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While the monolayer sheet is well-established as a Mott-insulator with a finite energy gap, the insulating nature of bulk 1T-TaS2 crystals remains ambiguous due to their varying dimensionalities and alterable interlayer coupling. In this study, we present a unique approach to unlock the intertwined two-dimensional Mott-insulator and three-dimensional band-insulator states in bulk 1T-TaS2 crystals by structuring a laddering stack along the out-of-plane direction. Through modulating the interlayer coupling, the insulating nature can be switched between band-insulator and Mott-insulator mechanisms. Our findings demonstrate the duality of insulating nature in 1T-TaS2 crystals. By manipulating the translational degree of freedom in layered crystals, our discovery presents a promising strategy for exploring fascinating physics, independent of their dimensionality, thereby offering a "three-dimensional" control for the era of slidetronics. While monolayer of 1T-TaS2 is considered to be a Mott insulator, the nature of the bulk insulating state is debated. Here the authors introduce a ladder-type structures with fractional misalignment of adjacent layers, showing that it becomes a Mott insulator due to decoupling between the layers. [ABSTRACT FROM AUTHOR]

Phase transition during annealing in the two‐step sequential deposition has drawn intensive attention as its significance in fabricating superior perovskite films. However, previous works have not paid enough attention to the importance of the purified phase transition path in the crystallization process. Herein, different from the mixed paths in the conventional cognition, purified phase transition path for α‐FAPbI3 crystallization is achieved by introducing dimethylurea (DMU) into lead iodide (PbI2) precursor solution. The multifunctional molecule is found to design a penetrable porous PbI2 film and fundamentally regulate the perovskite crystallization by forming single phase transition path via the complete δ‐phase during annealing of perovskite. The role of DMU in purified transition path for α‐FAPbI3 crystallization is unraveled with in situ photoluminescence and grazing incidence wide‐angle x‐ray scattering (GIWAXS) investigation. The crystal quality of perovskite films is significantly improved, resulting in single crystal‐like film. The best‐performing perovskite solar cells (PSCs) deliver a power conversion efficiency of 24.75%, resulting from the higher FF of 83.25% and an improved long‐term stability up to 3600 h. This work highlights the importance of purified phase transition path for the superior crystal quality toward high‐performance perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

The deviated crystallization kinetics of solution‐processed perovskite layers caused by the bottom interface is a barrier to comprehensively suppressing the defect formation and further to efficaciously improve the film quality and device performance. Herein, it is reported that the incorporation of a PEA2PbBr4 interlayer can effectively modify the crystallization process of the quasi‐2D mixed‐halide perovskite layers, resulting in enhanced Lewis acid‐base interaction and improved film homogeneity, which contributes to the strong defect passivation efficacy toward efficient sky‐blue emission. As a result, the devices with the bottom‐interface modification show a maximum external quantum efficiency of 14.2%, impressively an outstanding power efficiency of 17.0 lm W−1, and an external quantum efficiency of 12.3% at 1000 cd m−2. This work provides an insight into crystallization kinetics for defect suppression of the perovskite layer and further highlights the defect passivation efficacy of 2D perovskite‐based bottom‐interface modification toward high‐efficiency sky blue‐emitting diodes. [ABSTRACT FROM AUTHOR]

Tin halide perovskite solar cells are promising for the next generation of highly efficient photovoltaics. Their commercialization can be accelerated by increasing their stability in moisture and oxygen. Herein, an n‐type organic molecule (IO‐4Cl) is applied as an interlayer between the perovskite films and electron transport layers in p‐i‐n structured devices. The electron‐rich indacenodithieno‐[3,2‐b]thiophene enhances electron transport, while the hydrocarbon side chains and rigid conjugated backbone isolate air. It is also shown that the C═O in IO‐4Cl can coordinate with Sn2+ on perovskite films' surface and grain boundaries to enhance perovskite crystal stability. In addition, IO‐4Cl slows down crystallization dynamics, resulting in lower non‐radiation recombination. The moisture ingress in the perovskite films is tracked under high relative humidity (RH) and it is found that IO‐4Cl can mitigate moisture infiltration. Finally, the devices with IO‐4Cl maintain 95% of the initial power conversion efficiency after 1200 h of storage in a nitrogen‐filled glovebox, and their stability in ambient air (60–80% RH) is significantly improved against pristine devices, thus demonstrating the beneficial effects of IO‐4Cl interlayer on device stability. [ABSTRACT FROM AUTHOR]