Non-Adiabatic Excited State Molecular Dynamics Methodologies: comparison and convergence

Freixas, Victor M.; White, Alexander James; Nelson, Tammie Renee; Song, Huajing; Makhov, Dmitry V.; Shalashilin, Dmitrii; Fernandez-Alberti, S.; Tretiak, Sergei

doi:10.1021/acs.jpclett.1c00266

Title: Non-Adiabatic Excited State Molecular Dynamics Methodologies: comparison and convergence

Journal Article · Wed Mar 17 00:00:00 EDT 2021 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.1c00266· OSTI ID:1841929

Freixas, Victor M. ^[1];

^[2];

^[2]; Makhov, Dmitry V. ^[3]; Shalashilin, Dmitrii ^[4]; Fernandez-Alberti, S. ^[1];

^[2]

Universidad Nacional de Quilmes, Bernal (Argentina)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Leeds (United Kingdom); Bristol Univ. (United Kingdom)
Univ. of Leeds (United Kingdom)

Direct atomistic simulation of nonadiabatic molecular dynamics is a challenging goal that allows important insights into fundamental physical phenomena. A variety of frameworks, ranging from fully quantum treatment of nuclei to semiclassical and mixed quantum–classical approaches, were developed. These algorithms are then coupled to specific electronic structure techniques. Such diversity and lack of standardized implementation make it difficult to compare the performance of different methodologies when treating realistic systems. Here, we compare three popular methods for large chromophores: Ehrenfest, surface hopping, and multiconfigurational Ehrenfest with ab initio multiple cloning (MCE-AIMC). These approaches are implemented in the NEXMD software, which features a common computational chemistry model. The resulting comparisons reveal the method performance for population relaxation and coherent vibronic dynamics. Finally, we study the numerical convergence of MCE-AIMC algorithms by considering the number of trajectories, cloning thresholds, and Gaussian wavepacket width. Our results provide helpful reference data for selecting an optimal methodology for simulating excited-state molecular dynamics.

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

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

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1841929

Report Number(s):: LA-UR-21-20549

Journal Information:: Journal of Physical Chemistry Letters, Vol. 12, Issue 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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