{"title":"Grassmann Extrapolation for Accelerating Geometry Optimization.","authors":"Zahra Askarpour, Michele Nottoli, Benjamin Stamm","doi":"10.1021/acs.jctc.4c01417","DOIUrl":null,"url":null,"abstract":"<p><p>This study extends the Grassmann extrapolation (G-Ext) method, which was introduced for Born-Oppenheimer molecular dynamics, to the context of geometry optimization. Using density matrices from previous optimization steps, the G-Ext approach applies a nonlinear, structure-preserving mapping onto the Grassmann manifold to provide an initial guess which accelerates the convergence of the self-consistent field (SCF) procedure. Using the optimal parameters identified by employing various descriptors and computational strategies across a diverse set of molecules, G-Ext shows excellent performance improvements, particularly with large molecular systems.</p>","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":" ","pages":""},"PeriodicalIF":5.7000,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.4c01417","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
This study extends the Grassmann extrapolation (G-Ext) method, which was introduced for Born-Oppenheimer molecular dynamics, to the context of geometry optimization. Using density matrices from previous optimization steps, the G-Ext approach applies a nonlinear, structure-preserving mapping onto the Grassmann manifold to provide an initial guess which accelerates the convergence of the self-consistent field (SCF) procedure. Using the optimal parameters identified by employing various descriptors and computational strategies across a diverse set of molecules, G-Ext shows excellent performance improvements, particularly with large molecular systems.
期刊介绍:
The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.