期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 118, 期 34, 页码 19608-19617出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp505942k
关键词
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资金
- Center for Energy Nanoscience, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001013]
- Scientific Discovery through Advanced Computing (SciDAC) program - U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research and Basic Energy Sciences
- Welch Foundation [C-1559]
- National Science Foundation [NSF PHY11-25915]
The effect of morphology on singlet fission (SF) efficiency was investigated by using a combination of high-level electronic structure methods and a simple three-state kinetic model. The calculations reproduce the observed differences in SF efficiency in different polymorphs of 1,3-diphenylisobenzofuran (DPBF) and 1,6-diphenyl-1,3,5-hexatriene (DPH), as well as make predictions about 5,12-diphenyltetracene (DPT). The analysis of different factors contributing to the rates reveals that (i) there is more than one pair of adjacent chromophores that contribute to SF; (ii) not only slip-stacked configurations show efficient fission; and (iii) both electronic couplings and energy differences are responsible for different rates. The model predicts that the difference in SF efficiency in DPBF and DPH polymorphs increases at low temperature. In contrast, temperature dependence of the relative rates in the two DPT forms is predicted to be small. Our model predicts similar rates for the two polymorphs of DPT, although one form features much more favorable electronic couplings. This prediction depends strongly on the magnitude of Davydov's splitting; small changes in its value may change the ratio in favor of faster SF in xylene-grown crystals of DPT.
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