Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers
Abstract
Photon upconversion employing semicon- ductor nanocrystals (NCs) makes use of their large and tunable absorption to harvest light in the near-infrared (NIR) wavelengths as well as their small gap between singlet and triplet excited states to reduce energy losses. In this work, we report the highest QY (11.8%) thus far for the conversion of NIR to yellow photons by improving the quality of the PbS NC. This high QY was achieved by using highly purified lead and thiourea precursors. This QY is 2.6 times higher than from NCs prepared with commercially available lead and sulfide precursors. Transient absorption spectroscopy reveals two reasons for the enhanced QY: longer intrinsic exciton lifetimes of PbS NCs and the ability to support a longer triplet lifetime for the surface-bound transmitter molecule. Overall, this results in a higher efficiency of triplet exciton transfer from the PbS NC light absorber to the emitter and thus a higher photon upconversion QY.
- Authors:
-
- Univ. of California, Riverside, CA (United States)
- Emory Univ., Atlanta, GA (United States)
- Univ. of Kentucky, Lexington, KY (United States)
- Publication Date:
- Research Org.:
- Univ. of California, Riverside, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1773887
- Grant/Contract Number:
- SC0018969; FG02-12ER16347; SC0018208
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 25; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 30 DIRECT ENERGY CONVERSION; Excitons; Light absorption; Luminescence; Energy transfer; Precursors
Citation Formats
Huang, Zhiyuan, Xu, Zihao, Mahboub, Melika, Liang, Zhiming, Jaimes, Paulina, Xia, Pan, Graham, Kenneth R., Tang, Ming L., and Lian, Tianquan. Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b03385.
Huang, Zhiyuan, Xu, Zihao, Mahboub, Melika, Liang, Zhiming, Jaimes, Paulina, Xia, Pan, Graham, Kenneth R., Tang, Ming L., & Lian, Tianquan. Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers. United States. https://doi.org/10.1021/jacs.9b03385
Huang, Zhiyuan, Xu, Zihao, Mahboub, Melika, Liang, Zhiming, Jaimes, Paulina, Xia, Pan, Graham, Kenneth R., Tang, Ming L., and Lian, Tianquan. Mon .
"Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers". United States. https://doi.org/10.1021/jacs.9b03385. https://www.osti.gov/servlets/purl/1773887.
@article{osti_1773887,
title = {Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers},
author = {Huang, Zhiyuan and Xu, Zihao and Mahboub, Melika and Liang, Zhiming and Jaimes, Paulina and Xia, Pan and Graham, Kenneth R. and Tang, Ming L. and Lian, Tianquan},
abstractNote = {Photon upconversion employing semicon- ductor nanocrystals (NCs) makes use of their large and tunable absorption to harvest light in the near-infrared (NIR) wavelengths as well as their small gap between singlet and triplet excited states to reduce energy losses. In this work, we report the highest QY (11.8%) thus far for the conversion of NIR to yellow photons by improving the quality of the PbS NC. This high QY was achieved by using highly purified lead and thiourea precursors. This QY is 2.6 times higher than from NCs prepared with commercially available lead and sulfide precursors. Transient absorption spectroscopy reveals two reasons for the enhanced QY: longer intrinsic exciton lifetimes of PbS NCs and the ability to support a longer triplet lifetime for the surface-bound transmitter molecule. Overall, this results in a higher efficiency of triplet exciton transfer from the PbS NC light absorber to the emitter and thus a higher photon upconversion QY.},
doi = {10.1021/jacs.9b03385},
journal = {Journal of the American Chemical Society},
number = 25,
volume = 141,
place = {United States},
year = {Mon Jun 10 00:00:00 EDT 2019},
month = {Mon Jun 10 00:00:00 EDT 2019}
}
Web of Science
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