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Thermalization of Photoexcited Molecules in Solution

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Analysis of the steady-state absorption/fluorescence spectra of several laser dyes in room temperature solution suggests that the fluorescing molecules, if initially formed in a vibrationally excited state, lose their excess energy surprisingly slowly, remaining significantly warm on a nanosecond time scale. A similar analysis of the steady-state absorption/fluorescence spectra of GaAs confirms that in this case the carriers are fully thermalized, possessing no excess energy when they recombine on a microsecond time scale. A classical model which accounts qualitatively for slow molecular cooling is presented. We conclude that rapid molecular photoconversion processes are likely to involve incompletely cooled (thermalized) excited states.

Affiliations: 1: Department of Biochemistry, Imperial College, London SW7 2AZ, U.K.; 2: Department of Chemistry, The University of Western Ontario, London, Ontario, Canada N6A 5B7; 3: Department of Applied Mathematics and Theoretical Physics, Silver Street, Cambridge CB3 9EW, U.K.


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