Origin of giant permittivity and high-temperature dielectric anomaly behavior in Na0.5Y0.5Cu3Ti4O12 ceramics

Abstract

Na0.5Y0.5Cu3Ti4O12 ceramics prepared by the conventional solid-state reaction method under various sintering conditions were found to exhibit a giant dielectric constant over 10 000 around room temperature. Two electrical responses were observed in the combined modulus and impedance plots, indicating the presence of Maxwell-Wagner relaxation. The contributions of semiconducting grains and insulating grain boundaries (corresponding to high-frequency and low-frequency electrical response, respectively) played important roles in the dielectric properties of Na0.5Y0.5Cu3Ti4O12 ceramics. The correlations between grain boundaries resistance and low frequency dielectric loss, grains resistance and the position of dielectric loss peak were addressed. Mixed-valent structures of Cu2+/Cu3+ and Ti3+/Ti4+ had been determined using X-ray photoelectron spectroscopy. Electron hopping between Cu2+ and Cu3+ and electron transport in Ti3+–O–Ti4+ paths were proposed as the origin of the semiconducting nature of Na0.5Y0.5Cu3Ti4O12 ceramics. In particular, high-temperature dielectric anomaly behavior was investigated in detail. A dielectric peak exhibiting relaxor-like behavior was observed around 200 °C, which was linked with the formation of oxygen vacancies. Based on the electric modulus results, this behavior was explored in the light of the defect formation and explained in terms of a competition process depending on the combinational contribution to polarization between n- and p-type carriers rather than a relaxation process.