Droop-Free Colloidal Quantum Dot Light-Emitting Diodes
Abstract
Colloidal semiconductor quantum dots (QDs) are a highly promising materials platform for implementing solution-processable light-emitting diodes (LEDs). They combine high photostability of traditional inorganic semiconductors with chemical flexibility of molecular systems, which makes them well-suited for large-area applications such as television screens, solid-state lighting, and outdoor signage. Additional beneficial features include size-controlled emission wavelengths, narrow bandwidths, and nearly perfect emission efficiencies. State-of-the-art QD-LEDs exhibit high internal quantum efficiencies approaching unity. However, these peak values are observed only at low current densities (J) and correspondingly low brightnesses, whereas at higher J, the efficiency usually exhibits a quick roll-off. This efficiency droop limits achievable brightness levels and decreases device longevity due to excessive heat generation. We demonstrate QD-LEDs operating with high internal efficiencies (up to 70%) virtually droop-free up to unprecedented brightness of >100,000 cd m–2 (at ~500 mA cm–2). This exceptional performance is derived from specially engineered QDs that feature a compositionally graded interlayer and a final barrier layer. This QD design allows for improved balance between electron and hole injections combined with considerably suppressed Auger recombination, which helps mitigate efficiency losses due to charge imbalance at high currents. Finally, these results indicate a significant potential of newly developed QDs asmore »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Ajou Univ., Suwon (Korea, Republic of). Dept. of Chemical Engineering. Dept. of Energy System Research
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States). Center for High Technology Materials
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); LANL Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1477674
- Report Number(s):
- LA-UR-18-28788
Journal ID: ISSN 1530-6984
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 18; Journal Issue: 10; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Nanocrystal quantum dots Light emitting diode Droop-free
Citation Formats
Lim, Jaehoon, Park, Young -Shin, Wu, Kaifeng, Yun, Hyeong Jin, and Klimov, Victor I. Droop-Free Colloidal Quantum Dot Light-Emitting Diodes. United States: N. p., 2018.
Web. doi:10.1021/acs.nanolett.8b03457.
Lim, Jaehoon, Park, Young -Shin, Wu, Kaifeng, Yun, Hyeong Jin, & Klimov, Victor I. Droop-Free Colloidal Quantum Dot Light-Emitting Diodes. United States. https://doi.org/10.1021/acs.nanolett.8b03457
Lim, Jaehoon, Park, Young -Shin, Wu, Kaifeng, Yun, Hyeong Jin, and Klimov, Victor I. Mon .
"Droop-Free Colloidal Quantum Dot Light-Emitting Diodes". United States. https://doi.org/10.1021/acs.nanolett.8b03457. https://www.osti.gov/servlets/purl/1477674.
@article{osti_1477674,
title = {Droop-Free Colloidal Quantum Dot Light-Emitting Diodes},
author = {Lim, Jaehoon and Park, Young -Shin and Wu, Kaifeng and Yun, Hyeong Jin and Klimov, Victor I.},
abstractNote = {Colloidal semiconductor quantum dots (QDs) are a highly promising materials platform for implementing solution-processable light-emitting diodes (LEDs). They combine high photostability of traditional inorganic semiconductors with chemical flexibility of molecular systems, which makes them well-suited for large-area applications such as television screens, solid-state lighting, and outdoor signage. Additional beneficial features include size-controlled emission wavelengths, narrow bandwidths, and nearly perfect emission efficiencies. State-of-the-art QD-LEDs exhibit high internal quantum efficiencies approaching unity. However, these peak values are observed only at low current densities (J) and correspondingly low brightnesses, whereas at higher J, the efficiency usually exhibits a quick roll-off. This efficiency droop limits achievable brightness levels and decreases device longevity due to excessive heat generation. We demonstrate QD-LEDs operating with high internal efficiencies (up to 70%) virtually droop-free up to unprecedented brightness of >100,000 cd m–2 (at ~500 mA cm–2). This exceptional performance is derived from specially engineered QDs that feature a compositionally graded interlayer and a final barrier layer. This QD design allows for improved balance between electron and hole injections combined with considerably suppressed Auger recombination, which helps mitigate efficiency losses due to charge imbalance at high currents. Finally, these results indicate a significant potential of newly developed QDs as enablers of future ultrabright, highly efficient devices for both indoor and outdoor applications.},
doi = {10.1021/acs.nanolett.8b03457},
journal = {Nano Letters},
number = 10,
volume = 18,
place = {United States},
year = {Mon Sep 10 00:00:00 EDT 2018},
month = {Mon Sep 10 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
Degradation Mechanisms and Reactions in Organic Light-Emitting Devices
journal, July 2015
- Scholz, Sebastian; Kondakov, Denis; Lüssem, Björn
- Chemical Reviews, Vol. 115, Issue 16
Spectroscopic and Device Aspects of Nanocrystal Quantum Dots
journal, September 2016
- Pietryga, Jeffrey M.; Park, Young-Shin; Lim, Jaehoon
- Chemical Reviews, Vol. 116, Issue 18
White-Light-Emitting Diodes with Quantum Dot Color Converters for Display Backlights
journal, May 2010
- Jang, Eunjoo; Jun, Shinae; Jang, Hyosook
- Advanced Materials, Vol. 22, Issue 28
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking
journal, February 2013
- Chen, Ou; Zhao, Jing; Chauhan, Vikash P.
- Nature Materials, Vol. 12, Issue 5
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
Colloidal Spherical Quantum Wells with Near-Unity Photoluminescence Quantum Yield and Suppressed Blinking
journal, October 2016
- Jeong, Byeong Guk; Park, Young-Shin; Chang, Jun Hyuk
- ACS Nano, Vol. 10, Issue 10
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
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
Quantum Dot Light-Emitting Devices with Electroluminescence Tunable over the Entire Visible Spectrum
journal, July 2009
- Anikeeva, Polina O.; Halpert, Jonathan E.; Bawendi, Moungi G.
- Nano Letters, Vol. 9, Issue 7
Bright and Efficient Full-Color Colloidal Quantum Dot Light-Emitting Diodes Using an Inverted Device Structure
journal, April 2012
- Kwak, Jeonghun; Bae, Wan Ki; Lee, Donggu
- Nano Letters, Vol. 12, Issue 5
High-efficiency quantum-dot light-emitting devices with enhanced charge injection
journal, April 2013
- Mashford, Benjamin S.; Stevenson, Matthew; Popovic, Zoran
- Nature Photonics, Vol. 7, Issue 5
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
Double-heterojunction nanorods
journal, April 2014
- Oh, Nuri; Nam, Sooji; Zhai, You
- Nature Communications, Vol. 5, Issue 1
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
High-Efficiency Silicon Nanocrystal Light-Emitting Devices
journal, May 2011
- Cheng, Kai-Yuan; Anthony, Rebecca; Kortshagen, Uwe R.
- Nano Letters, Vol. 11, Issue 5
Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control
journal, May 2012
- Sun, Liangfeng; Choi, Joshua J.; Stachnik, David
- Nature Nanotechnology, Vol. 7, Issue 6
High-Performance Shortwave-Infrared Light-Emitting Devices Using Core-Shell (PbS-CdS) Colloidal Quantum Dots
journal, January 2015
- Supran, Geoffrey J.; Song, Katherine W.; Hwang, Gyu Weon
- Advanced Materials, Vol. 27, Issue 8
Highly efficient quantum dot near-infrared light-emitting diodes
journal, February 2016
- Gong, Xiwen; Yang, Zhenyu; Walters, Grant
- Nature Photonics, Vol. 10, Issue 4
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
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
Origins of Low Quantum Efficiencies in Quantum Dot LEDs
journal, January 2013
- Bozyigit, Deniz; Yarema, Olesya; Wood, Vanessa
- Advanced Functional Materials, Vol. 23, Issue 24
Origin of Efficiency Roll-Off in Colloidal Quantum-Dot Light-Emitting Diodes
journal, May 2013
- Shirasaki, Yasuhiro; Supran, Geoffrey J.; Tisdale, William A.
- Physical Review Letters, Vol. 110, Issue 21
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
High efficiency quantum dot light emitting diodes from positive aging
journal, January 2017
- Acharya, Krishna P.; Titov, Alexandre; Hyvonen, Jake
- Nanoscale, Vol. 9, Issue 38
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
Suppression of Auger Processes in Confined Structures
journal, January 2010
- Cragg, George E.; Efros, Alexander L.
- Nano Letters, Vol. 10, Issue 1
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
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
Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots
journal, August 2017
- Park, Young-Shin; Lim, Jaehoon; Makarov, Nikolay S.
- Nano Letters, Vol. 17, Issue 9
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
Towards zero-threshold optical gain using charged semiconductor quantum dots
journal, October 2017
- Wu, Kaifeng; Park, Young-Shin; Lim, Jaehoon
- Nature Nanotechnology, Vol. 12, Issue 12
Optical gain in colloidal quantum dots achieved with direct-current electrical pumping
journal, November 2017
- Lim, Jaehoon; Park, Young-Shin; Klimov, Victor I.
- Nature Materials, Vol. 17, Issue 1
Photochemical Electronic Doping of Colloidal CdSe Nanocrystals
journal, December 2013
- Rinehart, Jeffrey D.; Schimpf, Alina M.; Weaver, Amanda L.
- Journal of the American Chemical Society, Vol. 135, Issue 50
Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime
journal, April 2003
- Crooker, S. A.; Barrick, T.; Hollingsworth, J. A.
- Applied Physics Letters, Vol. 82, Issue 17
High-efficiency inverted dithienogermole–thienopyrrolodione-based polymer solar cells
journal, December 2011
- Small, Cephas E.; Chen, Song; Subbiah, Jegadesan
- Nature Photonics, Vol. 6, Issue 2, p. 115-120
Efficiency Roll-Off in Organic Light-Emitting Diodes
journal, September 2013
- Murawski, Caroline; Leo, Karl; Gather, Malte C.
- Advanced Materials, Vol. 25, Issue 47
The effect of Auger heating on intraband carrier relaxation in semiconductor quantum rods
journal, July 2006
- Achermann, Marc; Bartko, Andrew P.; Hollingsworth, Jennifer A.
- Nature Physics, Vol. 2, Issue 8
Works referencing / citing this record:
Quantum‐Dot Light‐Emitting Diodes for Outdoor Displays with High Stability at High Brightness
journal, October 2019
- Li, Xinyu; Lin, Qingli; Song, Jiaojiao
- Advanced Optical Materials, Vol. 8, Issue 2
Optically pumped colloidal-quantum-dot lasing in LED-like devices with an integrated optical cavity
journal, January 2020
- Roh, Jeongkyun; Park, Young-Shin; Lim, Jaehoon
- Nature Communications, Vol. 11, Issue 1
High‐Performance Quantum‐Dot Light‐Emitting Diodes Using NiO x Hole‐Injection Layers with a High and Stable Work Function
journal, November 2019
- Lin, Jian; Dai, Xingliang; Liang, Xiaoyong
- Advanced Functional Materials, Vol. 30, Issue 5
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
Inverted quantum dot light-emitting diodes with conductive interlayers of zirconium acetylacetonate
journal, January 2019
- Li, Yifei; Dai, Xingliang; Chen, Desui
- Journal of Materials Chemistry C, Vol. 7, Issue 11
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
Effects of 1,2-ethanedithiol concentration on performance improvement of quantum-dot LEDs
journal, January 2019
- Nguyen, Huu Tuan; Ryu, Shin Young; Duong, Anh Tuan
- RSC Advances, Vol. 9, Issue 66
Reduced Efficiency Roll‐Off and Improved Stability of Mixed 2D/3D Perovskite Light Emitting Diodes by Balancing Charge Injection
journal, July 2019
- Fakharuddin, Azhar; Qiu, Weiming; Croes, Guillaume
- Advanced Functional Materials, Vol. 29, Issue 37
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
Impact of 1,2-ethanedithiol treatment on luminescence and charge-transport characteristics in colloidal quantum-dot LEDs
journal, September 2019
- Nguyen, Huu Tuan; Ryu, Shin Young; Duong, Anh Tuan
- Nanotechnology, Vol. 30, Issue 50
Engineering Auger recombination in colloidal quantum dots via dielectric screening
journal, April 2019
- Hou, Xiaoqi; Kang, Jun; Qin, Haiyan
- Nature Communications, Vol. 10, Issue 1
Colloidal-annealing of ZnO nanoparticles to passivate traps and improve charge extraction in colloidal quantum dot solar cells
journal, January 2019
- Woo, Ho Kun; Kang, Min Su; Park, Taesung
- Nanoscale, Vol. 11, Issue 37
Waterproof Flexible InP@ZnSeS Quantum Dot Light‐Emitting Diode
journal, March 2020
- Shin, Dong‐Wook; Suh, Yo‐Han; Lee, Sanghyo
- Advanced Optical Materials, Vol. 8, Issue 6
Waterproof Flexible InP@ZnSeS Quantum Dot Light-Emitting Diode
text, January 2020
- Shin, Dong-Wook; Suh, Yh; Lee, S.
- Apollo - University of Cambridge Repository
Engineering the Band Alignment in QD Heterojunction Films via Ligand Exchange
journal, November 2019
- Grimaldi, Gianluca; van den Brom, Mark J.; du Fossé, Indy
- The Journal of Physical Chemistry C, Vol. 123, Issue 49
Spectroscopic Evidence for the Contribution of Holes to the Bleach of Cd-Chalcogenide Quantum Dots
journal, March 2019
- Grimaldi, Gianluca; Geuchies, Jaco J.; van der Stam, Ward
- Nano Letters, Vol. 19, Issue 5
Engineering Auger recombination in colloidal quantum dots via dielectric screening
journal, April 2019
- Hou, Xiaoqi; Kang, Jun; Qin, Haiyan
- Nature Communications, Vol. 10, Issue 1
Optically pumped colloidal-quantum-dot lasing in LED-like devices with an integrated optical cavity
journal, January 2020
- Roh, Jeongkyun; Park, Young-Shin; Lim, Jaehoon
- Nature Communications, Vol. 11, Issue 1
Electrochemically-stable ligands bridge photoluminescence-electroluminescence gap of quantum dots
text, January 2019
- Pu, Chaodan; Dai, Xingliang; Shu, Yufei
- arXiv