Electron transfer rates for asymmetric reactions

Details Electron transfer rates for asymmetric reactions Electron transfer rates for asymmetric reactions

2003-06-11

arxiv.org/abs/cond-mat/0306269v1

Chem. Phys. 296, 193 (2004)

Physics

Condensed Matter

13 pages, 4 figures, submitted to Chemical Physics Special Issue on the Spin-Boson Problem, ed. by H. Grabert and A. Nitzan

Scientific paper

10.1016/j.chemphys.2003.08.021

We use a numerically exact real-time path integral Monte Carlo scheme to compute electron transfer dynamics between two redox sites within a spin-boson approach. The case of asymmetric reactions is studied in detail in the least understood crossover region between nonadiabatic and adiabatic electron transfer. At intermediate-to-high temperature, we find good agreement with standard Marcus theory, provided dynamical recrossing effects are captured. The agreement with our data is practically perfect when temperature renormalization is allowed. At low temperature we find peculiar electron transfer kinetics in strongly asymmetric systems, characterized by rapid transient dynamics and backflow to the donor.

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