Advancements in Halide Perovskite Large Single Crystal Photodetectors: Bridging Optical and Ionizing Radiation

Abstract Halide perovskite large single crystals (HPLSCs, with millimeter‐scale dimensions) are promising materials for photodetection, effectively bridging optical and ionizing radiation regimes with superior optoelectronic properties. This review explores recent advancements in HPLSC‐based photodetectors, emphasizing synthesis methods, device architectures, and performance enhancements. Techniques like temperature‐lowering crystallization, inverse‐temperature crystallization, and antisolvent vapor‐assisted crystallization produce high‐quality HPLSCs with minimal defects, extended carrier diffusion, and improved storage stability. These crystals excel across spectral domains: visible detectors achieve responsivities over 100 A W ⁻¹ , UV devices offer microsecond response speeds, and infrared detectors utilize defect engineering for broadband sensitivity. In ionizing radiation detection, HPLSCs perform well due to high atomic number constituents and substantial thickness, yielding X‐ray sensitivities above 10 ⁵ µC Gy _air ⁻¹ cm ⁻² and γ‐ray energy resolutions comparable to commercial detectors. Lead‐free alternatives address toxicity concerns while maintaining efficacy. Future research is expected to focus on hybrid growth techniques, AI‐driven material discovery, and integrated multispectral imaging, highlighting HPLSCs' potential in medical imaging, environmental monitoring, and aerospace applications.