Exciton dynamics in chromophore aggregates with correlated environment fluctuations

We study the effects of correlated molecular transition energy fluctuations in molecular aggregates on the density matrix dynamics, and their signatures in the optical response. Correlated fluctuations do not affect single-exciton dynamics and can be described as a nonlocal contribution to the spectral broadening, which appears as a multiplicative factor in the time-domain response function. Intraband coherences are damped only by uncorrelated transition energy fluctuations. The signal can then be expressed as a spectral convolution of a local contribution of the uncorrelated fluctuations and the nonlocal contribution of the correlated fluctuations. (C) 2011 American Institute of Physics. [doi:10.1063/1.3579455]