Li Huwei, Li Kai, Li Zheyu, Fu Xinyu, Yang Qingxing, Wang Nan, Wang Xinyu, Feng Jing, Song Shuyan, Zhang Hongjie
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, China.
Light Sci Appl. 2025 May 14;14(1):195. doi: 10.1038/s41377-025-01839-5.
Lanthanide (Ln)-based metal halides with excellent luminescence properties, large Stokes shifts, and low toxicity have aroused wide attention as scintillators for X-ray imaging. However, the lack of fast and mild synthesis methods of Ln-based metal halides, as one of the technical challenges, limits their applications. Here, benefiting from the innovative selection of methanol and ethanol as the solvent and anti-solvent, respectively, a series of CsLnCl (Ln = Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu) microcrystals (MCs) were prepared via the recrystallization method at room temperature for the first time. This recrystallization method could also realize large-scale production at one time and recyclable recrystallization of single-element MCs and the preparation of high-entropy five-element Cs{TbDyHoErTm}Cl crystals. Among these CsLnCl MCs, CsTbCl MCs with 4f → 5d absorption transition possess the highest photoluminescence quantum yield of 90.8%. Besides, under X-ray irradiation, CsTbCl MCs show a high light yield of ~51,800 photons MeV and the as-fabricated thin films possess promising X-ray imaging ability and excellent spatial resolutions (12 lp mm). This work provides a new method for ultrafast preparing Ln-based metal halides under mild synthetic conditions and highlights their excellent potential as scintillators for X-ray imaging.
具有优异发光性能、大斯托克斯位移和低毒性的镧系（Ln）基金属卤化物作为X射线成像闪烁体引起了广泛关注。然而，作为技术挑战之一，缺乏快速温和的Ln基金属卤化物合成方法限制了它们的应用。在此，分别得益于创新性地选择甲醇和乙醇作为溶剂和反溶剂，首次通过重结晶法在室温下制备了一系列CsLnCl（Ln = Ce、Pr、Nd、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Lu）微晶（MCs）。这种重结晶方法还可以一次性实现大规模生产以及单元素MCs的可循环重结晶，并制备高熵五元Cs{TbDyHoErTm}Cl晶体。在这些CsLnCl MCs中，具有4f → 5d吸收跃迁的CsTbCl MCs具有90.8%的最高光致发光量子产率。此外，在X射线照射下，CsTbCl MCs显示出约51,800光子/MeV的高光产率，并且所制备的薄膜具有良好的X射线成像能力和出色的空间分辨率（12 lp mm）。这项工作为在温和合成条件下超快制备Ln基金属卤化物提供了一种新方法，并突出了它们作为X射线成像闪烁体的优异潜力。
