The 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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- New Mexico State Univ., Las Cruces, NM (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) (SC-22)
- 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 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.. The 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.. The design and synthesis of heterostructured quantum dots with dual emission in the visible and infrared. United States. doi: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.. Wed .
"The design and synthesis of heterostructured quantum dots with dual emission in the visible and infrared". United States. doi:10.1021/nn505793y.
@article{osti_1413786,
title = {The 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},
journal = {ACS Nano},
issn = {1936-0851},
number = 1,
volume = 9,
place = {United States},
year = {2014},
month = {11}
}
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