Thermostating extended Lagrangian Born-Oppenheimer molecular dynamics

Martínez, Enrique; Cawkwell, Marc J.; Voter, Arthur F.; Niklasson, Anders M.  N.

doi:10.1063/1.4917546

Thermostating extended Lagrangian Born-Oppenheimer molecular dynamics

Journal Article · Tue Apr 21 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4917546· OSTI ID:1422959

Martínez, Enrique ^[1]; Cawkwell, Marc J. ^[1]; Voter, Arthur F. ^[1]; Niklasson, Anders M. N. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Here, Extended Lagrangian Born-Oppenheimer molecular dynamics is developed and analyzed for applications in canonical (NVT) simulations. Three different approaches are considered: the Nosé and Andersen thermostats and Langevin dynamics. We have tested the temperature distribution under different conditions of self-consistent field (SCF) convergence and time step and compared the results to analytical predictions. We find that the simulations based on the extended Lagrangian Born-Oppenheimer framework provide accurate canonical distributions even under approximate SCF convergence, often requiring only a single diagonalization per time step, whereas regular Born-Oppenheimer formulations exhibit unphysical fluctuations unless a sufficiently high degree of convergence is reached at each time step. Lastly, the thermostated extended Lagrangian framework thus offers an accurate approach to sample processes in the canonical ensemble at a fraction of the computational cost of regular Born-Oppenheimer molecular dynamics simulations.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Laboratory Directed Research and Development (LDRD); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1422959

Report Number(s):: LA-UR--14-29698

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 15 Vol. 142; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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