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- Timothy C. Berkelbach
- Columbia University 1 Department of Chemistry, , 3000 Broadway, New York, New York 10027, USA
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- Mark S. Hybertsen
- Brookhaven National Laboratory 2 Center for Functional Nanomaterials, , Upton, New York 11973-5000, USA
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- David R. Reichman
- Columbia University 1 Department of Chemistry, , 3000 Broadway, New York, New York 10027, USA
説明
<jats:p>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.</jats:p>
収録刊行物
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- The Journal of Chemical Physics
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The Journal of Chemical Physics 138 (11), 114102-, 2013-03-15
AIP Publishing