Molecule‐Induced p‐Doping in Perovskite Nanocrystals Enables Efficient Color‐Saturated Red Light‐Emitting Diodes

Color‐saturated red light‐emitting diodes (LEDs) with emission wavelengths at around 620–640 nm are an essential part of high‐definition displays. Metal halide perovskites with very narrow emission linewidth are promising emitters, and rapid progress has been made in perovskite‐based LEDs (PeLEDs); however, the efficiency of the current color—pure red PeLEDs—still far lags behind those of other‐colored ones. Here, a simple but efficient strategy is reported to gradually down‐shift the Fermi level of perovskite nanocrystals (NCs) by controlling the interaction between NCs and their surface molecular electron acceptor—benzyl iodide with aromatic rings—and realize p‐doping in the color‐saturated 625 nm emitting NCs, which significantly reduces the hole injection barrier in devices. Besides, both the luminescence efficiency and electric conductivity of perovskite NCs are enhanced as additional advantages as the result of surface defects passivation. As a result, the external quantum efficiency for the resulting LED is increased from 4.5% to 12.9% after benzyl iodide treatment, making this device the best‐performing color‐saturated red PeLED so far. It is further found that the hole injection plays a more critical role than the photoluminescence efficiency of perovskite emitter in determining the LED performance, which implies design principles for efficient thin‐film planar LEDs.     

High‐Efficiency Perovskite Light‐Emitting Diodes with Synergetic Outcoupling Enhancement

Perovskite light‐emitting diodes (PeLEDs) show great application potential in high‐quality flat‐panel displays and solid‐state lighting due to their steadily improved efficiency, tunable colors, narrow emission peak, and easy solution‐processing capability. However, because of high optical confinement and nonradiative charge recombination during electron–photon conversion, the highest reported efficiency of PeLEDs remains far behind that of their conventional counterparts, such as inorganic LEDs, organic LEDs, and quantum‐dot LEDs. Here a facile route is demonstrated by adopting bioinspired moth‐eye nanostructures at the front electrode/perovskite interface to enhance the outcoupling efficiency of waveguided light in PeLEDs. As a result, the maximum external quantum efficiency and current efficiency of the modified cesium lead bromide (CsPbBr₃) green‐emitting PeLEDs are improved to 20.3% and 61.9 cd A^?1, while retaining spectral and angular independence. Further reducing light loss in the substrate mode using a half‐ball lens, efficiencies of 28.2% and 88.7 cd A^?1 are achieved, which represent the highest values reported to date for PeLEDs. These results represent a substantial step toward achieving practical applications of PeLEDs.     

Perovskite Light‐Emitting Diodes with Improved Outcoupling Using a High‐Index Contrast Nanoarray

Organic–inorganic hybrid perovskite light‐emitting diodes (PeLEDs) are promising for next‐generation optoelectronic devices due to their potential to achieve high color purity, efficiency, and brightness. Although the external quantum efficiency (EQE) of PeLEDs has recently surpassed 20%, various strategies are being pursued to increase EQE further and reduce the EQE gap compared to other LED technologies. A key point to further boost EQE of PeLEDs is linked to the high refractive index of the perovskite emissive layer, leading to optical losses of more than 70% of emitted photons. Here, it is demonstrated that a randomly distributed nanohole array with high‐index contrast can effectively enhance outcoupling efficiency in PeLEDs. Based on a comprehensive optical analysis on the perovskite thin film and outcoupling structure, it is confirmed that the nanohole array effectively distributes light into the substrate for improved outcoupling, allowing for 1.64 times higher light extraction. As a result, highly efficient red/near‐infrared PeLEDs with a peak EQE of 14.6% are demonstrated.     

High‐Performance Blue Perovskite Light‐Emitting Diodes Enabled by Efficient Energy Transfer between Coupled Quasi‐2D Perovskite Layers

While there has been extensive investigation into modulating quasi‐2D perovskite compositions in light‐emitting diodes (LEDs) for promoting their electroluminescence, very few reports have studied approaches involving enhancement of the energy transfer between quasi‐2D perovskite layers of the film, which plays very important role for achieving high‐performance perovskite LEDs (PeLEDs). In this work, a bifunctional ligand of 4‐(2‐aminoethyl)benzoic acid (ABA) cation is strategically introduced into the perovskite to diminish the weak van der Waals gap between individual perovskite layers for promoting coupled quasi‐2D perovskite layers. In particular, the strengthened interaction between coupled quasi‐2D perovskite layers favors an efficient energy transfer in the perovskite films. The introduced ABA can also simultaneously passivate the perovskite defects by reducing metallic Pb for less nonradiative recombination loss. Benefiting from the advanced properties of ABA incorporated perovskites, highly efficient blue PeLEDs with external quantum efficiency of 10.11% and a very long operational stability of 81.3 min, among the best performing blue quasi‐2D PeLEDs, are achieved. Consequently, this work contributes an effective approach for high‐performance and stable blue PeLEDs toward practical applications.     

High Performance Quasi‐2D Perovskite Sky‐Blue Light‐Emitting Diodes Using a Dual‐Ligand Strategy

For quasi‐2D perovskite light‐emitting diodes, the introduction of insulating bulky cation reduces the charge transport property, leading to lowered brightness and increased turn‐on voltage. Herein, a dual‐ligand strategy is adopted to prepare perovskite films by using an appropriate ratio of i‐butylammonium (iBA) and phenylethylammonium (PEA) as capping ligands. The introduction of iBA enhances the binding energy of the ligands on the surface of the quasi‐2D perovskite, and effectively controls the proportion of 2D perovskite to allow more efficient energy transfer, resulting in the great enhancement of the electric and luminescent properties of the perovskite. The photoluminescence (PL) mapping of the perovskite films exhibits that enhanced photoluminescence performance with better uniformity and stronger intensity can be achieved with this dual‐ligand strategy. By adjusting the proportion of the two ligands, sky‐blue perovskite light‐emitting diodes (PeLEDs) with electroluminescence (EL) peak located 485 nm are achieved with a maximum luminance up to 1130 cd m^?2 and a maximum external quantum efficiency (EQE) up to 7.84%. In addition, the color stability and device stability are significantly enhanced by using a dual‐ligand strategy. This simple and feasible method paves the way for improving the performance of quasi‐2D PeLEDs.     

Room‐Temperature Triple‐Ligand Surface Engineering Synergistically Boosts Ink Stability,Recombination Dynamics,and Charge Injection toward EQE‐11.6% Perovskite QLEDs

Developing low‐cost and high‐quality quantum dots (QDs) or nanocrystals (NCs) and their corresponding efficient light‐emitting diodes (LEDs) is crucial for the next‐generation ultra‐high‐definition flexible displays. Here, there is a report on a room‐temperature triple‐ligand surface engineering strategy to play the synergistic role of short ligands of tetraoctylammonium bromide (TOAB), didodecyldimethylammonium bromide (DDAB), and octanoic acid (OTAc) toward “ideal” perovskite QDs with a high photoluminescence quantum yield (PLQY) of >90%, unity radiative decay in its intrinsic channel, stable ink characteristics, and effective charge injection and transportation in QD films, resulting in the highly efficient QD‐based LEDs (QLEDs). Furthermore, the QD films with less nonradiative recombination centers exhibit improved PL properties with a PLQY of 61% through dopant engineering in A‐site. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on CsPbBr₃ QDs with the peak external quantum efficiency (EQE) of 11.6%, and the corresponding peak internal quantum efficiency (IQE) and power efficiency are 52.2% and 44.65 lm W^?1, respectively, which are the most‐efficient perovskite QLEDs with colloidal CsPbBr₃ QDs as emitters up to now. These results demonstrate that the as‐obtained QD inks have a wide range application in future high‐definition QD displays and high‐quality lightings.     

Conjugated Polyelectrolytes as Multifunctional Passivating and Hole‐Transporting Layers for Efficient Perovskite Light‐Emitting Diodes

Metal halide perovskites (MHPs) have attracted significant attention as light‐emitting materials owing to their high color purities and tunabilities. A key issue in perovskite light‐emitting diodes (PeLEDs) is the fabrication of an optimal charge transport layer (CTL), which has desirable energy levels for efficient charge injection while blocking opposite charges and enabling perovskite layer growth with reduced interfacial defects. Herein, two poly(fluorene‐phenylene)‐based anionic conjugated polyelectrolytes (CPEs) with different counterions (K⁺ and tetramethylammonium (TMA⁺)) are presented as multifunctional passivating and hole‐transporting layers (HTLs). The crystal growth of MHPs grown on different HTLs is investigated through X‐ray photoelectron spectroscopy, X‐ray diffraction, and density functional theory calculation. The CPE bearing the TMA⁺ counterions remarkably improves the growth of perovskites with suppressed interfacial defects, leading to significantly enhanced emission properties and device performance. The luminescent properties are further enhanced via aging and electrical stress application with effective rearrangement of the counterions on the interfacial defects in the perovskites. Finally, efficient formamidinium lead tribromide‐based quasi‐2D PeLEDs with an external quantum efficiency of 10.2% are fabricated. Using CPEs with varying counterions as a CTL can serve as an effective method for controlling the interfacial defects and improving perovskite‐based optoelectronic device properties.     

Fast Postmoisture Treatment of Luminescent Perovskite Films for Efficient Light‐Emitting Diodes

Despite the recent advances in the performance of perovskite light‐emitting diodes (PeLEDs), the effects of water on the perovskite emissive layer and its electroluminescence are still unclear, even though it has been previously demonstrated that moisture has a significant impact on the quality of perovskite films in the fabrication process of perovskite solar cells and is a prerequisite for obtaining high‐performance PeLEDs. Here, the effects of postmoisture on the luminescent CH₃NH₃PbBr₃ (MAPbBr₃) perovskite films are systematically investigated. It is found that postmoisture treatment can efficiently control the morphology and growth of perovskite films and only a fast moisture exposure at a 60% high relative humidity results in significantly improved crystallinity, carrier lifetime, and photoluminescence quantum yield of perovskite films. With the optimized moisture‐treated perovskite films, a high‐performance PeLED is fabricated, exhibiting a maximum current efficiency of 20.4 cd A^?1, which is an almost 20‐fold enhancement when compared with perovskite films without moisture treatment. The results provide valuable insights into the moisture‐assisted growth of luminescent perovskite films and will aid in the development of high‐performance perovskite light‐emitting devices.     

Blue light-emitting diodes based on halide perovskites: Recent advances and strategies

Metal halide perovskites, as a new generation of semiconductor materials, have been widely applied in various optoelectronic devices, especially in the field of perovskite light-emitting diodes (PeLEDs). The external quantum efficiencies (EQEs) of green, red, and near-infrared PeLEDs have exceeded 20% for the last few years, which are comparable to those of the state-of-the-art organic light-emitting diodes (OLEDs) and quantum-dot light-emitting diodes (QLEDs). However, the performances of blue PeLEDs lag far behind those of their counterparts, presumably due to the low quantum yields of blue perovskite films, the instability of the emission spectra, and the difficulties in charge injection for the devices under operation conditions. In this review, the structures and physical properties of blue emissive perovskite materials and the preparation methods of the corresponding perovskite films are firstly addressed. Then, the recent advances and strategies to improve the efficiency of blue PeLEDs are outlined, and the main challenges faced with the blue PeLEDs are also discussed. Finally, an outlook on blue LEDs based on perovskite materials is proposed.     

Morphology Engineering for High‐Performance and Multicolored Perovskite Light‐Emitting Diodes with Simple Device Structures

The film morphology is extremely significant for solution processed perovskite devices. Through fine morphology engineering without using any additives or further posttreatments, a full‐coverage and high quantum yield perovskite film has been achieved based on one‐step spin‐coating method. The morphologies and film characteristics of MAPbBr₃ with different MABr:PbBr₂ starting material ratios are in‐depth investigated by scanning electron microscopy, atomic force microscopy, X‐ray diffraction, photoluminescence, and time resolved photoluminescence. High performance organometal halide perovskite light‐emitting didoes (PeLEDs) based on simple device structure of indium tin oxide/poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS)/perovskite/TPBi/Ca/Al are demonstrated. The green PeLED based on MAPbBr₃ shows a maximum luminance of 8794 cd m^?2 (at 7.3 V) and maximum current efficiency of 5.1 cd A^?1 (at 5.1 V). Furthermore, a class of hybrid PeLEDs by adjusting the halide ratios of methylammonium lead halide (MAPbX₃, where X is Cl, Br, or I) are also demonstrated at room temperature. These mix‐halogenated PeLEDs show bright luminance (above 100 cd m^?2) with narrow and clean emission bands over the wide color gamut.     

Electrical Stress Influences the Efficiency of CH3NH3PbI3 Perovskite Light Emitting Devices

Organic–inorganic hybrid perovskite materials are emerging as semiconductors with potential application in optoelectronic devices. In particular, perovskites are very promising for light‐emitting devices (LEDs) due to their high color purity, low nonradiative recombination rates, and tunable bandgap. Here, using pure CH₃NH₃PbI₃ perovskite LEDs with an external quantum efficiency (EQE) of 5.9% as a platform, it is shown that electrical stress can influence device performance significantly, increasing the EQE from an initial 5.9% to as high as 7.4%. Consistent with the enhanced device performance, both the steady‐state photoluminescence (PL) intensity and the time‐resolved PL decay lifetime increase after electrical stress, indicating a reduction in nonradiative recombination in the perovskite film. By investigating the temperature‐dependent characteristics of the perovskite LEDs and the cross‐sectional elemental depth profile, it is proposed that trap reduction and resulting device‐performance enhancement is due to local ionic motion of excess ions, likely excess mobile iodide, in the perovskite film that fills vacancies and reduces interstitial defects. On the other hand, it is found that overstressed LEDs show irreversibly degraded device performance, possibly because ions initially on the perovskite lattice are displaced during extended electrical stress and create defects such as vacancies.     

Stretchable Organometal‐Halide‐Perovskite Quantum‐Dot Light‐Emitting Diodes

Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A^?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.     

Stretchable Light‐Emitting Diodes with Organometal‐Halide‐Perovskite–Polymer Composite Emitters

Intrinsically stretchable light‐emitting diodes (LEDs) are demonstrated using organometal‐halide‐perovskite/polymer composite emitters. The polymer matrix serves as a microscale elastic connector for the rigid and brittle perovskite and induces stretchability to the composite emissive layers. The stretchable LEDs consist of poly(ethylene oxide)‐modified poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate as a transparent and stretchable anode, a perovskite/polymer composite emissive layer, and eutectic indium–gallium as the cathode. The devices exhibit a turn‐on voltage of 2.4 V, and a maximum luminance intensity of 15 960 cd m^?2 at 8.5 V. Such performance far exceeds all reported intrinsically stretchable LEDs based on electroluminescent polymers. The stretchable perovskite LEDs are mechanically robust and can be reversibly stretched up to 40% strain for 100 cycles without failure.     

A Strategy for Architecture Design of Crystalline Perovskite Light‐Emitting Diodes with High Performance

All present designs of perovskite light‐emitting diodes (PeLEDs) stem from polymer light‐emitting diodes (PLEDs) or perovskite solar cells. The optimal structure of PeLEDs can be predicted to differ from PLEDs due to the different fluorescence dynamics and crystallization between perovskite and polymer. Herein, a new design strategy and conception is introduced, “insulator–perovskite–insulator” (IPI) architecture tailored to PeLEDs. As examples of FAPbBr₃ and MAPbBr₃, it is experimentally shown that the IPI structure effectively induces charge carriers into perovskite crystals, blocks leakage currents via pinholes in the perovskite film, and avoids exciton quenching simultaneously. Consequently, as for FAPbBr₃, a 30‐fold enhancement in the current efficiency of IPI‐structured PeLEDs compared to a control device with poly(3,4ethylenedioxythiophene):poly(styrene sulfonate) as hole‐injection layer is achieved—from 0.64 to 20.3 cd A^?1—while the external quantum efficiency is increased from 0.174% to 5.53%. As the example of CsPbBr₃, compared with the control device, both current efficiency and lifetime of IPI‐structured PeLEDs are improved from 1.42 and 4 h to 9.86 cd A^?1 and 96 h. This IPI architecture represents a novel strategy for the design of light‐emitting didoes based on various perovskites with high efficiencies and stabilities.     

Perovskite Materials for Light‐Emitting Diodes and Lasers

Organic–inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light‐emitting diodes, lasers, and light‐emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light‐emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A^?1 have been achieved. Although perovskite light‐emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light‐emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower‐dimensionality layered and three‐dimensional perovskites, nanostructures, charge‐transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light‐emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light‐emitting devices.     

Mixed Lead–Tin Halide Perovskites for Efficient and Wavelength‐Tunable Near‐Infrared Light‐Emitting Diodes

Near‐infrared (NIR) light‐emitting diodes (LEDs), with emission wavelengths between 800 and 950 nm, are useful for various applications, e.g., night‐vision devices, optical communication, and medical treatments. Yet, devices using thin film materials like organic semiconductors and lead based colloidal quantum dots face certain fundamental challenges that limit the improvement of external quantum efficiency (EQE), making the search of alternative NIR emitters important for the community. In this work, efficient NIR LEDs with tunable emission from 850 to 950 nm, using lead–tin (Pb‐Sn) halide perovskite as emitters are demonstrated. The best performing device exhibits an EQE of 5.0% with a peak emission wavelength of 917 nm, a turn‐on voltage of 1.65 V, and a radiance of 2.7 W Sr^?1 m^?2 when driven at 4.5 V. The emission spectra of mixed Pb‐Sn perovskites are tuned either by changing the Pb:Sn ratio or by incorporating bromide, and notably exhibit no phase separation during device operation. The work demonstrates that mixed Pb‐Sn perovskites are promising next generation NIR emitters.     

Highly Efficient Spectrally Stable Red Perovskite Light‐Emitting Diodes

Perovskite light‐emitting diodes (LEDs) have recently attracted great research interest for their narrow emissions and solution processability. Remarkable progress has been achieved in green perovskite LEDs in recent years, but not blue or red ones. Here, highly efficient and spectrally stable red perovskite LEDs with quasi‐2D perovskite/poly(ethylene oxide) (PEO) composite thin films as the light‐emitting layer are reported. By controlling the molar ratios of organic salt (benzylammonium iodide) to inorganic salts (cesium iodide and lead iodide), luminescent quasi‐2D perovskite thin films are obtained with tunable emission colors from red to deep red. The perovskite/polymer composite approach enables quasi‐2D perovskite/PEO composite thin films to possess much higher photoluminescence quantum efficiencies and smoothness than their neat quasi‐2D perovskite counterparts. Electrically driven LEDs with emissions peaked at 638, 664, 680, and 690 nm have been fabricated to exhibit high brightness and external quantum efficiencies (EQEs). For instance, the perovskite LED with an emission peaked at 680 nm exhibits a brightness of 1392 cd m^?2 and an EQE of 6.23%. Moreover, exceptional electroluminescence spectral stability under continuous device operation has been achieved for these red perovskite LEDs.     

Efficient and Tunable Electroluminescence from In Situ Synthesized Perovskite Quantum Dots

Semiconductor quantum dots (QDs) are among the most promising next‐generation optoelectronic materials. QDs are generally obtained through either epitaxial or colloidal growth and carry the promise for solution‐processed high‐performance optoelectronic devices such as light‐emitting diodes (LEDs), solar cells, etc. Herein, a straightforward approach to synthesize perovskite QDs and demonstrate their applications in efficient LEDs is reported. The perovskite QDs with controllable crystal sizes and properties are in situ synthesized through one‐step spin‐coating from perovskite precursor solutions followed by thermal annealing. These perovskite QDs feature size‐dependent quantum confinement effect (with readily tunable emissions) and radiative monomolecular recombination. Despite the substantial structural inhomogeneity, the in situ generated perovskite QDs films emit narrow‐bandwidth emission and high color stability due to efficient energy transfer between nanostructures that sweeps away the unfavorable disorder effects. Based on these materials, efficient LEDs with external quantum efficiencies up to 11.0% are realized. This makes the technologically appealing in situ approach promising for further development of state‐of‐the‐art LED systems and other optoelectronic devices.     

Strategies to Improve Luminescence Efficiency of Metal‐Halide Perovskites and Light‐Emitting Diodes

Metal‐halide perovskites (MHPs) are well suited to be vivid natural color emitters due to their superior optical and electrical properties, such as narrow emission linewidths, easily and widely tunable emission wavelengths, low material cost, and high charge carrier mobility. Since the first development of MHP light‐emitting diodes (PeLEDs) in 2014, many researchers have tried to understand the properties of MHP emitters and the limitations to luminescence efficiency (LE) of PeLEDs, and have devoted efforts to increase the LE of MHP emitters and PeLEDs. Within three and half years, PeLEDs have shown rapidly increased LE from external quantum efficiency ≈0.1% to ≈14.36%. Herein, the factors that limit the LE of PeLEDs are reviewed; the factors are characterized into the following groups: i) photophysical properties of MHP crystals, ii) morphological factors of MHP layers, and iii) problems caused by device architectures. Then, the strategies to overcome those luminescence‐limiting factors in MHP emitters and PeLEDs are critically evaluated. Finally, research directions to further increase the LE of MHP emitters and the potential of MHPs as a core component in next‐generation displays and solid‐state lightings are suggested.     

High‐Efficiency Solution‐Processed Inorganic Metal Halide Perovskite Light‐Emitting Diodes

This paper reports highly bright and efficient CsPbBr₃ perovskite light‐emitting diodes (PeLEDs) fabricated by simple one‐step spin‐coating of uniform CsPbBr₃ polycrystalline layers on a self‐organized buffer hole injection layer and stoichiometry‐controlled CsPbBr₃ precursor solutions with an optimized concentration. The PeLEDs have maximum current efficiency of 5.39 cd A^?1 and maximum luminance of 13752 cd m^?2. This paper also investigates the origin of current hysteresis, which can be ascribed to migration of Br^? anions. Temperature dependence of the electroluminescence (EL) spectrum is measured and the origins of decreased spectrum area, spectral blue‐shift, and linewidth broadening are analyzed systematically with the activation energies, and are related with Br^? anion migration, thermal dissociation of excitons, thermal expansion, and electron–phonon interaction. This work provides simple ways to improve the efficiency and brightness of all‐inorganic polycrystalline PeLEDs and improves understanding of temperature‐dependent ion migration and EL properties in inorganic PeLEDs.