In Situ Crystal Growth and Fusing-Confined Engineering of Quasi-Monocrystalline Perovskite Thick Junctions for X-ray Detection and Imaging

Metal halide perovskites exhibit great promise for utilization in X-ray detection owing to their excellent optoelectronic properties and high X-ray attenuation capabilities. However, fabricating large-area thick films for high-performance perovskite X-ray detection remains challenging. This study develops an in situ crystal growth and fusing-confined approach to prepare high-quality, large-scale perovskite quasi-monocrystalline thick junctions. The perovskite crystals are grown in situ using a highly concentrated perovskite colloidal solution in 2-methoxyethanol. Introducing methylammonium chloride enhances grain reorganization during in situ growth and fusing-confined processes, effectively reducing grain boundaries and surface defects. This allows for the preparation of quasi-monocrystalline thick junctions of large grains (>100 μm) with high crystallinity, uniform orientation, and vertical penetration across the film thickness. Additionally, the carrier mobility and lifetime of the thick junctions are significantly enhanced. The optimized MAPbI₃ detectors demonstrate an X-ray sensitivity of 2.6 × 10⁴ μC Gy_air^-1 cm^-2 and an exceptionally low detection limit of 1 nGy_air s^-1. Furthermore, inspired by a honeycomb structure, these detectors realize X-ray imaging in 64 × 64 pixels through a pixelated separation design, effectively reducing the charge-sharing effect. This study offers valuable insights into the preparation of large-scale perovskite quasi-monocrystalline thick junctions for highly sensitive X-ray detection and imaging applications.