Anomalous efficiency elevation of quantum-dot light-emitting diodes induced by operational degradation.

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.

Highly Efficient Light-Emitting Diodes Based on Self-Assembled Colloidal Quantum Wells.

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.

Obviating Ligand Exchange Preserves the Intact Surface of HgTe Colloidal Quantum Dots and Enhances Performance of Short Wavelength Infrared Photodetectors.

A large volume, scalable synthesis procedure of HgTe quantum dots (QDs) capped initially with short-chain conductive ligands ensures ligand exchange-free and simple device fabrication. An effective n- or p-type self-doping of HgTe QDs is achieved by varying cation-anion ratio, as well as shifting the Fermi level position by introducing single- or double-cyclic thiol ligands, that is, 2-furanmethanethiol (FMT) or 2,5-dimercapto-3,4-thiadiasole (DMTD) in the synthesis. This allows for preserving the intact surface of the HgTe QDs, thus ensuring a one order of magnitude reduced surface trap density compared with HgTe subjected to solid-state ligand exchange. The charge carrier diffusion length can be extended from 50 to 90 nm when the device active area consists of a bi-layer of cation-rich HgTe QDs capped with DMTD and FMT, respectively. As a result, the responsivity under 1340 nm illumination is boosted to 1 AW-1 at zero bias and up to 40 AW-1 under -1 V bias at room temperature. Due to high noise current density, the specific detectivity of these photodetectors reaches up to 1010 Jones at room temperature and under an inert atmosphere. Meanwhile, high photoconductive gain ensures a rise in the external quantum efficiency of up to 1000% under reverse bias.

Transparent dynamic infrared emissivity regulators.

Dynamic infrared emissivity regulators, which can efficiently modulate infrared radiation beyond vision, have emerged as an attractive technology in the energy and information fields. The realization of the independent modulation of visible and infrared spectra is a challenging and important task for the application of dynamic infrared emissivity regulators in the fields of smart thermal management and multispectral camouflage. Here, we demonstrate an electrically controlled infrared emissivity regulator that can achieve independent modulation of the infrared emissivity while maintaining a high visible transparency (84.7% at 400-760 nm). The regulators show high degree of emissivity regulation (0.51 at 3-5 µm, 0.41 at 7.5-13 µm), fast response ( < 600 ms), and long cycle life ( > 104 cycles). The infrared emissivity regulation is attributed to the modification of the carrier concentration in the surface depletion layer of aluminum-doped zinc oxide nanocrystals. This transparent infrared emissivity regulator provides opportunities for applications such as on-demand smart thermal management, multispectral displays, and adaptive camouflage.

All-Solution-Processed Perovskite Light-Emitting Diodes Based on a Thiol-Modified ZnO Electron-Transporting Layer.

All-solution-processed perovskite light-emitting diodes (LEDs) have the potential to be inexpensive and easily manufactured on a large scale without requiring vacuum thermal deposition of the emissive and charge transport layers. Zinc oxide (ZnO), which possesses superior optical and electronic properties, is commonly used in all-solution-processed optoelectronic devices. However, the polar solvent of ZnO inks can corrode the perovskite layer and cause severe photoluminescence quenching. In this work, we report the successful dispersion of ZnO nanoparticles in nonpolar n-octane by controlling the surface ligands from acetates to thiols. The nonpolar ink prevents the destruction of perovskite films. In addition, thiol ligands upshift the conduction band energy level, which also helps inhibit exciton quenching. Consequently, we demonstrate the fabrication of high-performance all-solution-processed green perovskite LEDs with a brightness of 21 000 cd/m2 and an external quantum efficiency of 6.36%. Our work provides a ZnO ink for fabricating efficient all-solution-processed perovskite LEDs.

Electrochemically Stable Ligands of ZnO Electron-Transporting Layers for Quantum-Dot Light-Emitting Diodes.

Thin films of ZnO nanocrystals are actively pursued as electron-transporting layers (ETLs) in quantum-dot light-emitting diodes (QLEDs). However, the developments of ZnO-based ETLs are highly engineering oriented and the design of ZnO-based ETLs remains empirical. Here, we identified a previously overlooked efficiency-loss channel associated with the ZnO-based ETLs: i.e., interfacial exciton quenching induced by surface-bound ethanol. Accordingly, we developed a general surface-treatment procedure to replace the redox-active surface-bound ethanol with electrochemically inert alkali carboxylates. Characterization results show that the surface treatment procedure does not change other key properties of the ETLs, such as the conductance and work function. Our single-variable experimental design unambiguously demonstrates that improving the electrochemical stabilities of the ZnO ETLs leads to QLEDs with a higher efficiency and longer operational lifetime. Our work provides a crucial guideline to design ZnO-based ETLs for optoelectronic devices.

ZnO-Based Electron-Transporting Layers for Perovskite Light-Emitting Diodes: Controlling the Interfacial Reactions.

Perovskite light-emitting diodes (PeLEDs) provide new opportunities for cost-effective and large-area electroluminescent devices. It is of interest to use ZnO-based electron-transport layers (ETLs), which demonstrate superior performance in other solution-processed LEDs, in PeLEDs. However, the notorious deprotonation reaction between ZnO and perovskite casts doubt on the long-term stability of PeLEDs with ZnO-based ETLs. This Perspective presents an overview of the chemical reactions that may occur at the interfaces between perovskite and ZnO-based ETLs. We highlight that other interfacial reactions during the fabrication of PeLEDs, including the reactions between ZnO and the intermediate phase during perovskite crystallization and the amidation reactions catalyzed by ZnO, demonstrate critical utilities in the fabrication of high-efficiency and stable PeLEDs. Considering these recent advances, we propose future directions and prospects to design and control the interfacial reactions, aiming to fully exploit the potential of ZnO-based ETLs for realizing high-performance PeLEDs.

Synthesis of Cu-Modified Nickel Oxide Nanocrystals and Their Applications as Hole-Injection layers for Quantum-Dot Light-Emitting Diodes.

Solution-processed NiOx thin films have been applied as hole-injection layers (HILs) in quantum-dot light-emitting diodes (QLEDs). The commonly used NiOx HILs are prepared by the precursor-based route, which requires high annealing temperatures of over 275 °C to in situ convert the precursors into oxide films. Such high processing temperatures of NiOx HILs hinder their applications in flexible devices. Herein, we report a low-temperature approach based on Cu-modified NiOx (NiOx -Cu) nanocrystals to prepare HILs. A simple post-synthetic surface-modification step, which anchors the copper agents onto the surfaces of oxide nanocrystals, is developed to improve the electrical conductivity of the low-temperature-processed (135 °C) oxide-nanocrystal thin films. In consequence, QLEDs based on the NiOx -Cu HILs exhibit an external quantum efficiency of 17.5 % and a T95 operational lifetime of ∼2,800 h at an initial brightness of 1,000 cd m-2 , meeting the commercialization requirements for display applications. The results shed light on the potential of using NiOx -Cu HILs for realizing high-performance flexible QLEDs.

Shelf-Stable Quantum-Dot Light-Emitting Diodes with High Operational Performance.

Quantum-dot light-emitting diodes (QLEDs) promise a new generation of high-performance, large-area, and cost-effective electroluminescent devices for both display and solid-state lighting technologies. However, a positive ageing process is generally required to improve device performance for state-of-the-art QLEDs. Here, it is revealed that the in situ reactions induced by organic acids in the commonly used encapsulation acrylic resin lead to positive ageing and, most importantly, the progression of in situ reactions inevitably results in negative ageing, i.e., deterioration of device performance after long-term shelf storage. In-depth mechanism studies focusing on the correlations between the in situ chemical reactions and the shelf-ageing behaviors of QLEDs inspire the design of an electron-transporting bilayer, which delivers both improved electrical conductivity and suppressed interfacial exciton quenching. This material innovation enables red QLEDs exhibiting neglectable changes of external quantum efficiency (>20.0%) and ultralong operational lifetime (T95 : 5500 h at 1000 nits) after storage for 180 days. This work provides design principles for oxide electron-transporting layers to realize shelf-stable and high-operational-performance QLEDs, representing a new starting point for both fundamental studies and practical applications.

Design of the Hole-Injection/Hole-Transport Interfaces for Stable Quantum-Dot Light-Emitting Diodes.

Extensive efforts have been devoted to improving the operational performance of quantum-dot light-emitting diodes (QLEDs). However, the fundamental understanding of the relationship between the design of the hole-injection layer (HIL)/hole-transporting layer (HTL) interface and the operational stability of QLEDs is limited. Here, we demonstrate that in the operation of red QLEDs, the leakage electrons induce in situ electrochemical reduction reactions of the polyfluorene HTLs, which in consequence create trap states and deteriorate charge-transport properties. We invoke an oxygen-plasma treatment on the PEDOT:PSS HILs, resulting in HIL/HTL interfaces with enhanced hole-injection properties. This simple method leads to more efficient exciton generation in the QDs layer and mitigated leakage electron-induced degradation of the HTLs, enabling red-emitting QLEDs with improved operational performance, i.e., high external quantum efficiency of >20.0% at a brightness ranging from 1000 to 10 000 cd m-2 and a long T95 operational lifetime of ∼4200 h at 1000 cd m-2.

Synthesis of Highly Monodisperse Cu2 O Nanocrystals and Their Applications as Hole-Transporting Layers in Solution-Processed Light-Emitting Diodes.

The synthesis of phase-pure, narrow-size-distributed and highly stable Cu2 O nanocrystals is reported, which can be processed as hole-transporting layers (HTLs) in solution-processed optoelectronic devices. The synthesis is based on a thermal decomposition process with a ligand protection strategy. The reactivity of precursor can be tuned by simply modulating the concentration of oleylamine in non-coordinated solvent, resulting in effectively controlling the size and size distribution of Cu2 O nanocrystals. Combined with ligand protection strategy of using lithium stearate and moderate reaction temperature of 170 °C, in situ aggregation of Cu2 O nanocrystals could be inhibited, exhibiting excellent stability in hexane for several months. The resulting phase-pure colloidal Cu2 O particles (after ozone-treatment) were applied as HTLs in polymer light-emitting diodes, the performance of which are comparable to that of the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) based devices.