, which reveal magnetic and electric order, are in the focus of recent solid state research [1][2][3][4] . Especially the simultaneous occurrence of ferroelectricity and ferromagnetism, combined with an intimate coupling of magnetization and polarization via magneto-capacitive effects, could pave the way for a new generation of electronic devices. Here we present measurements on a simple cubic spinel with unusual properties: It shows ferromagnetic order and simultaneously relaxor ferroelectricity, i.e. a ferroelectric cluster state, reached by a smeared-out phase transition, both with sizable ordering temperatures and moments. Close to the ferromagnetic ordering temperature the magneto-capacitive coupling, characterized by a variation of the dielectric constant in an external magnetic field, reaches colossal values of nearly 500%. We attribute the relaxor properties to geometric frustration, which is well known for magnetic moments, but here is found to impede long-range order of the structural degrees of freedom.The coexistence of ferroelectricity and ferromagnetism would constitute a mile stone for modern electronics and functionalised materials. The most appealing applications are new types of storage media using both magnetic and electric polarization and the possibility of electrically reading/writing magnetic memory devices (and vice versa). However, it is clear now that ferroelectric ferromagnets are rare 5,6 and mostly exhibit rather weak ferromagnetism. Spinel compounds are an important class of materials and their electronic properties are in the focus of research since the famous work of Verwey on magnetite 7 . Recent reports on geometrical frustration of the spin and orbital degrees of freedom 8 , and the observation of an orbital-glass state 9 in sulpho spinels, demonstrate the rich and complex physics, characteristic of these compounds. Here we report on another interesting experimental observation in a spinel system: R elaxor ferroelectricity in ferromagnetic CdCr 2 S 4 and the occurrence of colossal magnetocapacitive effects.CdCr 2 S 4 crystallizes in the normal cubic spinel structure (space group Fd3m, a = 1.024 nm), with Cr 3+ octahedrally surrounded by sulphur ions, yielding a half-filled lower t 2g triplet with a spin S = 3/2. Ferromagnetism in CdCr 2 S 4 is well known 10 , but early experimental observations of a number of mysterious features have fallen into oblivion: For example, reports of an anomalous expansion coefficient at low temperatures 11,12 , an unexpected concomitant broadening of the d iffraction lines 11 , a strong blue shift of the absorption edge on passing the ferromagnetic phase transition 13 , the observation of anomalously large phonon shifts and damping effects close to T c 14 and the observation of large magneto-resistance effects 15 . Figure 1a shows the inverse magnetic susceptibility χ -1 and the low-temperature magnetization M. The straight line indicates a fit to the paramagnetic susceptibility, which results in a Curie-Weiss temperature of 155 K and a paramagneti...

SrTiO 3 , a quantum paraelectric 1 , becomes a metal with a superconducting instability after removal of an extremely small number of oxygen atoms 2 . It turns into a ferroelectric upon substitution of a tiny fraction of strontium atoms with calcium 3 . The two orders may be accidental neighbours or intimately connected, as in the picture of quantum critical ferroelectricity 4 . Here, we show that in Sr 1−x Ca x TiO 3−δ (0.002 < x < 0.009, δ < 0.001) the ferroelectric order coexists with dilute metallicity and its superconducting instability in a finite window of doping. At a critical carrier density, which scales with the Ca content, a quantum phase transition destroys the ferroelectric order. We detect an upturn in the normal-state scattering and a significant modification of the superconducting dome in the vicinity of this quantum phase transition. The enhancement of the superconducting transition temperature with calcium substitution documents the role played by ferroelectric vicinity in the precocious emergence of superconductivity in this system, restricting possible theoretical scenarios for pairing.A perovskite of the ABO 3 family, SrTiO 3 is a quantum paraelectric whose dielectric constant rises to ∼20,000 at low temperature 1 , but avoids long-range ferroelectric order. It becomes a metal by substituting Sr with La, Ti with Nb, or by removing O. It has been known for half a century that this metal is a superconductor at low temperatures 2 . More recently, a sharp Fermi surface and a superconducting ground state have been found to persist down to a carrier concentration of 10 17 cm −3 in SrTiO 3−δ (refs 5,6 However, mobile electrons screen polarization and therefore only insulating solids are expected to host a ferroelectric order. Hitherto, as a paradigm, ferroelectric quantum criticality, in contrast to its magnetic counterpart, was deprived of an experimental phase diagram in which a superconducting phase and a ferroelectric order share a common boundary.Here, we produce such a phase diagram in the case of Sr 1−x Ca x TiO 3−δ . The main new observations are the following: metallic Sr 1−x Ca x TiO 3−δ hosts a phase transition structurally indistinguishable from the ferroelectric phase transition in insulating Sr 1−x Ca x TiO 3 ; the coexistence between this ferroelectric-like order and superconductivity ends beyond a threshold carrier concentration; and, in the vicinity of this quantum phase transition, calcium substitution enhances the superconducting critical temperature and induces an upturn in the normal-state resistivity.Figure 1 summarizes what we know about the emergence of ferroelectricity, metallicity and superconductivity in this system. When a small fraction of Sr atoms (x > 0.002) is replaced with isovalent Ca, Sr 1−x Ca x TiO 3 becomes ferroelectric 3 , with a Curie temperature steadily increasing with Ca content in the dilute limit 0.002 < x < 0.02 (refs 3,13,14). Macroscopic polarization below the Curie temperature has been observed in dielectric and linear birefringence measurements, a...

We report on the discovery of a novel triangular phase regime in the system La1-xSrxMnO3 by means of electron spin resonance and magnetic susceptibility measurements. This phase is characterized by the coexistence of ferromagnetic entities within the globally paramagnetic phase far above the magnetic ordering temperature. The nature of this phase can be understood in terms of Griffiths singularities arising due to the presence of correlated quenched disorder in the orthorhombic phase.

We report on structural, magnetic, dielectric, and thermodynamic properties of Eu 1−x Y x MnO 3 for Y doping levels 0 ഛ x Ͻ 1. This system resembles the multiferroic perovskite manganites RMnO 3 ͑with R = Gd, Dy, Tb͒ but without the interference of magnetic contributions of the 4f ions. In addition, it offers the possibility to continuously tune the influence of the A-site ionic radii. For small concentrations x ഛ 0.1 we find a canted antiferromagnetic and paraelectric ground state. For higher concentrations x ജ 0.3 ferroelectric polarization coexists with the features of a presumably spiral magnetic phase analogous to the observations in TbMnO 3 . In the intermediate concentration range around x Ϸ 0.2 a multiferroic scenario is realized combining weak ferroelectricity and weak ferromagnetism, presumably due to a conelike magnetic structure.

Crystal structure, magnetic susceptibility, and specific heat were measured in the normal cubic spinel compounds MnSc2S4 and FeSc2S4. Down to the lowest temperatures, both compounds remain cubic and reveal strong magnetic frustration. Specifically the Fe compound is characterized by a Curie-Weiss (CW) temperature ThetaCW = -45 K and does not show any indications of order down to 50 mK. In addition, the Jahn-Teller ion Fe2+ is orbitally frustrated. Hence, FeSc2S4 belongs to the rare class of spin-orbital liquids. MnSc2S4 is a spin liquid for temperatures T>TN approximately 2 K.