A Universal Doping Strategy for Boosting Luminescence Efficiency of Blue-Emitting Hybrid Zn Halides as Ultrastable and Underwater Scintillators

IF 13.7 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhi-Wei Chen, Na Lin, Xin-Yue Zhang, Yu-Sha Yan, Li Xiao, Yi-Fan Wu, Cheng-Yang Yue, Dongpeng Yan, Xiao-Wu Lei
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Abstract

Underwater blue-emitting X-ray scintillator is important for the resource exploration and communication in deep sea, but remains a significant challenge for perovskites. Herein, we proposed a universal Pb2+-doping strategy toward a family of stable 0D Zn halide AnZnBr4 realizing highly efficient blue-emitting scintillation. First-principles calculations indicate that doped-Pb2+ introduced extremely narrow impurity bands, which prompt more carriers into conduction bands, leading to near-unity PLQY. Meanwhile, these halides can withstand complex aqueous solutions containing various chemical substances in wide pH range (1–14) demonstrating ultrahigh water-resistance stabilities. More significantly, these halides exhibit satisfactory scintillation and imaging performance with highest light yield (31,500 photons MeV−1), low detection limit (141.2 nGyair s−1) and large spatial resolution (15.10 lp/mm), ranking among the top-performing Zn halide scintillators reported to date. The high water-resistance stabilities and satisfactory scintillation performance endow these halides advanced underwater X-ray imaging. This work not only provides a universal strategy to explore highly-efficient blue-emitting perovskite scintillators, but also realizes application of high-resolution X-ray imaging in underwater environment.

Abstract Image

一种提高蓝光杂化卤化锌超稳定水下闪烁体发光效率的通用掺杂策略
水下蓝光x射线闪烁体对深海资源勘探和通信具有重要意义,但对钙钛矿来说仍然是一个重大挑战。在此,我们提出了一种通用的Pb2+掺杂策略,用于稳定的0D卤化锌家族AnZnBr4,实现高效的蓝色闪烁。第一性原理计算表明,掺杂的pb2 +引入了极窄的杂质带,促使更多的载流子进入导带,导致接近统一的PLQY。同时,这些卤化物可以在宽pH范围(1-14)内承受含有各种化学物质的复杂水溶液,表现出超高的耐水性稳定性。更重要的是,这些卤化物具有令人满意的闪烁和成像性能,具有最高的产光量(31,500光子MeV−1),低检测限(141.2 nGyair s−1)和大空间分辨率(15.10 lp/mm),是迄今为止报道的表现最好的卤化锌闪烁体之一。高耐水稳定性和令人满意的闪烁性能使这些卤化物具有先进的水下x射线成像能力。这项工作不仅为探索高效蓝光钙钛矿闪烁体提供了一种通用策略,而且实现了高分辨率x射线成像在水下环境中的应用。
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来源期刊
CiteScore
17.40
自引率
0.00%
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审稿时长
7 weeks
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