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:
-
- 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
- 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
- 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}
}
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1021/nn505793y
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 26 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referencing / citing this record:
Biomineralization of PbS and PbS–CdS core–shell nanocrystals and their application in quantum dot sensitized solar cells
journal, January 2016
- Spangler, Leah C.; Lu, Li; Kiely, Christopher J.
- Journal of Materials Chemistry A, Vol. 4, Issue 16
Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking‐Suppressed Two‐Color Emission
journal, June 2019
- Dennis, Allison M.; Buck, Matthew R.; Wang, Feng
- Advanced Functional Materials, Vol. 29, Issue 37
Band Gap Engineering Improves the Efficiency of Double Quantum Dot Upconversion Nanocrystals
journal, April 2019
- Yang, Gaoling; Meir, Noga; Raanan, Dekel
- Advanced Functional Materials, Vol. 29, Issue 23
Ultrasensitive, Biocompatible, Self-Calibrating, Multiparametric Temperature Sensors
journal, October 2015
- Zhao, Haiguang; Vomiero, Alberto; Rosei, Federico
- Small, Vol. 11, Issue 43
Light‐Emitting Diodes with Cu‐Doped Colloidal Quantum Wells: From Ultrapure Green, Tunable Dual‐Emission to White Light
journal, August 2019
- Liu, Baiquan; Sharma, Manoj; Yu, Junhong
- Small, Vol. 15, Issue 38
Highly efficient large-area colourless luminescent solar concentrators using heavy-metal-free colloidal quantum dots
journal, August 2015
- Meinardi, Francesco; McDaniel, Hunter; Carulli, Francesco
- Nature Nanotechnology, Vol. 10, Issue 10
Photoinduced electron transfer in novel CdSe–Cu 2 Se type II core–shell quantum dots
journal, January 2019
- Simi, N. J.; Vinayakan, R.; Ison, V. V.
- RSC Advances, Vol. 9, Issue 26
Sub–single-exciton lasing using charged quantum dots coupled to a distributed feedback cavity
journal, August 2019
- Kozlov, Oleg V.; Park, Young-Shin; Roh, Jeongkyun
- Science, Vol. 365, Issue 6454