Novel Sol-Gel Route to Prepare Eu³⁺-Doped 80SiO₂-20NaGdF₄ Oxyfluoride Glass-Ceramic for Photonic Device Applications

Oxyfluoride glass-ceramics (OxGCs) with the molar composition 80SiO₂-20(1.5Eu³⁺: NaGdF₄) were prepared with sol-gel following the "pre-crystallised nanoparticles route" with promising optical results. The preparation of 1.5 mol % Eu³⁺-doped NaGdF₄ nanoparticles, named 1.5Eu³⁺: NaGdF₄, was optimised and characterised using XRD, FTIR and HRTEM. The structural characterisation of 80SiO₂-20(1.5Eu³⁺: NaGdF₄) OxGCs prepared from these nanoparticles' suspension was performed by XRD and FTIR revealing the presence of hexagonal and orthorhombic NaGdF₄ crystalline phases. The optical properties of both nanoparticles' phases and the related OxGCs were studied by measuring the emission and excitation spectra together with the lifetimes of the ⁵D₀ state. The emission spectra obtained by exciting the Eu³⁺-O^2- charge transfer band showed similar features in both cases corresponding the higher emission intensity to the ⁵D₀→⁷F₂ transition that indicates a non-centrosymmetric site for Eu³⁺ ions. Moreover, time-resolved fluorescence line-narrowed emission spectra were performed at a low temperature in OxGCs to obtain information about the site symmetry of Eu³⁺ in this matrix. The results show that this processing method is promising for preparing transparent OxGCs coatings for photonic applications.