期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 121, 期 39, 页码 21262-21271出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.7b07870
关键词
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资金
- Chemical Sciences, Geo-sciences, and Biosciences Division, Office of Basic Energy Sciences, U.S. Department of Energy (DOE) [DE-FG02-99ER14999]
- Swiss National Science Foundation [SNF 200020_159802]
- MRSEC of the National Science Foundation at the Materials Research Center of Northwestern University [DMR-1121262]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205, NSF ECCS-1542205]
- Keck-II of Northwestern University's NUANCE Center
- MRSEC at the Materials Research Center [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
Cyano-substituted tetracenes (5,11-dicyano-6,12-diphenyltetracene, Tet) undergo exoergic singlet fission (SF), a spin-allowed photophysical process that generates a pair of triplet excitons from one singlet exciton. To elucidate substituent effects on SF, we have measured the SF dynamics and triplet yields of thin films, formed by Tet bearing hydrogen (H), methyl (Me), fluoro (F), and trimethylsilyl (TMS) substituents on the p-phenyl positions and on the 3 and 9 positions of the tetracene core, by time-resolved spectroscopy in the vis-NIR and IR regions. The H-, Me-, and F-Tet display strong intramolecular electronic coupling (pi-pi distances <4 angstrom), and SF gives high triplet exciton yields up to 200% (quantitative). In addition, a charge-transfer state mediates SF in F-Tet films, while H-Tet and Me-Tet show no evidence for such a state. Correlations between the SF yields and the crystal structure show that chromophore slippage along both their short and long axes allows efficient SF and that a large degree of pi contact between the chromophores is not necessary for rapid and efficient SF in the solid state. As expected, the large interchromophore distance in TMS-Tet (>4 angstrom) reduces its SF triplet yield to about 60%.
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