Defect Dynamics Governed Radiation Hardness in Single-Crystal CsPbBr₃ γ-Ray Detectors

CsPbBr₃ is a reliable and cost-effective semiconductor material with significant potential for radiation detection applications. However, a crucial challenge is maintaining both high performance and radiation stability, particularly under extreme irradiation conditions. Here, the intrinsic origin of the exceptional radiation hardness of CsPbBr₃ single-crystal detectors is revealed by integrating performance changes with the evolution of point defects. It is shown that the detectors maintain exceptional radiation hardness under ⁶⁰Co γ-radiation (1.17 and 1.33 MeV) doses as high as 5 Mrad, with the crystal structure remaining stable, and no degradation, decomposition or phase segregation is observed. The combination of pulse height spectra response and deep level transient spectroscopy demonstrates that CsPbBr₃ detectors exhibit a self-healing capability through efficient defect migration at room temperature. Low-dose irradiation (≤500 krad) passivates intrinsic defects and reduces trap density, while high-dose irradiation (≥1 Mrad) generates new defects and degrades energy resolution. The self-healing behavior is attributed to the defect repair mechanism of radiation-induced damage in CsPbBr₃ through efficient defect migration. These findings position CsPbBr₃ as a leading candidate for radiation-hardened applications and provide critical insights into self-healing semiconductor materials for extreme environments.