Theoretical Studies of Excited State Reaction Dynamics, Surface Chemistry, and Condensed Phase Processes

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David Coker, of Boston University, is supported by a grant from the Theoretical and Computational Chemistry Program to perform theoretical studies of excited state reaction dynamics, surface chemistry and condensed-phase processes. The theoretical methods address a class of chemical problems in which there is strong mixing between the electronic and vibrational degrees of freedom. In these instances, the more common adiabatic approximation is insufficient. Coker uses his new method for computing real-time correlation functions, which is based on semi-classical expressions for the propagator. This approach enables a consistent treatment of nuclear and electronic degrees of freedom and opens up the possibility for treating problems of biochemical and environmental significance and to address the role of the solvent on fundamental chemical processes.Many industrial, biochemical and environmental chemical reactions involve multiple energy surfaces, which are due to different electronic configurations. In the stratosphere a single-chlorine containing molecule can degrade numerous ozone molecules before it is neutralized into a hydrogen-chloride molecule. Understanding which chlorine-containing molecules are easily photolyzed to reactive ClO containing species will aid in alleviating ozone depletion. Such reactions reside in the class of chemical reactions amenable to study using the methods developed under this grant.