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Title: Cu-Catalyzed Synthesis of CdZnSe–CdZnS Alloy Quantum Dots with Highly Tunable Emission

Abstract

Fabrication of quantum dots (QDs) with emission covering a wide spectral region has been persistently intriguing because of their potentials in a range of practical applications such as biological labeling and imaging, solar cells, light-emitting diodes, and next-generation displays. We report the synthesis of CdZnSe–CdZnS core–shell alloy QDs through a Cu-catalyzed solid solution alloying strategy starting from CdSe–CdS core–shell QDs. The resulting CdZnSe–CdZnS alloy QDs exhibit emission profiles covering a wide wavelength range of 470–650 nm while maintaining high photoluminescence quantum yields. In addition, high morphological uniformity of the starting CdSe–CdS QDs can be largely retained in the final alloy QDs. We attribute this alloying process to the high mobility nature of Cu cations in Cd-chalcogenide crystals at elevated reaction temperatures, which allows Cu cations to act as transporting agents to transfer a Zn component into the CdSe–CdS QDs while maintaining the particle integrity. We show that this unique alloying strategy is independent of the shape of the starting QDs and can also be applied to the synthesis of CdZnSe–CdZnS nanorods. We anticipate that our study will instigate the synthesis of various high-quality alloy QDs and other alloy nanocrystals beyond what can be achieved currently.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States). Dept. of Chemistry
  2. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Brown Univ., Providence, RI (United States); Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Inst. of Health (NIH) (United States)
OSTI Identifier:
1504402
Report Number(s):
BNL-211474-2019-JAAM
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
SC0012704; OIA-1538893; CHE-1554800; U54GM115677
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 7; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Yuan, Yucheng, Zhu, Hua, Wang, Xudong, Cui, Dingzhou, Gao, Zehua, Su, Dong, Zhao, Jing, and Chen, Ou. Cu-Catalyzed Synthesis of CdZnSe–CdZnS Alloy Quantum Dots with Highly Tunable Emission. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b00557.
Yuan, Yucheng, Zhu, Hua, Wang, Xudong, Cui, Dingzhou, Gao, Zehua, Su, Dong, Zhao, Jing, & Chen, Ou. Cu-Catalyzed Synthesis of CdZnSe–CdZnS Alloy Quantum Dots with Highly Tunable Emission. United States. https://doi.org/10.1021/acs.chemmater.9b00557
Yuan, Yucheng, Zhu, Hua, Wang, Xudong, Cui, Dingzhou, Gao, Zehua, Su, Dong, Zhao, Jing, and Chen, Ou. Thu . "Cu-Catalyzed Synthesis of CdZnSe–CdZnS Alloy Quantum Dots with Highly Tunable Emission". United States. https://doi.org/10.1021/acs.chemmater.9b00557. https://www.osti.gov/servlets/purl/1504402.
@article{osti_1504402,
title = {Cu-Catalyzed Synthesis of CdZnSe–CdZnS Alloy Quantum Dots with Highly Tunable Emission},
author = {Yuan, Yucheng and Zhu, Hua and Wang, Xudong and Cui, Dingzhou and Gao, Zehua and Su, Dong and Zhao, Jing and Chen, Ou},
abstractNote = {Fabrication of quantum dots (QDs) with emission covering a wide spectral region has been persistently intriguing because of their potentials in a range of practical applications such as biological labeling and imaging, solar cells, light-emitting diodes, and next-generation displays. We report the synthesis of CdZnSe–CdZnS core–shell alloy QDs through a Cu-catalyzed solid solution alloying strategy starting from CdSe–CdS core–shell QDs. The resulting CdZnSe–CdZnS alloy QDs exhibit emission profiles covering a wide wavelength range of 470–650 nm while maintaining high photoluminescence quantum yields. In addition, high morphological uniformity of the starting CdSe–CdS QDs can be largely retained in the final alloy QDs. We attribute this alloying process to the high mobility nature of Cu cations in Cd-chalcogenide crystals at elevated reaction temperatures, which allows Cu cations to act as transporting agents to transfer a Zn component into the CdSe–CdS QDs while maintaining the particle integrity. We show that this unique alloying strategy is independent of the shape of the starting QDs and can also be applied to the synthesis of CdZnSe–CdZnS nanorods. We anticipate that our study will instigate the synthesis of various high-quality alloy QDs and other alloy nanocrystals beyond what can be achieved currently.},
doi = {10.1021/acs.chemmater.9b00557},
journal = {Chemistry of Materials},
number = 7,
volume = 31,
place = {United States},
year = {Thu Mar 21 00:00:00 EDT 2019},
month = {Thu Mar 21 00:00:00 EDT 2019}
}

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