Theoretical Studies of Charge Shift Processes in Solution: Role of Solute-Solvent Electronic Structure and Solvation Dynamics

点击翻译按钮获取中文摘要

Hyung Kim of Carnegie Mellon University is supported by a grant from the Theoretical and Computational Chemistry Program to perform theoretical studies of charge shift processes in solution. He will study solute-solvent electronic structure variation with a fluctuating nonequilibrium solvent environment and it's effect on charge shift processes. A novel quantum chemical method will incorporate the solute-solvent electron correlation within a dielectric continuum solvent description. An improved solvent coordinate description, which properly accounts for solvent response to variations in the solute geometry during reaction, will also be developed. The theory will be applied to the first singlet electronic transition in formaldehyde, dissociative electron attachment, ultrafast excited-state electron transfer and state-dependent rotational dynamics in solution. Excellent theories are now available for understanding gas phase chemical reactions involving binary encounters between molecules. However, most chemical reactions of technological importance occur in condensed phases consisting of reacting solutes dissolved in non-reacting solvents. The effect which the solvent has on chemical reactions, and theoretical methods for dealing with this complex interaction are still very much in their infancy. Nevertheless, progress in this area of research can have an important long range impact on our fundamental understanding of chemical reactions of industrial significance. Kim's research is helping to provide a theoretical basis for the interpretation of solvent effects on chemical reactions in condensed phase systems.