期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 6, 页码 2326-2335出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b12662
关键词
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资金
- David and Lucile Packard Fellowship for Science and Engineering
- STROBE, A National Science Foundation Science & Technology Center [DMR 1548924]
- Center for Computational Study of Excited-State Phenomena in Energy Materials (C2SEPEM) at the Lawrence Berkeley National Laboratory - U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC02-05CH11231]
- National Science Foundation [DGE 1106400]
- Alfred P. Sloan Research Fellowship
- David and Lucile Packard Foundation
- Camille and Henry Dreyfus Teacher Scholar Award
Singlet fission is the spin-conserving process by which a singlet exciton splits into two triplet excitons. Singlet fission occurs via a correlated triplet pair intermediate, but direct evidence of this state has been scant, and in films of TIPS-pentacene, a small molecule organic semiconductor, even the rate of fission has been unclear. We use polarization-resolved transient absorption microscopy on individual crystalline domains of TIPS-pentacene to establish the fission rate and demonstrate that the initially created triplets remain bound for a surprisingly long time, hundreds of picoseconds, before separating. Furthermore, using a broadband probe, we show that it is possible to determine absorbance spectra of individual excited species in a crystalline solid. We find that triplet interactions perturb the absorbance, and provide evidence that triplet interaction and binding could be caused by the p-stacked geometry. Elucidating the relationship between the lattice structure and the electronic structure and dynamics has important implications for the creation of photovoltaic devices that aim to boost efficiency via singlet fission.
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