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Nickel oxide is one of the most promising hole‐transporting materials in inverted perovskite solar cells (PSCs) but suffers from undesired reactions with perovskite which leads to limited device performance and stability. Self‐assembled monolayers (SAMs) are demonstrated to effectively optimize the NiOx/perovskite interface, but the significance of the compactness of the SAM at the interface is less investigated. Here, a series of methoxy‐substituted triphenylamine functionalized benzothiadiazole (TBT) based SAM molecules, TBT‐BA, TBT‐FBA, and TBT‐DBA, with benzoic acid, 2‐fluorobenzoic acid and isophthalic acids as anchoring groups are used to modify NiOx. TBT‐BA with the simplest structure is demonstrated to form the densest SAM on NiOx, thus optimized NiOx/SAM/perovskite interface is achieved with enhanced charge collection and suppressed interfacial reaction and recombination. TBT‐BA can also passivate the perovskite most effectively due to the highest binding energy toward perovskite, thus the corresponding inverted PSCs show the highest PCE of 24.8% and maintain 88.7% of the initial PCE after storage at 60 °C for 2635 h in the glovebox. The work provides important insights into designing SAM molecules for modification transporting layers for efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

The inorganic perovskite solar cells (IPSC) are promising in the context of simultaneously delivering high efficiency and good stability. Developing a high‐performance and larger band gap IPSC is particularly in demand for commercialization due to their suitability to match with the prevailing silicon solar cells for tandem devices, while this is hindered by the poor morphology and phase stability of inorganic perovskite films. To address this issue, this work develops a combined method of nonstoichiometric composition and post‐cation exchange to improve the morphology and phase stability of the CsPbI2Br IPSCs, and achieves a record efficiency of 17.80%. This work finds that excessive PbI2 regulates the CsPbI2Br film crystallization, and thus, a high‐quality perovskite film with enlarged grains is obtained. Further depositing the formamidinium iodide on top of the CsPbI2Br perovskite induces cation exchange during the post‐annealing process, which increases the phase stability of the perovskite film and significantly improves the device efficiency and stability. Therefore, this work provides an avenue toward high‐performance IPSCs, via the nonstoichiometric and ion exchange method. [ABSTRACT FROM AUTHOR]

2D Dion–Jacobson (DJ) perovskites show structural stability and tunability and are regarded as promising photovoltaic materials. The spacer cations play an important impact on exciton separation and charge transport of 2D perovskites. Herein, a novel spacer with thiazole as core, 2‐thiazolemethanammonium (AMT), owning characters of small molecular size, delocalized π‐electrons, and strong electron‐withdrawing ability, is introduced to construct 2D DJ perovskites. Owing to the strong orbital coupling between AMT spacer and inorganic layers, the AMT‐based perovskite exhibits type II quantum well structure, which is favorable for exciton separation. On contrary, such interaction does not appear in the DJ perovskite when aliphatic propyldiammonium (PDA), with a similar length, is used as spacer. The AMT spacer can also induce better crystallinity, resulting in reduced defect density and improved charge transport ability. The optimized device based on (AMT)MA3Pb4I13 exhibits a power conversion efficiency (PCE) of 19.69%, which is a record for 2D DJ perovskite solar cells (PSCs) (n ≤ 4). This work provides deep understanding of the impact of aromatic spacer on the electronic structure of 2D DJ perovskites and the corresponding photovoltaic performance and provides a new opportunity toward highly efficient and stable PSCs. [ABSTRACT FROM AUTHOR]