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:
-
[1];
[1];
[2]
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States). Center for High Technology Materials (CHTM)
- 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:
- 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. Thu .
"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},
journal = {Nano Letters},
number = 9,
volume = 17,
place = {United States},
year = {Thu Jul 27 00:00:00 EDT 2017},
month = {Thu Jul 27 00:00:00 EDT 2017}
}
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Works referenced in this record:
Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots
journal, February 2000
- Klimov, V. I.
- Science, Vol. 287, Issue 5455
Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer
journal, August 1994
- Colvin, V. L.; Schlamp, M. C.; Alivisatos, A. P.
- Nature, Vol. 370, Issue 6488
Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000
- Klimov, V. I.; Mikhailovsky, A. A.; Xu, Su
- Science, Vol. 290, Issue 5490, p. 314-317
Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces
journal, October 2015
- Park, Young-Shin; Bae, Wan Ki; Baker, Thomas
- Nano Letters, Vol. 15, Issue 11
Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals
journal, May 2009
- Robel, István; Gresback, Ryan; Kortshagen, Uwe
- Physical Review Letters, Vol. 102, Issue 17, Article No. 177404
Multicarrier Interactions in Semiconductor Nanocrystals in Relation to the Phenomena of Auger Recombination and Carrier Multiplication
journal, March 2014
- Klimov, Victor I.
- Annual Review of Condensed Matter Physics, Vol. 5, Issue 1
Single-exciton optical gain in semiconductor nanocrystals
journal, May 2007
- Klimov, Victor I.; Ivanov, Sergei A.; Nanda, Jagjit
- Nature, Vol. 447, Issue 7143
Type-II Core/Shell CdS/ZnSe Nanocrystals: Synthesis, Electronic Structures, and Spectroscopic Properties
journal, September 2007
- Ivanov, Sergei A.; Piryatinski, Andrei; Nanda, Jagjit
- Journal of the American Chemical Society, Vol. 129, Issue 38
Towards non-blinking colloidal quantum dots
journal, June 2008
- Mahler, Benoit; Spinicelli, Piernicola; Buil, Stéphanie
- Nature Materials, Vol. 7, Issue 8
“Giant” Multishell CdSe Nanocrystal Quantum Dots with Suppressed Blinking
journal, April 2008
- Chen, Yongfen; Vela, Javier; Htoon, Han
- Journal of the American Chemical Society, Vol. 130, Issue 15
Reduced Auger Recombination in Single CdSe/CdS Nanorods by One-Dimensional Electron Delocalization
journal, September 2013
- Rabouw, Freddy T.; Lunnemann, Per; van Dijk-Moes, Relinde J. A.
- Nano Letters, Vol. 13, Issue 10
Suppression of Biexciton Auger Recombination in CdSe/CdS Dot/Rods: Role of the Electronic Structure in the Carrier Dynamics
journal, August 2010
- Zavelani-Rossi, Margherita; Lupo, Maria Grazia; Tassone, Francesco
- Nano Letters, Vol. 10, Issue 8
Multiexciton Engineering in Seeded Core/Shell Nanorods: Transfer from Type-I to Quasi-type-II Regimes
journal, October 2009
- Sitt, Amit; Sala, Fabio Della; Menagen, Gabi
- Nano Letters, Vol. 9, Issue 10
Biexciton Auger Recombination in CdSe/CdS Core/Shell Semiconductor Nanocrystals
journal, March 2016
- Vaxenburg, Roman; Rodina, Anna; Lifshitz, Efrat
- Nano Letters, Vol. 16, Issue 4
Small Bright Charged Colloidal Quantum Dots
journal, December 2013
- Qin, Wei; Liu, Heng; Guyot-Sionnest, Philippe
- ACS Nano, Vol. 8, Issue 1
Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield
journal, May 2015
- Nasilowski, Michel; Spinicelli, Piernicola; Patriarche, Gilles
- Nano Letters, Vol. 15, Issue 6
Auger Recombination Suppression in Nanocrystals with Asymmetric Electron-Hole Confinement
journal, January 2012
- Climente, Juan I.; Movilla, Jose L.; Planelles, Josep
- Small, Vol. 8, Issue 5
Suppression of Auger Processes in Confined Structures
journal, January 2010
- Cragg, George E.; Efros, Alexander L.
- Nano Letters, Vol. 10, Issue 1
Effect of the Core/Shell Interface on Auger Recombination Evaluated by Single-Quantum-Dot Spectroscopy
journal, January 2014
- Park, Young-Shin; Bae, Wan Ki; Padilha, Lazaro A.
- Nano Letters, Vol. 14, Issue 2
Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes
journal, October 2013
- Bae, Wan Ki; Park, Young-Shin; Lim, Jaehoon
- Nature Communications, Vol. 4, Issue 1
Controlled Alloying of the Core–Shell Interface in CdSe/CdS Quantum Dots for Suppression of Auger Recombination
journal, April 2013
- Bae, Wan Ki; Padilha, Lazaro A.; Park, Young-Shin
- ACS Nano, Vol. 7, Issue 4
Suppressed Auger Recombination in “Giant” Nanocrystals Boosts Optical Gain Performance
journal, October 2009
- García-Santamaría, Florencio; Chen, Yongfen; Vela, Javier
- Nano Letters, Vol. 9, Issue 10
Biexciton Quantum Yield of Single Semiconductor Nanocrystals from Photon Statistics
journal, March 2011
- Nair, Gautham; Zhao, Jing; Bawendi, Moungi G.
- Nano Letters, Vol. 11, Issue 3
Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared
journal, December 2014
- Lin, Qianglu; Makarov, Nikolay S.; Koh, Weon-kyu
- ACS Nano, Vol. 9, Issue 1
Lifetime blinking in nonblinking nanocrystal quantum dots
journal, January 2012
- Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea
- Nature Communications, Vol. 3, Issue 1
Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
journal, November 2011
- Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea
- Nature, Vol. 479, Issue 7372
Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals
journal, February 2013
- Javaux, C.; Mahler, B.; Dubertret, B.
- Nature Nanotechnology, Vol. 8, Issue 3
Auger Recombination of Biexcitons and Negative and Positive Trions in Individual Quantum Dots
journal, June 2014
- Park, Young-Shin; Bae, Wan Ki; Pietryga, Jeffrey M.
- ACS Nano, Vol. 8, Issue 7
Superposition Principle in Auger Recombination of Charged and Neutral Multicarrier States in Semiconductor Quantum Dots
journal, August 2017
- Wu, Kaifeng; Lim, Jaehoon; Klimov, Victor I.
- ACS Nano, Vol. 11, Issue 8
Explanation of quantum dot blinking without the long-lived trap hypothesis
journal, October 2005
- Frantsuzov, Pavel A.; Marcus, R. A.
- Physical Review B, Vol. 72, Issue 15
Model of Fluorescence Intermittency of Single Colloidal Semiconductor Quantum Dots Using Multiple Recombination Centers
journal, November 2009
- Frantsuzov, Pavel A.; Volkán-Kacsó, Sándor; Jankó, Bolizsár
- Physical Review Letters, Vol. 103, Issue 20
Influence of Shell Thickness on the Performance of Light-Emitting Devices Based on CdSe/Zn 1-X Cd X S Core/Shell Heterostructured Quantum Dots
journal, November 2014
- Lim, Jaehoon; Jeong, Byeong Guk; Park, Myeongjin
- Advanced Materials, Vol. 26, Issue 47
High efficiency and ultra-wide color gamut quantum dot LEDs for next generation displays: Quantum dot LEDs for next generation displays
journal, November 2015
- Manders, Jesse R.; Qian, Lei; Titov, Alexandre
- Journal of the Society for Information Display, Vol. 23, Issue 11
Cadmium-Free InP/ZnSeS/ZnS Heterostructure-Based Quantum Dot Light-Emitting Diodes with a ZnMgO Electron Transport Layer and a Brightness of Over 10 000 cd m −2
journal, January 2017
- Wang, Hung Chia; Zhang, Heng; Chen, Hao Yue
- Small, Vol. 13, Issue 13
Economic and Size-Tunable Synthesis of InP/ZnE (E = S, Se) Colloidal Quantum Dots.
journal, June 2015
- Tessier, Mickael D.; Dupont, Dorian; De Nolf, Kim
- Chemistry of Materials, Vol. 27, Issue 13
Probing Surface Defects of InP Quantum Dots Using Phosphorus Kα and Kβ X-ray Emission Spectroscopy
journal, August 2018
- Stein, Jennifer L.; Holden, William M.; Venkatesh, Amrit
- Chemistry of Materials, Vol. 30, Issue 18
Interfacial Oxidation and Photoluminescence of InP-Based Core/Shell Quantum Dots
journal, September 2018
- Tessier, Mickael D.; Baquero, Edwin A.; Dupont, Dorian
- Chemistry of Materials, Vol. 30, Issue 19
A Layer-by-Layer Growth Strategy for Large-Size InP/ZnSe/ZnS Core–Shell Quantum Dots Enabling High-Efficiency Light-Emitting Diodes
journal, October 2018
- Cao, Fan; Wang, Sheng; Wang, Feijiu
- Chemistry of Materials, Vol. 30, Issue 21
Synthesis of Semiconductor Nanocrystals, Focusing on Nontoxic and Earth-Abundant Materials
journal, July 2016
- Reiss, Peter; Carrière, Marie; Lincheneau, Christophe
- Chemical Reviews, Vol. 116, Issue 18
Blue Quantum Dot Light-Emitting Diodes with High Electroluminescent Efficiency
journal, October 2017
- Wang, Lishuang; Lin, Jie; Hu, Yongsheng
- ACS Applied Materials & Interfaces, Vol. 9, Issue 44
Bright and Uniform Green Light Emitting InP/ZnSe/ZnS Quantum Dots for Wide Color Gamut Displays
journal, February 2019
- Kim, Yongwook; Ham, Sujin; Jang, Hyosook
- ACS Applied Nano Materials, Vol. 2, Issue 3
Shape Control of CdSe Nanocrystals with Zinc Blende Structure
journal, November 2009
- Liu, Liping; Zhuang, Zhongbin; Xie, Ting
- Journal of the American Chemical Society, Vol. 131, Issue 45
Stoichiometry-Controlled InP-Based Quantum Dots: Synthesis, Photoluminescence, and Electroluminescence
journal, April 2019
- Li, Yang; Hou, Xiaoqi; Dai, Xingliang
- Journal of the American Chemical Society, Vol. 141, Issue 16
Core−Shell Quantum Dots of Lattice-Matched ZnCdSe 2 Shells on InP Cores: Experiment and Theory
journal, December 2000
- Mićić, Olga I.; Smith, Barton B.; Nozik, Arthur J.
- The Journal of Physical Chemistry B, Vol. 104, Issue 51
Optical, Electronic, and Structural Properties of Uncoupled and Close-Packed Arrays of InP Quantum Dots
journal, December 1998
- Mićić, Olga I.; Jones, Kim M.; Cahill, Andrew
- The Journal of Physical Chemistry B, Vol. 102, Issue 49
Highly Efficient Cadmium-Free Quantum Dot Light-Emitting Diodes Enabled by the Direct Formation of Excitons within InP@ZnSeS Quantum Dots
journal, September 2013
- Lim, Jaehoon; Park, Myeongjin; Bae, Wan Ki
- ACS Nano, Vol. 7, Issue 10
Electroluminescence from single monolayers of nanocrystals in molecular organic devices
journal, December 2002
- Coe, Seth; Woo, Wing-Keung; Bawendi, Moungi
- Nature, Vol. 420, Issue 6917
Solution-processed, high-performance light-emitting diodes based on quantum dots
journal, October 2014
- Dai, Xingliang; Zhang, Zhenxing; Jin, Yizheng
- Nature, Vol. 515, Issue 7525
Stable and efficient quantum-dot light-emitting diodes based on solution-processed multilayer structures
journal, August 2011
- Qian, Lei; Zheng, Ying; Xue, Jiangeng
- Nature Photonics, Vol. 5, Issue 9
High-efficiency light-emitting devices based on quantum dots with tailored nanostructures
journal, March 2015
- Yang, Yixing; Zheng, Ying; Cao, Weiran
- Nature Photonics, Vol. 9, Issue 4
Highly stable QLEDs with improved hole injection via quantum dot structure tailoring
journal, July 2018
- Cao, Weiran; Xiang, Chaoyu; Yang, Yixing
- Nature Communications, Vol. 9, Issue 1
High efficiency and stability of ink-jet printed quantum dot light emitting diodes
journal, April 2020
- Xiang, Chaoyu; Wu, Longjia; Lu, Zizhe
- Nature Communications, Vol. 11, Issue 1
Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency
journal, February 2019
- Shen, Huaibin; Gao, Qiang; Zhang, Yanbin
- Nature Photonics, Vol. 13, Issue 3
High-efficiency red electroluminescent device based on multishelled InP quantum dots
journal, January 2016
- Jo, Jung-Ho; Kim, Jong-Hoon; Lee, Ki-Heon
- Optics Letters, Vol. 41, Issue 17
Works referencing / citing this record:
Nanostructured colloidal quantum dots for efficient electroluminescence devices
journal, January 2019
- Bae, Wan Ki; Lim, Jaehoon
- Korean Journal of Chemical Engineering, Vol. 36, Issue 2
Perspective: Toward highly stable electroluminescent quantum dot light-emitting devices in the visible range
journal, January 2020
- Davidson-Hall, Tyler; Aziz, Hany
- Applied Physics Letters, Vol. 116, Issue 1
Insights on heterogeneity in blinking mechanisms and non-ergodicity using sub-ensemble statistical analysis of single quantum-dots
journal, August 2019
- Mukherjee, Amitrajit; Ray, Korak Kumar; Phadnis, Chinmay
- The Journal of Chemical Physics, Vol. 151, Issue 8
Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes
journal, November 2019
- Won, Yu-Ho; Cho, Oul; Kim, Taehyung
- Nature, Vol. 575, Issue 7784
Effects of interface-potential smoothness and wavefunction delocalization on Auger recombination in colloidal CdSe-based core/shell quantum dots
journal, December 2019
- Hou, Xiaoqi; Li, Yang; Qin, Haiyan
- The Journal of Chemical Physics, Vol. 151, Issue 23
Reducing the Chromaticity Shifts of Light‐Emitting Diodes Using Gradient‐Alloyed Cd x Zn 1− x Se y S 1− y @ZnS Core Shell Quantum Dots with Enhanced High‐Temperature Photoluminescence
journal, February 2019
- Tang, Jialun; Li, Fei; Yang, Gaoling
- Advanced Optical Materials, Vol. 7, Issue 10
The effects of discrete and gradient mid-shell structures on the photoluminescence of single InP quantum dots
journal, January 2019
- Lee, Sang Hyeon; Kim, Yongwook; Jang, Hyosook
- Nanoscale, Vol. 11, Issue 48