We investigated the microstructure, crystal structure, dielectric, and elecromechanical strain properties of lead-free BaTiO₃ (BT)-modified (Bi_1/2Na_1/2)TiO₃-SrTiO₃ (BNT-ST) piezoelectric ceramics. Samples were prepared by a conventional ceramic processing route. Temperature dependent dielectric properties confirmed that a phase transition from a nonergodic relaxor to an ergodic relaxor was induced when the BT concentration reached 1.5 mol%, interestingly, where the average grain size reached a maximum value of 4.5 μm. At the same time, enhanced electromechanical strain (S_max/E_max = 600 pm/V) was obtained. It is suggested that the induced ferroelectric-relaxor phase transition by the BT modification is responsible for the enhancement of electromechanical strain in 1.5 mol% BT-modified BNT-ST ceramics.

Bulk-sized PbTiO₃ (PT), which is widely known as a high-performance ferroelectric oxide but cannot be fabricated into a monolithic ceramic due to its high c/a ratio, was successfully prepared with a high tetragonality by partially substituting Ni ions for Pb ions using a solid-state reaction method. We found that Ni-doped PT was well-fabricated as a bulk monolith with a significant c/a ratio of ~1.06. X-ray diffraction on as-sintered and crushed samples revealed that NiTiO₃ secondary phase was present at the doping level of more than 2 at.%. Scanning electron microscopic study showed that NiTiO₃ secondary phase grew on the surface of PT specimens regardless of the doping level possibly due to the evaporation of Pb during sintering. We demonstrated that an unconventional introduction of Ni ions into A-site plays a key role on the fabrication of bulk PT, though how Ni ion functions should be studied further. We expect that this study contributes to a further development of displacive ferroelectric oxides with a high c/a ratio.

We investigated the origin of magnetic behaviors induced by an asymmetric spin exchange interaction in Fe-site engineered lead iron niobate [Pb(Fe_1/2Nb_1/2)O₃, PFN], which exhibits a room-temperature multiferroicity. The magnitude of spin exchange interaction was regulated by the introduced transition metals with a distinct Bohr magneton, i.e., Cr, Co, and Ni. All compositions were found to have a single-phase perovskite structure keeping their ferroelectric order except for Cr introduction. We discovered that the incorporation of each transition metal imposes a distinct magnetic behavior on the lead iron niobate system; antiferro-, hard ferro-, and soft ferromagnetism for Cr, Co, and Ni, respectively. This indicates that orbital occupancy and interatomic distance play key roles in the determination of magnetic behavior rather than the magnitude of the individual Bohr magneton. Further investigations are planned, such as X-ray absorption spectroscopy, to clarify the origin of magnetic properties in this system.