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

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.