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The origin of giant dielectric relaxation behavior and related electrical properties of grains and grain boundaries (GBs) of W6+-doped CaCu3Ti4O12 ceramics were studied using admittance and impedance spectroscopy analyses based on the brick–work layer model. Substitution of 1.0 at. % W6+ caused a slight decrease in GB capacitance, leading to a small decrease in the low-frequency dielectric constant. Surprisingly, W6+ doping ions have remarkable effects on the macroscopic dielectric relaxation and electrical properties of grains. X-ray photoelectron spectroscopy analysis suggested that the large enhancements of grain resistance and conduction activation energy of grains for the W6+-doped CaCu3Ti4O12 ceramic are caused by reductions in concentrations of Cu3+ and Ti3+ ions. Considering variation of dielectric properties together with changes in electrical properties of the W6+-doped CaCu3Ti4O12 ceramic, correlation between giant dielectric properties and electrical responses of grains and GBs can be described well by the internal barrier layer capacitor model. This model can ascribe mechanisms related to giant dielectric response and relaxation behavior in CaCu3Ti4O12 ceramics.

Giant dielectric permittivity (Li, Ti)-doped NiO (LTNO) ceramics are prepared by a simple PVA sol–gel method. The dielectric properties are investigated as a function of frequency (102–106 Hz) at different temperatures (233–473 K). The concentration of Li has a remarkable effect on the dielectric properties of the LTNO ceramics. The modified Cole–Cole equation, including the conductivity term, is used to describe the experimental dielectric spectra of a high permittivity response with excellent agreement over a wide range of frequencies (103–106 Hz) and temperatures (233–313 K). A frequency dielectric dispersion phenomenon in an LTNO ceramic is also analyzed by impedance spectroscopy. A separation of the grain and grain boundary properties is achieved using an equivalent circuit model. The grain and grain boundary conduction and the dielectric relaxation time of the Li0.05Ti0.02Ni0.93O follows the Arrhenius law associated with estimated activation energies of 0.216, 0.369 and 0.391 eV, respectively. Through the analysis by the modified relaxation model and impedance spectroscopy, it is strongly believed that the high dielectric permittivity response of the LTNO is not only contributed by the space charge polarization (Maxwell–Wagner polarization) mechanism at low frequency regions, but also by the defect-dipole polarization mechanism at high frequency regions.