Resonant Magnetoelectric X-ray Scattering in GaFeO3: Observation of Ordering of Toroidal Moments

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.

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 multiferroics. Despite the possible coexistence of ferroelectricity and magnetism, a pronounced interplay between these properties has rarely been observed. This has prevented the realization of multiferroic devices offering such functionality. 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.

The quest for higher data density in information storage is motivating investigations into approaches for manipulating magnetization by means other than magnetic fields. This is evidenced by the recent boom in magnetoelectronics and 'spintronics', where phenomena such as carrier effects in magnetic semiconductors and high-correlation effects in colossal magnetoresistive compounds are studied for their device potential. The linear magnetoelectric effect-the induction of polarization by a magnetic field and of magnetization by an electric field-provides another route for linking magnetic and electric properties. It was recently discovered that composite materials and magnetic ferroelectrics exhibit magnetoelectric effects that exceed previously known effects by orders of magnitude, with the potential to trigger magnetic or electric phase transitions. Here we report a system whose magnetic phase can be controlled by an external electric field: ferromagnetic ordering in hexagonal HoMnO3 is reversibly switched on and off by the applied field via magnetoelectric interactions. We monitor this process using magneto-optical techniques and reveal its microscopic origin by neutron and X-ray diffraction. From our results, we identify basic requirements for other candidate materials to exhibit magnetoelectric phase control.