLike[float]]): List of Hamiltonian integrals for up to 3-coupled vibrational modes. + Look at the `Usage Details` for more details on dimensions of tensors. + d_integrals (list[TensorLike[float]]): List of dipole integrals for up to 3-coupled vibrational modes. + Look at the `Usage Details` for more details on dimensions of tensors. modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. cutoff (float): threshold value for including matrix elements into operator @@ -406,15 +410,43 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto **Example** >>> h1 = np.array([[[0.00968289, 0.00233724, 0.0007408, 0.00199125], - ... [0.00233724, 0.02958449, 0.00675431, 0.0021936], - ... [0.0007408, 0.00675431, 0.0506012, 0.01280986], - ... [0.00199125, 0.0021936, 0.01280986, 0.07282307]]]) - >>> qml.qchem.vcf_integrals(h_integrals=[h1], modals=[4,4,4]) - ([[[ 9.36124041e-03, 3.63798208e-19, -3.42019607e-19, -3.83743044e-19], - [ 9.59982270e-19, 2.77803512e-02, 5.18290259e-18, -4.82000376e-18], - [-2.73826508e-19, 4.88583546e-18, 4.63297357e-02, -2.87022759e-18], - [-1.94549340e-19, -5.48544743e-18, -1.41379640e-18, 7.92203227e-02]]], - None) + [0.00233724, 0.02958449, 0.00675431, 0.0021936], + [0.0007408, 0.00675431, 0.0506012, 0.01280986], + [0.00199125, 0.0021936, 0.01280986, 0.07282307]]]) + >>> qml.qchem.vscf_integrals(h_integrals=[h1], modals=[4,4,4]) + ( + [array([[[ 9.36124041e-03, 3.63798208e-19, -3.42019607e-19, + -3.83743044e-19], + [ 9.59982270e-19, 2.77803512e-02, 5.18290259e-18, + -4.82000376e-18], + [-2.73826508e-19, 4.88583546e-18, 4.63297357e-02, + -2.87022759e-18], + [-1.94549340e-19, -5.48544743e-18, -1.41379640e-18, + 7.92203227e-02]]])], None + ) + + + .. details:: + :title: Usage Details + + Required dimensions of h_integral tensors are as follows: + + - 1-mode coupled integrals: `(n, m)` + - 2-mode coupled integrals: `(n, n, m, m, m, m)` + - 3-mode coupled integrals: `(n, n, n, m, m, m, m, m, m)` + + where ``n`` is the number of vibrational modes in the molecule and ``m`` represents the number + of modals. + + Required dimensions of d_integral tensors are as follows: + + - 1-mode coupled integrals: `(3, n, m)` + - 2-mode coupled integrals: `(3, n, n, m, m, m, m)` + - 3-mode coupled integrals: `(3, n, n, n, m, m, m, m, m, m)` + + where ``n`` is the number of vibrational modes in the molecule, ``m`` represents the number + of modals and the first axis represents the ``x, y, z`` component of the dipole. Default is ``None``. + """ if len(h_integrals) > 3: From 137efb007b7703a5290996e3fc5131e3ff718211 Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Fri, 13 Dec 2024 10:21:32 -0500 Subject: [PATCH 19/35] Improved docstring --- pennylane/qchem/vibrational/vscf.py | 4 ++-- 1 file changed, 2 insertions(+), 2 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 3412741678a..654256d3995 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -403,8 +403,8 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto Returns: tuple: A tuple of the following: - - List[TensorLike[float]]: List of n-mode expansion of Hamiltonian integrals in VSCF basis. - - List[TensorLike[float]]: List of n-mode expansion of dipole integrals in VSCF basis, + - List[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3-coupled vibrational modes. + - List[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3-coupled vibrational modes. returns ``None`` if d_integrals are not provided. **Example** From 7ba5853a34e8d3baabbbb9c6730737902c270aee Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 11:32:21 -0500 Subject: [PATCH 20/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 654256d3995..21df262135f 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -383,7 +383,7 @@ def _rotate_hamiltonian(h_integrals, mode_rots, modals): def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cutoff_ratio=1e-6): - r"""Generates vibrational self-consistent field rotated integrals for vibrational Hamiltonian. + r"""Generates vibrational self-consistent field rotated integrals. This function converts the Christiansen vibrational Hamiltonian integrals obtained in the harmonic oscillator basis to integrals in the vibrational self-consistent field (VSCF) basis. From 8376957bed14e9b01b1eaf441a6ce362cc50c3b7 Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 11:32:39 -0500 Subject: [PATCH 21/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 8 ++++---- 1 file changed, 4 insertions(+), 4 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 21df262135f..33e3114ef9e 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -391,10 +391,10 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto `J. Chem. Theory Comput. 2010, 6, 235–248 `_. Args: - h_integrals (list[TensorLike[float]]): List of Hamiltonian integrals for up to 3-coupled vibrational modes. - Look at the `Usage Details` for more details on dimensions of tensors. - d_integrals (list[TensorLike[float]]): List of dipole integrals for up to 3-coupled vibrational modes. - Look at the `Usage Details` for more details on dimensions of tensors. + h_integrals (list[TensorLike[float]]): list of Hamiltonian integrals for up to 3 coupled vibrational modes. + Look at the Usage Details for more information. + d_integrals (list[TensorLike[float]]): list of dipole integrals for up to 3 coupled vibrational modes. + Look at the Usage Details for more information. modals (list[int]): list containing the maximum number of modals to consider for each vibrational mode. Default value is the maximum number of modals. cutoff (float): threshold value for including matrix elements into operator From 5d7a50bc5bc23237d9a2be45216a29996841b31c Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 11:32:48 -0500 Subject: [PATCH 22/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 33e3114ef9e..1044b789ba5 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -438,7 +438,7 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto where ``n`` is the number of vibrational modes in the molecule and ``m`` represents the number of modals. - Required dimensions of d_integral tensors are as follows: + The ``d_integral`` tensor must have one of these dimensions: - 1-mode coupled integrals: `(3, n, m)` - 2-mode coupled integrals: `(3, n, n, m, m, m, m)` From db4998ed5efa3d63e9be191661484ac87c2ec00c Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 11:33:09 -0500 Subject: [PATCH 23/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 7 +++---- 1 file changed, 3 insertions(+), 4 deletions(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 1044b789ba5..8c3b22df0e9 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -402,10 +402,9 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto Default value is ``1e-6``. Returns: - tuple: A tuple of the following: - - List[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3-coupled vibrational modes. - - List[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3-coupled vibrational modes. - returns ``None`` if d_integrals are not provided. + tuple: a tuple containing: + - List[TensorLike[float]]: List of Hamiltonian integrals in VSCF basis for up to 3 coupled vibrational modes. + - List[TensorLike[float]]: List of dipole integrals in VSCF basis for up to 3 coupled vibrational modes. Returns ``None`` if d_integrals are not provided. **Example** From 02076777ff0544a699394fc90db2cb339cb3d4cc Mon Sep 17 00:00:00 2001 From: Diksha Dhawan <40900030+ddhawan11@users.noreply.github.com> Date: Fri, 13 Dec 2024 11:33:19 -0500 Subject: [PATCH 24/35] Update pennylane/qchem/vibrational/vscf.py Co-authored-by: Soran Jahangiri <40344468+soranjh@users.noreply.github.com> --- pennylane/qchem/vibrational/vscf.py | 2 +- 1 file changed, 1 insertion(+), 1 deletion(-) diff --git a/pennylane/qchem/vibrational/vscf.py b/pennylane/qchem/vibrational/vscf.py index 8c3b22df0e9..7a01850774a 100644 --- a/pennylane/qchem/vibrational/vscf.py +++ b/pennylane/qchem/vibrational/vscf.py @@ -428,7 +428,7 @@ def vscf_integrals(h_integrals, d_integrals=None, modals=None, cutoff=None, cuto .. details:: :title: Usage Details - Required dimensions of h_integral tensors are as follows: + The ``h_integral`` tensor must have one of these dimensions: - 1-mode coupled integrals: `(n, m)` - 2-mode coupled integrals: `(n, n, m, m, m, m)` From 937d39e099401b9dd0b57a4bb67113491592ea1d Mon Sep 17 00:00:00 2001 From: ddhawan11 Date: Fri, 13 Dec 2024 12:06:16 -0500 Subject: [PATCH 25/35] Updated changelog --- doc/releases/changelog-dev.md | 2 ++ 1 file changed, 2 insertions(+) diff --git a/doc/releases/changelog-dev.md b/doc/releases/changelog-dev.md index cec024e6693..7611ef4245e 100644 --- a/doc/releases/changelog-dev.md +++ b/doc/releases/changelog-dev.md @@ -195,6 +195,8 @@ such as `shots`, `rng` and `prng_key`. * Implemented wrapper function for vibrational Hamiltonian calculation and dataclass for storing the data. [(#6652)](https://github.com/PennyLaneAI/pennylane/pull/6652) + * Implemented functions for generating the vibrational Hamiltonian in vscf basis + [(#6688)](https://github.com/PennyLaneAI/pennylane/pull/6688)