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MgO-doped stoichiometric LiTaO3 (MgO:SLT) is one of the most promising nonlinear materials. However, its industrial application is limited by the poor optical quality caused by the nonhomogeneous distribution of magnesium. Herein, an MgO:SLT polycrystalline powder was synthesized with a homogenous magnesium distribution by a wet-chemical spray-drying method. A comparative investigation of the coordination state of Ta ions in MgO:SLT powders synthesized by this method and by a conventional solid-state reaction method was performed by X-ray photoelectron spectroscopy. It is proved that the Ta-Li antisite was completely eliminated as a result of the homogeneous Mg doping in the SLT lattice using the wet-chemical spray-drying method. However, for MgO:LT powder produced by the solid-state reaction method, element analysis after acid treatment shows that some Mg ions did not enter the LT lattice after high-temperature calcination. Also, scanning electron microscopy and transmission electron microscopy energy dispersive spectroscopy verified that some MgO particles still exist in the as-synthesized MgO:LT powder. This synthesis method can be used for mass production of high-quality polycrystalline powders for doped crystal growth and some other doped oxide powder products with high melt point.

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