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.

Multiferroics exhibiting the coexistence and a possible coupling of ferromagnetic and ferroelectric order are attracting widespread interest in terms of academic interests and possible applications. However, room-temperature single-phase multiferroics with soft ferromagnetic and displacive ferroelectric properties are still rare owing to the contradiction in the origin of ferromagnetism and ferroelectricity. In this study, we demonstrated that sizable ferromagnetic properties are induced in the ferroelectric bismuth ferrite-barium titanate system simply by introducing Co ions into the A-site. It is noted that all modified compositions exhibit well-saturated magnetic hysteresis loops at room temperature. Especially, 70Bi_0.95Co_0.05FeO₃-30Ba_0.95Co_0.05TiO₃ manifests noticeable ferroelectric and ferromagnetic properties; the spontaneous polarization and the saturation magnetization are 42 μC/㎠ and 3.6 emu/g, respectively. We expect that our methodology will be widely used in the development of perovskite-structured multiferroic oxides.

Magnetoelectric multiferroics, where a ferromagnetic and a ferroelectric order coexist and are coupled in a single phase, have been a hot topic in condensed matter physics for a long time owing to their ability to facilitate nextgeneration applications. In this review, we briefly introduce basic concept of the magnetoelectric multiferroic oxides as well as their history, physical origins, and significant achievements. The key moments contributing to the progress of magnetoelectric multiferroics are snapshotted chronologically, and then a discussion on the major magnetic exchange interactions and the ferroelectric origins are presented along with their coupling behavior. Furthermore, we argue a need for modifying the present classification of magnetoelectric multiferroics before presenting the evolution of multiferroics using representative examples with their properties such as magnetic/ferroelectric transition temperature, magnetization/electric polarization, and magnetoelectric coefficient. We hope that this brief review will provide the community researchers with insights into magnetoelectric multiferroic oxides.

Multiferroic BFO/PZT(5/95) multilayer films were fabricated by spin-coating method on the Pt/Ti/SiO2/Si substrate alternately using BFO and PZT(9/95) alkoxide solutions. The structural and dielectric properties were investigated with variation of the solvent and the number of coatings. All films showed the typical XRD patterns of the perovskite polycrystalline structure without presence of the second phase such as Bi2Fe4O3. BFO/PZT multilayer thin films showed the typical dielectric relaxation properties with increase an applied frequency. The average thickness of 6-coated BFO/PZT multilayer film was about 600 nm. The dielectric properties such as dielectric constant, dielectric loss and remnant polarization were superior to those of single composition BFO film, and those values for BFO/PZT multilayer film were 1199, 0.23% and 12 μC/cm2.

Nd and Ti co-doped bismuth ferrite (Bi1-xNdx)(Fe1-yTiy)O3 (x, y=0, 0.05, 0.1, 0.2) ceramics and thin films were synthesized through the conventional mixed-oxide process and pulsed laser deposition (PLD), respectively. Nd and Ti co-doping effect was examined with emphasis on how these impurities affect phase formation behavior as there could be the improvement in leakage current problems often associated with multiferroic BiFeO3 (BFO) thin films. The lattice constants of BFO ceramics decreased with Nd doping concentration up to 10mol%, while they further decreased with Nd and Ti co-doping to about 20%. BFO thin films obtained by the PLD process revealed random polycrystalline structure. Similar to bulk BFO ceramic, Nd and Ti co-doping effectively suppressed the formation of unwanted secondary phase and thus stabilized the perovskite phase in BFO thin films.