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Perovskite solar cells (PSCs) have experienced exceptional development in recent years, due to their outstanding photoelectronic properties and low‐cost solution processing. Many state‐of‐the‐art PSC designs have been effectively demonstrated using a stacked 3D perovskite/2D perovskite heterostructure, yet limitations arise due to the low conductivity of the 2D perovskite, the hidden buried interface of 3D perovskite, and halide ion migration within 3D/2D PSC device under operational bias. Here, these limitations are overcome by developing a novel and universal post‐synthetic metal (Zn2+) doping strategy and realizing 3D/2D PSCs with superior efficiency and stability. Informed by ab initio calculations and synchrotron fine structure experiments, it is revealed that the introduced zinc ions are energetically favored at interstitial crystal sites, subsequently hindering the migration of halide ions and producing a beneficial shift toward a more n‐type character in the buried 3D perovskite interface. Combined with extensive photophysical characterization, the Zn2+‐modified 3D/2D perovskite thin film is shown to strongly recover its photo‐carrier conductivity compared with the 3D/2D perovskite film, boosting the efficiency (22.90%) of PSCs while exhibiting improved humidity and operational stability. [ABSTRACT FROM AUTHOR]

Metal halide perovskite light‐emitting diodes (PeLEDs) are expected to be the next‐generation display technology due to their unique optoelectronic properties. Currently, the external quantum efficiencies of PeLEDs based on solution‐processed fabrication methods already exceed 20%. However, there are still many challenges existing in solution‐based PeLEDs that inhibit their commercialization. Recently, vacuum deposition techniques of perovskites have drawn much attention because of the ability to grow dense and uniform large‐area perovskite films with precisely controlled thickness, which is compatible with state‐of‐the‐art organic LED manufacturing processes. Despite the promising prospects of vacuum‐based PeLEDs, some challenges remain to be addressed to achieve PeLEDs with both high efficiency and high stability that are required for practical applications such as active‐matrix displays. This requires precise control of the film morphology, composition, and interface during the deposition process through fine‐tuning of the substrate temperature, deposition rate, vacuum level, precursor formulation, and post‐treatment conditions. In this review, it focuses on the key requirements for vacuum‐processed PeLEDs, highlights the recent advances in materials and devices of PeLEDs, and emphasize vacuum evaporation methods as well as the corresponding device performance. Possible approaches to improve the efficiency and the long‐term operational stability of vacuum‐processed PeLEDs are discussed. [ABSTRACT FROM AUTHOR]

Self‐assembly of nanocrystals into controlled structures while uncompromising their properties is one of the key steps in optoelectronic device fabrication. Herein, zigzag CsPbBr3 perovskite nanocrystals are demonstrated with a precise number of components with nanocube morphology, these can be successfully obtained through a dipole‐induced self‐assembly process. The addition of a trace amount of deionized water facilitates the transfer from CsPbBr3 nanocubes to intermediates of CsPb2Br5 and Cs3In2Br9, which then fastly release reaction monomers leading to further homogenous nucleation of CsPbBr3 nanocubes, followed by the formation of zigzag CsPbBr3 nanocrystals through a dipole‐induced self‐assembly process. Dipole moment along <110> axis is found to be the driving force for the assembly of nanocubes into zigzag nanocrystals. The zigzag CsPbBr3 nanocrystals exhibit desirable optical properties comparable to their nanocube counterparts and offer advantages for amplified spontaneous emission and lasing applications with low pump thresholds of 3.1 and 6.02 µJ cm−2, respectively. This study not only develops a strategy for producing highly controlled zigzag perovskite nanocrystals and provides insights on the dipole‐induced self‐assembly mechanisms, but also opens an avenue for their application in lasing. [ABSTRACT FROM AUTHOR]

Quasi‐2D Ruddlesden‐Popper perovskites receive tremendous attention for application in light‐emitting diodes (LEDs). However, the role of organic ammonium spacers on perovskite film has not been fully‐understood. Herein, a spacer cation assisted perovskite nucleation and growth strategy, where guanidinium (GA+) spacer is introduced into the perovskite precursor and at the interface between the hole transport layer (HTL) and the perovskite, to achieve dense and uniform perovskite films with enhanced optical and electrical performance is developed. A thin GABr interface pre‐formed on HTL provides more nucleation sites for perovskite crystal; while the added GA+ in perovskite reduces the crystallization rate due to strong hydrogen bonding interacts with intermediates, which promotes the growth of enhanced‐quality quasi‐2D perovskite films. The ionized ammonium group (NH3+) of GA+ also favors formation of polydisperse domain distribution, and amine or imine (NH2 or NH) group interact with perovskite defects through coordination bonding. The spacer cation assisted nucleation and growth strategy is advantageous for producing efficient and high‐luminance perovskite LEDs, with a peak external quantum efficiency of over 20% and a luminance up to 100 000 cd m−2. This work can inform and underpin future development of high‐performance perovskite LEDs with concurrent high efficiency and brightness. [ABSTRACT FROM AUTHOR]

Lead halide perovskite nanocrystals (PeNCs) are promising materials for applications in optoelectronics. However, their environmental instability remains to be addressed to enable their advancement into industry. Here the development of a novel synthesis method is reported for monodispersed PeNCs coated with all inorganic shell of cesium lead bromide (CsPbBr3) grown epitaxially on the surface of formamidinium lead bromide (FAPbBr3) NCs. The formed FAPbBr3/CsPbBr3 NCs have photoluminescence in the visible range 460–560 nm with narrow emission linewidth (20 nm) and high optical quantum yield, photoluminescence quantum yield (PLQY) up to 93%. The core/shell perovskites have enhanced optical stability under ambient conditions (70 d) and under ultraviolet radiation (50 h). The enhanced properties are attributed to overgrowth of FAPbBr3 with all‐inorganic CsPbBr3 shell, which acts as a protective layer and enables effective passivation of the surface defects. The use of these green‐emitting core/shell FAPbBr3/CsPbBr3 NCs is demonstrated in light‐emitting diodes (LEDs) and significant enhancement of their performance is achieved compared to core only FAPbBr3‐LEDs. The maximum current efficiency observed in core/shell NC LED is 19.75 cd A‐1 and the external quantum efficiency of 8.1%, which are approximately four times and approximately eight times higher, respectively, compared to core‐only devices. [ABSTRACT FROM AUTHOR]