ABSTRACT
Inorganic Bi-based perovskites have shown great potential in X-ray detection for their large absorption to X-rays, diverse low-dimensional structures, and eco-friendliness without toxic metals. However, they suffer from poor carrier transport properties compared to Pb-based perovskites. Here, we propose a mixed-halogen strategy to tune the structural dimensions and optoelectronic properties of Cs3 Bi2 I9-n Brn (0≤n≤9). Ten centimeter-sized single crystals are successfully grown by the Bridgman technique. Upon doping bromine to zero-dimensional Cs3 Bi2 I9 , the crystal transforms into a two-dimensional structure as the bromine content reaches Cs3 Bi2 I8 Br. Correspondingly, the optoelectronic properties are adjusted. Among these crystals, Cs3 Bi2 I8 Br exhibits negligible ion migration, moderate resistivity, and the best carrier transport capability. The sensitivities in 100â keV hard X-ray detection are 1.33×104 and 1.74×104 â µC Gyair -1 cm-2 at room temperature and 75 °C, respectively, which are the highest among all reported bismuth perovskites. Moreover, the lowest detection limit of 28.6â nGyair s-1 and ultralow dark current drift of 9.12×10-9 â nA cm-1 s-1 V-1 are obtained owing to the high ionic activation energy. Our work demonstrates that Br incorporation is an effective strategy to enhance the X-ray detection performance by tuning the dimensional and optoelectronic properties.
ABSTRACT
Halide perovskites are promising candidates for soft X-ray detection (<80 keV) owing to their high X-ray absorption coefficient, resistivity, and mobility lifetime product. However, the lack of large high-quality single crystals (SCs) renders it challenging to manufacture robust hard X-ray imaging systems (>100 keV) with a low detection limit and stable dark current. Herein, high-quality inch-size two-dimensional (2D) Cs3Bi2Br9 (CBB) single crystals are grown from a melt via the Bridgman method. The crystal quality is enhanced by eliminating inclusions of CsBr-rich phases and restraining the trap-state density, leading to an enhanced resistivity of 1.41 × 1012 Ω cm and a mobility lifetime product of 8.32 × 10-4 cm2 V-1. The Au/CBB/Au single-crystal device exhibits a high sensitivity of 1705 µC Gyair-1 cm-2 in all-inorganic bismuth-based perovskites and an ultralow detection limit of 0.58 nGyair s-1 in all of the bismuth-based perovskites for 120 keV hard X-ray detection. The CBB detector exhibits high work stability with an ultralow dark current drift of 2.8 × 10-10 nA cm-1 s-1 V-1 and long-term air environment reliability under a high electric field of 10â¯000 V cm-1 owing to the ultrahigh ionic activation energy of the 2D structure. The proposed robust imaging system based on CBB SC is a promising tool for X-ray medical imaging and diagnostics.
