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J Chem Phys. 2008 Nov 7;129(17):174106. doi: 10.1063/1.3002335.

Environment-assisted quantum walks in photosynthetic energy transfer.

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1
Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford St., Cambridge, Massachusetts 02138, USA.

Abstract

Energy transfer within photosynthetic systems can display quantum effects such as delocalized excitonic transport. Recently, direct evidence of long-lived coherence has been experimentally demonstrated for the dynamics of the Fenna-Matthews-Olson (FMO) protein complex [Engel et al., Nature (London) 446, 782 (2007)]. However, the relevance of quantum dynamical processes to the exciton transfer efficiency is to a large extent unknown. Here, we develop a theoretical framework for studying the role of quantum interference effects in energy transfer dynamics of molecular arrays interacting with a thermal bath within the Lindblad formalism. To this end, we generalize continuous-time quantum walks to nonunitary and temperature-dependent dynamics in Liouville space derived from a microscopic Hamiltonian. Different physical effects of coherence and decoherence processes are explored via a universal measure for the energy transfer efficiency and its susceptibility. In particular, we demonstrate that for the FMO complex, an effective interplay between the free Hamiltonian evolution and the thermal fluctuations in the environment leads to a substantial increase in energy transfer efficiency from about 70% to 99%.

PMID:
19045332
DOI:
10.1063/1.3002335
[Indexed for MEDLINE]
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