A ferroelectric crystal exhibits a stable and switchable electrical polarization that is manifested in the form of cooperative atomic displacements. A ferromagnetic crystal exhibits a stable and switchable magnetization that arises through the quantum mechanical phenomenon of exchange. There are very few 'multiferroic' materials that exhibit both of these properties, but the 'magnetoelectric' coupling of magnetic and electrical properties is a more general and widespread phenomenon. Although work in this area can be traced back to pioneering research in the 1950s and 1960s, there has been a recent resurgence of interest driven by long-term technological aspirations.

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Multiferroic and magnetoelectric materials

The magnetoelectric effect--the induction of magnetization by means of an electric field and induction of polarization by means of a magnetic field--was first presumed to exist by Pierre Curie, and subsequently attracted a great deal of interest in the 1960s and 1970s (refs 2-4). More recently, related studies on magnetic ferroelectrics have signalled a revival of interest in this phenomenon. From a technological point of view, the mutual control of electric and magnetic properties is an attractive possibility, but the number of candidate materials is limited and the effects are typically too small to be useful in applications. Here we report the discovery of ferroelectricity in a perovskite manganite, TbMnO3, where the effect of spin frustration causes sinusoidal antiferromagnetic ordering. The modulated magnetic structure is accompanied by a magnetoelastically induced lattice modulation, and with the emergence of a spontaneous polarization. In the magnetic ferroelectric TbMnO3, we found gigantic magnetoelectric and magnetocapacitance effects, which can be attributed to switching of the electric polarization induced by magnetic fields. Frustrated spin systems therefore provide a new area to search for magnetoelectric media.

Magnetic control of ferroelectric polarization

Magnetism and ferroelectricity are essential to many forms of current technology, and the quest for multiferroic materials, where these two phenomena are intimately coupled, is of great technological and fundamental importance. Ferroelectricity and magnetism tend to be mutually exclusive and interact weakly with each other when they coexist. The exciting new development is the discovery that even a weak magnetoelectric interaction can lead to spectacular cross-coupling effects when it induces electric polarization in a magnetically ordered state. Such magnetic ferroelectricity, showing an unprecedented sensitivity to ap plied magnetic fields, occurs in 'frustrated magnets' with competing interactions between spins and complex magnetic orders. We summarize key experimental findings and the current theoretical understanding of these phenomena, which have great potential for tuneable multifunctional devices.

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Multiferroics: a magnetic twist for ferroelectricity

Ferroelectric and magnetic materials are a time-honoured subject of study and have led to some of the most important technological advances to date. Magnetism and ferroelectricity are involved with local spins and off-centre structural distortions, respectively. These two seemingly unrelated phenomena can coexist in certain unusual materials, termed multiferroics1,2,3,4,5,6,7,8,9,10,11. Despite the possible coexistence of ferroelectricity and magnetism, a pronounced interplay between these properties has rarely been observed6,12. This has prevented the realization of multiferroic devices offering such functionality13. Here, we report a striking interplay between ferroelectricity and magnetism in the multiferroic TbMn2O5, demonstrated by a highly reproducible electric polarization reversal and permanent polarization imprint that are both actuated by an applied magnetic field. Our results point to new device applications such as magnetically recorded ferroelectric memory.

Electric polarization reversal and memory in a multiferroic material induced by magnetic fields.

Multiferroics, defined for those multifunctional materials in which two or more kinds of fundamental ferroicities coexist, have become one of the hottest topics of condensed matter physics and materials science in recent years. The coexistence of several order parameters in multiferroics brings out novel physical phenomena and offers possibilities for new device functions. The revival of research activities on multiferroics is evidenced by some novel discoveries and concepts, both experimentally and theoretically. In this review, we outline some of the progressive milestones in this stimulating field, especially for those single-phase multiferroics where magnetism and ferroelectricity coexist. First, we highlight the physical concepts of multiferroicity and the current challenges to integrate the magnetism and ferroelectricity into a single-phase system. Subsequently, we summarize various strategies used to combine the two types of order. Special attention is paid to three novel mechanisms for multiferroicity generation: (1) the ferroelectricity induced by the spin orders such as spiral and E-phase antiferromagnetic spin orders, which break the spatial inversion symmetry; (2) the ferroelectricity originating from the charge-ordered states; and (3) the ferrotoroidic system. Then, we address the elementary excitations such as electromagnons, and the application potentials of multiferroics. Finally, open questions and future research opportunities are proposed.

Multiferroicity: the coupling between magnetic and polarization orders

We have investigated the structural, magnetic, and electric properties of ferromagnetic ${\mathrm{BiMnO}}_{3}$ with a highly distorted perovskite structure. At ${T}_{E}=750--770\mathrm{K},$ a centrosymmetric--to--non-centrosymmetric structural transition takes place, which describes of the ferroelectricity in the system. The changes in the dielectric constant were induced by the magnetic ordering ${(T}_{M}\ensuremath{\approx}100\mathrm{K})$ as well as by the application of magnetic fields near ${T}_{M}.$ These features are attributed to the inherent coupling between the ferroelectric and ferromagnetic orders in the multiferroic system.

S. Kawamoto

Papers

Magnetocapacitance effect in multiferroic BiMnO 3