期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 6, 页码 2203-2210出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c00058
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资金
- National Science Foundation [CHE-1428479, DMR-1905401]
- Natural Sciences and Engineering Council of Canada (NSERC)
- Institute for Complex Adaptive Matter (ICAM) fellowship by Kent State University
- NSF [CHE-1362504, CHE-1464477, CHE-1800325]
- DOE [DE-SC0016501]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0017971]
- Mcubed Program by the University of Michigan
- University of Michigan ICAM
- U.S. Department of Energy (DOE) [DE-SC0016501, DE-SC0017971] Funding Source: U.S. Department of Energy (DOE)
Efficient organic photovoltaics (OPVs) require broadband charge photogeneration with near-unity quantum yield. This can only be achieved by exploiting all pathways that generate charge. Electron transfer from organic donors to acceptors has been well-studied and is considered the primary path to charge photogeneration in OPVs. In contrast, much less is known about the hole transfer pathway. Here we study charge photogeneration in an archetypal system comprising tetraphenyldibenzoperiflanthene:C-70 blends using our recently developed multispectral two-dimensional electronic spectroscopy (M-2DES), supported by time-dependent density functional theory and fully quantum-mechanical Fermi's golden rule rate calculations. Our approach identifies in real time two rapid charge transfer pathways that are confirmed through computational analysis. Surprisingly, we find that both electron and hole transfer occur with comparable rates and efficiencies, facilitated by donor-acceptor electronic interactions. Our results highlight the importance of the hole transfer pathway for optimizing the efficiency of OPV devices employing small-molecule heterojunctions.
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