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Despite their low exciton-binding energies, metal halide perovskites are extensively studied as light-emitting materials owing to narrow emission with high color purity, easy/wide color tunability, and high photoluminescence quantum yields. To improve the efficiency of perovskite light-emitting diodes (PeLEDs), much effort has been devoted to controlling the emitting layer morphologies to induce charge confinement and decrease the nonradiative recombination. The interfaces between the emitting layer and charge transporting layer (CTL) are vulnerable to various defects that deteriorate the efficiency and stability of the PeLEDs. Therefore, the establishment of multifunctional CTLs that can improve not only charge transport but also critical factors that influence device performance, such as defect passivation, morphology/phase control, ion migration suppression, and light outcoupling efficiency, are highly required. Herein, the fundamental limitations of perovskites as emitters (i.e., defects, morphological and phase instability, high refractive index with poor outcoupling) and the recent developments with regard to multifunctional CTLs to compensate such limitations are summarized, and their device applications are also reviewed. Finally, based on the importance of multifunctional CTLs, the outlook and research prospects of multifunctional CTLs for the further improvement of PeLEDs are discussed.

In this study, uniform Cs distribution in an organometal halide perovskite (OHP) film was achieved via sequential deposition method entailing the dissolution of Cs compounds in dimethyl formamide (DMF) with inorganic components, as opposed to using isopropyl alcohol with organic components, and the thermal stability and crystallinity of the OHP film were enhanced by improving the structural stability through Cs incorporation. Additionally, the device performance and thermal stability of OHP solar cells were enhanced by Cs incorporation, which led to fewer defect sites and the suppression of defect generation in OHP films, as confirmed by optical and electrical analysis, improving the overall film quality. The sequential deposition method was more amenable to scaling up than the anti-solvent assisted one-step spin-casting method, as demonstrated by the sequential deposition of the OHP film uniformly over a substrate with size of 8 cm × 8 cm. The uniformly sequentially deposited OHP film was used to create a large-area 1 cm2 OHP solar cell, which exhibited a high power conversion efficiency (PCE) of 16.77%. Further scalability of the sequentially deposited OHP solar cell was confirmed by highly uniform device performances by three cells on a single substrate with a negligible PCE standard deviation of 0.94%.

Charge carrier confinement and defect passivation are the main research struggle for the development of efficient perovskite light-emitting diodes (PeLEDs). In this study, we report a green-emitting PeLED by adding an anionic conjugated polyelectrolyte containing tetraethylammonium counter ions (MPS2-TEA) into formamidinium lead tribromide quasi-2D perovskites. X-ray diffraction shows that perovskite films with MPS2-TEA are more randomly oriented compared to the films without MPS2-TEA. Interestingly, the incorporation of MPS2-TEA reduces the roughness of surfaces and grain sizes of the perovskite films. The increases in photoluminescence intensity (by three times) and lifetime (18.11 vs. 9.81 ns) of perovskite films with MPS2-TEA compared to those of the pristine films suggest improved radiative recombination by intermixing perovskite with MPS2-TEA. Defect density in perovskite films with MPS2-TEA is significantly suppressed owing to defect passivation at the grain boundaries by MPS2-TEA. The PeLED with MPS2-TEA shows a significantly improved external quantum efficiency of up to 15.47%, the current efficiency of 69.02 cd/A, and maximum luminance of 12,252 cd/m 2, compared to a device without MPS2-TEA.

A series of anionic conjugated polyelectrolytes (CPEs) is synthesized based on poly(fluorene-co-phenylene) by varying the side-chain ionic density from two to six per repeat units (MPS2-TMA, MPS4-TMA, and MPS6-TMA). The effect of MPS2, 4, 6-TMA as interlayers on top of a hole-extraction layer of poly(bis(4-phenyl)-2,4,6-trimethylphenylamine (PTAA) is investigated in inverted perovskite solar cells (PeSCs). Owing to the improved wettability of perovskites on hydrophobic PTAA with the CPEs, the PeSCs with CPE interlayers demonstrate a significantly enhanced device performance, with negligible device-to-device dependence relative to the reference PeSC without CPEs. By increasing the ionic density in the MPS-TMA interlayers, the wetting, interfacial defect passivation, and crystal growth of the perovskites are significantly improved without increasing the series resistance of the PeSCs. In particular, the open-circuit voltage increases from 1.06 V for the PeSC with MPS2-TMA to 1.11 V for the PeSC with MPS6-TMA. The trap densities of the PeSCs with MPS2,4,6-TMA are further analyzed using frequency-dependent capacitance measurements. Finally, a large-area (1 cm2 ) PeSC is successfully fabricated with MPS6-TMA, showing a power conversion efficiency of 18.38% with negligible hysteresis and a stable power output under light soaking for 60 s.

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.

Metal halide perovskites (MHPs) have emerged as promising materials for light‐emitting diodes owing to their narrow emission spectrum and wide range of color tunability. However, the low exciton binding energy in MHPs leads to a competition between the trap‐mediated nonradiative recombination and the bimolecular radiative recombination. Here, efficient and stable green emissive perovskite light‐emitting diodes (PeLEDs) with an external quantum efficiency of 14.6% are demonstrated through compositional, dimensional, and interfacial modulations of MHPs. The interfacial energetics and optoelectronic properties of the perovskite layer grown on a nickel oxide (NiOx) and poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate hole injection interfaces are investigated. The better interface formed between the NiOx/perovskite layers in terms of lower density of traps/defects, as well as more balanced charge carriers in the perovskite layer leading to high recombination yield of carriers are the main reasons for significantly improved device efficiency, photostability of perovskite, and operational stability of PeLEDs.

Metal halide perovskites (MHPs) have emerged as promising emitters because of their excellent optoelectronic properties, including high photoluminescence quantum yields (PLQYs), wide-range color tunability, and high color purity. However, a fundamental limitation of MHPs is their low exciton binding energy, which results in a low radiative recombination rate and the dependence of PLQY on the excitation intensity. Under the operating conditions of light-emitting diodes (LEDs), the injected current densities are typically lower than the trap density, leading to a low actual PLQY. Moreover, the defects not only initiate the decomposition of MHPs caused by extrinsic factors, but also intrinsically stimulate ion migration across the interface and lead to the corrosion of electrodes due to interaction between those electrodes, even under inert conditions. The passivation of defects has proven to be effective for mitigating the effects of defects in MHPs. Herein, the origins and theoretical calculations of the defect tolerance in MHPs and the impact of defects on both the performance and stability of perovskite LEDs are reviewed. The passivation methods and materials for MHP bulk films and nanocrystals are discussed in detail. Based on the currently reported advances, specific requirements and future research directions for display applications are suggested.

Conjugated polyelectrolytes (CPEs) with π-delocalized main backbones and ionic pendant groups are intensively studied as interfacial layers for efficient polymer-based optoelectronic devices (POEDs) because they facilitate facile control of charge injection/extraction barriers. Here, a simple and effective method of performing precise interfacial energy level adjustment is presented by employing CPEs with different thicknesses and various ion densities under electric poling to realize efficient charge injection/extraction of POEDs. The effects of the CPE ion densities and electric (positive or negative) poling on the energy level tuning process are investigated by measuring the open-circuit voltages and current densities of devices with the structure indium tin oxide/zinc oxide/CPE/organic active layer/molybdenum oxide/gold while changing the CPE film thickness. The performances of inverted polymer light-emitting diodes and inverted polymer solar cells are remarkably improved by precisely controlling the interfacial energy level matching using optimum CPE conditions.