Dipolar chemical bridge induced CsPbI${}_3$ perovskite solar cells with 21.86 % efficiency

CsPbI${}_3$ perovskite receives tremendous attention for photovoltaic applications due to its ideal band gap and good thermal stability. However, CsPbI${}_3$ perovskite solar cells (PSCs) significantly suffer from photovoltage deficits because of serious interfacial energy losses within the PSCs, which to a large extent affects the photovoltaic performance of PSCs. Herein, a dipolar chemical bridge (DCB) is constructed between the perovskite and TiO${}_2$ layers to lower interfacial energy losses and thus improve the charge extraction of PSCs. The results reveal that the DCB could form a beneficial interfacial dipole between the perovskite and TiO${}_2$ layers, which could optimize the interfacial energetics of perovskite/TiO${}_2$ layers and thus improve the energy level alignment within the PSCs. Meanwhile, the constructed DCB could also simultaneously passivate the surface defects of perovskite and TiO${}_2$ layers, greatly lowering interfacial recombination. Consequently, the photovoltage deficit of CsPbI${}_3$ PSCs is largely reduced, leading to a record efficiency of 21.86 % being realized. Meanwhile, the operation stability of PSCs is also largely improved due to the high-quality perovskite films with released interfacial tensile strain being obtained after forming the DCB within the PSCs. (© 2024 Wiley‐VCH GmbH)