Two-dimensional van der Waals (2D vdW) magnets have attracted enormous attention as an emerging material platform for magnetism, spintronics, and multifunctional applications. Their single-crystalline layered structures, layer-number controllability, and unique 2D properties provide unique opportunities that are difficult to achieve in conventional magnetic materials. However, the discovery and development of new 2D magnetic compounds require considerable time and effort, and only a limited number of these materials have been reported to be suitable for practical use. Therefore, materials engineering based on already established 2D vdW magnets has become an important research direction to explore new characteristics and find a practical route for device applications. This review summarizes recent materials engineering pathways for 2D vdW magnets. The main contents focus on the engineering strategy through electrostatic, chemical, lattice, symmetry, and heterostructure ways. These approaches provide practical design routes for tailoring magnetic properties beyond intrinsic 2D vdW magnets. Further progress will require broader application to various types of materials and delicate optimization that connects expanding fundamental magnetism with electromagnetic device applications.
We investigated the origin of magnetic behaviors induced by an asymmetric spin exchange interaction in Fe-site engineered lead iron niobate [Pb(Fe1/2Nb1/2)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, 70Bi0.95Co0.05FeO3-30Ba0.95Co0.05TiO3 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.
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