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

Robert Silbey提交了一份更新提案，以继续他对玻璃和液体中发色团随时间变化的光谱学的理论研究。 本研究将探讨单分子光谱学与光子回波、烧孔和超快泵浦-探测研究等实验中分子分布光谱之间的联系。 各种分子的过程所造成的生色团与凝聚相的模式，并证明在光谱的相互作用将被检查。 将探讨的具体议题是激子和激发能量转移，光谱扩散，能量转移引起的光谱扩散。 所有这些工作都将与感兴趣的实验小组合作进行。嵌入在玻璃和液体中的分子的激光光谱研究，使相互作用和弛豫过程的凝聚相系统，包括生物相关的光合反应中心和蛋白质的理解得到了改善。 在大多数研究中，同时监测许多分子，因此测量它们的平均行为。 现在的方法正在发展，允许对单个分子进行测量，人们可以测量线形并观察分子在真实的时间内的扩散。 Silbey正在开发新的理论解释，将单分子的实验结果与分子分布的研究联系起来。 从这方面的努力所产生的见解将导致更好地欣赏凝聚相系统中的化学动力学，无论是实验上还是理论上。

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.