Robust Thermal Neutron Detection by LiInP₂Se₆ Bulk Single Crystals

Direct neutron detection based on semiconductor crystals holds promise to transform current neutron detector technologies and further boosts their widespread applications. It is, however, long impeded by the dearth of suitable materials in the form of sizeable bulk crystals. Here, high-quality centimeter-sized LiInP₂Se₆ single crystals are developed using the Bridgman method and their structure and property characteristics are systematically investigated. The prototype detectors fabricated from the crystals demonstrate an energy resolution of 53.7% in response to α-particles generated from an ²⁴¹Am source and robust, well-defined response spectra to thermal neutrons that exhibit no polarization or degradation effects under prolonged neutron/γ-ray irradiation. The primary mechanisms of Se-vacancy and In_Li antisite defects in the carrier trapping process are also identified. Such insights are critical for further enhancing the energy resolution of LiInP₂Se₆ bulk crystals toward the intrinsic level (≈8.6% as indicated by the chemical vapor transport-grown thin crystals). These results pave the way for practically adopting LiInP₂Se₆ single crystals in new-generation solid-state neutron detectors.