Electron Transfer Assisted by Vibronic Coupling from Multiple Modes

Journal of Chemical Theory and Computation
Subhajyoti ChaudhuriVictor S Batista

Abstract

Understanding the effect of vibronic coupling on electron transfer (ET) rates is a challenge common to a wide range of applications, from electrochemical synthesis and catalysis to biochemical reactions and solar energy conversion. The Marcus-Jortner-Levich (MJL) theory offers a model of ET rates based on a simple analytic expression with a few adjustable parameters. However, the MJL equation in conjunction with density functional theory (DFT) has yet to be established as a predictive first-principles methodology. A framework is presented for calculating transfer rates modulated by molecular vibrations, that circumvents the steep computational cost which has previously necessitated approximations such as condensing the vibrational manifold into a single empirical frequency. Our DFT-MJL approach provides robust and accurate predictions of ET rates spanning over 4 orders of magnitude in the 106-1010s-1range. We evaluate the full MJL equation with a Monte Carlo sampling of the entire active space of thermally accessible vibrational modes, while using no empirical parameters. The contribution to the rate of individual modes is illustrated, providing insight into the interplay between vibrational degrees of freedom and changes in el...Continue Reading

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Citations

Oct 17, 2019·Nature Communications·Jorge A Campos-Gonzalez-AnguloJoel Yuen-Zhou
Aug 14, 2020·Physical Chemistry Chemical Physics : PCCP·James B DerrValentine I Vullev
Nov 27, 2019·Nature Chemistry·Natalie A PaceObadiah G Reid
May 18, 2020·The Journal of Chemical Physics·William W Parson
Jul 3, 2020·The Journal of Chemical Physics·Eric R Heller, Jeremy O Richardson
Jul 20, 2021·The Journal of Physical Chemistry. B·William W Parson
Aug 13, 2021·Journal of Chemical Theory and Computation·Leonardo Evaristo de Sousa, Piotr de Silva
Sep 5, 2018·The Journal of Physical Chemistry. B·William W Parson
Apr 17, 2020·The Journal of Physical Chemistry Letters·Igor VurgaftmanJeffrey C Owrutsky
Jul 10, 2019·The Journal of Physical Chemistry. B·Dmitry V Matyushov, Marshall D Newton
May 6, 2019·The Journal of Physical Chemistry Letters·Subhajyoti ChaudhuriVictor S Batista
Sep 30, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Hyuk-Yong KwonElena Jakubikova

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