Exciton Coherence Lifetimes from Electronic Structure

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Exciton Coherence Lifetimes from Electronic Structure

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dc.contributor.author Parkhill, John Anthony
dc.contributor.author Aspuru-Guzik, Alan
dc.contributor.author Tempel, David Gabriel
dc.date.accessioned 2012-04-06T15:24:19Z
dc.date.issued 2012-04-06
dc.identifier.citation Parkhill, 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.issn 0021-9606 en_US
dc.identifier.issn 1089-7690 en_US
dc.identifier.uri http://nrs.harvard.edu/urn-3:HUL.InstRepos:8514994
dc.description.abstract We 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.sponsorship Chemistry and Chemical Biology en_US
dc.description.sponsorship Physics en_US
dc.language.iso en_US en_US
dc.publisher American Institute of Physics en_US
dc.relation.isversionof doi:10.1063/1.3689858 en_US
dash.license LAA
dc.subject ab initio calculations en_US
dc.subject density functional theory en_US
dc.subject electronic structure en_US
dc.subject excitons en_US
dc.subject fluorescence en_US
dc.subject organic compounds en_US
dc.title Exciton Coherence Lifetimes from Electronic Structure en_US
dc.type Journal Article en_US
dc.description.version Author's Original en_US
dc.relation.journal Journal of Chemical Physics en_US
dash.depositing.author Aspuru-Guzik, Alan
dash.waiver 2012-02-12
dc.date.available 2012-04-06T15:24:19Z

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  • FAS Scholarly Articles [7262]
    Peer reviewed scholarly articles from the Faculty of Arts and Sciences of Harvard University

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