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Incorporating bromide into metal‐iodide perovskites is a commonly used approach for widening the bandgap of lead‐halide perovskites. Here, mixing of iodide and bromide is explored in narrow‐bandgap lead‐tin perovskites to create a Cs0.1FA0.6MA0.3Pb0.5Sn0.5I2.5Br0.5 perovskite composition, achieving the optimal bandgap of 1.34 eV for single‐junction solar cells. Introducing bromide into the precursor solution, markedly influenced film formation and resulted in singular 40 µm‐sized perovskite crystals. Supported by in situ absorption measurements, it is found that the delay time between starting the spin‐coating of the perovskite precursor and depositing the antisolvent is key in controlling the film morphology. By drastically reducing this delay time, homogenous nucleation is induced and smooth closed films are obtained. The Cs0.1FA0.6MA0.3Pb0.5Sn0.5I2.5Br0.5 perovskite do not show signs of light‐induced halide segregation during prolonged illumination. Using ammonium thiocyanate (NH4SCN) as additive in the precursor solution, the grain size could be further controlled. In solar cells, NH4SCN improved reproducibility and decreased hysteresis is observed. Applying passivation to reduce non‐radiative recombination at the perovskite ‐ electron transport layer interface and optimizing the device configuration results in a power conversion efficiency of 19.0%. This is among the highest for perovskites in the 1.3−1.4 eV bandgap range reported to date. Carefully tuning the composition of mixed lead‐tin mixed iodide‐bromide perovskites results in an optimal‐bandgap semiconductor for solar energy conversion. Homogenous crystallization of this perovskite involves a short time delay between deposition of the precursor solution and applying an antisolvent. Using a bulk additive and top surface passivation to increase grain size and reduce non‐radiative recombination, the power conversion efficiency attains 19%.

Charge extraction (or injection) at the transport layer/lead halide perovskite interface is a decisive process in determining the efficiency of optoelectronic devices. To elucidate the influence of band offsets on the hole transfer process, a series of perovskite thin films with systematically tuned valence band positions (FA0.83Cs0.17Pb(IxBr1‐x)3) are fabricated and deposited on mesoporous NiO hole transport layers. In this work, transient absorption spectroscopy is performed to study the kinetics of hole transfer through the NiO/perovskite interface. It is revealed that a larger valence band offset is beneficial for hole extraction. To understand how hole depletion/accumulation influences the hole extraction process, in situ transient spectroelectrochemical measurements are also employed. These results highlight that, at negative applied electrochemical biases, an acceleration of the hole transfer process is found for different perovskite compositions. A more pronounced increase in the hole extraction rate can be tied to a larger valence band offset at the NiO/perovskite interface. These results provide a better understanding of the charge extraction process at NiO/perovskite interfaces, enabling more rational design of these systems. The influence of hole depletion/accumulation on the hole extraction is evaluated in NiO/perovskite bilayers by transient spectroelectrochemical measurements. Metal‐halide perovskite thin films with different valence band positions are prepared, and the influence of band offset on the hole extraction kinetics is studied. It is found that a larger valence band offset can result in a more pronounced increase in the hole extraction rate.

Understanding the statistical behaviors from films to devices is crucial for performance prediction and materials innovation. Here, we present the first fully automated high‐throughput experimental platform for metal‐halide perovskite research in China, integrating solution preparation, film fabrication, electrode evaporation, and comprehensive optical/optoelectronic characterization. This platform enables human‐interference‐free data collection with high repeatability, facilitating reliable statistical analysis. Through systematic investigation of over 1000 perovskite samples, we first identify the key factor of solvent atmosphere affecting experimental repeatability, and then introduce a super‐absorbent resin to effectively mitigate solvent‐related variability. By quantitative tracking of statistical distributions across the film‐to‐device transformation, we reveal that the deposition of charge transport layers also alters the bulk properties of perovskite films, as manifested by statistical changes in bandgap and Urbach energy. Finally, we develop a machine learning‐based predictive model that links thin‐film optical features to device performance, demonstrating the feasibility of AI‐driven approaches to accelerate the evolution of perovskite materials. We have developed a fully automated high‐throughput experimental platform for electronic thin films and devices. Through statistical analysis, we demonstrated the transformative potential of combining high‐throughput experimentation with statistical methods to accelerate materials research, offering a new paradigm for material discovery and performance optimization.

Visible‐light‐driven C─N bond formation from non‐preactivated partners remains a central challenge in oxidative synthesis, particularly when selective control over N‐centered radical intermediates is required. Here, lead‐halide perovskite microcrystals are shown to mediate cross‐dehydrogenative C─N coupling of aromatic heterocyclic amines in air at room temperature by controlling complementary radical species at semiconductor interfaces. Phenoxazine undergoes efficient oxidative dimerization, whereas closely related scaffolds such as phenothiazine and 9,9‐dimethyl‐9,10‐dihydroacridine display markedly different reactivity profiles despite comparable oxidation potentials. Combined electrochemical, spectroscopic, and radical‐trapping experiments reveal that efficient C─N bond formation correlates with the concurrent generation of radical cation and neutral aminyl species at the catalyst–substrate interface. UV–vis monitoring under controlled atmospheres establishes the necessity of oxygen for sustaining complementary radical populations, while spin‐unrestricted DFT calculations identify substrate‐dependent spin localization, as well as distinct N─H activation barriers, as key factors of coupling efficiency. Interception of the photogenerated aminyl radicals enables hetero‐cross‐dehydrogenative coupling with naphthol and naphthylamine derivatives. These findings delineate mechanistic principles governing C─N bond formation at semiconductor surfaces and position metal‐halide perovskites as tunable and recyclable platforms for N‐centered radical chemistry under mild conditions. Visible‐light‐excited CsPbBr3 perovskite microcrystals enable selective C─N bond formation from non‐preactivated aromatic amines via controlled generation of complementary aminyl and aminium radicals at the catalyst surface. Radical interplay governs reactivity, allowing efficient homo‐ and hetero‐cross‐dehydrogenative coupling under mild aerobic conditions with recyclable semiconductor photocatalysts.

Precise control of exciton confinement in metal halide perovskites is critical to the development of high‐performance, stable optoelectronic devices. A significant hurdle is the swift completion of ionic metathesis reactions, often within seconds, making consistent control challenging. Herein, the introduction of different steric hindrances in a Cs+ sublattice within CsYb2F7 is reported, which effectively modulates the reaction rate of Cs+ with lead (Pb2+) and halide ions in solution, extending the synthesis time for perovskite nanostructures to tens of minutes. Importantly, the Cs+ sublattice provides a crystal facet‐dependent preference for perovskite growth and thus exciton confinement, allowing the simultaneous occurrence of up to six emission bands of CsPbBr3. Moreover, the rigid CsYb2F7 nano template offers high activation energy and enhances the stability of the resulting perovskite nanostructures. This methodology provides a versatile approach to synthesizing functional heterostructures. Its robustness is demonstrated by in‐situ growth of perovskite nanostructures on Cs+‐mediated metal‐organic frameworks. Efficient steric hindrance management enables precise control of lead‐halide perovskite growth and emission from Cs+‐preconfined nanocrystals. Introducing diverse steric hindrances adjusts the Cs+ reaction rate with lead and halide ions in the solution, prolonging perovskite nanostructure synthesis to several tens of minutes. This approach has the potential to offer fresh perspectives in atomic‐scale nanocrystal engineering.

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), A BBʹX , 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.

The properties of films of organic-inorganic perovskites CH 3 NH 3 PbI 2.98 Cl 0.02 depending on the ratio of starting reagents in solutions (PbI 2 :{CH 3 NH 3 I + CH 3 NH 3 Cl}) has been investigated. It was found that the formation of the perovskite structure with the ratio of the initial reagents PbI 2 : CH 3 NH 3 I = 1:1 occurs at 70–80 °C, and with the increase of the temperature of thermal treatment to 120 °C, the thermal destruction of the perovskite begins. When the ratio of the starting reagents PbI 2 : CH 3 NH 3 I = 1:2, the formation of the perovskite structure occurs through the intermediate compound (CH 3 NH 3 ) 2 PbI 4 , and when the ratio is 1:3—(CH 3 NH 3 ) 3 PbI 5 and (CH 3 NH 3 ) 2 PbI 4 . Independent on the ratio of the initial components (CH 3 NH 3 I:PbI 2 ), the ratio between the content of lead and iodine in the films remains unchanged, that is why a significant difference in the film properties could be explained by the anisotropy of the particle shape, which is consistent with the data of electron microscopy and X-ray diffractometry.

Perovskites are attracting an increasing interest in the wide community of photovoltaics, optoelectronic, and detection, traditionally relying on lead‐based systems. This Minireview provides an overview of the current status of experimental and computational results available on Ge‐containing 3D and low‐dimensional halide perovskites. While stability issues analogous to those of tin‐based materials are present, some strategies to afford this problem in Ge metal halide perovskites (MHPs) for photovoltaics have already been identified and successfully employed, reaching efficiencies of solar devices greater than 7 % at up to 500 h of illumination. Interestingly, some Ge‐containing MHPs showed promising nonlinear optical responses as well as quite broad emissions, which are worthy of further investigation starting from the basic materials chemistry perspective, where a large space for properties modulation through compositions/alloying/fnanostructuring is present. Germane to germanium: This Minireview provides an overview of current experimental and computational research in the field of Ge‐based 3D and low‐dimensional halide perovskites. Materials properties, including stability issues and structure‐property correlations are discussed, as well as present and future applications in various fields ranging from photovoltaics to nonlinear optics and optoelectronics.

Metal halide perovskites (MHPs), emerging as innovative and promising semiconductor materials with prominent optoelectronic properties, has been pioneering a new era of light management (ranging from emission, absorption, modulation, to transmission) for next-generation optoelectronic technology. Notably, the exploration of fundamental characteristics of MHPs and their devices is the main research theme during the past decade, while in the next decade, it will be primarily critical to promote their implantation in the next-generation optoelectronics. In this review, we first retrospect the historical research milestones of MHPs and their optoelectronic devices. Thereafter, we introduce the origin of the unique optoelectronic features of MHPs, based on which we highlight the tunability of these features via regulating the phase, dimensionality, composition, and geometry of MHPs. Then, we show that owing to the convenient property control of MHPs, various optoelectronic devices with target performance can be designed. At last, we emphasize on the revolutionary applications of MHPs-based devices on the existing optoelectronic systems. This review demonstrates the key role of MHPs played in the development of modern optoelectronics, which is expected to inspire the novel research directions of MHPs and promote the widespread applications of MHPs in the next-generation optoelectronics.

Over the past decade, metal halide perovskite photovoltaics have been a major focus of research, with single-junction perovskite solar cells evolving from an initial power conversion efficiency of 3.8% to reach 25.5%. The broad bandgap tunability of perovskites makes them versatile candidates as the subcell in a tandem photovoltaics architecture. Stacking photovoltaic absorbers with cascaded bandgaps in a multi-junction device can potentially overcome the Shockley–Queisser efficiency limit of 33.7% for single-junction solar cells. There is now intense activity in developing tandem solar cells that pair perovskite with either itself or with a variety of mature photovoltaic technologies such as silicon and Cu(In,Ga)(S,Se)2 (CIGS). In this review, we survey recent advances in the field and discuss its outlook.A discussion of the evolution, present status and future outlook for tandem solar cells employing perovskite materials.