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Interfacial properties of a hole‐transport material (HTM) and a perovskite layer are of high importance, which can influence the interfacial charge transfer dynamics as well as the growth of perovskite bulk crystals particularly in inverted structure. The halogen bonding (XB) has been recognized as a powerful functional group to be integrated with new small molecule HTMs. Herein, a carbazole‐based halo (iodine)‐functional HTM (O1), is synthesized for the first time, demonstrating a high hole mobility and suitable energy levels that align well with those of perovskites. The strong interaction between O1 and perovskite, i.e., I···I−, induces the formation of an ordered interlayer, which are verified by both theoretical and experimental studies. Compared to the reference HTM (O2) without any halo‐function, the XB‐induced interlayer effectively enhances the interfacial charge extraction efficiency, while significantly hindering the non‐radiative charge recombination by reducing the surface traps upon the strong passivation effect. This is reflected as a big increase in the open‐circuit voltage by up to 114 mV in the fabrication of inverted devices with the highest power conversion efficiency of 22.34%. Moreover, the ordered XB‐driven interlayer at the interface of O1 and perovskite is mainly responsible for the extended lifespan under the operational conditions. [ABSTRACT FROM AUTHOR]

Reducing non‐radiative recombination caused by defects at buried interfaces is crucial to the development of efficient and stable perovskite solar cells (PSCs). Herein, supramolecular cucurbit[5]uril (CB[5]) is introduced into the SnO2 layer, where it engages in host–guest interactions to suppress oxygen vacancies in SnO2, prevent particle aggregation, and enhance the electron mobility of SnO2. By serving as a bridging agent at the buried interface between SnO2 and the perovskite layer, CB[5] reduces the defect density and improves the carrier extraction efficiency. It also enhanced the surface energy of the SnO2 substrate, facilitates the formation of large grains in the perovskite film, alleviates residual lattice stresses, and enhances the film quality. Consequently, the PSC with CB[5] shows a champion power conversion efficiency of 24.83%. Moreover, an unencapsulated device incorporating CB[5] retains more than 87% of its initial PCE under continuous illumination at the maximum power point tracking for 1000 h. This study pioneers the utilization of cucurbiturils in PSCs and provides insights into how supramolecular compounds can regulate buried interfaces. [ABSTRACT FROM AUTHOR]

Despite numerous studies have reported the inhibition of tin (II) oxidation in mixed tin‐lead halide perovskite, there remains a dearth of mechanistic information regarding how tin (II) undergoes oxidation in the precursor solution, particularly in terms of the involvement of DMSO. We here take advantage of density functional theory (DFT) to uncover that SnI2 can coordinate with DMSO and react with singlet oxygen, resulting in the generation of Sn (IV). Moreover, our DFT simulations reveal that benzaldehyde oxime (BZHO) competes with SnI2 in reacting with oxygen through the Alder‐ene reaction, hence effectively restraining the oxidation of tin (II), which is further verified by several experimental characterizations. Besides, the introduction of BZHO has also regulated the crystallization of the perovskite film and modified the electronic structure of the perovskite surface. As a result, the perovskite solar cells with the addition of BZHO demonstrate superior performance and operational stability, retaining 82 % of the initial PCE under continuous 1‐sun illumination for 800 hours. Furthermore, the efficiency of all‐perovskite tandem solar cells treated with BZHO reached 26.76 %. Therefore, this work presents a promising strategy for designing high‐performance and stable all‐perovskite tandem solar cells. [ABSTRACT FROM AUTHOR]

The migration of ions is known to be associated with various detrimental phenomena, including current density‐voltage hysteresis, phase segregation, etc. which significantly limit the stability and performance of perovskite solar cells, impeding their progress toward commercial applications. To address these challenges, we propose incorporating a polymerizable organic small molecule monomer, N‐carbamoyl‐2‐propan‐2‐ylpent‐4‐enamide (Apronal), into the perovskite film to form a crosslinked polymer (P‐Apronal) through thermal crosslinking. The carbonyl and amino groups in Apronal effectively interact with shallow defects, such as uncoordinated Pb2+ and iodide vacancies, leading to the formation of high‐quality films with enhanced crystallinity and reduced lattice strain. Furthermore, the introduction of P‐Apronal improves energy level alignment, and facilitates charge carrier extraction and transport, resulting in a champion efficiency of 25.09 %. Importantly, P‐Apronal can effectively suppress the migration of I− ions and improve the long‐term stability of the devices. The present strategy sets forth a path to attain long‐term stability and enhanced efficiency in perovskite solar cells. [ABSTRACT FROM AUTHOR]

Carbonyl functional materials as additives are extensively applied to reduce the defects density of the perovskite film. However, there is still a lack of comprehensive understanding for the effect of carbonyl additives to improve device performance. In this work, we systematically study the effect of carbonyl additive molecules on the passivation of defects in perovskite films. After a comprehensive investigation, the results confirm the importance of molecular dipole in amplifying the passivation effect of additive molecules. The additive with strong molecular dipole possesses the advantages of enhancing the efficiency and stability of perovskite solar cells (PSCs). After optimization, the companion efficiency of PSCs is 23.20 %, and it can maintain long‐term stability under harsh conditions. Additionally, a large‐area solar cell module‐modified DLBA was 20.18 % (14 cm2). This work provides an important reference for the selection and designing of efficient carbonyl additives. [ABSTRACT FROM AUTHOR]