Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 25, Pages 11270-11278Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c04583
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Funding
- National Natural Science Foundation of China [21975253, 21903084]
- Ministry of Science and Technology of China [2018YFA0208703]
- Strategic Pilot Science and Technology Project of Chinese Academy of Sciences [XDA21010206]
- LiaoNing Revitalization Talents Program [XLYC1807154]
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Triplet energy transfer from colloidal nanocrystals is a novel approach to sensitizing molecular triplets that are important for many applications. Recent studies suggest that this triplet transfer can be mediated by a hole transfer process when it is energetically allowed. In contrast, electrontransfer-mediated triplet transfer has not been observed yet, which is likely due to hole-trapping in typical II-VI group nanocrystals inhibiting the hole transfer step following initial electron transfer and hence disrupting a complete triplet exciton transfer. Here we report electron-transfer-mediated triplet energy transfer from CsPbCI3 and CsPbBr(3 )perovskite nanocrystals to surface-anchored rhodamine molecules. The mechanism was unambiguously established by ultrafast spectroscopy; control experiments using CdS nanocrystals also confirmed the role of hole-trapping in inhibiting this mechanism. The sensitized rhodamine triplets engaged in a variety of applications such as photon upconversion and singlet oxygen generation. Compared to conventional one-step triplet transfer, the electron-transfer-mediated mechanism is less demanding in terms of interfacial electronic coupling and hence is more generally implementable. Overall, this study not only establishes a complete framework of triplet energy transfer across nanocrystal/molecule interfaces but also greatly expands the scope of molecular triplet sensitization using nanocrystals.
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