Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion
Abstract
Inorganic semiconductor nanocrystals interfaced with spin-triplet exciton-accepting organic molecules have emerged as promising materials for converting incoherent long-wavelength light into the visible range. However, these materials to date have made exclusive use of nanocrystals containing toxic elements, precluding their use in biological or environmentally sensitive applications. In this paper, we address this challenge by chemically functionalizing non-toxic silicon nanocrystals with triplet-accepting anthracene ligands. Photoexciting these structures drives spin-triplet exciton transfer from silicon to anthracene through a single 15 ns Dexter energy transfer step with a nearly 50% yield. When paired with 9,10-diphenylanthracene emitters, these particles readily upconvert 488–640 nm photons to 425 nm violet light with efficiencies as high as 7 ± 0.9% and can be readily incorporated into aqueous micelles for biological use. Our demonstration of spin-triplet exciton transfer from silicon to molecular triplet acceptors can critically enable new technologies for solar energy conversion, quantum information and near-infrared driven photocatalysis.
- Authors:
-
[1];
[1];
[1];
[2]
- Univ. of California, Riverside, CA (United States)
- Univ. of Texas, Austin, TX (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Riverside, CA (United States)
- Sponsoring Org.:
- USDOE; National Science Foundation (NSF); Robert A. Welch Foundation; Research Corporation for Science Advancement; US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1773889
- Grant/Contract Number:
- SC0018969; CHE-1610412; F-1885; 24489; FA9550-19-1-0092; CHE-1351663; 1351386
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Chemistry
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 2; Journal ID: ISSN 1755-4330
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Xia, Pan, Raulerson, Emily K., Coleman, Devin, Gerke, Carter S., Mangolini, Lorenzo, Tang, Ming Lee, and Roberts, Sean T. Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion. United States: N. p., 2019.
Web. doi:10.1038/s41557-019-0385-8.
Xia, Pan, Raulerson, Emily K., Coleman, Devin, Gerke, Carter S., Mangolini, Lorenzo, Tang, Ming Lee, & Roberts, Sean T. Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion. United States. https://doi.org/10.1038/s41557-019-0385-8
Xia, Pan, Raulerson, Emily K., Coleman, Devin, Gerke, Carter S., Mangolini, Lorenzo, Tang, Ming Lee, and Roberts, Sean T. Mon .
"Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion". United States. https://doi.org/10.1038/s41557-019-0385-8. https://www.osti.gov/servlets/purl/1773889.
@article{osti_1773889,
title = {Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion},
author = {Xia, Pan and Raulerson, Emily K. and Coleman, Devin and Gerke, Carter S. and Mangolini, Lorenzo and Tang, Ming Lee and Roberts, Sean T.},
abstractNote = {Inorganic semiconductor nanocrystals interfaced with spin-triplet exciton-accepting organic molecules have emerged as promising materials for converting incoherent long-wavelength light into the visible range. However, these materials to date have made exclusive use of nanocrystals containing toxic elements, precluding their use in biological or environmentally sensitive applications. In this paper, we address this challenge by chemically functionalizing non-toxic silicon nanocrystals with triplet-accepting anthracene ligands. Photoexciting these structures drives spin-triplet exciton transfer from silicon to anthracene through a single 15 ns Dexter energy transfer step with a nearly 50% yield. When paired with 9,10-diphenylanthracene emitters, these particles readily upconvert 488–640 nm photons to 425 nm violet light with efficiencies as high as 7 ± 0.9% and can be readily incorporated into aqueous micelles for biological use. Our demonstration of spin-triplet exciton transfer from silicon to molecular triplet acceptors can critically enable new technologies for solar energy conversion, quantum information and near-infrared driven photocatalysis.},
doi = {10.1038/s41557-019-0385-8},
journal = {Nature Chemistry},
number = 2,
volume = 12,
place = {United States},
year = {Mon Dec 02 00:00:00 EST 2019},
month = {Mon Dec 02 00:00:00 EST 2019}
}
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