Peter Rossky is supported by a grant from the Theoretical and Computational Chemistry Program to continue his work in the area of quantum simulation of chemical dynamics in solution. This research focuses on both the development and application of mixed quantum and classical mechanical simulation methods for the description of chemical processes in solution. Emphasis is placed on the simulation of nonadiabatic quantum dynamics. The work will address in detail: 1) The fundamental molecular level description of the solvent modes associated with the non-radiative relaxation of solute excited electronic states in liquid solution; 2) New applications of algorithms for quantum nonadiabatic simulation to the dynamics of molecular photoionization and to intramolecular charge transfer dynamics in both aqueous and non-aqueous solution; 3) The development and implementation of new algorithms for nonadiabatic quantum dynamics; and 4) Generalization and testing of current nonadiabatic algorithms with emphasis on an analysis of the role of quantum coherence in the results obtained in the condensed phase. The majority of chemical reactions occur in solution. This fact has stimulated a tremendous research effort to elucidate a set of unifying principles describing chemical dynamics in liquids. To fully address this issue requires a detailed understanding of both the molecular motions that occur during the course of a chemical event and the energy flow within the solute and between the solute and the solvent. Exceptional recent progress in clarifying these aspects has been made. Advances in laser technology enable direct experimental measurement of dynamical behavior of chemical systems on the time scale of the fundamental events. At the same time, significant advances have been made in theoretical methods and models used in describing solution chemistry. Rossky's research in the development of new computational algorithms will allow for both cl assical and quantum mechanical dynamical simulations of phenomena on time scales accessible by these new experimental techniques.
