Communication: Calculation of interatomic forces and optimization of molecular geometry with auxiliary-field quantum Monte Carlo

The Journal of Chemical Physics
Mario Motta, Shiwei Zhang

Abstract

We propose an algorithm for accurate, systematic, and scalable computation of interatomic forces within the auxiliary-field quantum Monte Carlo (AFQMC) method. The algorithm relies on the Hellmann-Feynman theorem and incorporates Pulay corrections in the presence of atomic orbital basis sets. We benchmark the method for small molecules by comparing the computed forces with the derivatives of the AFQMC potential energy surface and by direct comparison with other quantum chemistry methods. We then perform geometry optimizations using the steepest descent algorithm in larger molecules. With realistic basis sets, we obtain equilibrium geometries in agreement, within statistical error bars, with experimental values. The increase in computational cost for computing forces in this approach is only a small prefactor over that of calculating the total energy. This paves the way for a general and efficient approach for geometry optimization and molecular dynamics within AFQMC.

References

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Oct 21, 2017·Journal of Chemical Theory and Computation·Mario Motta, Shiwei Zhang

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Citations

Feb 24, 2019·The Journal of Chemical Physics·Edgar Josué Landinez BordaMiguel A Morales
Nov 6, 2018·The Journal of Chemical Physics·Shuai ZhangMiguel A Morales
Aug 6, 2020·The Journal of Chemical Physics·Joonho Lee, David R Reichman
May 22, 2020·Journal of Chemical Theory and Computation·Fionn D MaloneMiguel A Morales
May 16, 2019·Journal of Chemical Theory and Computation·Mario MottaGarnet Kin-Lic Chan
Dec 20, 2018·Journal of Chemical Theory and Computation·Fionn D MaloneMiguel A Morales

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