Influence of Complex Exciton-Phonon Coupling on Optical Absorption and Energy Transfer of Quantum Aggregates

Abstract

We present a theory that efficiently describes the quantum dynamics of an electronic excitation that is coupled to a continuous, highly structured phonon environment. Based on a stochastic approach to non-Markovian open quantum systems, we develop a dynamical framework that allows us to handle realistic systems where a fully quantum treatment is desired yet the usual approximation schemes fail. The capability of the method is demonstrated by calculating spectra and energy transfer dynamics of mesoscopic molecular aggregates, elucidating the transition from fully coherent to incoherent transfer.