2024年4月18日，福州大学Qiushui Chen研究组在《德国应用化学》杂志发表论文，报道了他们对用于超级X射线成像的纳米晶体亚晶格的能量漏斗动力学的研究。

据了解，由于其独特的转换和存储X射线能量的能力，长期放射发光闪烁体最近引起了研究和工业团体的大量关注。然而，这些纳米晶体的能量转化动力学的测定仍未被探索。

在该文中，团队通过Gd³⁺驱动的微环境工程和Mn²⁺介导的辐射发光分析，研究了NaLuF₄:Mn²⁺/Gd³⁺纳米晶体亚晶格中的能量漏斗动力学。他们的光物理研究揭示了能量漏斗动力学的有效控制，并证明了电子陷阱深度在0.66至0.96 eV之间的可调性，相应的陷阱密度在2.38 × 10⁵至1.34 × 10⁷ cm^-3之间变化。这使得捕获的电子能够在几秒钟到30天的持续时间内被控制释放。此外，它可以在520-580 nm范围内定制辐射发光，并在313-403 K之间微调热激温度。

研究组进一步利用这些闪烁体制造高密度、大面积的闪烁屏幕，其X射线灵敏度提高了6倍，具有22 lp/mm的高分辨率X射线成像和30天的光存储。这使得通过快速热刺激辐射发光，读出受伤小鼠的高对比度成像成为可能。这些发现为辐射发光动力学与能量漏斗动力学的相关性提供了新的见解，从而有助于推进高能纳米光子的应用。

附：英文原文

Title: Probing Energy-Funneling Kinetics in Nanocrystal Sublattices for Superior X-ray Imaging

Author: Qinxia Wu, Xinqi Xu, Xiaokun Li, Hao Jiang, Xian Qin, Zhongzhu Hong, Xiaofeng Chen, Zhijian Yang, Xiangyu Ou, Lili Xie, Yu He, Sanyang Han, Qiushui Chen, Huanghao Yang

Issue&Volume: 2024-04-18

Abstract: Long-lasting radioluminescence scintillators have recently attracted substantial attention from both research and industrial communities, primarily due to their distinctive capabilities of converting and storing X-ray energy. However, determination of energy-conversion kinetics in these nanocrystals remaines unexplored. Here we investigate energy funneling kinetics in NaLuF4:Mn2+/Gd3+ nanocrystal sublattices via Gd3+-driven microenvironment engineering and Mn2+-mediated radioluminescence profiling. Our photophysical studies reveal effective control of energy-funneling kinetics and demonstrate the tunability of electron trap depth ranging from 0.66 to 0.96 eV, with the corresponding trap density varying between 2.38 × 105 and 1.34 × 107 cm-3. This enables controlled release of captured electrons over durations spanning from seconds to 30 days. Furthermore, it allows tailorable radioluminescence emission within the range of 520-580 nm and fine-tuning of thermally-stimulated temperature between 313-403 K. We further utilize these scintillators to fabricate high-density, large-area scintillation screens that exhibit a 6-fold improvement in X-ray sensitivity, 22 lp/mm high-resolution X-ray imaging, and a 30-day-long optical memory. This enables high-contrast imaging of injured mice through fast thermally-stimulated radioluminescence readout. These findings offer new insights into the correlation of radioluminescence dynamics with energy funneling kinetics, thereby contributing to the advancement of high-energy nanophotonic applications.

DOI: 10.1002/anie.202404177

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202404177