Transparent crystallized glass with a surface crystallization layer of sub-millimeter thickness was found in the glass compositions of 35BaO–15TiO2–50GeO2 (BTG50), 28BaO–18TiO2–54SiO2 (BTS54), and 35SrO–20TiO2–45SiO2 (STS45), and the precipitated fresnoite-type crystalline phase showed nonlinear optical properties. XRD measurements confirmed that BTS54 and STS45 crystallized glasses precipitate as a single phase of the fresnoite-type crystallites Ba2TiSi2O8 and Sr2TiSi2O8, respectively. On the other hand, BTG50 crystallized glass precipitated two phases with mainly fresnoite-type BTG, Ba2TiGe2O8 and BaGe4O9. The results of the XRD analysis of STS45 crystallized glass demonstrated high crystal orientation in the (002) direction from the glass surface.
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