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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]

Core–shell perovskite nanocrystals (NCs) have emerged as a promising class of materials for optoelectronic applications due to their unique properties and stability. Although much research has been conducted on the shell growth mechanism and properties of the core–shell NCs, little is known about the role of shell thickness in determining their optical properties. Herein, a heteroepitaxial method is employed to prepare a series of core–shell FAPbBr3/CsPbBr3 NCs with different shell thicknesses. Through temperature‐dependent photoluminescence measurement, it is found that the electronic structure of core–shell FAPbBr3/CsPbBr3 NCs evolves from quasi‐type‐II to type‐I with the increase in shell thickness. This abnormal transition can be attributed to the thickened gradient alloy layer FA1‐xCsxPbBr3, which effectively relieves the lattice mismatch and releases strain in the NCs, resulting in variations in the bandgap between the core and the shell. Furthermore, the biexciton Auger lifetimes in these samples exhibit a non‐monotonic dependence on shell thickness, indicating the electronic structure transition. These results provide valuable insights into the relationship between shell thickness, electronic structure, and optical properties in core–shell perovskite NCs, which may offer guidance for the design of high‐performance optoelectronic devices. [ABSTRACT FROM AUTHOR]

The facile oxidation of Sn2+ to Sn4+ poses an inherent challenge that limits the efficiency and stability of tin‐lead mixed (Sn−Pb) perovskite solar cells (PSCs) and all‐perovskite tandem devices. In this work, we discover the sustainable redox reactions enabling self‐healing Sn−Pb perovskites, where their intractable oxidation degradation can be recovered to their original state under light soaking. Quantitative and operando spectroscopies are used to investigate the redox chemistry, revealing that metallic Pb0 from the photolysis of perovskite reacts with Sn4+ to regenerate Pb2+ and Sn2+ spontaneously. Given the sluggish redox reaction kinetics, V3+/V2+ ionic pair is designed as an effective redox shuttle to accelerate the recovery of Sn−Pb perovskites from oxidation. The target Sn−Pb PSCs enabled by V3+/V2+ ionic pair deliver an improved power conversion efficiency (PCE) of 21.22 % and excellent device lifespan, retaining nearly 90 % of its initial PCE after maximum power point tracking under light for 1,000 hours. [ABSTRACT FROM AUTHOR]

Performance of blue solution‐processed perovskite light‐emitting diodes (LEDs) is limited by availability of blue perovskite materials. Herein, 4‐(trifluoromethyl)benzoyl ammonium bromide (4‐TMBABr) is used with abundant NH and CO groups to passivate the defects and produce highly stable PEAxPA2‐x(CsPbBr3)n‐1PbBr4 perovskites for blue LED applications. The NH group in the 4‐TMBABr suppresses the Br‐ion mismatch through hydrogen bonds (N‐H···Br) and CO group coordinates the unsaturated lead dangling bonds (CO:Pb). The effective defect passivation by 4‐TMBABr reduces the nonradiative recombination in the perovskite films, hence enhancing its optical performance. In the LED structure, the sodium bis(trifluoromethanesulfonyl)imide (SBTI) modified NiOx films are used to improve the hole transport and to inhibit the fluorescence quenching of the perovskite layer. The dual‐defect manipulation strategy is advantageous for producing efficient and spectrally stable blue perovskite LEDs, and the authors demonstrate an LED with maximum luminance of 1094 cd m−2 and external quantum efficiency of 10.3%. This work can inform and underpin future development of blue perovskite LEDs with highly efficient and stabile performance. [ABSTRACT FROM AUTHOR]

Metal halide perovskite quantum dots (QDs) have emerged as potential materials for high brightness, wide color gamut, and cost‐effective backlight emission due to their high photoluminescence quantum yields, narrow emission linewidths, and tunable bandgaps. Herein, CsPbX3/SBA‐15 nanocomposites are prepared with outstanding optical properties and high stability through an in situ growth strategy using mesoporous silica particles. According to finite‐difference time‐domain simulations, the mesoporous structure provides a strong waveguide effect on perovskite QDs and the uniform dispersion suppresses reabsorption losses, improving the overall photoconversion efficiency of perovskite QDs. The as‐fabricated perovskite monochromatic light‐emitting diode (LED) has a maximum luminous efficiency of 183 lm W−1, which is the highest for monochromatic perovskite LEDs reported to date. A further benefit of this work is that the white devices, which combine the green and red perovskite nanocomposites with commercial blue LED, exhibit a high luminous efficiency of 116 lm W−1 and a wide color gamut (125% for NTSC and 94% for Rec. 2020) with coordinates of (0.33,0.31). [ABSTRACT FROM AUTHOR]

Stable all‐inorganic CsPbX3 perovskite nanocrystals (PNCs) with high optical yield can be used in combination with graphene as photon sensors with high responsivity (up to 106 A W−1) in the VIS‐UV range. The performance of these perovskite/graphene field effect transistors (FET) is mediated by charge transfer processes at the perovskite – graphene interface. Here, the effects of high electric (up to 3000 kV cm−1) and magnetic (up to 60 T) fields applied perpendicular to the graphene plane on the charge transfer are reported. The authors demonstrate electric‐ and magnetic‐field dependent charge transfer and a slow (>100 s) charge dynamics. Magneto‐transport experiments in constant (≈0.005 T s−1) and pulsed (≈1000 T s−1) magnetic fields reveal pronounced hysteresis effects in the transfer characteristics of the FET. A magnetic time is used to explain and model differences in device behavior under fast (pulsed) and slowly (continuous) changing magnetic fields. The understanding of the dynamics of the charge transfer in perovskite/graphene heterostructures developed here is relevant for exploitation of these hybrid systems in electronics and optoelectronics, including ultrasensitive photon detectors and FETs for metrology. [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]

Perovskite solar cells (PSCs) have witnessed an unprecedentedly rapid development, especially in terms of power conversion efficiency (PCE). However, the solution‐processed perovskite films inevitably possess numerous crystallographic defects (e.g., halide vacancies), which has been shown to incur non‐radiative charge recombination and ion migration, thus limiting the enhancement of the PCE and stability of PSCs. Here, a novel dual metal (i.e., divalent and monovalent metal ions) modification strategy is reported for simultaneously reducing the defects, immobilizing the halide anions, and preventing ion loss from perovskite during post‐annealing process. Accordingly, this strategy significantly reduces non‐radiative recombination, enhancing the PCE by ≈12% and mitigating the current density‐voltage (J–V) hysteresis effect in resultant devices compared to undoped counterparts. As a result, a champion PCE exceeding 22% and a high open‐circuit voltage (Voc) of 1.16 V is obtained for dual metal ions‐modified PSCs. The optimized devices also exhibit extended lifespan upon the dual metal treatment. The study provides a new defect engineering strategy toward more efficient and stable perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

Quasi-two-dimensional (quasi-2D) perov- skites possess the preponderances of large exciton binding energy and quantum confinement effects compared with three-dimensional (3D) perovskites. The unique properties of quasi-2D perovskite have attracted extensive attention in the field of optoelectronic devices, especially in the light emitting diode (LED) direction. However, the adverse effects between the perovskite emission layer and the popularly used hole transport layer (HTL) Poly(3,4-ethylenedioxythiophene):poly (styrene sulfonate) (PEDOT:PSS) have degrade the device performance, such as large energy level barrier and exciton quenching. Here we demonstrated high performance of LED with enhanced brightness and efficiency by modifying the PEDOT:PSS with NdBr3, which not only decreases exciton quenching, but also decreases HOMO level of the PEDOT:PSS, thereby improving the charge balance. The final performance of the perovskite light-emitting diode (PeLED) device was obtained with a maximum luminance of 18684 cd m−2, a maximum current efficiency (CE) of 48.4 cd A−1 and an external quantum efficiency (EQE) of up to 15.5% when using NdBr3 modified PEDOT:PSS. [ABSTRACT FROM AUTHOR]

Simplified perovskite solar cells (PSCs) were fabricated with the perovskite layer sandwiched and encapsulated between carbon‐based electron transport layer (ETL) and counter electrode (CE) by a fully blade‐coated process. A self‐assembled monolayer of amphiphilic silane (AS) molecules on transparent conducting oxide (TCO) substrate appeals to the fullerene ETL deposition and preserves its integrity against the solvent damage. The AS serves as a "molecular glue" to strengthen the adhesion toughness at the TCO/ETL interface via robust chemical interaction and bonding, facilitating the interfacial charge extraction, increasing PCEs by 77 % and reducing hysteresis. A PCE of 18.64 % was achieved for the fully printed devices, one of the highest reported for carbon‐based PSCs. AS‐assisted interfacial linkage and carbon‐material‐assisted self‐encapsulation enhance the stability of the PSCs, which did not experience performance degradation when stored at ambient conditions for over 3000 h. [ABSTRACT FROM AUTHOR]

Inorganic perovskite nanocrystals (NCs) have demonstrated a number of unique optical and electronic properties for optoelectronic applications. However, the physical properties of these nanostructures, such as the dynamics of charge carriers on different timescales and their effect on the optical recombination of carriers, are not yet fully understood. This work reports on a slow (>1 s) reversible quenching of the NC photoluminescence due to a light‐induced Stark effect involving defects on the surface of the NCs and the redistribution of photoexcited carriers onto the NC surface. This phenomenon can influence the operation of optoelectronic devices based on these NCs, including hybrid photosensors based on graphene decorated with inorganic perovskite NCs, revealing their prospects and limitations. [ABSTRACT FROM AUTHOR]

Core/shell structured metal halide perovskite nanocrystals (NCs) are emerging as a type of material with remarkable optical and electronic properties. Research into this field has been developing and expanding rapidly in recent years, with significant advances in the studies of the shell growth mechanism and in understanding of properties of these materials. Significant enhancement of both the stability and the optical performance of core/shell perovskite NCs are of particular importance for their applications in optoelectronic technologies. In this review, the recent advances in core/shell structured perovskite NCs are summarized. The band structures and configurations of core/shell perovskite NCs are elaborated, the shell classification and shell engineering approaches, such as perovskites and their derivative shells, semiconductor shell, oxide shell, polymer shell, etc. are reviewed, and the shell growth mechanisms are discussed. The prospective of these NCs in lighting and displays, solar cells, photodetectors, and other devices is discussed in the light of current knowledge, remaining challenges, and future opportunities. [ABSTRACT FROM AUTHOR]

Quasi-two-dimensional (quasi-2D) Ruddlesden–Popper (RP) perovskites such as BA2Csn–1PbnBr3n+1 (BA = butylammonium, n > 1) are promising emitters, but their electroluminescence performance is limited by a severe non-radiative recombination during the energy transfer process. Here, we make use of methanesulfonate (MeS) that can interact with the spacer BA cations via strong hydrogen bonding interaction to reconstruct the quasi-2D perovskite structure, which increases the energy acceptor-to-donor ratio and enhances the energy transfer in perovskite films, thus improving the light emission efficiency. MeS additives also lower the defect density in RP perovskites, which is due to the elimination of uncoordinated Pb2+ by the electron-rich Lewis base MeS and the weakened adsorbate blocking effect. As a result, green light-emitting diodes fabricated using these quasi-2D RP perovskite films reach current efficiency of 63 cd A−1 and 20.5% external quantum efficiency, which are the best reported performance for devices based on quasi-2D perovskites so far. Owing to large exciton binding energy, quasi-2D perovskite is promising for light-emitting application, yet inhomogeneous phases distribution limits the potential. Here, the authors improve the performance by using MeS additive to regulate the phase distribution and to reduce defect density in the films. [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]

Metal halide perovskite nanocrystals (NCs) have shown significant potential in light‐emitting applications due to the unique luminous properties, such as high color purity, tunability, and solution processability. However, the large‐scale production of perovskite NCs with high‐quality for meeting the commercial applications is still a challenge. Herein, a facile room‐temperature synthesis of ten‐gram‐scale FAPbX3 (FA+ = HC(NH2)2+, X = Br, or mixed halide system Cl/Br and Br/I) NCs by a high‐power ultrasonic‐assisted strategy and the electroluminescence for light‐emitting diodes (LEDs) is reported. The uniform high‐power radiation avoids the adverse effects caused by heating and stirring unevenness, and no inert gas is needed in the reaction process. Meanwhile, the room temperature reaction reduces the crystallization rate of the NCs, leading to the successful synthesis of ten‐gram‐scale high‐quality FAPbX3 perovskite NCs. The resulting NCs show size‐focus distribution and high photoluminescence quantum yields of 93%, and the adjustable photoluminescence spectra from 453 to 695 nm by manipulating halide compositions. Attributed to the acquired FAPbBr3 NCs, a high‐efficiency green LED with the maximum current efficiency of 61.3 cd A−1 and external quantum efficiency of 14.1% is also obtained. [ABSTRACT FROM AUTHOR]

Recent years have witnessed an incredibly high fever in metal halide perovskite materials due to their promising applications in a wide range of optoelectronic applications. The morphologies and optoelectronic properties of the perovskite layers play critical roles in affecting the optoelectronic performances. This review summarizes the recent advances in the fabrication of a variety of perovskite morphologies and their promising progress achieved in different optoelectronic applications, including solar cells, light‐emitting diodes, photodetectors, lasers, photocatalysis, X‐ray detectors/imagers, and luminescent solar concentrators. Several blossoming representatives, including 0D perovskite quantum dots, 1D perovskite nanowires, 2D perovskite nanosheets/nanoplatelets, and 3D textured perovskite assemblies (i.e., cuboid‐like, inverse opal‐like, coral‐like, or maze‐like morphologies, etc.), are highlighted to demonstrate their fascinating properties and outstanding capabilities for efficient optoelectronic applications. Finally, a perspective on the remaining challenges and future directions of fabricating unique perovskite morphologies for next‐generation high‐performance optoelectronic devices is provided. [ABSTRACT FROM AUTHOR]

Highlights: [•] La1–x Ca x NiO3 perovskite-type oxides were investigated in glycerol steam reforming. [•] The perovskite structure facilitates the uniform distribution of the containing elements. [•] The partial substitution of La by Ca significantly affected the surface properties of La1–x Ca x NiO3. [•] Nickel dispersion and metal-support interaction were critical to the catalytic performance. [ABSTRACT FROM AUTHOR]

This review highlights the recent advances of employing the perovskite crystals redissolution strategy in perovskite photovoltaics, with particular emphasis on comparing different methodologies for synthesizing perovskites, elucidating the distinct solution chemistry, analyzing the cost advantages, as well as underlining the desirable thin-film superiority with improved quality and enhanced optoelectronic properties. [Display omitted] High-efficiency perovskite solar cells (PSCs) normally rely on costly, high purity (>99.99%), air-sensitive raw materials that vary batch-to-batch. The perovskite films and devices derived from conventional raw materials mixture method suffer from inferior reproducibility of optoelectronic properties and performance, as well as discounted promise towards low-cost scalable manufacturing. Distinguished from the direct mixing of raw materials, the preparation of perovskite films with precursors made by the redissolution of perovskite crystals holds the promise to make PSCs more affordable, reproducible, efficient and stable. The resultant perovskite films inherit the exceptional characteristics of the parent perovskite crystals, such as high crystallinity, high purity, accurate stoichiometric ratio, and low trap-state density, as well as good ambient and phase stability. Herein, we summarize recent progress on the employment of the perovskite crystals redissolution strategy for achieving low-cost, efficient perovskite-based solar-to-electricity conversion, which will help both popularize the redissolution strategy and reveal unprecedented advantages gained by its adoption. [ABSTRACT FROM AUTHOR]