The mixed caesium and formamidinium lead triiodide perovskite system (Cs1-xFAxPbI3) in the form of quantum dots (QDs) offers a new pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective ligand-assisted cation exchange strategy that enables controllable synthesis of Cs1-xFAxPbI3 QDs across the whole composition range (x: 0-1), which is inaccessible in large-grain polycrystalline thin films. The surface ligands play a key role in driving the cross-exchange of cations for the rapid formation of Cs1-xFAxPbI3 QDs with suppressed defect density. The hero Cs0.5FA0.5PbI3 QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that QD devices exhibit substantially enhanced photostability compared to their thin film counterparts because of the suppressed phase segregation, retaining 94% of the original PCE under continuous 1-sun illumination for 600 hours.

Lead halide perovskites have witnessed significant progress in low-cost and high-efficiency photovoltaics, with a rapid increase in photovoltaic efficiencies from 3.8% to a certified record of 25.2% in the past decade. [1-4] However, the viability and practical scale-up implementation are limited by the stability and toxicity of the lead halide perovskites. [5,6] To circumvent these two

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The phenethylammonium cation significantly promotes the formation of fully-covered thin-films of hybrid bismuth organohalides with low surface roughness and excellent stability.

Charge carrier transport in materials is of essential importance for photovoltaic and photonic applications. Here, the authors demonstrate a controllable acceleration or deceleration of charge carrier transport in specially structured metal‐alloy perovskite (MACs)PbI3 (MA= CH3NH3) single‐crystals with a gradient composition of CsPbI3/(MA1−xCsx)PbI3/MAPbI3. Depending on the Cs‐cation distribution in the structure and therefore the energy band alignment, two different effects are demonstrated: i) significant acceleration of electron transport across the depth driven by the gradient band alignment and suppression of electron–hole recombination, benefiting for photovoltaic and detector applications; and ii) decelerated electron transport and thus improved radiative carrier recombination and emission efficiency, highly beneficial for light and display applications. At the same time, the top Cs‐layer results in hole localization in the top layer and surface passivation. This controllable acceleration and deceleration of electron transport is critical for various applications in which efficient electron–hole separation and suppressed nonradiative electron–hole recombination is demanded.

Lead (Pb) halide perovskites have witnessed highly promising achievements for high-efficiency solar cells, light-emitting diodes (LEDs), and photo/radiation detectors due to their exceptional optoelectronic properties. However, compound stability and Pb toxicity are still two main obstacles towards the commercialization of halide perovskite-based devices. Therefore, it is of substantial interest to search for non-toxic candidates with comparable photophysical characteristics. Metal-halide double perovskites (MHDPs), A2BBʹX6, are recently booming as promising alternatives for Pb-based halide-perovskites for their non-toxicity and significantly enhanced chemical and thermodynamic stability. Moreover, this family exhibits rich combinatorial chemistry with tuneable optoelectronic properties and thus a great potential for a broad range of optoelectronic/electronic applications. Herein, we present a comprehensive review of the MHDPs synthesized so far, and classified by their optical and electronic properties. We systematically generalize their electronic structure by both theoretical and experimental efforts to prospect the relevant optoelectronic properties required by different applications. The progress of the materials in various applications is explicated in view of the material structure-function relationship. Finally, a perspective outlook to improve the physical and optoelectronic properties of the materials is proposed aiming at fostering their future development and applications.

Organometal perovskite single crystals have been recognized as a promising platform for high-performance optoelectronic devices, featuring high crystallinity and stability. However, a high trap density and structural nonuniformity at the surface have been major barriers to the progress of single crystal-based optoelectronic devices. Here, the formation of a unique nanoisland structure is reported at the surface of the facet-controlled cuboid MAPbI 3 (MA = CH 3 NH 3 +) single crystals through a cation interdiffusion process enabled by energetically vaporized CsI. The interdiffusion of mobile ions between the bulk and the surface is triggered by thermally activated CsI vapor, which reconstructs the surface that is rich in MA and CsI with reduced dangling bonds. Simultaneously, an array of Cs-Pb-rich nanoislands is constructed on the surface of the MAPbI 3 single crystals. This newly reconstructed nanoisland surface enhances the light absorbance over 50% and increases the charge carrier mobility from 56 to 93 cm 2 V −1 s −1 . As confirmed by Kelvin probe force microscopy, the nanoislands form a gradient band bending that prevents recombination of excess carriers, and thus, enhances lateral carrier transport properties. This unique engineering of the single crystal surface provides a pathway towards developing high-quality perovskite single-crystal surface for optoelectronic applications.

Metal halide perovskites (MHPs) as a new generation of optoelectronic materials, have attracted a surge of attention due to their remarkable intrinsic properties. Despite the tremendous advances for their polycrystalline...