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Crossover from nonadiabatic to adiabatic electron transfer reactions: Multilevel blocking Monte Carlo simulations

L. Muehlbacher·R. Egger
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Abstract

The crossover from nonadiabatic to adiabatic electron transfer has been theoretically studied under a spin-boson model (dissipative two-state system) description. We present numerically exact data for the thermal transfer rate and the time-dependent occupation probabilities in largely unexplored regions of parameter space, using real-time path-integral Monte Carlo simulations. The dynamical sign problem is relieved by employing a variant of the recently proposed multilevel blocking algorithm. We identify the crossover regime between nonadiabatic and adiabatic electron transfer, both in the classical (high-temperature) and the quantum (low-temperature) limit. The electron transfer dynamics displays rich behaviors, including multi-exponential decay and the breakdown of a rate description due to vibrational coherence.

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L. Muehlbacher, R. Egger. 2002-05-19. Crossover from nonadiabatic to adiabatic electron transfer reactions: Multilevel blocking Monte Carlo simulations. https://doi.org/10.1063/1.1523014

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