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The stability of hybrid organic-inorganic halide perovskite semiconductors remains a significant obstacle to their application in photovoltaics. To this end, the use of low-dimensional (LD) perovskites, which incorporate hydrophobic organic moieties, provides an effective strategy to improve their stability, yet often at the expense of their performance. To address this limitation, supramolecular engineering of noncovalent interactions between organic and inorganic components has shown potential by relying on hydrogen bonding and conventional van der Waals interactions. Here, the capacity to access novel LD perovskite structures that uniquely assemble through unorthodox S-mediated interactions is explored by incorporating benzothiadiazole-based moieties. The formation of S-mediated LD structures is demonstrated, including one-dimensional (1D) and layered two-dimensional (2D) perovskite phases assembled via chalcogen bonding and S-π interactions. This involved a combination of techniques, such as single crystal and thin film X-ray diffraction, as well as solid-state NMR spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities of S-mediated LD perovskites. The resulting materials are applied in n-i-p and p-i-n perovskite solar cells, demonstrating enhancements in performance and operational stability that reveal a versatile supramolecular strategy in photovoltaics., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Doping of all-inorganic lead halide perovskites to enhance their photovoltaic performance and stability has been reported to be effective. Up to now most studies have focused on the doping of elements in to the perovskite lattice. However, most of them cannot be doped into the perovskite lattice and the roles of these dopants are still controversial. Herein,the authors introduce CdI 2 as an additive into CsPbI 3-x Br x and use it as active layer to fabricate high-performance inorganic perovskite solar cells (PSCs). Cd with a smaller radius than Pb can partially substitute Pb in the perovskite lattice by up to 2 mol%. Meanwhile, the remaining Cd stays on the surface and grain boundaries (GB) of the perovskite film in the form of Cs 2 CdI 4-x Br -x , which is found to reduce non-radiative recombination. These effects result in prolonged charge carrier lifetime, suppressed defect formation, decreased GBs, and an upward shift of energybands in the Cd-containing film. A champion efficiency of 20.8% is achieved for Cd-incorporated PSCs, together with improved device ambient stability. This work highlights the importance of simultaneous lattice engineering, defectcontrol and atomic-level characterization in achieving high-performance inorganic PSCs with well-defined structure-property relationships., (© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.)