Enhancing the Upconversion Luminescence and Sensitivity of Nanothermometry through Advanced Design of Dumbbell-Shaped Structured Nanoparticles

Abstract

The core-shell engineering of lanthanide-doped nanoparticles has captured considerable attention because it can safeguard the luminescence intensity of the core by reducing surface defects. However, the limited surface area of the traditional spherical core-shell structure hinders the further breakthrough of the brightness. Herein, a unique NaYF₄:Yb³⁺/RE³⁺@NaYF₄:Yb³⁺/RE³⁺@NaNdF₄:Yb³⁺ (RE³⁺ = Ho³⁺ or Er³⁺) dumbbell-shaped multilayer nanoparticle featuring a high surface area is reported. Its upconversion luminescence intensity is higher than that of the conventional spherical core-shell structure. A thorough investigation is performed on the luminescence and thermometric mechanisms of Ho³⁺/Er³⁺ distributed in the core and the first shell. Remarkably, when Ho³⁺/Er³⁺ ions are distributed in the first shell, the relative sensitivity of the biological luminescence nanothermometer composed of downshifting near-infrared emissions is increased to 2.543% K^-1 (328 K), which considerably exceeds most reported values. The increased value is attributed to the more thermal-sensitive phonon-assisted energy transfer. For potential biological applications, dumbbell-shaped nanoparticles (DSNPs) with hydrophilic modification show excellent thermometric performance and high tissue penetration depth. Overall, the insights provided by this work will broaden the scope of novel DSNPs in the fields of luminescence and nanothermometry.