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dc.contributor.authorMa, Jian
dc.contributor.authorCao, Jianshu
dc.date.accessioned2016-08-11T20:57:37Z
dc.date.available2016-08-11T20:57:37Z
dc.date.issued2015-03
dc.date.submitted2014-08
dc.identifier.issn0021-9606
dc.identifier.issn1089-7690
dc.identifier.urihttp://hdl.handle.net/1721.1/103910
dc.description.abstractWe study the Förster resonant energy transfer rate, absorption and emission spectra in multichromophoric systems. The multichromophoric Förster theory (MCFT) is determined from an overlap integral of generalized matrices related to the donor’s emission and acceptor’s absorption spectra, which are obtained via a full 2nd-order cumulant expansion technique developed in this work. We calculate the spectra and MCFT rate for both localized and delocalized systems, and calibrate the analytical 2nd-order cumulant expansion with the exact stochastic path integral method. We present three essential findings: (i) The role of the initial entanglement between the donor and its bath is found to be crucial in both the emission spectrum and the MCFT rate. (ii) The absorption spectra obtained by the cumulant expansion method are nearly identical to the exact spectra for both localized and delocalized systems, even when the system-bath coupling is far from the perturbative regime. (iii) For the emission spectra, the cumulant expansion can give reliable results for localized systems, but fail to provide reliable spectra of the high-lying excited states of a delocalized system, when the system-bath coupling is large and the thermal energy is small. This paper also provides a simple golden-rule derivation of the MCFT, reviews existing methods, and motivates further developments in the subsequent papers.en_US
dc.description.sponsorshipNational Science Foundation (U.S.) (NSF award CHE-1112825)en_US
dc.description.sponsorshipUnited States. Defense Advanced Research Projects Agency (Grant No. N99001-10-1-4063)en_US
dc.language.isoen_US
dc.publisherAmerican Institute of Physics (AIP)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1063/1.4908599en_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.titleFörster resonance energy transfer, absorption and emission spectra in multichromophoric systems. I. Full cumulant expansions and system-bath entanglementen_US
dc.typeArticleen_US
dc.identifier.citationMa, Jian, and Jianshu Cao. "Förster resonance energy transfer, absorption and emission spectra in multichromophoric systems. I. Full cumulant expansions and system-bath entanglement." Journal of Chemical Physics 142, 094106 (2015).en_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Chemistryen_US
dc.contributor.mitauthorMa, Jianen_US
dc.contributor.mitauthorCao, Jianshuen_US
dc.relation.journalJournal 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.orderedauthorsMa, Jian; Cao, Jianshuen_US
dspace.embargo.termsNen_US
dc.identifier.orcidhttps://orcid.org/0000-0001-7616-7809
mit.licensePUBLISHER_POLICYen_US
mit.metadata.statusComplete


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