Microscopic theory of singlet exciton fission. III. Crystalline pentacene.
J Chem Phys
; 141(7): 074705, 2014 Aug 21.
Article
em En
| MEDLINE
| ID: mdl-25149804
ABSTRACT
We extend our previous work on singlet exciton fission in isolated dimers to the case of crystalline materials, focusing on pentacene as a canonical and concrete example. We discuss the proper interpretation of the character of low-lying excited states of relevance to singlet fission. In particular, we consider a variety of metrics for measuring charge-transfer character, conclusively demonstrating significant charge-transfer character in the low-lying excited states. The impact of this electronic structure on the subsequent singlet fission dynamics is assessed by performing real-time master-equation calculations involving hundreds of quantum states. We make direct comparisons with experimental absorption spectra and singlet fission rates, finding good quantitative agreement in both cases, and we discuss the mechanistic distinctions that exist between small isolated aggregates and bulk systems.
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01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
J Chem Phys
Ano de publicação:
2014
Tipo de documento:
Article
País de afiliação:
Estados Unidos