Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 138, Issue 11, Pages -Publisher
AIP Publishing
DOI: 10.1063/1.4794425
Keywords
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Funding
- Center for Re-Defining Photovoltaic Efficiency through Molecule Scale Control
- Energy Frontier Research Center
- U.S. 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)
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Singlet fission, a spin-allowed energy transfer process generating two triplet excitons from one singlet exciton, has the potential to dramatically increase the efficiency of organic solar cells. However, the dynamical mechanism of this phenomenon is not fully understood and a complete, microscopic theory of singlet fission is lacking. In this work, we assemble the components of a comprehensive microscopic theory of singlet fission that connects excited state quantum chemistry calculations with finite-temperature quantum relaxation theory. We elaborate on the distinction between localized diabatic and delocalized exciton bases for the interpretation of singlet fission experiments in both the time and frequency domains. We discuss various approximations to the exact density matrix dynamics and propose Redfield theory as an ideal compromise between speed and accuracy for the detailed investigation of singlet fission in dimers, clusters, and crystals. Investigations of small model systems based on parameters typical of singlet fission demonstrate the numerical accuracy and practical utility of this approach. (C) 2013 American Institute of Physics. [http://dx.doi.org/10.1063/1.4794425]
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