Spectral analysis of electron transfer kinetics II

Details Spectral analysis of electron transfer kinetics II Spectral analysis of electron transfer kinetics II

2002-03-29

arxiv.org/abs/cond-mat/0203620v1

Journal of Chemical Physics, vol. 117, pp. 3822-3836, 2002

Physics

Condensed Matter

Statistical Mechanics

submitted for a publication in Journal of Chemical Physics

Scientific paper

10.1063/1.1491241

Electron transfer processes in Debye solvents are studied using a spectral analysis method recently proposed. Spectral structure of a nonadiabatic two-state diffusion equation is investigated to reveal various kinetic regimes characterized by a broad range of physical parameters; electronic coupling, energy bias, reorganization energy, and solvent relaxation rate. Within this unified framework, several kinetic behaviors of the electron transfer kinetics, including adiabatic Rabi oscillation, crossover from the nonadiabatic to adiabatic limits, transition from the incoherent to coherent kinetic limits, and dynamic bath effect, are demonstrated and compared with results from previous theoretical models. Dynamics of the electron transfer system is also calculated with the spectral analysis method. It is pointed out that in the large reorganization energy case the nonadiabatic diffusion equation exhibits a non-physical behavior, yielding a negative eigenvalue.

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