Proton Coupled Electron Transfer and Charge Transfer Reactions at Solid-Liquid Interfaces and Homogeneous Environment
Proton coupled electron transfer (PCET) reactions are integral part of several catalytic processes that are crucial for energy storage, fuel cell research and several biological processes. On the other hand, excited state charge transfer reactions are at the heart of many photoinduced processes. In this presentation, I will discuss (i) computational study of PCET reaction between ZnO nanocrystal and an organic radical (ii) new theoretical methods to calculate solvent reorganization energies for electron transfer and PCET reactions in electrochemical systems, and (iii) implementation of a novel method to incorporate nuclear quantum effects in charge transfer dynamics. In the first part of the presentation I will show how to estimate rate constant for PCET between photoreduced ZnO nanocrystal and TEMPO. For reactions that involve a substantial redistribution of charge density in a polar environment, it is important to estimate the energy penalty involved in rearranging the solvent dipoles in order to estimate rate constant for the charge transfer process. In the second part of this talk I will describe a new method for calculating this important parameter, solvent reorganization energy, in the context of electrochemical electron transfer and PCET reactions. In the final part of this talk I will introduce my ongoing research on incorporating nuclear quantum effects in charge transfer dynamics within the framework of ring polymer surface hopping algorithm.