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dc.contributor.authorParkhill, John Anthony
dc.contributor.authorTempel, David Gabriel
dc.contributor.authorAspuru-Guzik, Alan
dc.date.accessioned2012-04-06T15:24:19Z
dc.date.issued2012-04-06
dc.identifier.citationParkhill, John A., David G. Tempel, and Alan Aspuru-Guzik. 2012. Exciton coherence lifetimes from electronic structure. Journal of Chemical Physics 136(10): 104510.en_US
dc.identifier.issn0021-9606en_US
dc.identifier.issn1089-7690en_US
dc.identifier.urihttp://nrs.harvard.edu/urn-3:HUL.InstRepos:8514994
dc.description.abstractWe model the coherent energy transfer of an electronic excitation within covalently linked aromatic homodimers from first-principles. Our results shed light on whether commonly used models of the bath calculated via detailed electronic structure calculations can reproduce the key dynamics. For the systems we model, the time scales of coherent transport are experimentally known from time-dependent polarization anisotropy measurements, and so we can directly assess whether current techniques are predictive for modeling coherent transport. The coupling of the electronic degrees of freedom to the nuclear degrees of freedom is calculated from first-principles rather than assumed, and the fluorescence anisotropy decay is directly reproduced. Surprisingly, we find that although time-dependent density functional theory absolute energies are routinely in error by orders of magnitude more than the coupling energy between monomers, the coherent transport properties of these dimers can be semi-quantitatively reproduced from these calculations. Future directions which must be pursued to yield predictive and reliable models of coherent transport are suggested.en_US
dc.description.sponsorshipChemistry and Chemical Biologyen_US
dc.description.sponsorshipPhysicsen_US
dc.language.isoen_USen_US
dc.publisherAmerican Institute of Physicsen_US
dc.relation.isversionofdoi:10.1063/1.3689858en_US
dash.licenseLAA
dc.subjectab initio calculationsen_US
dc.subjectdensity functional theoryen_US
dc.subjectelectronic structureen_US
dc.subjectexcitonsen_US
dc.subjectfluorescenceen_US
dc.subjectorganic compoundsen_US
dc.titleExciton Coherence Lifetimes from Electronic Structureen_US
dc.typeJournal Articleen_US
dc.description.versionAuthor's Originalen_US
dc.relation.journalJournal of Chemical Physicsen_US
dash.depositing.authorAspuru-Guzik, Alan
dash.waiver2012-02-12
dc.date.available2012-04-06T15:24:19Z
dc.identifier.doi10.1063/1.3689858*
dash.contributor.affiliatedParkhill, John Anthony
dash.contributor.affiliatedTempel, David
dash.contributor.affiliatedAspuru-Guzik, Alan


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