Rational synthesis of three-dimensional core-double shell upconversion nanodendrites with ultrabright luminescence...

Engineering the morphology of rare-earth doped NaYF₄-based upconversion nanoparticles (UCNPs) can effectively tune their upconversion luminescence emission (UCLE) properties. Herein, we rationally synthesized a new class of three-dimensional upconversion core-double-shell nanodendrites (UCNDs) including an active core (NaYF₄:Yb,Er,Ca) capped by a transition layer (NaYF₄:Yb,Ca) and an active outer shell (NaNdF₄:Yb,Ca). The high concentration of the Nd³⁺ sensitizer in the outer dendritic shell enhances the luminescence intensity, while the transition layer enriched with Yb³⁺ acts as an efficient energy migration network between the outer shell and inner core along with preventing the undesired quenching effects resulting from Nd³⁺. These unique structural and compositional merits enhanced the UCLE of UCNDs by 5 and 15 times relative to NaYF₄:Yb,Er,Ca@NaYF₄:Yb,Ca truncated core-shell UCNPs and NaYF₄:Yb,Er,Ca spherical core UCNPs, respectively, under excitation at 980 nm. The SiO₂-COOH layer coated UCNDs (UCND@SiO₂-COOH) were successfully used as efficient long-term luminescent probes for in vitro and in vivo bioimaging without any significant toxicity. The uptake and retention of UCND@SiO₂-COOH were mostly found in the liver and spleen. This study may open the way towards the preparation of three-dimensional UCND nanostructures for biomedical applications.