Charge-Transfer Excitations Steer the Davydov Splitting and Mediate Singlet Exciton Fission in Pentacene

Quantum-chemical calculations are combined to a model Frenkel-Holstein Hamiltonian to assess the nature of the lowest electronic excitations in the pentacene crystal. We show that an admixture of charge-transfer excitations into the lowest singlet excited states form the origin of the Davydov splitt...

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Bibliographic Details
Published in:	Physical review letters Vol. 110; no. 22; p. 226402
Main Authors:	Beljonne, D., Yamagata, H., Brédas, J. L., Spano, F. C., Olivier, Y.
Format:	Journal Article
Language:	English
Published:	United States 31.05.2013
ISSN:	0031-9007, 1079-7114, 1079-7114
Online Access:	Get full text
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Summary:	Quantum-chemical calculations are combined to a model Frenkel-Holstein Hamiltonian to assess the nature of the lowest electronic excitations in the pentacene crystal. We show that an admixture of charge-transfer excitations into the lowest singlet excited states form the origin of the Davydov splitting and mediate instantaneous singlet exciton fission by direct optical excitation of coherently coupled single and double exciton states, in agreement with recent experiments.
Bibliography:	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23
ISSN:	0031-9007 1079-7114 1079-7114
DOI:	10.1103/PhysRevLett.110.226402