Graphical Cerium-ion doped lead-free double perovskite crystals (Cs 2 NaTbCl 6 ), were found to have significantly improved sensitivity and the double perovskite crystals (Ce : Cs 2 NaTbCl 6 ) showed excellent ability to resist X-ray radiation damage. In addition the composite film of Ce : Cs 2 NaTbCl 6 crystals can reach a detection limit of 30 nGy ⋅ s −1 of X-ray detector, with the capability to clearly distinguishing the spatial resolution of 10 lp/mm. Scintillators are widely used for nondestructive testing, nuclear medicine imaging, space exploration and security inspection. Recently, lead halide perovskite scintillation crystals have been brought into focus due to their effective atomic number, fast scintillation decay time, strong luminous efficiency, and tunable band gap. However, their application is limited by lead toxicity. Here we report that Ce-doping can increase sensitivity in lead-free double perovskite crystals (Cs 2 NaTbCl 6 ) for X-ray detection and imaging. The introduction of Ce ions as sensitizer can be used to improve the radioluminescence of the crystals. The light output of Ce : Cs 2 NaTbCl 6 crystals is about 52153 ph/MeV, which is 25 % higher than that of un-doped crystal. The X-ray sensitivity is significantly enhanced. Based on our scintillation film X-ray detector the detection limit is 30 nGy ⋅ s −1 , which is about 1/183 of the typical medical imaging dose. Our scintillating film has excellent imaging ability with spatial resolution of up to 10 lp/mm. This research shows that Ce : Cs 2 NaTbCl 6 perovskite crystal scintillators are promising materials for X-ray imaging application.
Rare earth-based halide double perovskites are regarded as an emerging class of X-ray scintillation materials. However, the majority of related scintillator applications are still focused on single crystal and powder systems; the application of nanocrystal (NC) scintillators is rarely reported. Here, we present the synthesis of high-purity Cs2NaTbCl6 NCs by an improved hot-injection method. Interestingly, hollow Cs2NaTbCl6 NCs are observed, the monitoring of the growth process indicates that micrometer-sized NaCl is the initial product, and then the NaCl would convert into Cs2NaTbCl6 NCs through the diffusion of Cs+ and Tb3+ into NaCl lattice, and the faster outward diffusion of Na+ results in the formation of hollow NCs. The double perovskite NCs exhibit green light emission, and the photoluminescence intensity can be significantly enhanced through Ce3+ doping. In particular, the Cs2NaTbCl6:5%Ce3+ scintillator exhibits a linear response and a low detection limit of 79.09 nGy/s when exposed to X-rays. Furthermore, a flexible scintillator film for X-ray imaging is prepared by mixing NCs with polymer, showing a high spatial resolution imaging capability of 10 lp/mm. This work provides a new strategy for hollow perovskite NCs and may shed light on the synthesis of related hollow NCs and their applications in X-ray detection.
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