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Effect of partial nitridation on the dielectric constant of A5Ta4O15 (A=Sr, Ba)
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The anion lattice of dielectric oxides A5Ta4O15 (A=Sr, Ba) were modified using a mild ammonolysis treatment, which led to A5Ta4O15–3xN2x. N-doping was examined by varying the ammonolysis temperature and time in the ranges of 1023–1173 K and 2–20 h, respectively. Using sintered ceramics of A5Ta4O15, N-doping could be achieved up to 2x≈0.4 for both Sr5Ta4O15–3xN2x and Ba5Ta4O15–3xN2x. The nitridation of A5Ta4O15 was not accompanied by a significant change in the crystal structure but a substantial evolution of the electronic structure was observed, as indicated by the marked shift in the band gap. Capacitance measurements revealed a ≈50% increase in the dielectric constants (κ) of A5Ta4O15 upon N-doping. At 100 kHz and 295 K, κ was measured to be 37 for Sr5Ta4O15, 54 for Sr5Ta4O14.4N0.4, 26 for Ba5Ta4O15, and 43 for Ba5Ta4O14.4N0.4. All the Sr5Ta4O15, Ba5Ta4O15, and Ba5Ta4O14.4N0.4 displayed temperature-stable dielectric behavior in the range, 30–450 K. On the other hand, Sr5Ta4O14.4N0.4 exhibited a rapid increase in κ with increasing temperature, suggesting strong lattice anharmonicity.

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