Dielectric properties and impedance spectroscopy of NASICON type Na$_3$Zr$_2$Si$_2$PO$_{12}$

Abstract

We report the temperature dependent dielectric properties and impedance spectroscopy investigation of Na$_3$Zr$_2$Si$_2$PO$_{12}$ in the frequency range of 20 Hz--2 MHz. The Rietveld refinement of x-ray diffraction pattern confirms the monoclinic phase with C2/c space group. The {\it d.c.} resistivity behavior shows its strong insulating nature at low temperatures, and follows Arrhenius law of thermal conduction with an activation energy of 0.68 eV. The decrease in electric permittivity ($\epsilon_r$) with frequency is explained based on the space polarization mechanism and its increment with temperature by thermal activation of charge carriers. The dielectric loss (D=tan$\delta$) peak follows the Arrhenius law of thermal activation with an energy of 0.25 eV. We observe an enhancement in {\it a.c.} conductivity with frequency and temperature due to the decrease in the activation energy, which results in enhancing the conduction between defect states. Further, we observe an abrupt increase in the {\it a.c.} conductivity at high frequencies, which is explained using the universal Jonschers power law. The analysis of {\it a.c.} conductivity shows two types of conduction mechanisms namely correlated barrier hopping and non-overlapping small polaron tunnelling in the measured temperature range. The imaginary part of the electric modulus confirms the non-Debye type relaxation in the sample. The shifting of the relaxation peak towards higher frequency side with an increase in temperature ensures its thermally activated nature. The scaling behavior of the electric modulus shows similar type of relaxation over the measured temperature range. The combined analysis of electric modulus and impedance with frequency shows the short-range mobility of charge carriers.