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

Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory
Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory
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.
0021-9606
Vitale, Valerio
dc892a8a-70b3-4adf-9e30-f29eb1d1b965
Dziedzic, Jacek
8e2fdb55-dade-4ae4-bf1f-a148a89e4383
Albaugh, Alex
67df21c3-f950-46ed-9dc8-86be3a3bdd6e
Niklasson, Anders M.N.
20b49841-b66a-44dc-88bc-f3887aca1e5d
Head-Gordon, Teresa
11febdf4-20fa-4abb-97a1-3305c6e81b09
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Vitale, Valerio
dc892a8a-70b3-4adf-9e30-f29eb1d1b965
Dziedzic, Jacek
8e2fdb55-dade-4ae4-bf1f-a148a89e4383
Albaugh, Alex
67df21c3-f950-46ed-9dc8-86be3a3bdd6e
Niklasson, Anders M.N.
20b49841-b66a-44dc-88bc-f3887aca1e5d
Head-Gordon, Teresa
11febdf4-20fa-4abb-97a1-3305c6e81b09
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61

Vitale, Valerio, Dziedzic, Jacek, Albaugh, Alex, Niklasson, Anders M.N., Head-Gordon, Teresa and Skylaris, Chris-Kriton (2017) Performance of extended Lagrangian schemes for molecular dynamics simulations with classical polarizable force fields and density functional theory. The Journal of Chemical Physics, 146 (12). (doi:10.1063/1.4978684). (In Press)

Record type: Article

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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Revision_Performances_of_extended_Lagrangian - Accepted Manuscript
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More information

Accepted/In Press date: 1 March 2017
Organisations: Chemistry, Electronics & Computer Science, Computational Systems Chemistry

Identifiers

Local EPrints ID: 407980
URI: https://eprints.soton.ac.uk/id/eprint/407980
ISSN: 0021-9606
PURE UUID: 2d31b4b4-2c55-4620-93b5-cec7cad8c32a
ORCID for Jacek Dziedzic: ORCID iD orcid.org/0000-0003-4786-372X
ORCID for Chris-Kriton Skylaris: ORCID iD orcid.org/0000-0003-0258-3433

Catalogue record

Date deposited: 06 May 2017 01:02
Last modified: 14 Mar 2019 01:41

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