Triplet Energy Transfer from Perovskite Nanocrystals Mediated by Electron Transfer

Article abstract of DOI:10.1021/jacs.0c04583

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, electron-transfer-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 CsPbCl3 and CsPbBr3 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.

Full text of DOI:10.1021/jacs.0c04583

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Article
Triplet Energy Transfer from Perovskite
Nanocrystals Mediated by Electron Transfer
Xiao Luo, Guijie Liang, Yaoyao Han, Yulu Li, Tao Ding, Shan He, Xue Liu, and Kaifeng Wu
J. Am. Chem. Soc., Just Accepted Manuscript • DOI: 10.1021/jacs.0c04583 • Publication Date (Web): 01 Jun 2020
Downloaded from pubs.acs.org on June 1, 2020
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ACS Paragon Plus Environment

Journal of the American Chemical Society
Page 6 of 27
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ACS Paragon Plus Environment

Page 7 of 27
Journal of the American Chemical Society
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ACS Paragon Plus Environment

Journal of the American Chemical Society
Page 8 of 27
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ACS Paragon Plus Environment

Page 9 of 27
Journal of the American Chemical Society
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Journal of the American Chemical Society
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ACS Paragon Plus Environment

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ACS Paragon Plus Environment

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ACS Paragon Plus Environment

Journal of the American Chemical Society
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ACS Paragon Plus Environment

Page 17 of 27
Journal of the American Chemical Society
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ACS Paragon Plus Environment

Journal of the American Chemical Society
Page 18 of 27
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ACS Paragon Plus Environment

Page 19 of 27
Journal of the American Chemical Society
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ACS Paragon Plus Environment

Journal of the American Chemical Society
Page 20 of 27
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Journal of the American Chemical Society
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ACS Paragon Plus Environment

Journal of the American Chemical Society
Page 26 of 27
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ACS Paragon Plus Environment

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Journal of the American Chemical Society
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ACS Paragon Plus Environment