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Wide‐bandgap (WBG) perovskite solar cell (PSC) plays a pivotal role as the top subcell in all‐perovskite tandem solar cells (TSCs), facilitating the absorption of high‐energy photons and affording a large open‐circuit voltage (VOC). Nonetheless, the stability and efficiency of WBG PSCs are constrained by light‐induced halide segregation and non‐radiative recombination losses. In this study, this work presents an approach of utilizing 2‐methylpiperazinium bromide (2‐MePBr) via interfacial engineering to realize high‐efficiency WBG (1.77 eV) PSCs. The C─NH─C functional group in 2‐MePBr, serving as an electron donor, can interact with under‐coordinated lead defects at the perovskite surface. Consequently, the treatment with 2‐MePBr mitigates interfacial non‐radiative recombination, enhances charge transport, inhibits ion migration, and thus delivers an improved power conversion efficiency (PCE) of 19.30% with a VOC of 1.29 V, and a fill factor of 83.08%. Notably, the WBG PSCs manifest enhanced stability, preserving 80% of the initial PCE after 337 h of continuous operation under 1 sun illumination at the maximum power point. Furthermore, the all‐perovskite TSCs based on this WBG subcell achieve a PCE of 27.47%, showing its promising application in perovskite‐based tandem solar cells. [ABSTRACT FROM AUTHOR]

In recent years, the surface modification of perovskite by wide band‐gap insulating materials has been one of the main strategies to achieve efficient and stable perovskite solar cells (PSCs). Unfortunately, a significant hurdle in this approach is the dilemma surrounding the quality of passivation and the transport of charges. Here, this trade‐off is overcome by introducing self‐assembled diphenylphosphinic acid (DPPA) porous layer. Applying highly concentrated DPPA solution on the perovskite surface not only provides excellent passivation of entire surface, but also the excess DPPA will form a self‐assembled porous insulating layer (PIL), which forms random submicron‐sized openings at the interface of the insulating layer for accelerated charge transport. In addition, the energy level of the perovskite surface can be modulated by this insulating material to facilitate carrier transport. As a result, an impressive power conversion efficiency (PCE) over 24% has been achieved in methylammonium‐free p‐i‐n devices with an ultrahigh fill factor (FF) of 84.7%. The unencapsulated devices exhibit excellent thermal and operational stability. This work paves a way for establishment of an effective passivation and facilitated transport simultaneously. [ABSTRACT FROM AUTHOR]