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1.
J Phys Chem Lett ; 15(26): 6722-6727, 2024 Jul 04.
Artículo en Inglés | MEDLINE | ID: mdl-38900937

RESUMEN

Quantum dot light-emitting diodes (QLEDs) are promising electroluminescent devices for next-generation display and solid-state lighting technologies. Achieving shelf-stable and high-performance QLEDs is crucial for their practical applications. However, the successful demonstration of shelf-stable QLEDs with high efficiencies is limited to red devices. Here, we developed a solution-based amine ligand exchange strategy to passivate the surfaces of optical ZnO (O-ZnO) nanocrystals, leading to suppressed exciton quenching at the green and blue QD/oxide interface. Furthermore, we designed new bilayered oxide electron-transporting layers consisting of amine-modified O-ZnO/conductive ZnO. This design simultaneously offers suppressed interfacial exciton quenching and sufficient electron transport in the green and blue QLEDs, resulting in shelf-stable green and blue devices with high efficiencies. Our devices exhibit neglectable changes in external quantum efficiencies (maximum external quantum efficiencies of 22.4% for green and 14.3% for blue) after storage for 270 days. Our work represents a step forward in the practical applications of QLED technology.

2.
Nat Commun ; 14(1): 7785, 2023 Nov 27.
Artículo en Inglés | MEDLINE | ID: mdl-38012136

RESUMEN

Quantum-dot light-emitting diodes promise a new generation of high-performance and solution-processed electroluminescent light sources. Understanding the operational degradation mechanisms of quantum-dot light-emitting diodes is crucial for their practical applications. Here, we show that quantum-dot light-emitting diodes may exhibit an anomalous degradation pattern characterized by a continuous increase in electroluminescent efficiency upon electrical stressing, which deviates from the typical decrease in electroluminescent efficiency observed in other light-emitting diodes. Various in-situ/operando characterizations were performed to investigate the evolutions of charge dynamics during the efficiency elevation, and the alterations in electric potential landscapes in the active devices. Furthermore, we carried out selective peel-off-and-rebuild experiments and depth-profiling analyses to pinpoint the critical degradation site and reveal the underlying microscopic mechanism. The results indicate that the operation-induced efficiency increase results from the degradation of electron-injection capability at the electron-transport layer/cathode interface, which in turn leads to gradually improved charge balance. Our work provides new insights into the degradation of red quantum-dot light-emitting diodes and has far-reaching implications for the design of charge-injection interfaces in solution-processed light-emitting diodes.

3.
Adv Mater ; 35(49): e2305382, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37672560

RESUMEN

Nanocrystal-based light-emitting diodes (Nc-LEDs) have immense potential for next-generation high-definition displays and lighting applications. They offer numerous advantages, such as low cost, high luminous efficiency, narrow emission, and long lifetime. However, the external quantum efficiency (EQE) of Nc-LEDs, typically employing isotropic nanocrystals, is limited by the out-coupling factor. Here efficient, bright, and long lifetime red Nc-LEDs based on anisotropic nanocrystals of colloidal quantum wells (CQWs) are demonstrated. Through modification of the substrate's surface properties and control of the interactions among CQWs, a self-assembled layer with an exceptionally high distribution of in-plane transitions dipole moment of 95%, resulting in an out-coupling factor of 37% is successfully spin-coated. The devices exhibit a remarkable peak EQE of 26.9%, accompanied by a maximum brightness of 55 754 cd m-2 and a long operational lifetime (T95 @100 cd m-2 ) over 15 000 h. These achievements represent a significant advancement compared to previous studies on Nc-LEDs incorporating anisotropic nanocrystals. The work is expected to provide a general self-assembly strategy for enhancing the light extraction efficiency of Nc-LEDs based on anisotropic nanocrystals.

4.
J Phys Chem Lett ; 14(25): 5812-5817, 2023 Jun 29.
Artículo en Inglés | MEDLINE | ID: mdl-37338303

RESUMEN

Quantum-dot light-emitting diodes (QLEDs) show great potential in next-generation display and lighting technologies. Further reducing the resistances of the high-efficiency QLEDs is critical to improving their luminous efficiencies and lowering their power consumption. However, wet-chemistry methods to improve the conductivities of ZnO-based electron-transport layers (ETLs) often lead to trade-offs in the external quantum efficiencies (EQEs) of QLEDs. Here, we report a facile approach toward highly conductive QLEDs by in situ diffusion of Mg atoms into the ZnO-based ETLs. We demonstrate that thermally evaporated Mg can spread deep into the ZnO-based ETL with a long penetration length, generating oxygen vacancies that promote the electron-transport properties. The Mg-diffused ETLs enhance the conductivities and luminous efficiencies of state-of-the-art QLEDs without sacrificing the EQEs. This strategy is applied to QLEDs with various optical architectures, leading to significant enhancements in the current densities, luminances, and luminous efficiencies. We expect that our method could be extended to other solution-processed LEDs using ZnO-based ETLs.

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