Institute of Nanochemistry and Nanobiology, Shanghai University, Shanghai 200444, China.
Genome Institute of Singapore, Agency of Science Technology and Research, 138672, Singapore.
Nanoscale. 2022 Mar 24;14(12):4595-4603. doi: 10.1039/d1nr07329j.
Lanthanide-doped nanocrystals that simultaneously convert near-infrared (NIR) irradiation into emission of shorter (ultraviolet-C, UVC) and longer wavelengths (NIR) offer many exciting opportunities for application in drug release, photodynamic therapy, deep-tissue bioimaging, and solid-state lasing. However, a formidable challenge is the development of lanthanide-doped nanocrystals with efficient UVC and NIR emissions simultaneously due to their low conversion efficiency. Here, we report a dye-sensitized heterogeneous core-multishell architecture with enhanced UVC emission and NIR emission under 793 nm excitation. This nanocrystal design efficiently suppresses energy trapping induced by interior lattice defects and promotes upconverted UVC emission from Gd. Moreover, a significant downshifting emission from Yb at 980 nm was also observed owing to an efficient energy transfer from Nd to Yb. Furthermore, by taking advantage of ICG sensitization, we realized a largely enhanced emission from the UVC to NIR spectral region. This study provides a mechanistic understanding of the upconversion and downshifting processes within a heterogeneous architecture while offering exciting opportunities for important biological and energy applications.
镧系掺杂纳米晶能够将近红外(NIR)辐射同时转化为较短(紫外-C,UVC)和较长波长(NIR)的发射,为药物释放、光动力疗法、深层组织生物成像和固态激光等应用提供了许多令人兴奋的机会。然而,由于转换效率低,开发同时具有高效 UVC 和 NIR 发射的镧系掺杂纳米晶仍然是一个巨大的挑战。在这里,我们报告了一种染料敏化的异质核壳结构,在 793nm 激发下具有增强的 UVC 发射和 NIR 发射。这种纳米晶设计有效地抑制了内部晶格缺陷引起的能量捕获,并促进了 Gd 的上转换 UVC 发射。此外,由于 Nd 到 Yb 的有效能量转移,还观察到来自 Yb 的显著下转换发射,其位于 980nm。此外,通过利用 ICG 的敏化作用,我们实现了从 UVC 到 NIR 光谱区域的大幅增强发射。本研究为异质结构内的上转换和下转换过程提供了一种机制理解,同时为重要的生物和能源应用提供了令人兴奋的机会。