Centre d'Enseignement et de Recherche en Mathématiques et Calcul Scientifique (CERMICS), École des Ponts ParisTech (ENPC), Laboratoire de Mathématiques de Besançon (UMR 6623) (LMB), Centre National de la Recherche Scientifique (CNRS)-Université de Franche-Comté (UFC), Université Bourgogne Franche-Comté [COMUE] (UBFC)-Université Bourgogne Franche-Comté [COMUE] (UBFC), Simons Targeted Grant Award No. 89663, Italian Ministry of University and Research, grant 2020HT-SXMA 002 (PSI-MOVIE), DFG, under Germany’s Excellence Strategy – EXC 2075 – 390740016, ANR-15-IDEX-0003,BFC,ISITE ' BFC(2015), European Project: 810367,EMC2(2019)
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.
