화학공학소재연구정보센터
Journal of Physical Chemistry A, Vol.115, No.16, 3845-3858, 2011
Decoherence in Weakly Coupled Excitonic Complexes
Equations of motion for weakly, coupled excitonic complexes are derived. The description allows one 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 shown to be related to the well-known Forster type energy-transfer rate equations, but unlike Forster 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 the homogeneous limit, demonstrating a distinct delocalization effect and reduction of the resonance coupling due to interaction with the bath.