Title: Two-band optical gain and ultrabright electroluminescence from colloidal quantum dots at 1000 A cm−2

Journal Article · · Nature Communications

Abstract Colloidal quantum dots (QDs) are attractive materials for the realization of solution-processable laser diodes. Primary challenges towards this objective are fast optical-gain relaxation due to nonradiative Auger recombination and poor stability of colloidal QD solids under high current densities required to obtain optical gain. Here we resolve these challenges and achieve broad-band optical gain spanning the band-edge (1S) and the higher-energy (1P) transitions. This demonstration is enabled by continuously graded QDs with strongly suppressed Auger recombination and a current-focusing device design, combined with short-pulse pumping. Using this approach, we achieve ultra-high current densities (~1000 A cm −2 ) and brightness (~10 million cd m −2 ), and demonstrate an unusual two-band electroluminescence regime for which the 1P band is more intense than the 1S feature. This implies the realization of extremely large QD occupancies of up to ~8 excitons per-dot, which corresponds to complete filling of the 1S and 1P electron shells.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1874419
Report Number(s):
LA-UR-22-24389; 3734; PII: 31189
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (39)

Characterizing Joule Heating in Polymer Light-Emitting Diodes Using a Scanning Thermal Microscope journal February 2004
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
Quantum-dots based materials for temperature sensing: effect of cyclic heating-cooling on fluorescence journal August 2019
Thermally induced failure mechanisms of organic light emitting device structures probed by X-ray specular reflectivity journal October 1997
Thermally stable organic light-emitting diodes using new families of hole-transporting amorphous molecular materials journal June 2000
Highly efficient and low turn-on voltage quantum-dot light-emitting diodes using a ZnMgO/ZnO double electron transport layer journal September 2021
Failure mechanism of organic light emitting diodes (OLEDs) induced by hygrothermal effect journal May 2019
Advances and prospects of lasers developed from colloidal semiconductor nanostructures journal August 2018
Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces journal October 2015
Suppressing Efficiency Roll-Off at High Current Densities for Ultra-Bright Green Perovskite Light-Emitting Diodes journal April 2020
Unraveling the Origin of Operational Instability of Quantum Dot Based Light-Emitting Diodes journal September 2018
Investigation on Thermally Induced Efficiency Roll-Off: Toward Efficient and Ultrabright Quantum-Dot Light-Emitting Diodes journal September 2019
Tuning the Potentials of “Extra” Electrons in Colloidal n -Type ZnO Nanocrystals via Mg 2+ Substitution journal April 2012
High-Temperature Luminescence Quenching of Colloidal Quantum Dots journal September 2012
Single Molecule Quantum-Confined Stark Effect Measurements of Semiconductor Nanoparticles at Room Temperature journal October 2012
Single-exciton optical gain in semiconductor nanocrystals journal May 2007
Solution-processed, high-performance light-emitting diodes based on quantum dots journal October 2014
Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy journal March 2017
Optical gain in colloidal quantum dots achieved with direct-current electrical pumping journal November 2017
A bright future for colloidal quantum dot lasers journal August 2019
Optically pumped colloidal-quantum-dot lasing in LED-like devices with an integrated optical cavity journal January 2020
Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths journal January 2019
Bright colloidal quantum dot light-emitting diodes enabled by efficient chlorination journal February 2018
Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency journal February 2019
Colloidal quantum dot lasers journal February 2021
Efficient and stable blue quantum dot light-emitting diode journal October 2020
Bandgap tunable Zn 1−x Mg x O thin films as electron transport layers for high performance quantum dot light-emitting diodes journal January 2017
Quantum dots to probe temperature and pressure in highly confined liquids journal January 2018
Degradation of quantum dot light emitting diodes, the case under a low driving level journal January 2020
Thermal stability in oligomeric triphenylamine/tris(8-quinolinolato) aluminum electroluminescent devices journal April 1997
Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime journal April 2003
Control of carrier injection and transport in quantum dot light emitting diodes (QLEDs) via modulating Schottky injection barrier and carrier mobility journal November 2019
Temperature dependence of the photoluminescence properties of colloidal Cd Se ∕ Zn S core/shell quantum dots embedded in a polystyrene matrix journal June 2005
Duration Effect of Pulsed High-Brightness Organic Light-emitting Diodes conference August 2018
Weave Patterned Organic Transistors on Fiber for E-Textiles journal February 2005
Quantum-Confined Stark Effect in Single CdSe Nanocrystallite Quantum Dots journal December 1997
Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots journal February 2000
Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots journal October 2000
Carrier Injection and Transport of Steady-State High Current Density Exceeding 1000 A/cm 2 in Organic Thin Films * journal November 2003