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Title: Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared

Abstract

The unique optical properties exhibited by visible emitting core/shell quantum dots with especially thick shells are the focus of widespread study, but have yet to be realized in infrared (IR) -active nanostructures. We apply an effective-mass model to identify PbSe/CdSe core/shell quantum dots as a promising system for achieving this goal. We then synthesize colloidal PbSe/CdSe quantum dots with shell thicknesses of up to 4 nm that exhibit unusually slow hole intra-band relaxation from shell to core states, as evidenced by the emergence of dual emission, i.e., IR photoluminescence from the PbSe core observed simultaneously with visible emission from the CdSe shell. In addition to the large shell thickness, the development of slowed intraband relaxation is facilitated by the existence of a sharp core-shell interface without discernible alloying. Growth of thick shells without interfacial alloying or incidental formation of homogenous CdSe nanocrystals was accomplished using insights attained via a systematic study of the dynamics of the cation-exchange synthesis of both PbSe/CdSe as well as the related system PbS/CdS. Finally, we show that the efficiency of the visible photoluminescence can be greatly enhanced by inorganic passivation.

Authors:
 [1];  [2];  [2];  [2];  [2];  [3];  [2];  [2]
  1. Center for Advanced Solar Photophysics, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States, Department of Chemical and Materials Engineering, New Mexico State University, Las Cruces, New Mexico 88003, United States
  2. Center for Advanced Solar Photophysics, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
  3. Department of Chemical and Materials Engineering, New Mexico State University, Las Cruces, New Mexico 88003, United States
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1413786
Alternate Identifier(s):
OSTI ID: 1321751
Report Number(s):
LA-UR-14-28541
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Name: ACS Nano Journal Volume: 9 Journal Issue: 1; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
quantum dots; core/shell nanocrystal; dual emission; cation exchange; vacancy formation; effective mass model

Citation Formats

Lin, Qianglu, Makarov, Nikolay S., Koh, Weon-kyu, Velizhanin, Kirill A., Cirloganu, Claudiu M., Luo, Hongmei, Klimov, Victor I., and Pietryga, Jeffrey M. Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared. United States: N. p., 2014. Web. doi:10.1021/nn505793y.
Lin, Qianglu, Makarov, Nikolay S., Koh, Weon-kyu, Velizhanin, Kirill A., Cirloganu, Claudiu M., Luo, Hongmei, Klimov, Victor I., & Pietryga, Jeffrey M. Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared. United States. https://doi.org/10.1021/nn505793y
Lin, Qianglu, Makarov, Nikolay S., Koh, Weon-kyu, Velizhanin, Kirill A., Cirloganu, Claudiu M., Luo, Hongmei, Klimov, Victor I., and Pietryga, Jeffrey M. Thu . "Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared". United States. https://doi.org/10.1021/nn505793y.
@article{osti_1413786,
title = {Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared},
author = {Lin, Qianglu and Makarov, Nikolay S. and Koh, Weon-kyu and Velizhanin, Kirill A. and Cirloganu, Claudiu M. and Luo, Hongmei and Klimov, Victor I. and Pietryga, Jeffrey M.},
abstractNote = {The unique optical properties exhibited by visible emitting core/shell quantum dots with especially thick shells are the focus of widespread study, but have yet to be realized in infrared (IR) -active nanostructures. We apply an effective-mass model to identify PbSe/CdSe core/shell quantum dots as a promising system for achieving this goal. We then synthesize colloidal PbSe/CdSe quantum dots with shell thicknesses of up to 4 nm that exhibit unusually slow hole intra-band relaxation from shell to core states, as evidenced by the emergence of dual emission, i.e., IR photoluminescence from the PbSe core observed simultaneously with visible emission from the CdSe shell. In addition to the large shell thickness, the development of slowed intraband relaxation is facilitated by the existence of a sharp core-shell interface without discernible alloying. Growth of thick shells without interfacial alloying or incidental formation of homogenous CdSe nanocrystals was accomplished using insights attained via a systematic study of the dynamics of the cation-exchange synthesis of both PbSe/CdSe as well as the related system PbS/CdS. Finally, we show that the efficiency of the visible photoluminescence can be greatly enhanced by inorganic passivation.},
doi = {10.1021/nn505793y},
url = {https://www.osti.gov/biblio/1413786}, journal = {ACS Nano},
issn = {1936-0851},
number = 1,
volume = 9,
place = {United States},
year = {2014},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1021/nn505793y

Citation Metrics:
Cited by: 26 works
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