Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

Bjorgaard, Josiah August; Velizhanin, Kirill A.; Tretiak, Sergei

doi:10.1063/1.4946009

Title: Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

Journal Article · Fri Apr 15 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4946009· OSTI ID:1338760

^[1];

^[2]; Tretiak, Sergei ^[3]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division. Center for Nonlinear Studies
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division. Center for Nonlinear Studies. Center for Integrated Nanotechnologies

The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited state molecular dynamics. In this paper, we describe methods of simulating nonequilibrium solvent effects in excited state molecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Finally, molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission.

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

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1338760

Report Number(s):: LA-UR-16-20658

Journal Information:: Journal of Chemical Physics, Vol. 144, Issue 15; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
solvation
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Title: Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

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