Direct Simulation of Proton-Coupled Electron Transfer Reaction Dynamics and Mechanisms

Author: Kretchmer, Joshua S.

Year: 2015

Degree: Dissertation (Ph.D.)

Advisor: Miller, Thomas F.

Committee Members: Marcus, Rudolph A.; Okumura, Mitchio; Gray, Harry B.; Miller, Thomas F.

Option: Chemistry

DOI: 10.7907/Z98913T5

Abstract

Proton-coupled electron transfer (PCET) reactions are ubiquitous throughout chemistry and biology. However, challenges arise in both the the experimental and theoretical investigation of PCET reactions; the rare-event nature of the reactions and the coupling between quantum mechanical electron- and proton-transfer with the slower classical dynamics of the surrounding environment necessitates the development of robust simulation methodology. In the following dissertation, novel path-integral based methods are developed and employed for the direct simulation of the reaction dynamics and mechanisms of condensed-phase PCET.

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