The Effect of Site-Specific Spectral Densities on the High-Dimensional Exciton-Vibrational Dynamics in the FMO Complex

Abstract

The coupled exciton-vibrational dynamics of a three-site model of the FMO complex is investigated using the Multi-layer Multi-configuration Time-dependent Hartree (ML-MCTDH) approach. Emphasis is put on the effect of the spectral density on the exciton state populations as well as on the vibrational and vibronic non-equilibrium excitations. Models which use either a single or site-specific spectral densities are contrasted to a spectral density adapted from experiment. For the transfer efficiency, the total integrated Huang-Rhys factor is found to be more important than details of the spectral distributions. However, the latter are relevant for the obtained non-equilibrium vibrational and vibronic distributions and thus influence the actual pattern of population relaxation.

revised version

References in corpus (5)

• Multilayer multi-configuration time-dependent Hartree method: implementation and applications to a Henon-Heiles Hamiltonian and to pyrazine
• Long-Lived Electronic Coherence in Dissipative Exciton-Dynamics of Light-Harvesting Complexes
• On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
• Explicit Correlated Exciton-Vibrational Dynamics of the FMO Complex
• On the Applicability of the Caldeira-Leggett Model to Condensed Phase Vibrational Spectroscopy

Cited by in corpus (2)

• Systematic coarse-graining of environments for the non-perturbative simulation of open quantum systems
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