Antimony chalcogenides such as Sb2S3, Sb2Se3, and Sb2(SxSe1−x)3 have emerged as very promising alternative solar absorber materials due to their high stability, abundant elemental storage, nontoxicity, low‐cost, suitable tunable bandgap, and high absorption coefficient. Remarkable achievements have been made in antimony chalcogenide solar cells in the past few decades, with the power conversion efficiency (PCE) currently reaching 9.2%, which is close to the PCE level required for industrial applications. To facilitate the realization of highly efficient antimony chalcogenide solar cells in the future, a comprehensive review of antimony chalcogenide‐based materials and photovoltaic devices is presented. First, the fundamental physical properties and preparation methods of antimony chalcogenide‐based materials are outlined, and then, notable recent developments in antimony chalcogenide‐based photovoltaic devices with various architectures are highlighted. Finally, the most prominent limitations are described, and approaches to achieving remarkable advances in antimony chalcogenide solar cells in the future are provided.

Nickel oxide (NiOx) is desirable hole selective material (HSMs) for perovskite photovoltaics because of the characteristic in stability and low cost. However, they deliver limited open‐circuit voltage (VOC) compared to some organic HSMs. As it is known, the performance of perovskite solar cells is predominantly limited by trap‐assisted non‐radiative recombination at the perovskite/hole‐selective layer interfaces. A typical lithium‐doping strategy leads to the valence‐band maximum shift and the electronic levels of NiOx can be tuned robustly to match perovskite active layer in perovskite solar cells. More critically, carrier dynamics studies demonstrate another critical PN4N interlayer strategy reduced interfacial density of defect sites and trap‐assisted recombination. These merits contribute coordinately to lower energy loss across the perovskite/NiOx interface and facilitate charge transport process through the relevant interface, yielding VOC values increase to 1.14 V and power conversion efficiencies over 20%.

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A room-temperature solution-processed pillar[5]arene-based small molecule material, termed C3, has been designed, synthesized, and incorporated between a conventional PCBM electron transport layer (ETL) and a metal electrode to function as a single-layer cathode buffer layer (CBL) for efficient planar p-i-n perovskite solar cells (PVSCs). It has been found that C3 has a work function tunneling effect, which can decrease the work function of the Ag electrode; therefore, introduction of C3 successfully enhances the interface contact and reduces the interface barriers, which usually exist between fullerene derivatives and metal electrodes. It was also found that the C3 capping layer could improve the surface quality of PCBM, forming a smooth, dense and pinhole-free morphology with fewer surface defects. Thus, C3 can modify the interface between PCBM and Ag, enhance the diode properties of devices and facilitate electron transport through the devices; therefore, it is a very promising CBL material for PVSCs. A device with a hybrid PCBM ETL and a single cathode buffer layer of C3 exhibited a high power conversion efficiency (PCE) of 17.42% with negligible hysteresis, which was dramatically higher than that of a device based on a pure PCBM ETL. With the major advantages of a low-temperature solution process and interface modification, the excellent PCE of PVSCs on flexible substrates can exceed 13%. These results demonstrate that solution-processed pillar[5]arene-based small molecule materials can serve as high performance CBLs in PVSCs.

hybrid perovskite solar cells (PVSCs) have attracted more and more attention because of the decent properties of perovskites such as high absorption coefficient, tunable optical bandgap, long carrier lifetime, high mobility and long diffusion length. PVSCs have achieved great improvements with power conversion efficiency now reaching certified 25.2%, which showed huge potential for future commercialization. [1][2][3][4][5][6][7] State-ofthe-art PVSCs use solution-processed perovskite films to absorb incident light. The halide perovskite absorbers are generally regarded as soft ionic solids, which are prone to contain defects in polycrystalline films (e.g., vacancies, interstitials, and cation and antisite substitutions). [8] The widely used one-step spin-casting procedure represents the simplest solution process, in which stoichiometric organic and metal halide precursors are mixed in organic solvents and transformed into intermediate perovskite crystalline thin films by centrifugal force and solvent evaporation. Such a simple deposition route has cost advantages and potential of device scaling up, but a large number of defects will inevitably form during the spin-casting process. For example, the spin-casting process may cause the formation of some anomalous perovskite clusters which are easy to be decomposed, resulting in the formation of ionic defects such as iodide vacancies or uncoordinated lead/halide ions. The presence of such defects in perovskites has commonly been recognized as fatal, such that the perovskite properties (e.g., conductivity, free charge mobility, and charge lifetime) are significantly decreased. Defects will also cause serious carrier recombination including radiative and nonradiative recombination, which have been demonstrated to be the main reason for energy loss in perovskite photovoltaic devices and are detrimental to the carrier lifetime of perovskite film, the performance and stability of PVSCs. [9] Efficient control and engineering of defects distributed in light-absorbing semiconductor materials have been proven to be an effective way to accelerate the development of high-performance perovskite solar cells. [10] To reduce the defects and eliminate the recombination, researchers have Perovskite solar cells (PVSCs) have achieved excellent power conversion efficiency (PCE) but still suffer from instability issues. Defect passivation is an important route to simultaneously increase the efficiency and stability ofPVSCs. Here, a strategy of incorporating silica oligomer in perovskite films for surface and grain boundary defect passivation is reported. Silica oligomer passivation agent (PA) is in situ formed through hydrolysis and condensation reaction of tetraethyl orthosilicate additive in perovskite precursor. The passivation mechanism is elucidated by density functional theory calculation, revealing stable chelating interaction and hydrogen bond interaction between PA and perovskite. Spectroscopic and electrical characterizations demonstrate that silica oligomer can enlarge grain si...