Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.093
Publication date: 23rd September 2021
Ionizing radiation, wherever present, e.g., in medicine, nuclear environment, or homeland security, due to its strong impact on biological matter, should be closely monitored. Availability of semiconductor materials with distinctive characteristics required for an efficient high-energy photon detection, especially with high atomic numbers (high Z), in sufficiently large, single-crystalline forms, which would also be both chemically and mechanically robust, is still very limited.
Metal halide perovskite were indeed found to meet all aforementioned key requirements, at an extremely low cost. In this work γ-ray detectors based on crystals of methylammonium lead tribromide (MAPbBr3) equipped with carbon electrodes were fabricated, allowing radiation detection by photocurrent measurements at room temperatures with record sensitivities (333.8 μC Gy-1 cm-2 ). Importantly, the devices operated at low bias voltages (<1.0 V), which may enable future low-power operation in energy-sparse environments, including space. The detector prototypes were exposed to radiation from a 60Co source at dose rates up to 2.3 Gy h-1 under ambient and operational conditions for over 100 h, without any sign of degradation. We postulate that the excellent radiation tolerance stems from the intrinsic structural plasticity of the organic-inorganic halide perovskites, which can be attributed to a defect-healing process by fast ion migration at the nanoscale level.
Furthermore, since the sensitivity of the γ-ray detectors is proportional to the volume of the employed MAPbBr3 crystals, a unique crystal growth technique is introduced, baptized as the “oriented crystal-crystal intergrowth” or OC2G method, yielding crystal specimens with volume and mass of over 1000 cm3 and 3.8 kg, respectively. Large-volume specimens have a clear advantage for radiation detection; however, the demonstrated kilogram-scale crystallogenesis coupled with future cutting and slicing technologies may have additional benefits, for instance, enable the development for the first time of crystalline perovskite wafers, which may challenge the status quo of present and future performance limitations in all optoelectronic applications.
The work was supported by the Swiss National Science Foundation (No. 513733) and the ERC advanced grant “PICOPROP” (Grant No. 670918).