Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 6, Issue 10, Pages 1925-1929Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b00437
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Funding
- Ministry of Science and Technology of Taiwan, Republic of China [101-2628-M-001-003-MY4]
- Academia Sinica through the Research Project on Nano Science and Technology
- Academia Sinica through the Center for Sustainability Science
- National Center for Theoretical Sciences
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The electronic coupling for singlet fission, an important parameter for determining the rate, has been found to be too small unless charge-transfer (CT) components were introduced in the diabatic states, mostly through perturbation or a model Hamiltonian. In the present work, the fragment spin difference (FSD) scheme was generalized to calculate the singlet fission coupling. The largest coupling strength obtained was 14.8 meV for two pentacenes in a crystal structure, or 33.7 meV for a transition-state structure, which yielded a singlet fission lifetime of 239 or 37 fs, generally consistent with experimental results (80 fs). Test results with other polyacene molecules are similar. We found that the charge on one fragment in the S-1 diabatic state correlates well with FSD coupling, indicating the importance of the CT component. The FSD approach is a useful first-principle method for singlet fission coupling, without the need to include the CT component explicitly.
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