A Quasi Time-Reversible scheme based on density matrix extrapolation on the Grassmann manifold for Born-Oppenheimer Molecular Dynamics

TL;DR

This paper introduces a Quasi Time-Reversible scheme using Grassmann extrapolation of density matrices to improve initial guess accuracy in Born-Oppenheimer Molecular Dynamics, reducing computational effort while maintaining energy stability.

Contribution

It presents a novel Quasi Time-Reversible scheme based on Grassmann manifold extrapolation for density matrices in molecular dynamics simulations.

Findings

Reduces the number of self-consistent field iterations.

Maintains similar energy drift as existing methods.

Effective on large molecular systems with thousands of atoms.

Abstract

This article proposes a so-called Quasi Time-Reversible (QTR G-Ext) scheme based on Grassmann extrapolation of density matrices for an accurate calculation of initial guesses in Born-Oppenheimer Molecular Dynamics simulations. The method shows excellent results on four large molecular systems, ranging from 21 to 94 atoms simulated with Kohn-Sham density functional theory surrounded with a classical environment with 6k to 16k atoms. Namely, it clearly reduces the number of self-consistent field iterations, while keeping a similar energy drift as in the extended Lagrangian Born-Oppenheimer method.