Correlation-Dependent Coherent to Incoherent Transitions in Resonant Energy Transfer Dynamics

Abstract

I investigate energy transfer in a donor-acceptor pair beyond weak system-bath coupling. I identify a transition from coherent to incoherent dynamics with increasing temperature, due to multiphonon effects not captured by a standard weak-coupling treatment. The crossover temperature has a marked dependence on the degree of spatial correlation between fluctuations experienced at the two system sites. For strong correlations, this leads to the possibility of coherence surviving into a high-temperature regime.