Owing to the combination of good thermo-optical properties and inhomogeneously broadened fluorescence spectra suitable for ultrashort laser pulse generation, rare-earth doped solid solutions of sesquioxides (Y,Lu,Sc)2O3 have attracted considerable interest in recent years. In this study, compositionally disordered Tm3+-doped YScO3 transparent ceramic was fabricated using solid-state vacuum sintering of nanopowder produced using laser ablation of solid target in air flow. The as-synthesized powder consisted of weakly aggregated spherical particles having 20 nm diameter and a mostly monoclinic (space group C2/m) crystal structure, whose symmetry was transformed into cubic (space group Ia-3) by calcination at 1050 °C. From high resolution transmission electron microscopy (HRTEM) and energy dispersive X-ray analysis (EDX), we observed a homogeneous distribution of components both throughout individual nanoparticles and 100-nm-thick ceramic foil resulting in high structural and optical quality of the obtained samples. The sintered ceramic featured an optical transmission of 77% at 600 nm and above 81% near 2 μm, an average grain size of 24.2 μm and a content of scattering centers of 26.1 ppm. The absorption spectra at several temperatures, from 93 K to 293 K, were measured and the corresponding absorption coefficients were obtained by Lambert-Beer formula in the range from 600 nm to 900 nm and from 1400 nm to 2100 nm. In particular, the room temperature absorption cross section at 794 nm and 1634 nm were determined to be σabs = 4.25 × 10−21 cm2 and σabs = 5.01 × 10−21 cm2 respectively. Concerning the emission cross section it was calculated by Fuchtbauer-Ladenburg equation starting from the fluorescence spectrum acquired at the laser work temperature: at 1951 nm and 2106 nm corresponding to the main two emission peaks belonging the curve, it was found σem = 9.2 × 10−21 cm2 and σem = 4.9 × 10−21 cm2, respectively. Finally, it was tested the laser behavior of the ceramic: pumped at 793 nm in quasi-CW mode it delivered 1.27 W of output power with a slope efficiency of 10.33% at 2081 nm. The tunability curve spans from 1942 nm to 2110 nm (i.e. 168 nm).
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