Environment-assisted quantum walks in photosynthetic energy transfer

被引:963
作者
Mohseni, Masoud [1 ]
Rebentrost, Patrick [1 ]
Lloyd, Seth [2 ]
Aspuru-Guzik, Alan [1 ]
机构
[1] Harvard Univ, Dept Chem & Biol Chem, Cambridge, MA 02138 USA
[2] MIT, Dept Mech Engn, Cambridge, MA 02139 USA
关键词
excitons; fluctuations; free energy; molecular biophysics; photosynthesis; proteins; quantum theory; reaction kinetics theory;
D O I
10.1063/1.3002335
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 , 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%.
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页数:9
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