Quasi-Diabatic Propagation Scheme for Direct Simulation of Proton-Coupled Electron Transfer Reaction

Arkajit Mandal, Juan S.C. Sandoval, Farnaz A. Shakib, Pengfei Huo

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14 Scopus citations


We apply a recently developed quasi-diabatic (QD) propagation scheme to simulate proton-coupled electron transfer (PCET) reactions. This scheme enables a direct interface between an accurate diabatic dynamics approach and the adiabatic vibronic states of the coupled electron-proton subsystem. It explicitly avoids theoretical efforts to preconstruct diabatic states for the transferring electron and proton or reformulate a diabatic dynamics method to the adiabatic representation, both of which are nontrivial tasks. Using a partial linearized path-integral approach and symmetrical quasi-classical approach as the diabatic dynamics methods, we demonstrate that the QD propagation scheme provides accurate vibronic dynamics of PCET reactions and reliably predicts the correct reaction mechanism without any a priori assumptions. This work demonstrates the possibility to directly simulate challenging PCET reactions by using accurate diabatic dynamics approaches and adiabatic vibronic information.

Original languageEnglish (US)
Pages (from-to)2470-2482
Number of pages13
JournalJournal of Physical Chemistry A
Issue number12
StatePublished - Mar 28 2019
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry


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