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

Title: Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots

Abstract

Auger recombination is a nonradiative three-particle process wherein the electron–hole recombination energy dissipates as a kinetic energy of a third carrier. Auger decay is enhanced in quantum-dot (QD) forms of semiconductor materials compared to their bulk counterparts. Because this process is detrimental to many prospective applications of the QDs, the development of effective approaches for suppressing Auger recombination has been an important goal in the QD field. One such approach involves “smoothing” of the confinement potential, which suppresses the intraband transition involved in the dissipation of the electron–hole recombination energy. Here, the present study evaluates the effect of increasing “smoothness” of the confinement potential on Auger decay employing a series of CdSe/CdS-based QDs wherein the core and the shell are separated by an intermediate layer of a CdSexS1–x alloy comprised of 1–5 sublayers with a radially tuned composition. As inferred from single-dot measurements, use of the five-step grading scheme allows for strong suppression of Auger decay for both biexcitons and charged excitons. Further, due to nearly identical emissivities of neutral and charged excitons, these QDs exhibit an interesting phenomenon of lifetime blinking for which random fluctuations of a photoluminescence lifetime occur for a nearly constant emission intensity.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States). Center for High Technology Materials (CHTM)
  2. Los Alamos National Lab. (LANL), Los Alamos, 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). Chemical Sciences, Geosciences, and Biosciences Division; USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1469533
Report Number(s):
LA-UR-17-26004
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 9; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; Material Science; semiconductor nanocrystal; quantum dot; suppression of Auger recombination; interfacial alloy layer; lifetime blinking

Citation Formats

Park, Young-Shin, Lim, Jaehoon, Makarov, Nikolay Sergeevich, and Klimov, Victor Ivanovich. Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b02438.
Park, Young-Shin, Lim, Jaehoon, Makarov, Nikolay Sergeevich, & Klimov, Victor Ivanovich. Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots. United States. https://doi.org/10.1021/acs.nanolett.7b02438
Park, Young-Shin, Lim, Jaehoon, Makarov, Nikolay Sergeevich, and Klimov, Victor Ivanovich. 2017. "Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots". United States. https://doi.org/10.1021/acs.nanolett.7b02438. https://www.osti.gov/servlets/purl/1469533.
@article{osti_1469533,
title = {Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots},
author = {Park, Young-Shin and Lim, Jaehoon and Makarov, Nikolay Sergeevich and Klimov, Victor Ivanovich},
abstractNote = {Auger recombination is a nonradiative three-particle process wherein the electron–hole recombination energy dissipates as a kinetic energy of a third carrier. Auger decay is enhanced in quantum-dot (QD) forms of semiconductor materials compared to their bulk counterparts. Because this process is detrimental to many prospective applications of the QDs, the development of effective approaches for suppressing Auger recombination has been an important goal in the QD field. One such approach involves “smoothing” of the confinement potential, which suppresses the intraband transition involved in the dissipation of the electron–hole recombination energy. Here, the present study evaluates the effect of increasing “smoothness” of the confinement potential on Auger decay employing a series of CdSe/CdS-based QDs wherein the core and the shell are separated by an intermediate layer of a CdSexS1–x alloy comprised of 1–5 sublayers with a radially tuned composition. As inferred from single-dot measurements, use of the five-step grading scheme allows for strong suppression of Auger decay for both biexcitons and charged excitons. Further, due to nearly identical emissivities of neutral and charged excitons, these QDs exhibit an interesting phenomenon of lifetime blinking for which random fluctuations of a photoluminescence lifetime occur for a nearly constant emission intensity.},
doi = {10.1021/acs.nanolett.7b02438},
url = {https://www.osti.gov/biblio/1469533}, journal = {Nano Letters},
issn = {1530-6984},
number = 9,
volume = 17,
place = {United States},
year = {2017},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Evidence for Barrierless Auger Recombination in PbSe Nanocrystals: A Pressure-Dependent Study of Transient Optical Absorption
journal, November 2008


Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer
journal, August 1994


Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000


Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces
journal, October 2015


Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals
journal, May 2009


Multiexcitons in type-II colloidal semiconductor quantum dots
journal, January 2007


Single-exciton optical gain in semiconductor nanocrystals
journal, May 2007


Type-II Core/Shell CdS/ZnSe Nanocrystals:  Synthesis, Electronic Structures, and Spectroscopic Properties
journal, September 2007


Towards non-blinking colloidal quantum dots
journal, June 2008


“Giant” Multishell CdSe Nanocrystal Quantum Dots with Suppressed Blinking
journal, April 2008


Reduced Auger Recombination in Single CdSe/CdS Nanorods by One-Dimensional Electron Delocalization
journal, September 2013


Suppression of Biexciton Auger Recombination in CdSe/CdS Dot/Rods: Role of the Electronic Structure in the Carrier Dynamics
journal, August 2010


Multiexciton Engineering in Seeded Core/Shell Nanorods: Transfer from Type-I to Quasi-type-II Regimes
journal, October 2009


Biexciton Auger Recombination in CdSe/CdS Core/Shell Semiconductor Nanocrystals
journal, March 2016


Small Bright Charged Colloidal Quantum Dots
journal, December 2013


Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield
journal, May 2015


Auger Recombination Suppression in Nanocrystals with Asymmetric Electron-Hole Confinement
journal, January 2012


Suppression of Auger Processes in Confined Structures
journal, January 2010


Effect of the Core/Shell Interface on Auger Recombination Evaluated by Single-Quantum-Dot Spectroscopy
journal, January 2014


Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes
journal, October 2013


Controlled Alloying of the Core–Shell Interface in CdSe/CdS Quantum Dots for Suppression of Auger Recombination
journal, April 2013


Suppressed Auger Recombination in “Giant” Nanocrystals Boosts Optical Gain Performance
journal, October 2009


Biexciton Quantum Yield of Single Semiconductor Nanocrystals from Photon Statistics
journal, March 2011


Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared
journal, December 2014


Lifetime blinking in nonblinking nanocrystal quantum dots
journal, January 2012


Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
journal, November 2011


Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals
journal, February 2013


Auger Recombination of Biexcitons and Negative and Positive Trions in Individual Quantum Dots
journal, June 2014


Explanation of quantum dot blinking without the long-lived trap hypothesis
journal, October 2005


Model of Fluorescence Intermittency of Single Colloidal Semiconductor Quantum Dots Using Multiple Recombination Centers
journal, November 2009


High efficiency and ultra-wide color gamut quantum dot LEDs for next generation displays: Quantum dot LEDs for next generation displays
journal, November 2015


Economic and Size-Tunable Synthesis of InP/ZnE (E = S, Se) Colloidal Quantum Dots.
journal, June 2015


Probing Surface Defects of InP Quantum Dots Using Phosphorus Kα and Kβ X-ray Emission Spectroscopy
journal, August 2018


Interfacial Oxidation and Photoluminescence of InP-Based Core/Shell Quantum Dots
journal, September 2018


Synthesis of Semiconductor Nanocrystals, Focusing on Nontoxic and Earth-Abundant Materials
journal, July 2016


Blue Quantum Dot Light-Emitting Diodes with High Electroluminescent Efficiency
journal, October 2017


Bright and Uniform Green Light Emitting InP/ZnSe/ZnS Quantum Dots for Wide Color Gamut Displays
journal, February 2019


Shape Control of CdSe Nanocrystals with Zinc Blende Structure
journal, November 2009


Stoichiometry-Controlled InP-Based Quantum Dots: Synthesis, Photoluminescence, and Electroluminescence
journal, April 2019


Core−Shell Quantum Dots of Lattice-Matched ZnCdSe 2 Shells on InP Cores:  Experiment and Theory
journal, December 2000


Optical, Electronic, and Structural Properties of Uncoupled and Close-Packed Arrays of InP Quantum Dots
journal, December 1998


Electroluminescence from single monolayers of nanocrystals in molecular organic devices
journal, December 2002


Solution-processed, high-performance light-emitting diodes based on quantum dots
journal, October 2014


Stable and efficient quantum-dot light-emitting diodes based on solution-processed multilayer structures
journal, August 2011


High-efficiency light-emitting devices based on quantum dots with tailored nanostructures
journal, March 2015


Highly stable QLEDs with improved hole injection via quantum dot structure tailoring
journal, July 2018


High efficiency and stability of ink-jet printed quantum dot light emitting diodes
journal, April 2020


Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency
journal, February 2019


Long-range resonance transfer of electronic excitations in close-packed CdSe quantum-dot solids
journal, September 1996


High-efficiency red electroluminescent device based on multishelled InP quantum dots
journal, January 2016


Works referencing / citing this record:

Nanostructured colloidal quantum dots for efficient electroluminescence devices
journal, January 2019


Perspective: Toward highly stable electroluminescent quantum dot light-emitting devices in the visible range
journal, January 2020


Insights on heterogeneity in blinking mechanisms and non-ergodicity using sub-ensemble statistical analysis of single quantum-dots
journal, August 2019


Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes
journal, November 2019


Colloidal semiconductor nanocrystals in energy transfer reactions
journal, January 2019


The effects of discrete and gradient mid-shell structures on the photoluminescence of single InP quantum dots
journal, January 2019


Towards the commercialization of colloidal quantum dot solar cells: perspectives on device structures and manufacturing
journal, January 2020