Raman, dielectric and variable range hopping nature of Gd2O3-doped K0.5N0.5NbO3 piezoelectric ceramics

Abstract

(K0.5Na0.5)NbO3 (KNN) + x wt% Gd2O3 (x = 0 -1.5) ceramics have been prepared by conventional solid state reaction method. The effect of Gd2O3 on the structural, microstructural and dielectric properties of KNN ceramics were studied systematically. The effect of Gd2O3 on phase transformation from orthorhombic to psuedocubic structure is explained interms of changes in the internal vibration modes of NbO6 octahedra. The Raman intensity of the stretching mode v1 enhanced and shifted toward higher wavenumber with Gd2O3 concentration, which is attributed to the increase in polarizability and change in the O-Nb-O bond angles. Microstructural analysis revealed that the grain size of the KNN ceramics decreases from 2.26 ± 1.07 μm to 0.35 ± 0.13 μm and becomes homogenous with an increase in Gd2O3 concentration. The frequency dependent dielectric spectra are analyzed by using Havriliak-Negami function. The fitted symmetry parameter and relaxation time (τ) are found to be 0.914 and 8.78 × 10−10 ± 5.5 × 10−11 s, respectively for the sample doped with x = 1.0. The addition of Gd2O3 to the KNN shifted the polymorphic phase transition orthorhombic to tetragonal transition temperature (TO-T) from 199oC to 85oC with enhanced dielectric permittivity (ε′ = 1139 at 1 MHz). The sample with x = 1.0, shown a high dielectric permittivity (ε′ = 879) and low dielectric loss (<5%) in the broad temperature range (-140oC – 150oC) with the Curie temperature 307 oC can have the potential for high temperature piezoelectric and tunable RF circuit applications. The temperature dependent AC-conductivity follows the variable range hopping conduction mechanism by obtaining the slope -0.25 from the ln[ln(ρac)] versus ln(T) graph in the temperature range of 133 K-308 K. The effect of Gd2O3 on the Mott’s parameters such as density of states (N(EF)), hopping length (RH), and hopping energy (WH) have been discussed.