Significantly improved giant dielectric properties and enhanced nonlinear coefficient of Ni2+ doped CaCu3Ti4O12/CaTiO3 composites.

CaCu3-xNixTi4O12/CaTiO3 ceramic composites were fabricated using initial Ca2Cu2-xNixTi4O12 compositions (x = 0, 0.05, 0.10, and 0.20) to improve the dielectric properties (DPs) of the CaCu3Ti4O12 ceramics. CaCu3Ti4O12 and CaTiO3 phases were confirmed. Microstructural analysis and Rietveld refinement showed that the Ni2+ dopant might substitute the Cu2+ sites of the CaCu3Ti4O12 structure. The average grain sizes of CaCu3Ti4O12 (4.1-5.6 µm) and CaTiO3 (1.2-1.4 µm) changed slightly with the Ni2+ doping concentration. The best DPs were obtained for the CaCu3-xNixTi4O12/CaTiO3 with x = 0.2. The loss tangent was significantly reduced by an order of magnitude compared to that of the undoped composite, from tanδ∼0.161 to ∼0.016 at 1 kHz, while the dielectric permittivity slightly decreased from ε'∼5.7 × 103 to ∼4.0 × 103. Furthermore, the temperature dependence of ε' could be improved by doping with Ni2+. The improved DPs were caused by the enhanced electrical responses of the internal interfaces, which resulted in enhanced non-Ohmic properties. The largest nonlinear coefficient (α∼7.6) was obtained for the CaCu3-xNixTi4O12/CaTiO3 with x = 0.05. Impedance spectroscopy showed that the CaCu3-xNixTi4O12/CaTiO3 composites consisted of semiconducting and insulating components. The DPs of CaCu3-xNixTi4O12/CaTiO3 were explained based on the space-charge polarization at the active-interfaces.