Paper detail

Decoherence in Weakly Coupled Excitonic Complexes

Equations of motion for weakly coupled excitonic complexes are derived. The description allows to treat the system in the basis of electronic states localized on individual chromophores, while at the same time accounting for experimentally observable delocalization effects in optical spectra. The equations are show to be related to the well-known Foerster type energy transfer rate equations, but unlike Foerster equations, they provide a description of the decoherence processes leading to suppression of the resonance coupling by bath fluctuations. Linear absorption and two-dimensional photon echo correlation spectra are calculated for simple model systems in homogeneous limit demonstrating distinct delocalization effect and reduction of the resonance coupling due to interaction with the bath.