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dc.contributor.authorYamagata, H.en_US
dc.contributor.authorNorton, J.en_US
dc.contributor.authorHontz, E.en_US
dc.contributor.authorOlivier, Y.en_US
dc.contributor.authorBeljonne, Daviden_US
dc.contributor.authorBrédas, Jean-Lucen_US
dc.contributor.authorSilbey, R. J.en_US
dc.contributor.authorSpano, F. C.en_US
dc.date.accessioned2013-05-29T18:28:37Z
dc.date.available2013-05-29T18:28:37Z
dc.date.issued2011-03
dc.identifier.citationYamagata, H. and Norton, J. and Hontz, E. and Olivier, Y. and Beljonne, D. and Brédas, J. L. and Silbey, R. J. and Spano, F. C., "The nature of singlet excitons in oligoacene molecular crystals," Journal of Chemical Physics, 134, 20, (May 28 2011)en_US
dc.identifier.issn0021-9606
dc.identifier.urihttp://hdl.handle.net/1853/47106
dc.description© 2011 American Institute of Physics. The electronic version of this article is the complete one and can be found at: http://dx.doi.org/10.1063/1.3590871en_US
dc.descriptionDOI: 10.1063/1.3590871en_US
dc.description.abstractA theory for polarized absorption in crystalline oligoacenes is presented, which includes Frenkel exciton coupling, the coupling between Frenkel and charge-transfer (CT) excitons, and the coupling of all neutral and ionic excited states to the dominant ring-breathing vibrational mode. For tetracene, spectra calculated using all Frenkel couplings among the five lowest energy molecular singlet states predict a Davydov splitting (DS) of the lowest energy (0–0) vibronic band of only −32 cm ⁻¹, far smaller than the measured value of 631 cm ⁻¹ and of the wrong sign—a negative sign indicating that the polarizations of the lower and upper Davydov components are reversed from experiment. Inclusion of Frenkel-CT coupling dramatically improves the agreement with experiment, yielding a 0–0 DS of 601 cm ⁻¹ and a nearly quantitative reproduction of the relative spectral intensities of the 0–n vibronic components. Our analysis also shows that CT mixing increases with the size of the oligoacenes. We discuss the implications of these results on exciton dissociation and transport.en_US
dc.publisherGeorgia Institute of Technologyen_US
dc.subjectDavydov splittingen_US
dc.subjectExcited statesen_US
dc.subjectOrganic semiconductorsen_US
dc.subjectPhonon-exciton interactionsen_US
dc.subjectUltraviolet spectraen_US
dc.subjectVisible spectraen_US
dc.titleThe nature of singlet excitons in oligoacene molecular crystalsen_US
dc.typeArticleen_US
dc.contributor.corporatenameGeorgia Institute of Technology. Center for Organic Photonics and Electronicsen_US
dc.contributor.corporatenameTemple University. Dept. of Chemistryen_US
dc.contributor.corporatenameGeorgia Institute of Technology. School of Chemistry and Biochemistryen_US
dc.contributor.corporatenameUniversité de Mons. Laboratoire de Chimie des Matériaux nouveauxen_US
dc.contributor.corporatenameMassachusetts Institute of Technology. Dept. of Chemistry and Center for Excitonicsen_US
dc.publisher.originalAmerican Institute of Physicsen_US
dc.identifier.doi10.1063/1.3590871


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