Theoretical and Computational Studies of Multiple Charge Transfer Reactions in the Condensed Phase

University Of Notre Dame, Notre Dame IN

Investigators

Abstract

Sharon Hammes-Schiffer is supported by the Theoretical and Computational Chemistry Program to pursue investigations of multiple charge transfer reactions, including multiple proton transfer and proton-coupled electron transfer. The broad goal of this project is to elucidate the fundamental principles of multiple charge transfer reactions in the condensed phase. Two complementary approaches will be implemented to accomplish this goal. In the first approach, using mixed quantum/classical molecular dynamics methods, the solvent is represented as explicit molecules treated classically, while transferring protons and active electrons are treated quantum mechanically. In the second approach, based on multistate continuum theory, the solvent is represented as a dielectric continuum and the transferring protons and active electrons are treated quantum mechanically. Both approaches will be developed and tested by applications to model systems. This combination of the development of theoretical and computational methodology and subsequent application to chemically and biologically relevant systems will provide insight into the fundamental principles of multiple charge transfer reactions. Such reactions are important in proton wires (proton transport along chains of water molecules), asymmetric salt bridges, and enzyme reactions vital to metabolism.