Accurate nonadiabatic quantum dynamics on the cheap: making the most of mean field theory with master equations

The Journal of Chemical Physics
Aaron KellyThomas E Markland

Abstract

In this article, we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean field generalized quantum master equation (MF-GQME) approach is a non-perturbative and non-Markovian theory to treat open quantum systems without any restrictions on the form of the Hamiltonian that it can be applied to. By studying relaxation dynamics in a wide range of dynamical regimes, typical of charge and energy transfer, we show that MF-GQME provides a much higher accuracy than a direct application of mean field theory. In addition, these increases in accuracy are accompanied by computational speed-ups of between one and two orders of magnitude that become larger as the system becomes more nonadiabatic. This combination of quantum-classical theory and master equation techniques thus makes it possible to obtain the accuracy of much more computationally expensive approaches at a cost lower than even mean field dynamics, providing the ability to treat the quantum dynamics of atomistic condensed phase systems for long times.

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Citations

Feb 9, 2016·Journal of Chemical Theory and Computation·David B LingerfeltXiaosong Li
Nov 14, 2015·The Journal of Physical Chemistry Letters·William C PfalzgraffThomas E Markland
May 18, 2016·The Journal of Chemical Physics·Andrés Montoya-Castillo, David R Reichman
May 18, 2016·The Journal of Chemical Physics·Aaron KellyThomas E Markland
Apr 20, 2016·Annual Review of Physical Chemistry·Mi Kyung LeeDavid F Coker
Aug 9, 2016·The Journal of Chemical Physics·Wenjie Dou, Joseph E Subotnik
Mar 3, 2017·The Journal of Chemical Physics·Andrés Montoya-Castillo, David R Reichman
Jul 16, 2019·The Journal of Chemical Physics·Xin He, Jian Liu
Feb 24, 2019·The Journal of Chemical Physics·Maximilian A C SallerJeremy O Richardson
Aug 3, 2019·The Journal of Chemical Physics·Johan E Runeson, Jeremy O Richardson
Jul 1, 2019·The Journal of Chemical Physics·Sutirtha N Chowdhury, Pengfei Huo
Jun 9, 2020·The Journal of Chemical Physics·Yakov BraverAndrius Gelzinis
Jun 4, 2019·The Journal of Chemical Physics·Aaron Kelly
Jan 8, 2018·The Journal of Chemical Physics·Chang-Yu Hsieh, Jianshu Cao
Jul 10, 2020·The Journal of Chemical Physics·Siqin CaoXuhui Huang
Nov 22, 2020·The Journal of Chemical Physics·Jonathan R Mannouch, Jeremy O Richardson
Jan 10, 2020·The Journal of Physical Chemistry. a·Wenjie Dou, Joseph E Subotnik
Mar 1, 2021·The Journal of Chemical Physics·Chang Woo Kim, Ignacio Franco
Apr 4, 2021·The Journal of Chemical Physics·Sutirtha N Chowdhury, Pengfei Huo
Apr 21, 2021·Physical Chemistry Chemical Physics : PCCP·Fabrizio SantoroRoberto Improta
Nov 14, 2019·The Journal of Physical Chemistry. B·Sambarta Chatterjee, Nancy Makri
Aug 24, 2021·The Journal of Physical Chemistry. B·Ellen Mulvihill, Eitan Geva
Mar 1, 2018·Journal of Chemical Theory and Computation·Arkajit MandalPengfei Huo

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