Wang Wang, Feng Zhe, Li Bai, Chang Yulei, Li Xu, Yan Xu, Chen Runze, Yu Xiaoming, Zhao Huiying, Lu Geyu, Kong Xianggui, Qian Jun, Liu Xiaomin
State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, FineMechanics and Physics, Chinese Academy of Science, Changchun 130033, China.
J Mater Chem B. 2021 Mar 28;9(12):2899-2908. doi: 10.1039/d0tb02728f. Epub 2021 Mar 16.
Traditional sensitizer (Yb or Nd) and activator (Er) co-doped lanthanide-based nanoprobes possessing emission of Er at 1525 nm have attracted much attention in NIR-IIb bio-imaging. However, the 1525 nm fluorescence efficiency was not high enough in such co-doped systems due to the serious back energy transfer from the activator to the sensitizer, resulting in a lot of excitation energy loss. Herein, we have designed an efficient NIR-IIb nanoprobe Er self-sensitized NaErF:0.5%Tm@NaLuF, where substantially all the excitation energy could contribute to Er ions and most energy transfer processes were confined among Er ions, avoiding the energy dissipation by heterogeneous sensitizer ions. The influence of the types of epitaxial heterogeneous shells, the doping effect and optimal doping concentration of Tm ions, as well as the critical shell thickness for obtaining the surface quenching-assisted downshifting emission are systematically investigated to acquire the most efficient 1525 nm luminescence under 800 nm excitation. The quantum yield in the 1500-1700 nm region reached 13.92%, enabling high-resolution through-skull cerebrovascular microscopy imaging and large-depth in vivo physiological dynamic imaging with an extremely low excitation powder density of 35 mW cm. The designed nanoprobe can be potentially used for brain science research and clinical diagnosis.
传统的敏化剂(镱或钕)和激活剂(铒)共掺杂的基于镧系元素的纳米探针在1525 nm处具有铒的发射,在近红外IIb生物成像中引起了广泛关注。然而,在这种共掺杂体系中,由于激活剂向敏化剂的严重反向能量转移,1525 nm处的荧光效率不够高,导致大量激发能量损失。在此,我们设计了一种高效的近红外IIb纳米探针铒自敏化的NaErF:0.5%Tm@NaLuF,其中基本上所有的激发能量都可以贡献给铒离子,并且大多数能量转移过程都局限于铒离子之间,避免了异质敏化剂离子造成的能量耗散。系统地研究了外延异质壳的类型、铥离子的掺杂效果和最佳掺杂浓度,以及获得表面猝灭辅助下转换发射的临界壳层厚度,以在800 nm激发下获得最有效的1525 nm发光。在1500 - 1700 nm区域的量子产率达到13.92%,能够实现高分辨率的穿颅脑血管显微镜成像和大深度的体内生理动态成像,激发光功率密度极低,仅为35 mW/cm²。所设计的纳米探针具有用于脑科学研究和临床诊断的潜力。