期刊
JOURNAL OF CHEMICAL PHYSICS
卷 141, 期 7, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4892793
关键词
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资金
- Center for Re-Defining Photovoltaic Efficiency through Molecule Scale Control, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001085]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- Department of Energy Office of Science Graduate Fellowship Program (DOE SCGF)
- ORISE-ORAU [DE-AC05-06OR23100]
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. (C) 2014 AIP Publishing LLC.
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