Theoretical Studies of Energy Transfer, Relaxation and Spectroscopy in Condensed Phase Molecular Systems

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Robert Silbey has submitted a renewal proposal to continue his theoretical studies of the time dependent spectroscopy of chromophores in glasses and liquids. This research will explore the connection between single molecule spectroscopy and the spectrum of distributions of molecules in experiments such as photon echo, hole burning, and ultrafast pump-probe studies. Various molecular processes that are caused by the interaction of the chromophores with modes of the condensed phase and evidenced in the spectrum will be examined. Specific topics that will be explored are exciton and excitation energy transfer, spectral diffusion, and energy transfer induced spectral diffusion. All of this work will be carried out in collaboration with interested experimental groups. Laser spectroscopic studies of molecules embedded in glasses and liquids have enabled improved understanding of interactions and relaxation processes in condensed phase systems including biologically relevant photosynthetic reaction centers and proteins. In most studies, many molecules are monitored at once, so their averaged behavior is measured. Now methods are evolving that permit measurements on a single molecule where one can measure line shapes and watch the molecule diffuse in real time. Silbey is developing new theoretical interpretations that connect experimental results on single molecules with the studies on distributions of molecules. The insights resulting from this effort will lead to a better appreciation of chemical dynamics in condensed phase systems, both experimentally and theoretically.