High-efficiency and low-cost perovskite solar cells (PVKSCs) are an ideal candidate for addressing the scalability challenge of solar-based renewable energy. The dynamically evolving research field of PVKSCs has made immense progress in solving inherent challenges and capitalizing on their unique structure-property-processing-performance traits. This review offers a unique outlook on the paths toward commercialization of PVKSCs from the interfacial engineering perspective, relevant to both specialists and nonspecialists in the field through a brief introduction of the background of the field, current state-of-the-art evolution, and future research prospects. The multifaceted role of interfaces in facilitating PVKSC development is explained. Beneficial impacts of diverse charge-transporting materials and interfacial modifications are summarized. In addition, the role of interfaces in improving efficiency and stability for all emerging areas of PVKSC design are also evaluated. The authors' integral contributions in this area are highlighted on all fronts. Finally, future research opportunities for interfacial material development and applications along with scalability-durability-sustainability considerations pivotal for facilitating laboratory to industry translation are presented.

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Flexible perovskite solar cells (PSCs) using plastic substrates have become one of the most attractive points in the field of thin-film solar cells. Low-temperature and solution-processable nanoparticles (NPs) enable the fabrication of semiconductor thin films in a simple and low-cost approach to function as charge-selective layers in flexible PSCs. Here, we synthesized phase-pure p-type Cu-doped NiO NPs with good electrical properties, which can be processed to smooth, pinhole-free, and efficient hole transport layers (HTLs) with large-area uniformity over a wide range of film thickness using a room-temperature solution-processing technique. Such a high-quality inorganic HTL allows for the fabrication of flexible PSCs with an active area >1 cm, which have a power conversion efficiency over 15.01% without hysteresis. Moreover, the Cu/NiO NP-based flexible devices also demonstrate excellent air stability and mechanical stability compared to their counterpart fabricated on the pristine NiO films. This work will contribute to the evolution of upscaling flexible PSCs with a simple fabrication process and high device performances.

Although three-dimensional metal halide perovskite (ABX3) single crystals are promising next-generation materials for radiation detection, state-of-the-art perovskite X-ray detectors include methylammonium as A-site cations, limiting the operational stability. Previous efforts to improve the stability using formamidinium–caesium-alloyed A-site cations usually sacrifice the detection performance because of high trap densities. Here we successfully solve this trade-off between stability and detection performance by synergistic composition engineering, where we include A-site alloys to decrease the trap density and B-site dopants to release the microstrain induced by A-site alloying. As such, we develop high-performance perovskite X-ray detectors with excellent stability. Our X-ray detectors exhibit high sensitivity of (2.6 ± 0.1) × 104 μC Gyair−1 cm−2 under 1 V cm−1 and ultralow limit of detection of 7.09 nGyair s−1. In addition, they feature long-term operational stability over half a year and impressive thermal stability up to 125 °C. We further demonstrate the promise of our perovskite X-ray detectors for low-bias portable applications with high-quality X-ray imaging and monitoring prototypes.

Despite the dramatic rise in power conversion efficiencies (PCEs) of perovskite solar cells (PeSCs), concerns surrounding the long-term stability as well as the poor reproducibility in the archetypal three-dimensional (3D) perovskite, MAPbI3 (MA = CH3NH3), have the potential to derail commercialization. We have reported the fabrication and properties of a series of 2D perovskite compounds (PEI)2(MA) n−1Pb n I3n+1 (n = 3, 5, 7) by incorporating polyethylenimine (PEI) cations within the layered structure. The benefits of using intercalated polymer cations in the multilayered films are multiple: moisture resistance and film quality are greatly enhanced compared to that of their 3D MAPbI3 analogue; charge transport within solar cells can also be improved compared to that of 2D materials using small-molecule bulky ammonium. The moisture-stable nature of the multilayered perovskite materials allow for the simple one-step fabrication of cells with an aperture area of 2.32 cm2 under ambient humidity that have a PCE up to 8.77%. Overall, the 2D perovskite family offers rich multitudes of substituent and crystal structures, defining a promising class of stable and efficient light-absorbing materials.

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By embedding various types of colloidal silver nanoprisms into both interfacial layers, significant and general enhancement in the device performances of multiple polymer solar cell systems is demonstrated. The increased device efficiencies are due to the cooperative optical enhancement, resulting in enhanced short‐circuit current densities. These results provide a powerful, general, and tunable means to enhance light harvesting at desired wavelength bands in existing and emerging organic photovoltaic materials.