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Title: Towards zero-threshold optical gain using charged semiconductor quantum dots

Colloidal semiconductor quantum dots are attractive materials for the realization of solution-processable lasers. However, their applications as optical-gain media are complicated by a non-unity degeneracy of band-edge states, because of which multiexcitons are required to achieve the lasing regime. This increases the lasing thresholds and leads to very short optical gain lifetimes limited by nonradiative Auger recombination. Here, we show that these problems can be at least partially resolved by employing not neutral but negatively charged quantum dots. By applying photodoping to specially engineered quantum dots with impeded Auger decay, we demonstrate a considerable reduction of the optical gain threshold due to suppression of ground-state absorption by pre-existing carriers. Moreover, by injecting approximately one electron per dot on average, we achieve a more than twofold reduction in the amplified spontaneous emission threshold, bringing it to the sub-single-exciton level. Furthermore, these measurements indicate the feasibility of ‘zero-threshold’ gain achievable by completely blocking the band-edge state with two electrons.
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [3] ; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences, Dalian (China)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Report Number(s):
LA-UR-17-26002
Journal ID: ISSN 1748-3387; TRN: US1800810
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Nature Nanotechnology
Additional Journal Information:
Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 1748-3387
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science; Zero-threshold optical gain, colloidal quantum dot, lasing
OSTI Identifier:
1415416

Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor Ivanovich. Towards zero-threshold optical gain using charged semiconductor quantum dots. United States: N. p., Web. doi:10.1038/nnano.2017.189.
Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, & Klimov, Victor Ivanovich. Towards zero-threshold optical gain using charged semiconductor quantum dots. United States. doi:10.1038/nnano.2017.189.
Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor Ivanovich. 2017. "Towards zero-threshold optical gain using charged semiconductor quantum dots". United States. doi:10.1038/nnano.2017.189. https://www.osti.gov/servlets/purl/1415416.
@article{osti_1415416,
title = {Towards zero-threshold optical gain using charged semiconductor quantum dots},
author = {Wu, Kaifeng and Park, Young -Shin and Lim, Jaehoon and Klimov, Victor Ivanovich},
abstractNote = {Colloidal semiconductor quantum dots are attractive materials for the realization of solution-processable lasers. However, their applications as optical-gain media are complicated by a non-unity degeneracy of band-edge states, because of which multiexcitons are required to achieve the lasing regime. This increases the lasing thresholds and leads to very short optical gain lifetimes limited by nonradiative Auger recombination. Here, we show that these problems can be at least partially resolved by employing not neutral but negatively charged quantum dots. By applying photodoping to specially engineered quantum dots with impeded Auger decay, we demonstrate a considerable reduction of the optical gain threshold due to suppression of ground-state absorption by pre-existing carriers. Moreover, by injecting approximately one electron per dot on average, we achieve a more than twofold reduction in the amplified spontaneous emission threshold, bringing it to the sub-single-exciton level. Furthermore, these measurements indicate the feasibility of ‘zero-threshold’ gain achievable by completely blocking the band-edge state with two electrons.},
doi = {10.1038/nnano.2017.189},
journal = {Nature Nanotechnology},
number = 12,
volume = 12,
place = {United States},
year = {2017},
month = {10}
}

Works referenced in this record:

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Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals
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Exciton-Exciton Interaction and Optical Gain in Colloidal CdSe/CdS Dot/Rod Nanocrystals
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