THEORETICAL CALCULATION OF PUMP-PROBE STIMULATED EMISSION PROFILES OF ULTRAFAST ELECTRON TRANSFER

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1994

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Ohio State University

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Abstract

The photo-induced electron transfer (ET) has bean observed in many chemical and biological systems such as photosynthetic reaction center. The time resolved spectra of these phenomenon were well described by many researchers. Recent improvement of femtosecond technique lead to the discovery of ultrafast ET’s that take place in pico or femto second time $scale^{1,2,3}$. The conventional theory assumes that the vibrational relaxation of the photoexcited electronic state takes place much faster than the ET process. Considering the typical time scale of the vibrational relaxation (sub-pico second), above assumption should be examined for the cases of ultrafast ET. In this work, the theoretical model in which the ET and the vibrational relaxation are comparable rate will be presented. Also, the pump-probe stimulated emission profiles based on this model will be shown. The various features of these profiles such as quantum beat and temperature effect will be discussed in detail.

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1. M.H. Vos, F. Rappaport, J.C. Lambry, J. Breton, and J.L. Martin, Nature 363, 320 (1993) 2. T. Arlt, S. Schmidt, W. Kaiser, C. Lauterwasser, M. Meyer, H. Scheer, and W. Zinth, Proc. Natl. Acad. Sci. USA, 9D, 11757 (1993). 3. G.R. Fleming, J.L. Martin, and J. Breton. Nature, 333, 190 (1988).
Author Institution: Department of chemistry and Biochemistry, Arizona State University

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