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Layered halide perovskites (LHPs) with crystallographically 2D structures have gained increasing interest for photovoltaic applications due to their superior chemical stability and intriguing anisotropic properties, which are in contrast to their conventional 3D perovskite counterparts. The most frequently studied LHPs are Ruddlesden–Popper (RP) phases, which suffer from a carrier‐transport bottleneck due to the van der Waals gap associated with their intrinsic organic interlayer structures. To address this issue, Dion–Jacobson (DJ) and alternating‐cation‐interlayer (ACI) LHPs have rapidly emerged, which exhibit unique structural and (opto)electronic characteristics that may resemble those of the 3D counterparts owing to the eliminated or reduced van der Waals gap. Improved photophysical properties have been achieved in DJ and ACI LHPs, leading towards better photovoltaic performance. Here we provide a comprehensive discussion on the merits and promises of DJ and ACI LHPs from a chemistry perspective. Then, we review recent progress on the synthesis and tailoring of DJ and ACI LHP crystals and thin films, as well as their optoelectronic properties and photovoltaic performance. Finally, we discuss possible pathways to overcome critical challenges to realize the full potential of DJ and ACI LHPs for high‐performance solar cells and beyond. [ABSTRACT FROM AUTHOR]

Two pseudohalide thiocyanate ions (SCN−) have been used to replace two iodides in CH3NH3PbI3, and the resulting perovskite material was used as the active material in solar cells. In accelerated stability tests, the CH3NH3Pb(SCN)2I perovskite films were shown to be superior to the conventional CH3NH3PbI3 films as no significant degradation was observed after the film had been exposed to air with a relative humidity of 95 % for over four hours, whereas CH3NH3PbI3 films degraded in less than 1.5 hours. Solar cells based on CH3NH3Pb(SCN)2I thin films exhibited an efficiency of 8.3 %, which is comparable to that of CH3NH3PbI3 based cells fabricated in the same way. [ABSTRACT FROM AUTHOR]