Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare. Among such ferromagnetic ferroelectrics are conical spin spiral magnets
with a simultaneous reversal of magnetization and electric polarization that is still little understood. Such materials can feature various multiferroic domains that complicates their study. Here we study the multiferroic domains in ferromagnetic ferroelectric Mn$_{2}$GeO$_{4}$ using neutron diffraction, and show that it features a double-Q conical magnetic structure that, apart from trivial 180 degree commensurate magnetic domains, can be described by ferromagnetic and ferroelectric domains only. We show unconventional magnetoelectric couplings such as the magnetic-field-driven reversal of ferroelectric polarization with no change of spin-helicity, and present a phenomenological theory that successfully explains the magnetoelectric coupling. Our measurements establish Mn$_{2}$GeO$_{4}$ as a conceptually simple multiferroic in which the magnetic-field-driven flop of conical spin spirals leads to the simultaneous reversal of magnetization and electric polarization.
We have investigated the magnetoelectric and magnetodielectric response in FeVO$_4$, which exhibits a change in magnetic structure coincident with ferroelectric ordering at $T_{N2}$$approx$15 K. Using symmetry considerations, we construct a model for
the possible magnetoelectric coupling in this system, and present a discussion of the allowed spin structures in FeVO$_4$. Based on this model, in which the spontaneous polarization is caused by a trilinear spin-phonon interaction, we experimentally explore the magnetoelectric coupling in FeVO$_4$ thin films through measurements of the electric field induced shift of the multiferroic phase transition temperature, which exhibits an increase of 0.25 K in an applied field of 4 MV/m. The strong spin-charge coupling in fvo, is also reflected in the significant magnetodielectric shift, which is present in the paramagnetic phase due to a quartic spin-phonon interaction and shows a marked enhancement with the onset of magnetic order which we attribute to the trilinear spin-phonon interaction. We observe a clear magnetic field induced dielectric anomaly at lower temperatures, distinct from the sharp peak associated with the multiferroic transition, which we tentatively assign to a spin reorientation cross-over. We also present a magnetoelectric phase diagram for FeVO$_4$.
We report on the electric field control of magnetic phase transition temperatures in multiferroic Ni3V2O8 thin films. Using magnetization measurements, we find that the phase transition temperature to the canted antiferromagnetic state is suppressed
by 0.2 K in an electric field of 30 MV/m, as compared to the unbiased sample. Dielectric measurements show that the transition temperature into the magnetic state associated with ferroelectric order increases by 0.2 K when the sample is biased at 25 MV/m. This electric field control of the magnetic transitions can be qualitatively understood using a mean field model incorporating a tri-linear coupling between the magnetic order parameters and spontaneous polarization.
Competing interactions and geometric frustration provide favourable conditions for exotic states of matter. Such competition often causes multiple phase transitions as a function of temperature and can lead to magnetic structures that break inversion
symmetry, thereby inducing ferroelectricity [1-4]. Although this phenomenon is understood phenomenologically [3-4], it is of great interest to have a conceptually simpler system in which ferroelectricity appears coincident with a single magnetic phase transition. Here we report the first such direct transition from a paramagnetic and paraelectric phase to an incommensurate multiferroic in the triangular lattice antiferromagnet RbFe(MoO4)2 (RFMO). A magnetic field extinguishes the electric polarization when the symmetry of the magnetic order changes and ferroelectricity is only observed when the magnetic structure has chirality and breaks inversion symmetry. Multiferroic behaviour in RFMO provides a theoretically tractable example of ferroelectricity from competing spin interactions. A Landau expansion of symmetry-allowed terms in the free energy demonstrates that the chiral magnetic order of the triangular lattice antiferromagnet gives rise to a pseudoelectric field, whose temperature dependence agrees with that observed experimentally.
There is much interest in the physics of materials that show a strong coupling between magnetic and electric degrees of freedom. In a recent paper by Mostovoy a theory is presented that is based on symmetry arguments and leads to quite general claims
which we feel merit some further analysis. In particular, Mostovoy concludes that spiral magnets are, in general, ferroelectric. We argue that this conclusion is not generally valid, and that the symmetry of the unit cell has to be taken into account by any symmetry-based magneto-electric coupling theory. In an attempt to avoid further confusion in the search of new multiferroic materials, we identify in this Comment some of the necessary symmetry properties of spiral magnets that can lead to ferroelectricity.
TbMnO3 is an orthorhombic insulator where incommensurate spin order for temperature T_N < 41K is accompanied by ferroelectric order for T < 28K. To understand this, we establish the magnetic structure above and below the ferroelectric transition usin
g neutron diffraction. In the paraelectric phase, the spin structure is incommensurate and longitudinally-modulated. In the ferroelectric phase, however, there is a transverse incommensurate spiral. We show that the spiral breaks spatial inversion symmetry and can account for magnetoelectricity in TbMnO3.
