skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Chemistry of Materials

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.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States); Brown Univ., Providence, RI (United States); Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Inst. of Health (NIH) (United States)
Grant/Contract Number:
SC0012704; OIA-1538893; CHE-1554800; U54GM115677
OSTI ID:
1504402
Report Number(s):
BNL-211474-2019-JAAM
Journal Information:
Chemistry of Materials, Vol. 31, Issue 7; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 35 works
Citation information provided by
Web of Science

References (82)

Pure colors from core–shell quantum dots journal September 2013
Prospects of Nanoscience with Nanocrystals journal January 2015
Quantum Dot Solar Cells. Semiconductor Nanocrystals as Light Harvesters journal October 2008
Efficient CdSe Quantum Dot-Sensitized Solar Cells Prepared by an Improved Successive Ionic Layer Adsorption and Reaction Process journal December 2009
Highly Efficient Quantum-Dot-Sensitized Solar Cell Based on Co-Sensitization of CdS/CdSe journal February 2009
Improved performance and stability in quantum dot solar cells through band alignment engineering journal May 2014
Colloidal Quantum Dot Solar Cells journal June 2015
Time-gated biological imaging by use of colloidal quantum dots journal January 2001
Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules journal July 2001
Quantum dot bioconjugates for imaging, labelling and sensing journal June 2005
Continuous injection synthesis of indium arsenide quantum dots emissive in the short-wavelength infrared journal November 2016
In Vivo Whole Animal Fluorescence Imaging of a Microparticle-Based Oral Vaccine Containing (CuInSe x S 2– x )/ZnS Core/Shell Quantum Dots journal August 2013
Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer journal August 1994
Compact Biocompatible Quantum Dots Functionalized for Cellular Imaging journal January 2008
Prospects for LED lighting journal April 2009
White-Light-Emitting Diodes with Quantum Dot Color Converters for Display Backlights journal May 2010
Emergence of colloidal quantum-dot light-emitting technologies journal December 2012
Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes journal October 2013
High-efficiency quantum-dot light-emitting devices with enhanced charge injection journal April 2013
High-efficiency light-emitting devices based on quantum dots with tailored nanostructures journal March 2015
Bright colloidal quantum dot light-emitting diodes enabled by efficient chlorination journal February 2018
Probing cellular events, one quantum dot at a time journal March 2010
Single-component quasicrystalline nanocrystal superlattices through flexible polygon tiling rule journal December 2018
Superstructures generated from truncated tetrahedral quantum dots journal September 2018
Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites journal September 1993
Semiconductor Clusters, Nanocrystals, and Quantum Dots journal February 1996
Shape control of CdSe nanocrystals journal March 2000
Shape matters journal March 2003
Highly Emissive Colloidal CdSe/CdS Heterostructures of Mixed Dimensionality journal December 2003
Seeded Growth of Highly Luminescent CdSe/CdS Nanoheterostructures with Rod and Tetrapod Morphologies journal October 2007
Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach journal October 2007
Controlled Synthesis and Optical Properties of Colloidal Ternary Chalcogenide CuInS 2 Nanocrystals journal October 2008
“Giant” Multishell CdSe Nanocrystal Quantum Dots with Suppressed Blinking journal April 2008
Core/Shell Semiconductor Nanocrystals journal January 2009
Colloidal CdSe/CdS Dot-in-Plate Nanocrystals with 2D-Polarized Emission journal July 2012
Blue-UV-Emitting ZnSe(Dot)/ZnS(Rod) Core/Shell Nanocrystals Prepared from CdSe/CdS Nanocrystals by Sequential Cation Exchange journal January 2012
Chemical, Structural, and Quantitative Analysis of the Ligand Shells of Colloidal Quantum Dots journal September 2012
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking journal February 2013
Zinc Chalcogenide Seed-Mediated Synthesis of CdSe Nanocrystals: Nails, Chesses and Tetrahedrons journal April 2015
Atomic Structure of Wurtzite CdSe (Core)/CdS (Giant Shell) Nanobullets Related to Epitaxy and Growth journal October 2016
A Two-Step Synthetic Strategy toward Monodisperse Colloidal CdSe and CdSe/CdS Core/Shell Nanocrystals journal May 2016
Optoelectronic Properties of CuInS 2 Nanocrystals and Their Origin journal January 2016
Monodisperse Hexagonal Pyramidal and Bipyramidal Wurtzite CdSe-CdS Core–Shell Nanocrystals journal April 2017
Tight Binding of Carboxylate, Phosphonate, and Carbamate Anions to Stoichiometric CdSe Nanocrystals journal February 2017
Templated Growth of InP Nanocrystals with a Polytwistane Structure journal January 2018
Suppressed Blinking and Auger Recombination in Near-Infrared Type-II InP/CdS Nanocrystal Quantum Dots journal October 2012
Reducing Competition by Coordinating Solvent Promotes Morphological Control in Alternating Layer Growth of CdSe/CdS Core/Shell Quantum Dots journal October 2015
Bright Core–Shell Semiconductor Quantum Wires journal November 2012
Epitaxial Growth of Highly Luminescent CdSe/CdS Core/Shell Nanocrystals with Photostability and Electronic Accessibility
  • Peng, Xiaogang; Schlamp, Michael C.; Kadavanich, Andreas V.
  • Journal of the American Chemical Society, Vol. 119, Issue 30, p. 7019-7029 https://doi.org/10.1021/ja970754m
journal July 1997
(CdSe)ZnS Core−Shell Quantum Dots: Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites journal November 1997
Blue Luminescence from (CdS)ZnS Core–Shell Nanocrystals journal April 2004
Large-Scale Synthesis of Nearly Monodisperse CdSe/CdS Core/Shell Nanocrystals Using Air-Stable Reagents via Successive Ion Layer Adsorption and Reaction journal October 2003
Synthesis and Characterization of Strongly Luminescing ZnS-Capped CdSe Nanocrystals journal January 1996
Design and Synthesis of Antiblinking and Antibleaching Quantum Dots in Multiple Colors via Wave Function Confinement journal November 2016
Purple-, Blue-, and Green-Emitting Multishell Alloyed Quantum Dots: Synthesis, Characterization, and Application for Ratiometric Extracellular pH Sensing journal August 2017
Composition-Tunable ZnxCd1-xSe Nanocrystals with High Luminescence and Stability journal July 2003
Alloyed Zn x Cd 1 - x S Nanocrystals with Highly Narrow Luminescence Spectral Width journal November 2003
Engineering InAs x P 1- x /InP/ZnSe III−V Alloyed Core/Shell Quantum Dots for the Near-Infrared journal August 2005
Color-Saturated Green-Emitting QD-LEDs journal September 2006
Homogeneously Alloyed CdS x Se 1 - x Nanocrystals:  Synthesis, Characterization, and Composition/Size-Dependent Band Gap journal September 2006
Highly Luminescent Cd1−xZnxSe/ZnS Core/Shell Nanocrystals Emitting in the Blue–Green Spectral Range journal March 2007
A facile route to violet- to orange-emitting Cd x Zn 1− x Se alloy nanocrystals via cation exchange reaction journal August 2007
Gram-Scale One-Pot Synthesis of Highly Luminescent Blue Emitting Cd 1− x Zn x S/ZnS Nanocrystals journal August 2008
Tailoring ZnSe–CdSe Colloidal Quantum Dots via Cation Exchange: From Core/Shell to Alloy Nanocrystals journal August 2013
Highly Efficient, Color-Pure, Color-Stable Blue Quantum Dot Light-Emitting Devices journal July 2013
High-Efficient Deep-Blue Light-Emitting Diodes by Using High Quality Zn x Cd 1- x S/ZnS Core/Shell Quantum Dots journal December 2013
Quantum Dot Light-Emitting Devices with Electroluminescence Tunable over the Entire Visible Spectrum journal July 2009
Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths journal June 2013
Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths journal December 2015
Permanent dipole moment and charges in colloidal semiconductor quantum dots journal October 1999
Mechanisms of the Shape Evolution of CdSe Nanocrystals journal February 2001
Nanoheterostructure Cation Exchange: Anionic Framework Conservation journal July 2010
Luminescent Colloidal Semiconductor Nanocrystals Containing Copper: Synthesis, Photophysics, and Applications journal May 2016
Doping Cu in Semiconductor Nanocrystals: Some Old and Some New Physical Insights journal February 2011
Photoluminescence Blinking and Reversible Electron Trapping in Copper-Doped CdSe Nanocrystals journal May 2015
Cluster-Seeded Synthesis of Doped CdSe:Cu 4 Quantum Dots journal March 2013
One-Pot Synthesis of Monodisperse Colloidal Copper-Doped CdSe Nanocrystals Mediated by Ligand–Copper Interactions journal October 2016
Doping semiconductor nanocrystals journal July 2005
Absolute electronegativity and hardness: application to inorganic chemistry journal February 1988
Chemical hardness and bond dissociation energies journal November 1988
Highly Luminescent Nanocrystals From Removal of Impurity Atoms Residual From Ion-Exchange Synthesis journal January 2012
Absolute hardness: companion parameter to absolute electronegativity journal December 1983

Cited By (3)

Doping of Cu( i ) ions into CdS/ZnS core/shell nanocrystals through a cation exchange strategy journal January 2019
Rational Design and Synthesis of Highly Luminescent Multinary Cu‐In‐Zn‐S Semiconductor Nanocrystals with Tailored Nanostructures journal March 2020
Strategies for extending charge separation in colloidal nanostructured quantum dot materials journal January 2019

Similar Records

A facile route to synthesize CdZnSe core–shell-like alloyed quantum dots via cation exchange reaction in aqueous system
Journal Article · Mon Sep 15 00:00:00 EDT 2014 · Materials Research Bulletin · OSTI ID:1504402

Engineering of Lead Selenide Quantum Dot Based Devices and Core/Shell Heterostructures
Thesis/Dissertation · Fri May 01 00:00:00 EDT 2020 · OSTI ID:1504402

Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices
Journal Article · Wed Dec 30 00:00:00 EST 2020 · ACS Nano · OSTI ID:1504402

Related Subjects