TITLE

The role of different reorganization energies within the Zusman theory of electron transfer

AUTHOR(S)
Casado-Pascual, Jesús; Morillo, Manuel; Goychuk, Igor; Hänggi, Peter
PUB. DATE
January 2003
SOURCE
Journal of Chemical Physics;1/1/2003, Vol. 118 Issue 1, p291
SOURCE TYPE
Academic Journal
DOC. TYPE
Article
ABSTRACT
We consider the kinetics of electron transfer reactions in condensed media with different reorganization energies for the forward and backward processes. The starting point of our analysis is an extension of the well-known Zusman equations to the case of parabolic diabatic curves with different curvatures. A generalized master equation for the populations as well as formal expressions for their long-time limit is derived. We discuss the conditions under which the time evolution of the populations of reactants and products can be described at all times by a single exponential law. In the limit of very small tunnel splitting, a novel rate formula for the nonadiabatic transitions is obtained. It generalizes previous results derived within the contact approximation. For larger values of the tunnel splitting, we make use of the consecutive step approximation leading to a rate formula that bridges between the nonadiabatic and solvent-controlled adiabatic regimes. Finally, the analytical predictions for the long-time populations and for the rate constant are tested against precise numerical solutions of the starting set of partial differential equations.
ACCESSION #
8687044

 

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