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.     

Surface‐Plasmon‐Enhanced Perovskite Light‐Emitting Diodes

Perovskite light‐emitting diodes (PeLEDs) have attracted considerable attention because of their potential in display and lighting applications. To promote commercialization of PeLEDs, it is important to improve the external quantum efficiency of the devices, which depends on their internal quantum efficiency (IQE) and light extraction efficiency. Optical simulations have revealed that 20–50% of the light generated in the device will be lost to surface plasmon (SP) modes formed in the metal/dielectric interfaces. Therefore, extracting the optical energy in SP modes to the air will greatly increase the light extraction efficiency of PeLEDs. In addition, the SPs can accelerate radiative recombination of the emitter via near‐field effects. Thus, the IQE of a PeLED can also be enhanced by SP manipulation. In this review, first, general concepts of the SPs and how they can enhance the efficiency of LEDs are introduced. Then recent progresses in SP‐enhanced emission of perovskite films and LEDs are systematically reviewed. After that, the challenges and opportunities of the SP‐enhanced PeLEDs are shown, followed by an outlook of further development of the SPs in perovskite optoelectronic devices.     

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.     

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.     

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.     

Efficient Red Perovskite Light‐Emitting Diodes Based on Solution‐Processed Multiple Quantum Wells

This paper reports a facile and scalable process to achieve high performance red perovskite light‐emitting diodes (LEDs) by introducing inorganic Cs into multiple quantum well (MQW) perovskites. The MQW structure facilitates the formation of cubic CsPbI₃ perovskites at low temperature, enabling the Cs‐based QWs to provide pure and stable red electroluminescence. The versatile synthesis of MQW perovskites provides freedom to control the crystallinity and morphology of the emission layer. It is demonstrated that the inclusion of chloride can further improve the crystallization and consequently the optical properties of the Cs‐based MQW perovskites, inducing a low turn‐on voltage of 2.0 V, a maximum external quantum efficiency of 3.7%, a luminance of ≈440 cd m^?2 at 4.0 V. These results suggest that the Cs‐based MQW LED is among the best performing red perovskite LEDs. Moreover, the LED device demonstrates a record lifetime of over 5 h under a constant current density of 10 mA cm^?2. This work suggests that the MQW perovskites is a promising platform for achieving high performance visible‐range electroluminescence emission through high‐throughput processing methods, which is attractive for low‐cost lighting and display applications.     

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.     

Optimization of Low‐Dimensional Components of Quasi‐2D Perovskite Films for Deep‐Blue Light‐Emitting Diodes

Compared to efficient green and near‐infrared light‐emitting diodes (LEDs), less progress has been made on deep‐blue perovskite LEDs. They suffer from inefficient domain [various number of PbX₆^? layers (n)] control, resulting in a series of unfavorable issues such as unstable color, multipeak profile, and poor fluorescence yield. Here, a strategy involving a delicate spacer modulation for quasi‐2D perovskite films via an introduction of aromatic polyamine molecules into the perovskite precursor is reported. With low‐dimensional component engineering, the n₁ domain, which shows nonradiative recombination and retarded exciton transfer, is significantly suppressed. Also, the n₃ domain, which represents the population of emission species, is remarkably increased. The optimized quasi‐2D perovskite film presents blue emission from the n₃ domain (peak at 465 nm) with a photoluminescence quantum yield (PLQY) as high as 77%. It enables the corresponding perovskite LEDs to deliver stable deep‐blue emission (CIE (0.145, 0.05)) with an external quantum efficiency (EQE) of 2.6%. The findings in this work provide further understanding on the structural and emission properties of quasi‐2D perovskites, which pave a new route to design deep‐blue‐emissive perovskite materials.     

Degradation Mechanisms in Small‐Molecule and Polymer Organic Light‐Emitting Diodes

Degradation in organic light‐emitting diodes (OLEDs) is a complex problem. Depending upon the materials and the device architectures used, the degradation mechanism can be very different. In this Progress Report, using examples in both small molecule and polymer OLEDs, the different degradation mechanisms in two types of devices are examined. Some of the extrinsic and intrinsic degradation mechanisms in OLEDs are reviewed, and recent work on degradation studies of both small‐molecule and polymer OLEDs is presented. For small‐molecule OLEDs, the operational degradation of exemplary fluorescent devices is dominated by chemical transformations in the vicinity of the recombination zone. The accumulation of degradation products results in coupled phenomena of luminance‐efficiency loss and operating‐voltage rise. For polymer OLEDs, it is shown how the charge‐transport and injection properties affect the device lifetime. Further, it is shown how the charge balance is controlled by interlayers at the anode contact, and their effects on the device lifetime are discussed.