Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory

Valerio Vitale; Jacek Dziedzic; Alex Albaugh; Anders Niklasson; Teresa Head-Gordon; Chris-Kriton Skylaris

doi:10.1063/1.4978684

Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory

Abstract

Iterative energy minimization with the aim of achieving self-consistency is a common feature of Born-Oppenheimer molecular dynamics (BOMD) and classical molecular dynamics with polarizable force fields. In the former, the electronic degrees of freedom are optimized, while the latter often involves an iterative determination of induced point dipoles. The computational effort of the self-consistency procedure can be reduced by re-using converged solutions from previous time steps. However, this must be done carefully, as not to break time-reversal symmetry, which negatively impacts energy conservation. Self-consistent schemes based on the extended Lagrangian formalism, where the initial guesses for the optimized quantities are treated as auxiliary degrees of freedom, constitute one elegant solution. We report on the performance of two integration schemes with the same underlying extended Lagrangian structure, which we both employ in two radically distinct regimes—in classical molecular dynamics simulations with the AMOEBA polarizable force field and in BOMD simulations with the Onetep linear-scaling density functional theory (LS-DFT) approach. Both integration schemes are found to offer significant improvements over the standard (unpropagated) molecular dynamics formulation in both the classical and LS-DFT regimes.

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Authors (6)

Valerio Vitale
- University of Southampton School of Chemistry
Jacek Dziedzic dr hab. inż.
Alex Albaugh
- University of California, Berkeley Department of Chemical and Biomolecular Engineering
Anders Niklasson
- Los Alamos National Laboratory Theoretical Division
Teresa Head-Gordon
- University of California, Berkeley Department of Chemical and Biomolecular Engineering
Chris-Kriton Skylaris
- University of Southampton .

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DOI:: Digital Object Identifier (open in new tab) 10.1063/1.4978684
License: Copyright (2017 AIP Publishing)

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Category:: Articles
Type:: artykuł w czasopiśmie wyróżnionym w JCR
Published in:: JOURNAL OF CHEMICAL PHYSICS no. 146, edition 12, pages 1 - 17,
ISSN: 0021-9606
Language:: English
Publication year:: 2017
Bibliographic description:: Vitale V., Dziedzic J., Albaugh A., Niklasson A., Head-Gordon T., Skylaris C.: Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory// JOURNAL OF CHEMICAL PHYSICS. -Vol. 146, iss. 12 (2017), s.1-17
DOI:: Digital Object Identifier (open in new tab) 10.1063/1.4978684
Verified by:: Gdańsk University of Technology