Efficient Energy Transfer in Light-Harvesting Systems, II: Quantum-Classical Comparison, Flux Network, and Robustness Analysis

Details Efficient Energy Transfer in Light-Harvesting Systems, II: Quantum-Classical Comparison, Flux Network, and Robustness Analysis Efficient Energy Transfer in Light-Harvesting Systems, II: Quantum-Classical Comparison, Flux Network, and Robustness Analysis

2011-09-27

arxiv.org/abs/1109.5769v1

Physics

Chemical Physics

Scientific paper

Following the calculation of optimal energy transfer in thermal environment in our first paper (New J. Phys. {\bf 12}, 105012), full quantum dynamics and leading-order `classical' hopping kinetics are compared for the Fenna-Matthews-Olson (FMO) protein complex with the thermal bath described by classical white noise (the Haken-Strobl model) and by quantum Debye noise. Because the two-site quantum dynamics is fully captured by the hopping kinetics, the difference between the quantum dynamics and 'classical' kinetics is due to higher-order quantum corrections, which include non-local multi-site coherence, i.e. long-range coherence. We observe that higher-order quantum correction leads to small changes in the trapping time or in energy transfer efficiency. (1-2% in the Haken-Strobl model and $\lessapprox 10%$ in the quantum Debye model), suggesting that quantum coherence does not extend beyond a pair of sites in FMO and the optimal efficiency in FMO can be explained by Forster rate theory. However, using the population flux network, %instead of energy transfer efficiency, we can identify significant differences in the major energy transfer pathway between hopping kinetics and quantum dynamics due to multi-site quantum coherence. (26% in the Haken-Strobl model and 32% in the quantum Debye model for the initial site at BChl 1). In addition, the golden-rule rate expression for the hopping rate provides a simple and reliable estimation on the stability of the energy transfer against the change of internal (Hamiltonian) and external (dephasing rate, trapping rate, etc.) parameters. The quantum-classical comparison with the removal of the bottleneck site, BChl 4, demonstrates quantum protection by the mechanism via multi-site quantum coherence.

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