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dc.contributor.authorWu, Jianlan
dc.contributor.authorLiu, Fan
dc.contributor.authorMa, Jian
dc.contributor.authorSilbey, Robert J.
dc.contributor.authorCao, Jianshu
dc.date.accessioned2013-11-04T19:07:24Z
dc.date.available2013-11-04T19:07:24Z
dc.date.issued2012-11
dc.date.submitted2012-06
dc.identifier.issn00219606
dc.identifier.issn1089-7690
dc.identifier.urihttp://hdl.handle.net/1721.1/81985
dc.description.abstractFollowing the calculation of optimal energy transfer in thermal environment in our first paper [J. L. Wu, F. Liu, Y. Shen, J. S. Cao, and R. J. Silbey, New J. Phys.12, 105012 (2010)], full quantum dynamics and leading-order “classical” hopping kinetics are compared in the seven-site Fenna-Matthews-Olson (FMO) protein complex. The difference between these two dynamic descriptions is due to higher-order quantum corrections. Two thermal bath models, classical white noise (the Haken-Strobl-Reineker (HSR) model) and quantum Debye model, are considered. In the seven-site FMO model, we observe that higher-order corrections lead to negligible changes in the trapping time or in energy transfer efficiency around the optimal and physiological conditions (2% in the HSR model and 0.1% in the quantum Debye model for the initial site at BChl 1). However, using the concept of integrated flux, we can identify significant differences in branching probabilities of the energy transfer network between hopping kinetics and quantum dynamics (26% in the HSR model and 32% in the quantum Debye model for the initial site at BChl 1). This observation indicates that the quantum coherence can significantly change the distribution of energy transfer pathways in the flux network with the efficiency nearly the same. The quantum-classical comparison of the average trapping time with the removal of the bottleneck site, BChl 4, demonstrates the robustness of the efficient energy transfer by the mechanism of multi-site quantum coherence. To reconcile with the latest eight-site FMO model which is also investigated in the third paper [J. Moix, J. L. Wu, P. F. Huo, D. F. Coker, and J. S. Cao, J. Phys. Chem. Lett.2, 3045 (2011)], the quantum-classical comparison with the flux network analysis is summarized in Appendix C . The eight-site FMO model yields similar trapping time and network structure as the seven-site FMO model but leads to a more disperse distribution of energy transfer pathways.en_US
dc.description.sponsorshipNational Science Foundation (U.S.) (Grant CHE-1112825)en_US
dc.description.sponsorshipUnited States. Defense Advanced Research Projects Agency (Grant N66001-10-1-4063)en_US
dc.description.sponsorshipUnited States. Dept. of Energy. Office of Basic Energy Sciences (Grant DE-SC0001088)en_US
dc.language.isoen_US
dc.publisherAmerican Institute of Physics (AIP)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1063/1.4762839en_US
dc.rightsArticle is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.en_US
dc.sourceMIT web domainen_US
dc.titleEfficient energy transfer in light-harvesting systems: Quantum-classical comparison, flux network, and robustness analysisen_US
dc.typeArticleen_US
dc.identifier.citationWu, Jianlan, Fan Liu, Jian Ma, Robert J. Silbey, and Jianshu Cao. “Efficient energy transfer in light-harvesting systems: Quantum-classical comparison, flux network, and robustness analysis.” The Journal of Chemical Physics 137, no. 17 (2012): 174111. © 2012 American Institute of Physicsen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Chemistryen_US
dc.contributor.mitauthorWu, Jianlanen_US
dc.contributor.mitauthorMa, Jianen_US
dc.contributor.mitauthorSilbey, Robert J.en_US
dc.contributor.mitauthorCao, Jianshuen_US
dc.relation.journalThe Journal of Chemical Physicsen_US
dc.eprint.versionFinal published versionen_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dspace.orderedauthorsWu, Jianlan; Liu, Fan; Ma, Jian; Silbey, Robert J.; Cao, Jianshuen_US
dc.identifier.orcidhttps://orcid.org/0000-0001-7616-7809
mit.licensePUBLISHER_POLICYen_US


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