Explicit Correlated Exciton-Vibrational Dynamics of the FMO Complex
arXiv:1503.07059 · doi:10.1021/acs.jpcb.5b03928
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 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.
arXiv commentrevised and expanded version
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- Coherent quantum dynamics launched by incoherent relaxation in a quantum circuit simulator of a light-harvesting complex
- Effective Modeling of Open Quantum Systems by Low-rank Discretization of Structured Environments
- The Effect of Site-Specific Spectral Densities on the High-Dimensional Exciton-Vibrational Dynamics in the FMO Complex
- Exploring Disordered Quantum Spin Models with a Multi-Layer Multi-Configurational Approach
- Dissipation Pathways in a Photosynthetic Complex