Influence of core size on the upconversion luminescence properties of spherical Gd_2O_3:Yb~(3+)/Er~(3+)@SiO_2 particles with core-shell structures

摘要

Spherical SiO_2 particles with different sizes (30, 80, 120, and 180nm) have been coated with Gd_2O_3:Yb~(3+)/Er~(3+) layers by a heterogeneous precipitation method, leading to the formation of core-shell structural Gd_2O_3:Yb~(3+)/Er~(3+)@SiO_2 particles. The samples were characterized by using X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, upconversion (UC) emission spectra, and fluorescent dynamical analysis. The obtained core-shell particles have perfect spherical shape with narrow size distribution. Under the excitation of 980 nm diode laser, the core-shell samples showed size-dependent upconversion luminescence (UCL) properties. The inner SiO_2 cores in core-shell samples were proved to have limited effect on the total UCL intensities of Er~(3+) ions. The UCL intensities of core-shell particles were demonstrated much higher than the values obtained in pure Gd_2O_3:Yb~(3+)/Er~(3+) with the same phosphor volume. The dependence of the specific area of a UCL shell on the size of its inner SiO_2 particle was calculated and analyzed for the first time. It was confirmed that the surface effect came from the outer surfaces of emitting shells is dominant in influencing the UCL property in the core-shell samples. Three-photon UC processes for the green emissions were observed in the samples with small sizes of SiO_2 cores. The results of dynamical analysis illustrated that more nonradiative relaxation occurred in the core-shell samples with smaller SiO_2 core sizes.