期刊
NATURE CHEMISTRY
卷 8, 期 12, 页码 1120-1125出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2589
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资金
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, US Department of Energy (DOE) [DE-FG02-99ER14999]
- Argonne-Northwestern Solar Energy Research (ANSER) Center
- Argonne-Northwestern Solar Energy Research (ANSER) Center, an Energy Frontier Research Center - Office of Science, Office of Basic Energy Sciences, US DOE [DE-SC0001059]
When an assembly of two or more molecules absorbs a photon to form a singlet exciton, and the energetics and intermolecular interactions are favourable, the singlet exciton can rapidly and spontaneously produce two triplet excitons by singlet fission. To understand this process is important because it may prove to be technologically significant for enhancing solar-cell performance. Theory strongly suggests that charge-transfer states are involved in singlet fission, but their role has remained an intriguing puzzle and, up until now, no molecular system has provided clear evidence for such a state. Here we describe a terrylenediimide dimer that forms a charge-transfer state in a few picoseconds in polar solvents, and undergoes equally rapid, high-yield singlet fission in nonpolar solvents. These results show that adjusting the charge-transfer-state energy relative to those of the exciton states can serve to either inhibit or promote singlet fission.
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