Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers

Huang, Zhiyuan; Xu, Zihao; Mahboub, Melika; Liang, Zhiming; Jaimes, Paulina; Xia, Pan; Graham, Kenneth R.; Tang, Ming L.; Lian, Tianquan

doi:10.1021/jacs.9b03385

Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers

Journal Article · Mon Jun 10 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b03385· OSTI ID:1773887

^[1]; ^[2]; ^[3]; Liang, Zhiming ^[4]; Jaimes, Paulina ^[3]; ^[3]; ^[4]; ^[3]; ^[2]

Univ. of California, Riverside, CA (United States); UC Riverside
Emory Univ., Atlanta, GA (United States)
Univ. of California, Riverside, CA (United States)
Univ. of Kentucky, Lexington, KY (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Riverside, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0008798; SC0018208; SC0018969

OSTI ID:: 1773887

Alternate ID(s):: OSTI ID: 1611155

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 25 Vol. 141; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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A perspective on triplet fusion upconversion: triplet sensitizers beyond quantum dots VanOrman, Zachary A.; Bieber, Alexander S.; Wieghold, Sarah MRS Communications, Vol. 9, Issue 3 https://doi.org/10.1557/mrc.2019.115	journal	September 2019

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