Quantifying Efficiency Roll-Off Factors in Quantum-Dot Light-Emitting Diodes.

The application of quantum-dot light-emitting diodes (QLEDs) is hindered by efficiency roll-off at high current densities. Factors contributing to this roll-off include Auger recombination, electric field-induced quenching, Joule heating, and electron leakage into the hole transport layer. However, a method to quantitatively attribute the contribution of each factor to roll-off has not yet been available, leaving the primary cause of roll-off unidentified. This work addresses this gap using electrically pumped transient absorption spectroscopy, which measures the accumulated electrons and electric field in quantum dots (QDs). This study also introduces a method to quantify electron leakage in QLEDs using this spectroscopic technique. Based on the spectroscopic experimental results, the contribution of each factor to roll-off is quantified. A green QLED with a peak external quantum efficiency (EQE) of 26.8% is studied as an example. The EQE declines to 20.5% at a current density of 354 mA cm-2, where field-induced quenching accounts for 5% of the efficiency roll-off, and electron leakage contributes 95%. Contributions from Auger recombination and heat-induced quenching are negligible. This work demonstrates strong correlations between roll-off and electron leakage amplitude using statistical data obtained in multiple QLEDs, confirming that electron leakage is the primary factor in EQE roll-off.

Doping bilayer hole-transport polymer strategy stabilizing solution-processed green quantum-dot light-emitting diodes.

Quantum-dot light-emitting diodes (QLEDs) are solution-processed electroluminescence devices with great potential as energy-saving, large-area, and low-cost display and lighting technologies. Ideally, the organic hole-transport layers (HTLs) in QLEDs should simultaneously deliver efficient hole injection and transport, effective electron blocking, and robust electrochemical stability. However, it is still challenging for a single HTL to fulfill all these stringent criteria. Here, we demonstrate a general design of doping-bilayer polymer-HTL architecture for stabilizing high-efficiency QLEDs. We show that the bilayer HTLs combining the electrochemical-stable polymer and the electron-blocking polymer unexpectedly increase the hole injection barrier. We mitigated the problem by p-doping of the underlying sublayer of the bilayer HTLs. Consequently, green QLEDs with an unprecedented maximum luminance of 1,340,000 cd m-2 and a record-long operational lifetime (T95 lifetime at an initial luminance of 1000 cd m-2 is 17,700 hours) were achieved. The universality of the strategy is examined in various polymer-HTL systems, providing a general route toward high-performance solution-processed QLEDs.

Realizing Sunlight-Induced Efficiently Dynamic Infrared Emissivity Modulation Based on Aluminum-Doped zinc Oxide Nanocrystals.

Dynamic manipulation of an object's infrared radiation characteristics is a burgeoning technology with significant implications for energy and information fields. However, exploring efficient stimulus-spectral response mechanism and realizing simple device structures remains a formidable challenge. Here, a novel dynamic infrared emissivity regulation mechanism is proposed by controlling the localized surface plasmon resonance absorption of aluminum-doped zinc oxide (AZO) nanocrystals through ultraviolet photocharging/oxidative discharging. A straightforward device architecture that integrates an AZO nanocrystal film with an infrared reflective layer and a substrate, functioning as a photo-induced dynamic infrared emissivity modulator, which can be triggered by weak ultraviolet light in sunlight, is engineered. The modulator exhibits emissivity regulation amount of 0.72 and 0.61 in the 3-5 and 8-13 µm ranges, respectively. Furthermore, the modulator demonstrates efficient light triggering characteristic, broad spectral range, angular-independent emissivity, and long cyclic lifespan. The modulator allows for self-adaptive daytime radiative cooling and nighttime heating depending on the ultraviolet light in sunlight and O2 in air, thereby achieving smart thermal management for buildings with zero-energy expenditure. Moreover, the potential applications of this modulator can extend to rewritable infrared displays and deceptive infrared camouflage.

Shelf-Stable Green and Blue Quantum Dot Light-Emitting Diodes with High Efficiencies.

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.

Inner Doping of Carbon Nanotubes with Perovskites for Ultralow Power Transistors.

Semiconducting carbon nanotubes (CNTs) are considered as the most promising channel material to construct ultrascaled field-effect transistors, but the perfect sp2 C─C structure makes stable doping difficult, which limits the electrical designability of CNT devices. Here, an inner doping method is developed by filling CNTs with 1D halide perovskites to form a coaxial heterojunction, which enables a stable n-type field-effect transistor for constructing complementary metal-oxide-semiconductor electronics. Most importantly, a quasi-broken-gap (BG) heterojunction tunnel field-effect transistor (TFET) is first demonstrated based on an individual partial-filling CsPbBr3/CNT and exhibits a subthreshold swing of 35 mV dec-1 with a high on-state current of up to 4.9 µA per tube and an on/off current ratio of up to 105 at room temperature. The quasi-BG TFET based on the CsPbBr3/CNT coaxial heterojunction paves the way for constructing high-performance and ultralow power consumption integrated circuits.

Ion Migration in Lead-Halide Perovskites: Cation Matters.

Metal halide perovskites exhibit remarkable properties for optoelectronic applications, yet their susceptibility to ion migration poses challenges for device stability. Previous research has predominantly focused on the migration of the halide ions. However, the migration of cations, which also has a significant influence on the device performance, is largely overlooked. In this Perspective, we review the migration of cations and their impacts on perovskite materials and devices. Special attention shall be devoted to recent insights into the migration of L-site organic cations in 2D/3D perovskites. We outline inspirations and directions for further research into the cation migration of perovskites, highlighting new possibilities in advancing perovskite optoelectronics.

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.

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.

Mg-Diffusion of ZnO-Based Electron-Transport Layers for Highly Conductive Quantum-Dot Light-Emitting Diodes.

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.

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.

A Demulsification-Crystallization Model for High-Quality Perovskite Nanocrystals.

A room-temperature technique with all-nonpolar-solvent, which circumvents the sensitivity of ionic perovskite to polar solvent, has become attractive for the synthesis of metal halide perovskite nanocrystals (PNCs). However, the lack of understanding of the inner mechanism, especially for the state of the precursor and the crystallization process of the PNCs, hinders further development of this technique. Here, through systematic study of the Pb precursor and in situ characterization of the PNCs, it is revealed that the reverse micelle nature of the Pb precursor exactly creates a novel demulsification-crystallization (D-C) model, namely, a two-stage nucleation is divided by a demulsification process for the PNCs. On this basis, a top efficiency for green light-emitting diodes based on PNCs is obtained with a maximum external quantum efficiency of 22.5% through tailoring the D-C model using a multiple-acid-anion synergistic assisted strategy to obtain high-quality PNCs. Beyond the high efficiency, the work paves the way for diverse ideas in PNC synthesis.

Efficient and Bright Deep-Red Light-Emitting Diodes based on a Lateral 0D/3D Perovskite Heterostructure.

Bright and efficient deep-red light-emitting diodes (LEDs) are important for applications in medical therapy and biological imaging due to the high penetration of deep-red photons into human tissues. Metal-halide perovskites have potential to achieve bright and efficient electroluminescence due to their favorable optoelectronic properties. However, efficient and bright perovskite-based deep-red LEDs have not been achieved yet, due to either Auger recombination in low-dimensional perovskites or trap-assisted nonradiative recombination in 3D perovskites. Here, a lateral Cs4 PbI6 /FAx Cs1- x PbI3 (0D/3D) heterostructure that can enable efficient deep-red perovskite LEDs at very high brightness is demonstrated. The Cs4 PbI6 can facilitate the growth of low-defect FAx Cs1- x PbI3 , and act as low-refractive-index grids, which can simultaneously reduce nonradiative recombination and enhance light extraction. This device reaches a peak external quantum efficiency of 21.0% at a photon flux of 1.75 × 1021 m-2 s-1 , which is almost two orders of magnitude higher than that of reported high-efficiency deep-red perovskite LEDs. Theses LEDs are suitable for pulse oximeters, showing an error <2% of blood oxygen saturation compared with commercial oximeters.

CdSe/CdSeS Nanoplatelet Light-Emitting Diodes with Ultrapure Green Color and High External Quantum Efficiency.

Colloidal II-VI group nanoplatelets (NPLs) possess ultranarrow emission line widths, for which they have great promise in achieving the purest display color in solution-processed light-emitting diodes (LEDs). Red NPL-LEDs have shown extremely saturated red color with high efficiency, while the green and blue ones lag far behind. Herein, we report green NPL-LEDs with the purest color in accordance with the Rec. 2020 standard and the peak external quantum efficiency (EQE) of 9.78%. By carefully controlling the aspect ratio, capping ligands, and purifications of CdSe/CdSeS core/alloyed-crown NPLs, NPL films with excellent flatness and unity photoluminescence quantum yields (PLQYs) are realized, laying a solid foundation for improving LED performance. Furthermore, via tuning the carrier injection balance, the record-high EQE for green NPL-LEDs is achieved. The electroluminescence (EL) exhibits an extremely saturated green color with the Commission Internationale de L'Eclairage (CIE) coordinates of (0.163 0.786), which demonstrates their great potential in applications of ultrahigh-definition display technology. Our findings would help to further improve the performance of all NPL-LEDs.

Molecular Triplet Sensitization of Monolayer Semiconductors in 2D Organic/Inorganic Hybrid Heterostructures.

Hybrid heterostructures (HSs) comprising organic and two-dimensional (2D) monolayer semiconductors hold great promise for optoelectronic applications. So far, research efforts on organic/2D HSs have exclusively focused on coupling directly photoexcited singlets to monolayer semiconductors. It remains unexplored whether and how the optically dark triplets in organic semiconductors with intriguing properties (e.g., long lifetime) can be implemented for modulating light-matter interactions of hybrid HSs. Herein, we investigate the triplet sensitization of monolayer semiconductors by time-resolved spectroscopic studies on Pd-octaethylporphyrin (PdOEP)/WSe2 and PdOEP/WS2 HSs with type I and type II band alignment, respectively. We show that PdOEP triplets formed in ∼5 ps from intersystem crossing can transfer energy or charge to WSe2 or WS2 monolayers, respectively, leading to a significant photoluminescence enhancement (180%) in WSe2 or long-lived charge separation (>2 ns) in WS2. The triplet transfer occurs in ∼100 ns, which is more than 3 orders of magnitude slower than singlet and can be attributed to its tightly localized nature. Further study of thickness dependence reveals the dictating role of triplet diffusion for triplet sensitization in organic/2D HSs. This study shows the great promise of much less explored molecular triplets on sensitizing 2D monolayer semiconductors and provides the guidance to achieve long-range light harvesting and energy migration in organic/2D HSs for enhanced optoelectronic applications.

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.

Efficient light-emitting diodes based on oriented perovskite nanoplatelets.

Solution-processed planar perovskite light-emitting diodes (LEDs) promise high-performance and cost-effective electroluminescent devices ideal for large-area display and lighting applications. Exploiting emission layers with high ratios of horizontal transition dipole moments (TDMs) is expected to boost the photon outcoupling of planar LEDs. However, LEDs based on anisotropic perovskite nanoemitters remain to be inefficient (external quantum efficiency, EQE <5%) due to the difficulties of simultaneously controlling the orientations of TDMs, achieving high photoluminescence quantum yields (PLQYs) and realizing charge balance in the films of assembled nanostructures. Here, we demonstrate efficient electroluminescence from an in situ grown perovskite film composed of a monolayer of face-on oriented nanoplatelets. The ratio of horizontal TDMs of the perovskite nanoplatelet film is ~84%, which leads to a light-outcoupling efficiency of ~31%, substantially higher than that of isotropic emitters (~23%). In consequence, LEDs with a peak EQE of 23.6% are achieved, representing highly efficient planar perovskite LEDs.

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.

Efficient and bright warm-white electroluminescence from lead-free metal halides.

Solution-processed metal-halide perovskites are emerging as one of the most promising materials for displays, lighting and energy generation. Currently, the best-performing perovskite optoelectronic devices are based on lead halides and the lead toxicity severely restricts their practical applications. Moreover, efficient white electroluminescence from broadband-emission metal halides remains a challenge. Here we demonstrate efficient and bright lead-free LEDs based on cesium copper halides enabled by introducing an organic additive (Tween, polyethylene glycol sorbitan monooleate) into the precursor solutions. We find the additive can reduce the trap states, enhancing the photoluminescence quantum efficiency of the metal halide films, and increase the surface potential, facilitating the hole injection and transport in the LEDs. Consequently, we achieve warm-white LEDs reaching an external quantum efficiency of 3.1% and a luminance of 1570 cd m-2 at a low voltage of 5.4 V, showing great promise of lead-free metal halides for solution-processed white LED applications.