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Quasi‐two‐dimensional (quasi‐2D) perovskites are emerging as efficient emitters in blue perovskite light‐emitting diodes (PeLEDs), while the imbalanced crystallization of the halide‐mixed system limits further improvements in device performance. The rapid crystallization caused by Cl doping produces massive defects at the interface, leading to aggravated non‐radiative recombination. Meanwhile, unmanageable perovskite crystallization is prone to facilitate the formation of nonuniform low‐dimensional phases, which results in energy loss during the exciton transfer process. Here, we propose a multifunctional interface engineering for nucleation and phase regulation by incorporating the zwitterionic additive potassium sulfamate into the hole transport layer. By using potassium ions (K+) as heterogeneous nucleation seeds, finely controlled growth of interfacial K+‐guided grains is achieved. The sulfamate ions can simultaneously regulate the phase distribution and passivate defects through coordination interactions with undercoordinated lead atoms. Consequently, such synergistic effect constructs quasi‐2D blue perovskite films with smooth energy landscape and reduced trap states, leading to pure‐blue PeLEDs with a maximum external quantum efficiency (EQE) of 17.32 %, spectrally stable emission at 478 nm and the prolonged operational lifetime. This work provides a unique guide to comprehensively regulate the halide‐mixed blue perovskite crystallization by manipulating the characteristics of grain‐growth substrate. [ABSTRACT FROM AUTHOR]

The development of perovskite light‐emitting diodes (PeLEDs) with both high efficiency and excellent stability remains challenging. Herein, a strong correlation between the lattice strain in perovskite films and the stability of resulting PeLEDs is revealed. Based on high‐efficiency PeLEDs, the device lifetime is optimized by rationally tailoring the lattice strain in perovskite films. A PeLED with a high peak external quantum efficiency of 18.2% and a long lifetime of 151 h (T70, under a current density of 20 mA cm−2) is realized with a minimized lattice strain in the perovskite film. In addition, an increase in the lattice strain is found during the long‐time device stability test, indicating that the degradation of the local perovskite lattice structure could be one of the degradation mechanisms for long‐term stable PeLEDs. [ABSTRACT FROM AUTHOR]

Metal halide perovskite materials have demonstrated significant potential in various optoelectronic applications, such as photovoltaics, light emitting diodes, photodetectors, and lasers. However, the stability issues of perovskite materials continue to impede their widespread use. Many studies have attempted to understand the complex degradation mechanism and dynamics of these materials. Among them, in situ and/or operando approaches have provided remarkable insights into the degradation process by enabling precise control of degradation parameters and real-time monitoring. In this review, we focus on these studies utilizing in situ and operando approaches and demonstrate how these techniques have contributed to reveal degradation details, including structural, compositional, morphological, and other changes. We explore why these two approaches are necessary in the study of perovskite degradation and how they can be achieved by upgrading the corresponding ex situ techniques. With recent stability improvements of halide perovskite using various methods (compositional engineering, surface engineering, and structural engineering), the degradation of halide perovskite materials is greatly retarded. However, these improvements may turn into new challenges during the investigation into the retarded degradation process. Therefore, we also highlight the importance of enhancing the sensitivity and probing range of current in situ and operando approaches to address this issue. Finally, we identify the challenges and future directions of in situ and operando approaches in the stability research of halide perovskites. We believe that the advancement of in situ and operando techniques will be crucial in supporting the journey toward enhanced perovskite stability. [ABSTRACT FROM AUTHOR]

Perovskite light‐emitting didoes (PeLEDs) have shown considerable potential in solution‐processable display applications. However, the performance of blue PeLEDs in terms of efficiency and stability hinders their practicality on account of severe trap‐mediated nonradiative recombination losses and halide phase segregation. To ameliorate these issues, mixed‐halide sky‐blue perovskite materials are strategically modulated through crystal defect passivation with a trifurcate isocyanate oligomer, which leads to the synergistical suppression of charge trap density and halide ion migration. The proposed approach enables the performance improvement for sky‐blue PeLEDs, exhibiting a peak external quantum efficiency of 14.82% and spectrally stable emission at 487 nm. In addition, prolonged operational lifetime and enhanced capability of moisture resistance are achieved simultaneously, approaching a half‐lifetime of ≈2900 s at an initial brightness of 178 cd m–2. [ABSTRACT FROM AUTHOR]

Quasi‐2D metal halide perovskite light emitting diodes (PeLEDs) have attracted a lot of attentions in recent years, while their potential applications in displays and lighting are limited by the device stability. Although defect passivation in PeLEDs is an effective method to ameliorate the unstable problem, the underlying mechanisms need to be further explored. Herein, organic spacer cations with different charge distributions and formation energies in quasi‐2D CsPbBr3 perovskites are utilized to unravel the defect passivation mechanisms, including phenylmethanamine, 2‐phenylethanamine bromide, and 4‐phenylbutylammonium. The experimental findings and density functional theory calculation reveal that the defect passivation occurs by the electrostatic interaction between defective PbBr64− octahedrons and proper organic spacer cations during the annealing process, particularly at the grain boundaries. The thermal stability of the perovskite films and device performance are improved after the effective defect passivation process. The exploration of the defect passivation process in perovskites will be beneficial to the development of high‐performance PeLEDs. [ABSTRACT FROM AUTHOR]

Regardless of the rapid advance on perovskite light‐emitting diodes (PeLEDs), the lack of long‐term operational stability hinders the practicality of this technology. Particularly, thermal management is indispensable to control the Joule heating induced by charge transport and parasitic re‐absorption of internally confined photons. Herein, a synergetic device architecture is proposed for minimizing the optical energy losses in PeLEDs toward high efficiency and long lifetime. By adopting a carefully modified perovskite emitter in combination with an improved light outcoupling structure, red PeLEDs emitting at 666 nm achieve a peak external quantum efficiency of 21.2% and an operational half‐lifetime of 4806.7 h for an initial luminance of 100 cd m‐2. The enhanced light extraction from trapped modes can efficiently reduce the driving current and suppress optical energy losses in PeLEDs, which in turn ameliorate the heat‐induced device degradation during operation. This work paves the way toward high‐performance PeLEDs for display and lighting applications in the future. [ABSTRACT FROM AUTHOR]

Efficient and stable blue emission of perovskite light‐emitting diodes (PeLEDs) is a requisite toward their potential applications in full‐color displays and solid‐state lighting. Rational manipulation over the entire electroluminescence process is promising to break the efficiency limit of blue PeLEDs. Herein, a facile device architecture is proposed to achieve efficient blue PeLEDs for simultaneously reducing the energetic loss during electron‐photon conversion and boosting the light outcoupling. Effective interfacial engineering is employed to manipulate the perovskite crystallization nucleation, enabling highly compact perovskite nanocrystal assemblies and suppressing the trap‐induced carrier losses by means of interfacial hydrogen bonding interactions. This strategy contributes to a high external quantum efficiency (EQE) of 12.8% for blue PeLEDs emitting at 486 nm as well as improved operational stability. Moreover, blue PeLEDs reach a peak EQE of 16.8% with the incorporation of internal outcoupling structures for waveguided light, which can be further raised to 27.5% by integrating a lens‐based structure for substrate‐mode light. These results verify the validity of this strategy in producing efficient and stable blue PeLEDs for practical applications. [ABSTRACT FROM AUTHOR]

While tremendous progress has recently been made in perovskite light‐emitting diodes (PeLEDs), large‐area blue devices feature inferior performance due to uneven morphologies and vast defects in the solution‐processed perovskite films. To alleviate these issues, a facile and reliable interface engineering scheme is reported for manipulating the crystallization of perovskite films enabled by a multifunctional molecule 2‐amino‐1,3‐propanediol (APDO)‐triggered "anchoring effect" at the grain‐growth interface. Sky‐blue perovskite films with large‐area uniformity and low trap states are obtained, showing the distinctly improved radiative recombination and hole‐transport capability. Based on the APDO‐induced interface engineering, synergistical boost in device performance is achieved for large‐area sky‐blue PeLED (measuring at 100 mm2) with a peak external quantum efficiency (EQE) of 9.2% and a highly prolonged operational lifetime. A decent EQE up to 6.1% is demonstrated for the largest sky‐blue device emitting at 400 mm2. [ABSTRACT FROM AUTHOR]

Inkjet printing is a powerful technology for realizing high‐density pixelated perovskite light‐emitting diodes (PeLEDs). However, the coffee‐stain effect in the inkjet printing process often leads to uneven thickness and poor crystallization of printed perovskite features, which deteriorates the performance of PeLEDs. Here, a strategy is developed to suppress the coffee‐stain effect via enhancing Marangoni flow strength. An interfacial poly(vinylpyrrolidone) (PVP) layer is incorporated to tune the surface tension of the underlying hole transport layer (HTL) and enhance the perovskite crystallization. The substrate temperature is also carefully controlled to tune the printing solvent evaporation rate rationally. By optimizing the thickness of the PVP layer and the temperature of the printing stage, the coffee‐stain effect is dramatically restrained. In addition, the interfacial insulating PVP layers play a positive role in suppressing leakage current level of PeLEDs by avoiding any direct electrical contact between HTL and electron transporting layer. Finally, an inkjet‐printed PeLED with a brightness of 3640 cd m–2 and external quantum efficiency of 9.0% is achieved. This work highlights the availability of inkjet‐printing technology for fabricating patterned PeLEDs in information display applications. [ABSTRACT FROM AUTHOR]

Perovskite light‐emitting diodes (PeLEDs) are emerging candidates for the applications of solution‐processed full‐color displays. However, the device performance of deep‐blue PeLED still lags far behind that of their red and green counterparts, which is largely limited by low external quantum efficiency (EQE) and poor operational stability. Here, a facile and reliable crystallization strategy for perovskite grains is proposed, with improved deep‐blue emission through rational interfacial engineering. By modifying the substrate with potassium cation (K+) as the supplier of heterogeneous nucleation seeds, the interfacial K+‐guided grain growth is realized for well‐packed perovskite assemblies with high surface coverage and the controlled crystal orientation, leading to the enhanced radiative recombination and hole‐transport capabilities. Synergistical boost in device performance is achieved for deep‐blue PeLEDs emitting at 469 nm with a peak EQE of 4.14%, a maximum luminance of 451 cd m–2, and spectrally stable color coordinates of (0.125, 0.076) that matches well with the National Television System Committee (NTSC) standard blue. [ABSTRACT FROM AUTHOR]

Deep-Blue Emission: Interfacial Potassium-Guided Grain Growth for Efficient Deep-Blue Perovskite Light-Emitting Diodes (Adv. Funct. Keywords: crystallization manipulation; deep-blue emission; interface engineering; perovskite light-emitting diodes EN crystallization manipulation deep-blue emission interface engineering perovskite light-emitting diodes 1 1 1 02/05/21 20210203 NES 210203 In article number 2006736, Yan-Qing Li, Jian-Xin Tang, and co-workers demonstrate a facile and reliable crystallization strategy for interfacial potassium-guided perovskite grain growth, leading to efficient deep-blue light-emitting diodes with an external quantum efficiency of 4.14% and stable color coordinates of (0.125, 0.076). Crystallization manipulation, deep-blue emission, interface engineering, perovskite light-emitting diodes. [Extracted from the article]

Quasi‐2D Ruddlesden–Popper (RP) perovskites with quantum‐size‐tuned nanoplatelet crystallites are particularly attractive for light‐emitting diode (LED) applications because of their excellent charge transport, bandgap tunability, and narrow emission peaks. Favorable energy cascade structure in 2D RP perovskites can funnel the photoexcitation from large‐bandgap nanoplatelets to the lowest bandgap ones, which promises efficient radiative recombination. However, how to rationally control the nanoplatelet distribution as well as the crystallization characteristics to ensure efficient energy transfer and charge transport in perovskite films is still challenging. Here, a simple path to facilely tune the nanoplatelet distribution as well as the crystal orientation via carefully controlling postannealing condition is provided. With optimizing the thermal annealing time, compact and flat perovskite films with high photoluminescence quantum yield are obtained. Based on the optimized perovskite films, green LED with a current efficiency of 43.7 cd A−1, corresponding to an external quantum efficiency of 13.9%, is achieved. This work provides a simple path to target highly efficient perovskite LED devices. Efficient perovskite light‐emitting diodes (LEDs) are achieved via tuning nanoplatelet distribution and the crystallinity orientation of quasi‐2D perovskite films. By using the optimized perovskite film to build LED devices, a current efficiency of 43.7 cd A−1 and an external quantum efficiency of 13.9% are achieved, which are the one of the impressive performances in this field. [ABSTRACT FROM AUTHOR]