Efficient calculation of unbiased atomic forces in ab initio Variational Monte Carlo

Fuente: arXiv
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Main Authors: Nakano, Kousuke, Casula, Michele, Tenti, Giacomo
Format: Preprint
Published: 2023
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author Nakano, Kousuke
Casula, Michele
Tenti, Giacomo
author_facet Nakano, Kousuke
Casula, Michele
Tenti, Giacomo
contents Ab initio quantum Monte Carlo (QMC) is a state-of-the-art numerical approach for evaluating accurate expectation values of many-body wavefunctions. However, one of the major drawbacks that still hinders widespread QMC applications is the lack of an affordable scheme to compute unbiased atomic forces. In this study, we propose a very efficient method to obtain unbiased atomic forces and pressures in the Variational Monte Carlo (VMC) framework with the Jastrow-correlated Slater determinant ansatz, exploiting the gauge-invariant and locality properties of its geminal representation. We demonstrate the effectiveness of our method for H$_2$ and Cl$_2$ molecules and for the cubic boron nitride crystal. Our framework has a better algorithmic scaling with the system size than the traditional finite-difference method, and, in practical applications, is as efficient as single-point VMC calculations. Thus, it paves the way to study dynamical properties of materials, such as phonons, and is beneficial for pursuing more reliable machine-learning interatomic potentials based on unbiased VMC forces.
format Preprint
id arxiv_https___arxiv_org_abs_2312_17608
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Efficient calculation of unbiased atomic forces in ab initio Variational Monte Carlo
Nakano, Kousuke
Casula, Michele
Tenti, Giacomo
Materials Science
Chemical Physics
Computational Physics
Ab initio quantum Monte Carlo (QMC) is a state-of-the-art numerical approach for evaluating accurate expectation values of many-body wavefunctions. However, one of the major drawbacks that still hinders widespread QMC applications is the lack of an affordable scheme to compute unbiased atomic forces. In this study, we propose a very efficient method to obtain unbiased atomic forces and pressures in the Variational Monte Carlo (VMC) framework with the Jastrow-correlated Slater determinant ansatz, exploiting the gauge-invariant and locality properties of its geminal representation. We demonstrate the effectiveness of our method for H$_2$ and Cl$_2$ molecules and for the cubic boron nitride crystal. Our framework has a better algorithmic scaling with the system size than the traditional finite-difference method, and, in practical applications, is as efficient as single-point VMC calculations. Thus, it paves the way to study dynamical properties of materials, such as phonons, and is beneficial for pursuing more reliable machine-learning interatomic potentials based on unbiased VMC forces.
title Efficient calculation of unbiased atomic forces in ab initio Variational Monte Carlo
topic Materials Science
Chemical Physics
Computational Physics
url https://arxiv.org/abs/2312.17608