Distinct magnetic contributions for magnetoelectric coupling at room temperature in perovskite PZT-PFN solid solutions

Although a high technological interest, there are only a few single-phase solid solutions that exhibit multiferroic and magnetoelectric coupling at room temperature. In this work, such characteristics are reported for PZT-xPFN solid solutions. It is noticed that magnetoelectric coupling and its nature are anomalously dependent on the PFN concentration, resulting from linear magnetoelectric and paramagnetoelectric contributions. The origin of the multiferroicity and the magnetoelectric coupling is explained by considering the presence and evolution of complex defects and magnetic nanoregions caused by PFN addition. For the lower PFN (x = 0.10), the magnetic order is related to Fe-Vo complex defects. For intermediary Fe-Nb concentration (0.15 < x < 0.25), the equimolar Fe-Nb and well-distributed Fe3+ ions result in a paramagnetic system, without linear magnetoelectric coupling. Finally, for higher Fe-Nb concentrations (0.30 < x < 0.35), the magnetic order is related to the existence of Fe-rich nanoregions, resulting in a linear magnetoelectric coupling three times smaller than that measured for lower PFN content.(c) 2022 Elsevier B.V. All rights reserved.