New insights into the nonadiabatic state population dynamics of model proton-coupled electron transfer reactions from the mixed quantum-classical Liouville approach

The Journal of Chemical Physics
Farnaz A Shakib, Gabriel Hanna

Abstract

In a previous study [F. A. Shakib and G. Hanna, J. Chem. Phys. 141, 044122 (2014)], we investigated a model proton-coupled electron transfer (PCET) reaction via the mixed quantum-classical Liouville (MQCL) approach and found that the trajectories spend the majority of their time on the mean of two coherently coupled adiabatic potential energy surfaces. This suggested a need for mean surface evolution to accurately simulate observables related to ultrafast PCET processes. In this study, we simulate the time-dependent populations of the three lowest adiabatic states in the ET-PT (i.e., electron transfer preceding proton transfer) version of the same PCET model via the MQCL approach and compare them to the exact quantum results and those obtained via the fewest switches surface hopping (FSSH) approach. We find that the MQCL population profiles are in good agreement with the exact quantum results and show a significant improvement over the FSSH results. All of the mean surfaces are shown to play a direct role in the dynamics of the state populations. Interestingly, our results indicate that the population transfer to the second-excited state can be mediated by dynamics on the mean of the ground and second-excited state surfaces, as...Continue Reading

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Citations

May 28, 2016·Journal of Chemical Theory and Computation·Farnaz Shakib, Gabriel Hanna
Jun 21, 2017·The Journal of Physical Chemistry Letters·Farnaz A Shakib, Pengfei Huo
Dec 29, 2020·Physical Chemistry Chemical Physics : PCCP·Sandra E Brown, Farnaz A Shakib
Feb 28, 2019·The Journal of Physical Chemistry. a·Arkajit MandalPengfei Huo

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