期刊
JOURNAL OF CHEMICAL PHYSICS
卷 130, 期 23, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3155214
关键词
energy level crossing; molecular electronic states; molecule-photon collisions; nonradiative transitions; photosynthesis; quantum theory; solvent effects
资金
- Director, Office of Science, Office of Basic Energy Sciences, U. S. Department of Energy [DE-AC02-05CH11231]
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, U. S. Department of Energy [DE-AC03-76SF000098]
- JSPS Postdoctoral Fellowship for Research Abroad
The observation of long-lived electronic coherence in photosynthetic excitation energy transfer (EET) by Engel [Nature (London) 446, 782 (2007)] raises questions about the role of the protein environment in protecting this coherence and the significance of the quantum coherence in light harvesting efficiency. In this paper we explore the applicability of the Redfield equation in its full form, in the secular approximation and with neglect of the imaginary part of the relaxation terms for the study of these phenomena. We find that none of the methods can give a reliable picture of the role of the environment in photosynthetic EET. In particular the popular secular approximation (or the corresponding Lindblad equation) produces anomalous behavior in the incoherent transfer region leading to overestimation of the contribution of environment-assisted transfer. The full Redfield expression on the other hand produces environment-independent dynamics in the large reorganization energy region. A companion paper presents an improved approach, which corrects these deficiencies [A. Ishizaki and G. R. Fleming, J. Chem. Phys. 130, 234111 (2009)].
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