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Electron transfer reaction in the marcus inverted region: role of high frequency vibrational modes

Gayathri, N and Bagchi, B (1996) Electron transfer reaction in the marcus inverted region: role of high frequency vibrational modes. In: 5th International Meeting of Physical Chemistry - Fast Elementary Processes in Chemical and Biological Systems, JUN, 1995, FRANCE.

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Abstract

A theoretical study of the dynamics of photo-electron transfer reactions in the Marcus inverted regime is presented. This study is motivated partly by the recent proposal of Barbara et al. (J. Phys. Chem. 96, 3728, 1991) that a minimal model of an electron transfer reaction should consist of a polar solvent mode (X), a low frequency vibrational mode (Q) and one high frequency mode (q). Interplay between these modes may be responsible for the crossover observed in the dynamics from a solvent controlled to a vibrational controlled electron transfer. The following results have been obtained. (i) In the case of slowly relaxing solvents, the proximity of the point of excitation to an effective sink on the excited surface is critical in determining the decay of the reactant population. This is because the Franck-Condon overlap between the reactant ground and the product excited states decreases rapidly with increase in the quantum number of the product vibrational state. (ii) Non-exponential solvation dynamics has an important effect in determining the rates of electron transfer. Especially, a biphasic solvation and a large coupling between the reactant and the product states both may be needed to explain the experimental results. ©1996 American Institute of Physics

Item Type: Conference Paper
Additional Information: Copyright of this article belongs to American institute of physics.
Department/Centre: Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited: 28 Apr 2011 04:32
Last Modified: 28 Apr 2011 04:32
URI: http://eprints.iisc.ernet.in/id/eprint/37164

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