Abstract

We provide here a simple description of the coherent time evolution of a coordinate point or configuration distribution on an excited state energy surface, following excitation by a classical {delta}-like pulse. The configuration is probed by another {delta}-like pulse at a later time. The time evolution of the probe pulse absorption follows patterns which depend in characteristic ways on the probability of transition to other surfaces crossing the surface primarily excited, the frequency of the exciting light, and the friction of motion on the potential surfaces. The formalism is analytical and appropriate for use on the primary ultrafast charge separation involving special pair and auxiliary bacteriochlorophyll and bacteriopheophytin in the bacterial photosynthetic reaction center. In this respect the formalism also offers clues to the high-energy superexchange or low-energy coherently populated nature of the intermediate state chlorophyll. 23 refs., 2 figs.

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