Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China.
Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.
Nat Commun. 2021 May 14;12(1):2798. doi: 10.1038/s41467-021-23190-0.
Radiation dosimeters displaying conspicuous response of irradiance are highly desirable, owing to the growing demand of monitoring high-energy radiation and environmental exposure. Herein, we present a case of dosimetry based on a discrete nanocluster, Th(OH)(O)(HO)(HCOO)∙4DMF∙HO (Th-SINAP-100), by judiciously incorporating heavy Th polynuclear centers as radiation attenuator and organic linkers as photo-responsive sensor. Interestingly, dual-module photochromic transitions upon multiple external stimuli including UV, β-ray, and γ-ray are integrated into this single material. The striking color change, and more significantly, the visible color transition of luminescence in response to accumulating radiation dose allow an on-site quantitative platform for naked-eye detection of ionization radiations over a broad range (1-80 kGy). Single crystal X-ray diffraction and density functional theory calculations reveal that the dual-module photochromism can be attributed to the π(TPC) → π*(TPC) intermolecular charge transfer driven by enhanced π-π stacking interaction between the adjacent TPC moieties upon irradiation.
由于对监测高能辐射和环境暴露的需求不断增长,人们非常希望辐射剂量计能够显示出明显的辐照度响应。在此,我们提出了一种基于离散纳米团簇Th(OH)(O)(HO)(HCOO)∙4DMF∙HO(Th-SINAP-100)的剂量测定方法,巧妙地将重 Th 多核中心作为辐射衰减剂,将有机配体作为光响应传感器。有趣的是,这种单一材料中集成了双模块光致变色跃迁,可响应多种外部刺激,包括 UV、β射线和γ射线。显著的颜色变化,更重要的是,发光的可见颜色随累积辐射剂量的变化,可以实现在线定量检测宽范围(1-80 kGy)内的电离辐射。单晶 X 射线衍射和密度泛函理论计算表明,双模块光致变色可归因于相邻 TPC 部分之间增强的π-π堆积相互作用驱动的[TPC]→[TPC]*分子内电荷转移。