Ultrafast pump-probe transient absorption spectroscopy has been applied to study return electron transfer in the tetracyanoethylene- benzene electron donor-acceptor complex in several polar and non-polar solvents. Ultrafast excitation of the charge transfer band of the complex yields an excited Franck-Condon state, which relaxes to form a contact ion pair. The decay time of the ion pair is, in most cases, longer than the solvation time and is observed on a time scale from 2 picoseconds to 1 ns, depending on the solvent. Using the empirical solvent polarity scale ^vG153 and a conventional non-adiabatic theory of electron transfer, absolute rate constants for the non-radiative return electron transfer can be predicted in different solvents.
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