期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 134, 期 1, 页码 386-397出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja2080482
关键词
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资金
- Office of Naval Research [N00014-05-1-0021, N00014-05-1-0019]
- BP Solar, Inc.
- ANSER Center, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
- MRSEC of the National Science Foundation at the Materials Research Center of Northwestern University [DMR-0520513]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1121262] Funding Source: National Science Foundation
The photophysics and morphology of thin films of N,N-bis(2,6-diisopropylphenyl)perylene-3,4:9,10-bis(dicarboximide) (1) and the 1,7-diphenyl (2) and 1,7-bis(3,5-di-tert-butylphenyl) (3) derivatives blended with 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pn) were studied for their potential use as photoactive layers in organic photovoltaic (OPV) devices. Increasing the steric bulk of the 1,7-substituents of the perylene-3,4:9,10-bis(dicarboximide) (PDI) impedes aggregation in the solid state. Film characterization data using both atomic force microscopy and X-ray diffraction showed that decreasing the PDI aggregation by increasing the steric bulk in the order 1 < 2 < 3 correlates with a decrease in the density/size of crystalline TIPS-Pn domains. Transient absorption spectroscopy was performed on similar to 100 nm solution-processed TIPS-Pn:PDI blend films to characterize the charge separation dynamics. These results showed that selective excitation of the TIPS-Pn results in competition between ultrafast singlet fission ((1)*TIPS-Pn + TIPS-Pn -> 2 (3)*TIPS-Pn) and charge transfer from (1)*TIPS-Pn to PDIs 1-3. As the blend films become more homogeneous across the series TIPS-Pn:PDI 1 -> 2 -> 3, charge separation becomes competitive with singlet fission. Ultrafast charge separation forms the geminate radical ion pair state (1)(TIPS-Pn(+center dot)-PDI-center dot) that undergoes radical pair intersystem crossing to form (3)(TIPS-Pn(+center dot)-PDI-center dot), which then undergoes charge recombination to yield either (3)*PDI or (3)*TIPS-Pn. Energy transfer from (3)*PDI to TIPS-Pn also yields (3)*TIPS-Pn. These results show that multiple pathways produce the (3)*TIPS-Pn state, so that OPV design strategies based on this system must utilize this triplet state for charge separation.
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