Dielectric nonlinearity and spontaneous polarization of KTa1xNbxO3 in the diffuse transition range

Abstract
KTa1x Nbx O3 (KTN) in an intermediate-concentration range (x=15.7%) has been studied using dielectric-constant and spontaneous-polarization measurements. A large peak in the dielectric constant (εmax≃70 000) is observed at the temperature Tc*. From room temperature down to Tc*+20 K, ε obeys a Curie-Weiss law with T0∼142.3 K. Below, ε deviates from this law and P-E hysteresis loops are observed. These results indicate that the phase transition exhibits a diffuse character which is related to the appearance of microscopic polarized regions or cells. The ε peak at Tc* exhibits a cusp shape and becomes flattened upon application of low dc-bias fields. A corresponding dielectric loss peak is also observed, the position of which reveals the relaxational character of the transition. Through measurements of ε(E,T) for different dc-bias fields, we have characterized the dielectric nonlinearities in the transition range; the first nonlinear coefficient, ε(2), diverges in two distinct ranges, as (T-Tc* )n, with n∼9 initially and with n≃2 closer to Tc*. These results suggest that diffuse phase transitions in mixed ferroelectrics are due to the ordering of polar cells modified by mutual strain interactions.