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

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

doi:10.1021/jacs.9b03385

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

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

Research output: Contribution to journal › Article › peer-review

80 Scopus citations

Abstract

Photon upconversion employing semiconductor 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. Here, 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.

Original language	English
Pages (from-to)	9769-9772
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	141
Issue number	25
DOIs	https://doi.org/10.1021/jacs.9b03385
State	Published - Jun 26 2019

Bibliographical note

Publisher Copyright:
Copyright © 2019 American Chemical Society.

Funding

M.L.T. acknowledges the Alfred P. Sloan foundation. The U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Solar Photochemistry Program Award Numbers DE-FG02-12ER16347 to T.L and DE-SC0018969 to M.L.T supported this work. Z.L. and K.R.G. contributed the XPS measurements under work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences and the EPSCoR program, under Award Number DE-SC0018208.

Funders	Funder number
EPSCoR program	DE-SC0018208
Office of Basic Energy Sciences	DE-SC0018969, DE-FG02-12ER16347
U.S. Department of Energy
Office of Science Programs

ASJC Scopus subject areas

Catalysis
Biochemistry
General Chemistry
Colloid and Surface Chemistry

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title = "Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers",

abstract = "Photon upconversion employing semiconductor 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. Here, 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.",

author = "Zhiyuan Huang and Zihao Xu and Melika Mahboub and Zhiming Liang and Paulina Jaimes and Pan Xia and Graham, \{Kenneth R.\} and Tang, \{Ming L.\} and Tianquan Lian",

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AU - Huang, Zhiyuan

AU - Xu, Zihao

AU - Mahboub, Melika

AU - Liang, Zhiming

AU - Jaimes, Paulina

AU - Xia, Pan

AU - Graham, Kenneth R.

AU - Tang, Ming L.

AU - Lian, Tianquan

PY - 2019/6/26

Y1 - 2019/6/26

N2 - Photon upconversion employing semiconductor 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. Here, 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.

AB - Photon upconversion employing semiconductor 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. Here, 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.

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

Abstract

Bibliographical note

Funding

ASJC Scopus subject areas

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