Ferroic glass behavior in (Bi,Na)TiO3-based lead-free electroceramics

Abstract

Ferroic glass materials, that is, relaxors, spin glasses, and strain glasses attract special attention because of their intriguing physical properties and potential for novel technological applications. Here, several characterization techniques are used to demonstrate the occurrence of simultaneous relaxor and strain glass states in the ternary lead-free xBi0.5Na0.5TiO3-yBi0.5K0.5TiO3-zBaTiO3 (BNBK) system. Hysteresis and current density loops measurements at different temperatures for a BNBK ceramic showed typical characteristics observed in BNT based ceramics containing the tetragonal P4bm phase. Above 400 K, slim loops like those of ferroelectric relaxors are observed. A phase transition with simultaneous relaxor and strain glass character is revealed by the dielectric and anelastic characterizations, which opens up a wide spectrum of possible applications. The minimum of elastic modulus shifts to higher temperatures as the frequency increases, obeying the Vogel-Fulcher relation, which clearly shows the occurrence of a strain glass state in this material. Similar characteristics are observed in the imaginary part of the dielectric permittivity, which demonstrates the relaxor character of this phase transition. The origin of this phenomenon was elucidated with the help of structural characterizations, such as Raman spectroscopy and high-resolution synchrotron X-ray diffraction, at different temperatures. This work provides an in-depth understanding of the structural changes that determine the phenomenology behind the observed ferroic glass behavior and the ferroelectric, dielectric, and mechanical properties of this ternary ceramic composition.