Demonstration of Energy-Resolved γ-Ray Detection at Room Temperature by the CsPbCl₃ Perovskite Semiconductor

The detection of γ-rays at room temperature with high-energy resolution using semiconductors is one of the most challenging applications. The presence of even the smallest amount of defects is sufficient to kill the signal generated from γ-rays which makes the availability of semiconductors detectors a rarity. Lead halide perovskite semiconductors exhibit unusually high defect tolerance leading to outstanding and unique optoelectronic properties and are poised to strongly impact applications in photoelectric conversion/detection. Here we demonstrate for the first time that large size single crystals of the all-inorganic perovskite CsPbCl₃ semiconductor can function as a high-performance detector for γ-ray nuclear radiation at room temperature. CsPbCl₃ is a wide-gap semiconductor with a bandgap of 3.03 eV and possesses a high effective atomic number of 69.8. We identified the two distinct phase transitions in CsPbCl₃, from cubic (Pm-3m) to tetragonal (P4/mbm) at 325 K and finally to orthorhombic (Pbnm) at 316 K. Despite crystal twinning induced by phase transitions, CsPbCl₃ crystals in detector grade can be obtained with high electrical resistivity of ∼1.7 × 10⁹ Ω·cm. The crystals were grown from the melt with volume over several cubic centimeters and have a low thermal conductivity of 0.6 W m^-1 K^-1. The mobilities for electron and hole carriers were determined to ∼30 cm²/(V s). Using photoemission yield spectroscopy in air (PYSA), we determined the valence band maximum at 5.66 ± 0.05 eV. Under γ-ray exposure, our Schottky-type planar CsPbCl₃ detector achieved an excellent energy resolution (∼16% at 122 keV) accompanied by a high figure-of-merit hole mobility-lifetime product (3.2 × 10^-4 cm²/V) and a long hole lifetime (16 μs). The results demonstrate considerable defect tolerance of CsPbCl₃ and suggest its strong potential for γ-radiation and X-ray detection at room temperature and above.