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Title: Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots

Abstract

One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. This process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]
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  1. Center for Advanced Solar Photophysics, Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1413788
Alternate Identifier(s):
OSTI ID: 1416307
Report Number(s):
LA-UR-17-27775
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Name: ACS Nano Journal Volume: 10 Journal Issue: 12; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Auger recombination; Auger up-conversion; biexciton; core/shell PbSe/CdSe quantum dot; single exciton; trion; two-photon absorption; up-conversion

Citation Formats

Makarov, Nikolay S., Lin, Qianglu, Pietryga, Jeffrey M., Robel, István, and Klimov, Victor I. Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots. United States: N. p., 2016. Web. doi:10.1021/acsnano.6b04928.
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Makarov, Nikolay S., Lin, Qianglu, Pietryga, Jeffrey M., Robel, István, & Klimov, Victor I. Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots. United States. https://doi.org/10.1021/acsnano.6b04928
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Makarov, Nikolay S., Lin, Qianglu, Pietryga, Jeffrey M., Robel, István, and Klimov, Victor I. Mon . "Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots". United States. https://doi.org/10.1021/acsnano.6b04928.
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@article{osti_1413788,
title = {Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots},
author = {Makarov, Nikolay S. and Lin, Qianglu and Pietryga, Jeffrey M. and Robel, István and Klimov, Victor I.},
abstractNote = {One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. This process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.},
doi = {10.1021/acsnano.6b04928},
journal = {ACS Nano},
number = 12,
volume = 10,
place = {United States},
year = {Mon Dec 12 00:00:00 EST 2016},
month = {Mon Dec 12 00:00:00 EST 2016}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsnano.6b04928
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Works referencing / citing this record:

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