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The coupled quantum dynamics of excitonic and vibrational degrees of freedomis investigated for high-dimensional models of the Fenna-Matthews-Olson (FMO)complex. This includes a seven and an eight-site model with 518 and 592harmonic vibrational modes, respectively. The coupling between local electronictransitions and vibrations is described within the Huang-Rhys model usingparameters that are obtained by discretization of an experimental spectraldensity. Different pathways of excitation energy flow are analyzed in terms ofthe reduced one-exciton density matrix, focussing on the role of vibrationaland vibronic excitation. Distinct features due to both competing time scales ofvibrational and exciton motion and vibronically-assisted transfer are observed.The question of the effect of initial state preparation is addressed bycomparing the case of an instantaneous Franck-Condon excitation at a singlesite with that of a laser field excitation.

Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) Approach to the Correlated Exciton-Vibrational Dynamics in the FMO Complex