Understanding the Effects of Liquid Structure on Chemical Bonds and Solvated Electrons Using Ultrafast Spectroscopy and Mixed Quantum/Classical Molecular Dynamics Simulation

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In this award, funded by the Chemical Structure, Dynamics and Mechanisms-A Program of the Chemistry Division, Prof. Benjamin J. Schwartz of the University of California, Los Angeles and two graduate student colleagues will undertake a theoretical program of research, supplemented with some experiments, to develop a better understanding of solvated electrons and photodissociation reactions in solution through the study of simple, prototypical model systems. The theoretical work will center on molecular dynamics simulations incorporating a rigorous, mixed quantum/classical method that Schwartz and his colleagues have developed, including the development of new interaction potentials that can respond to changes in the local environment around different chemical species. The simulations' focus will be on 1) understanding whether or not different solvents have pre-existing cavities that can control the dynamics of electron transfer reactions and/or support solvated electrons, and 2) understanding how liquid structure and dynamics control chemical bond-breaking and bond formation in solution. Accompanying the simulations will be a limited number of femtosecond laser experiments that will directly measure the dynamics of charge-transfer-to-solvent reactions (that create solvated electrons) in a variety of different solvents and also possibly the photodissociation dynamics of simple diatomic molecules. Besides the broader scientific impacts of the research being supported, the young researchers working on this project will gain simultaneous experience in both cutting edge theoretical and experimental methods. Moreover, the project will provide these educational opportunities both to students from traditionally underrepresented groups in the sciences and to Los Angeles area high school students via an outreach program for high school teachers. Finally, because solution-phase electron transfer reactions and chemical bond dynamics are ubiquitous in chemistry and biology, the methods and measurements developed in this proposal will enhance many areas of research outside the immediate focus of this proposal.