Surface hopping outperforms secular Redfield theory when reorganization energies range from small to moderate (and nuclei are classical)

The Journal of Chemical Physics
Brian R Landry, Joseph E Subotnik

Abstract

We evaluate the accuracy of Tully's surface hopping algorithm for the spin-boson model in the limit of small to moderate reorganization energy. We calculate transition rates between diabatic surfaces in the exciton basis and compare against exact results from the hierarchical equations of motion; we also compare against approximate rates from the secular Redfield equation and Ehrenfest dynamics. We show that decoherence-corrected surface hopping performs very well in this regime, agreeing with secular Redfield theory for very weak system-bath coupling and outperforming secular Redfield theory for moderate system-bath coupling. Surface hopping can also be extended beyond the Markovian limits of standard Redfield theory. Given previous work [B. R. Landry and J. E. Subotnik, J. Chem. Phys. 137, 22A513 (2012)] that establishes the accuracy of decoherence-corrected surface-hopping in the Marcus regime, this work suggests that surface hopping may well have a very wide range of applicability.

References

Jul 23, 2004·The Journal of Chemical Physics·Chaoyuan ZhuDonald G Truhlar
Jul 23, 2004·The Journal of Chemical Physics·Qiang Shi, Eitan Geva
Apr 20, 2005·The Journal of Chemical Physics·Priya V Parandekar, John C Tully
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Dec 3, 2008·The Journal of Chemical Physics·Masoud MohseniAlán Aspuru-Guzik
Nov 18, 2009·The Journal of Chemical Physics·Patrick RebentrostAlán Aspuru-Guzik
Jan 19, 2011·The Journal of Chemical Physics·Joseph E Subotnik, Neil Shenvi
May 10, 2011·The Journal of Physical Chemistry. a·Dana NachtigallováHans Lischka
Mar 3, 2012·The Journal of Chemical Physics·Timothy C BerkelbachDavid R Reichman
Oct 30, 2012·Journal of Chemical Theory and Computation·Johan Strümpfer, Klaus Schulten
Dec 20, 2012·The Journal of Chemical Physics·Brian R Landry, Joseph E Subotnik
Jul 5, 2013·The Journal of Chemical Physics·Aaron Kelly, Thomas E Markland
Dec 11, 2013·The Journal of Chemical Physics·Brian R LandryJoseph E Subotnik
Mar 29, 2014·Accounts of Chemical Research·Tammie NelsonSergei Tretiak

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Citations

Dec 4, 2015·The Journal of Physical Chemistry Letters·Amber Jain, Joseph E Subotnik
Nov 23, 2015·The Journal of Chemical Physics·Andrés Montoya-CastilloDavid R Reichman
Oct 10, 2015·The Journal of Chemical Physics·Amber Jain, Joseph E Subotnik
Oct 10, 2015·The Journal of Chemical Physics·Amber JainJoseph E Subotnik
Sep 24, 2015·The Journal of Chemical Physics·Alexey D Kondorskiy, Shinkoh Nanbu
Jul 9, 2016·The Journal of Chemical Physics·Nicole BellonziJoseph E Subotnik
May 25, 2016·Annual Review of Physical Chemistry·Joseph E SubotnikNicole Bellonzi
Jun 15, 2018·Nature Communications·Tammie R NelsonSergei Tretiak
Jul 6, 2019·Chemical Reviews·Francesco SegattaBenedetta Mennucci

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