Selection and Optimization of a K_0.5Na_0.5NbO₃-Based Material for Environmentally-Friendly Magnetoelectric Composites

Li- and Ta-modified K ${}_{0.5}$ Na ${}_{0.5}$ NbO ${}_3$ compounds are among the most promising lead-free ferroelectrics for high-sensitivity piezoelectric ceramic materials, and are potentially capable of replacing Pb(Zr,Ti)O ${}_3$ . They are also being investigated as piezoelectric components in environmentally friendly magnetoelectric composites. However, most suitable modifications for this application have not been identified. We report here a simulation study of how the magnetoelectric voltage responses of layered composite structures based on Li ${}_x$ (K ${}_{0.5}$ Na ${}_{0.5}$ ) ${}_{1-x}$ Nb ${}_{1-y}$ Ta ${}_y$ O ${}_3$ varies with the chemical composition of the piezoelectric. Instead of relying on material coefficients from the literature, which would have required using different sources, an ad hoc set of materials was prepared. This demanded tailoring preparation by conventional means to obtain dense ceramics while controlling alkali volatilization, perovskite phase and microstructure, as well as characterizing their dielectric, elastic and electromechanical properties. This provided the set of relevant material coefficients as a function of composition, which was used to obtain the magnetoelectric responses of model layered structures including a reference magnetostrictive spinel oxide by simulation. The piezoelectric material leading to the highest magnetoelectric coefficient was identified, and shown to be different to that showing the highest piezoelectric coefficient. This reflects the dependence of the magnetoelectric response on all material coefficients, along with the complex interplay between composition, processing and properties in K ${}_{0.5}$ Na ${}_{0.5}$ NbO ${}_3$ -based ceramics.