Explicit Correlated Exciton-Vibrational Dynamics of the FMO Complex

Abstract

The coupled exciton-vibrational dynamics of a 3-site FMO model is investigated using the numerically exact multilayer multiconfiguration time-dependent Hartree approach. Thereby the vibrational mode specific coupling to local electronic transitions is adapted from a discretized experimental spectral density. The solution of the resulting time-dependent Schrödinger equation including three electronic and 450 vibrational degrees of freedom is analyzed in terms of excitonic populations and coherences. Emphasis is put onto the role of specific ranges of vibrational frequencies. It is observed that modes between 160 and 300 cm${}^{-1}$ are responsible for the subpicosecond population and coherence decay. Further, it is found that a mean-field approach with respect to the vibrational degrees of freedom is not applicable.

revised and expanded 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
• Enhanced quantum entanglement in the non-Markovian dynamics of biomolecular excitons
• On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
• Exploiting structured environments for efficient energy transfer: The phonon antenna mechanism

Cited by in corpus (1)

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