Zhao Xue, Fu Pengfei, Li Pan, Du Hainan, Zhu Jinsong, Ge Ciyu, Yang Longbo, Song Boxiang, Wu Haodi, Jin Tong, Guo Qingxun, Wang Liang, Li Jinghui, Xiao Zewen, Chang Jingjing, Niu Guangda, Luo Jiajun, Tang Jiang
School of Microelectronics, Xidian University, Xi'an 710071, China.
Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China.
Research (Wash D C). 2023 May 5;6:0125. doi: 10.34133/research.0125. eCollection 2023.
Lead halide perovskite nanocrystals have recently demonstrated great potential as x-ray scintillators, yet they still suffer toxicity issues, inferior light yield (LY) caused by severe self-absorption. Nontoxic bivalent europium ions (Eu) with intrinsically efficient and self-absorption-free transition are a prospective replacement for the toxic Pb. Here, we demonstrated solution-processed organic-inorganic hybrid halide BAEuI (BA denotes CHNH) single crystals for the first time. BAEuI was crystallized in a monoclinic space group of 2/, with photoactive sites of [EuI] octahedra isolated by BA cations, which exhibited high photoluminescence quantum yield of 72.5% and large Stokes shift of 97 nm. These properties enable an appreciable LY value of 79.6% of LYSO (equivalent to ~27,000 photons per MeV) for BAEuI. Moreover, BAEuI shows a short excited-state lifetime (151 ns) due to the parity-allowed transition, which boosts the potential of BAEuI for use in real-time dynamic imaging and computer tomography applications. In addition, BAEuI demonstrates a decent linear scintillation response ranging from 9.21 μGy s to 145 μGy s and a detection limit as low as 5.83 nGy s. The x-ray imaging measurement was performed using BAEuI polystyrene (PS) composite film as a scintillation screen, which exhibited clear images of objects under x-ray irradiation. The spatial resolution was determined to be 8.95 lp mm at modulation transfer function = 0.2 for BAEuI/PS composite scintillation screen. We anticipate that this work will stimulate the exploration of transition lanthanide metal halides for sensitive x-ray scintillators.
近年来,卤化铅钙钛矿纳米晶体作为X射线闪烁体展现出巨大潜力,然而它们仍存在毒性问题,且由于严重的自吸收导致光产额(LY)较低。具有本征高效且无自吸收跃迁的无毒二价铕离子(Eu)有望替代有毒的Pb。在此,我们首次展示了通过溶液法制备的有机-无机杂化卤化物BAEuI(BA表示CHNH)单晶。BAEuI结晶于单斜空间群2/,其中[EuI]八面体的光活性位点被BA阳离子隔离,其表现出72.5%的高光致发光量子产率和97 nm的大斯托克斯位移。这些特性使得BAEuI的可观光产额值达到LYSO的79.6%(相当于每兆电子伏特约27,000个光子)。此外,由于宇称允许跃迁,BAEuI的激发态寿命较短(151 ns),这提升了BAEuI在实时动态成像和计算机断层扫描应用中的潜力。此外,BAEuI在9.21 μGy s至145 μGy s范围内表现出良好的线性闪烁响应,检测限低至5.83 nGy s。使用BAEuI聚苯乙烯(PS)复合膜作为闪烁屏进行了X射线成像测量,该复合膜在X射线照射下呈现出清晰的物体图像。对于BAEuI/PS复合闪烁屏,在调制传递函数 = 0.2时,空间分辨率确定为8.95 lp mm。我们预计这项工作将激发对用于灵敏X射线闪烁体的跃迁镧系金属卤化物的探索。