Spin-reorientation, ferroelectricity, and magnetodielectric effect in YFe(1-x)Mn(x)O3(0.1 ≤ x ≤ 0.40)

We report the observation of magnetoelectric and magnetodielectric effects at different temperatures in Mn-substituted yttrium orthoferrite, YFe(1-x)Mn(x)O(3)(0.1 ≤ x ≤ 0.40). Substitution of Mn in antiferromagnetic YFeO(3)(T(N) = 640 K) induces a first-order spin-reorientation transition at a temperature, T(SR), which increases with x whereas the Néel temperature (T(N)) decreases. While the magnetodielectric effect occurs at T(SR) and T(N), the ferroelectricity appears rather at low temperatures. The origin of magnetodielectric effect is attributed to spin-phonon coupling as evidenced from the temperature dependence of Raman phonon modes. The large magnetocapacitance (18% at 50 kOe) near T(SR) = 320 K and high ferroelectric transition temperature (～115 K) observed for x = 0.4 suggest routes to enhance magnetoelectric effect near room temperature for practical applications.     

Magnetic field annealing effects on self-oriented BiFeO3 thin films prepared by chemical solution deposition

Self-oriented BiFeO₃ (BFO) thin films are prepared via chemical solution deposition method with magnetic field in-situ annealing process. The effects of magnetic annealing on the microstructure, magnetic and dielectric properties as well as magnetoelectric coupling effect of the BFO thin films are investigated. With increasing the annealing magnetic field, the crystallization quality, texture, grain boundary connectivity and densification of the films are enhanced, which is attributed to the improvement of connection and diffusion of components. The magnetization of the field-annealing films and dielectric constant as well as remanent polarization increases with increasing the strength of annealing magnetic field. In addition, it is observed that magnetocapacitance value of the magnetic-field-annealing BFO thin film is higher than the non-field-annealing one. Moreover the BFO thin films annealed at 3 kOe magnetic field show the magnetoelectric effect with 4% under 2 kOe at room temperature.     

Coexistence of magnetism and superconductivity in the iron-based compound Cs0.8(FeSe0.98)2

We report on muon-spin rotation and relaxation (μSR), electrical resistivity, magnetization and differential scanning calorimetry measurements performed on a high-quality single crystal of Cs(0.8)(FeSe(0.98))(2). Whereas our transport and magnetization data confirm the bulk character of the superconducting state below T(c)=29.6(2) K, the μSR data indicate that the system is magnetic below T(N)=478.5(3) K, where a first-order transition occurs. The first-order character of the magnetic transition is confirmed by differential scanning calorimetry data. Taken all together, these data indicate in Cs(0.8)(FeSe(0.98))(2) a microscopic coexistence between the superconducting phase and a strong magnetic phase. The observed T(N) is the highest reported to date for a magnetic superconductor.     

Magnetite (Fe3O4): a new variant of relaxor multiferroic?

The electric polarization, dielectric permittivity, magnetoelectric effect, heat capacity, magnetization and ac susceptibility of magnetite films and polycrystals were investigated. The electric polarization of magnetite films with saturation values between 4 and 8 μC cm(-2) was found to vanish between 32 and 38 K, but in polycrystals no phase transition was detected in this range by heat capacity. Both types of samples showed magnetoelectric effects at low temperatures below a frequency-dependent crossover. This is interpreted as arising from multiferroic relaxor behavior.     

Magnetoelectric and magnetoelastic interactions in NdFe3(BO3)4 multiferroics

Complex experimental and theoretical investigations of the magnetic, magnetoelectric, and magnetoelastic properties of neodymium iron borate NdFe₃(BO₃)₄ along various crystallographic directions have been carried out in strong pulsed magnetic fields up to 230 kOe in a temperature range of 4.2–50 K. It has been found that neodymium iron borate, as well as gadolinium iron borate, is a multiferroic. It has a much larger (above 300 μC/m²) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (～50 kOe) has been determined for the first time from experimental data. The theoretical analysis based on the magnetic symmetry and quantum properties of the Nd ion in the crystal provides an explanation of the unusual behavior of the magnetoelectric and magnetoelastic properties of neodymium iron borate in strong magnetic fields and correlation observed between them.     

Magnetoelectric effect and magnetostriction in the paramagnetic piezoelectric NiSO4 · 6H2O

The direct magnetoelectric effect, the magnetostriction, and the magnetic moment in piezoelectric paramagnetic NiSO₄ · 6H₂O single crystals is comprehensively studied over a wide temperature range in magnetic fields up to 14 T for several magnetic field directions with respect to crystallographic axes. At temperatures above 20 K, the magnetoelectric effect is rigorously quadratic in magnetic field over the entire magnetic field range. As the temperature decreases, the region of quadratic behavior shifts toward low fields. To explain the magnetoelectric effect, the contribution of the magnetostriction-induced piezoelectric effect is considered. It is shown that the piezoelectric effect may be neglected at the helium temperature, where the magnetoelectric effect is high, since its value does not exceed 1%. However, the relative contribution of the piezoelectric effect increases to 10% at T = 40 K, where the magnetoelectric polarization decreases strongly. In contrast to the earlier assumption that the magnetoelectric effect is rapidly and fully saturated in fields higher than 3 T, complete saturation is actually not detected even at 14 T.     

Magnetic behavior of Eu(3)Ni(4)Ga(4): antiferromagnetic order and large magnetoresistance

The results of the magnetic susceptibility, isothermal magnetization, heat capacity, electrical resistivity and magnetoresistance measurements on polycrystalline Eu(3)Ni(4)Ga(4) are presented. Eu(3)Ni(4)Ga(4) forms in Na(3)Pt(4)Ge(4)-type cubic crystal structure (space group [Formula: see text]). The temperature dependence of the magnetic susceptibility of Eu(3)Ni(4)Ga(4) confirms the divalent state (Eu(2+)) of Eu ions with an effective magnetic moment μ(eff)?=?7.98?μ(B). At low fields, e.g.?at 0.01?T, a magnetic phase transition to an antiferromagnetically ordered state occurs at T(N)?=?10.9?K, which is further confirmed by the temperature dependence of the heat capacity and electrical resistivity. The field dependence of isothermal magnetization at 2?K reveals the presence of two field induced metamagnetic transitions at H(c1) and H(c2)?=?0.55 and 1.2?T, respectively and a polarized phase above H(PO)?=?1.7?T. The reduced jump in the heat capacity at the transition temperature, ΔC|(T(N))?=?13.48?J/mol-Eu?K would indicate an amplitude modulated (AM) antiferromagnetic structure. An interesting feature is that a large negative magnetoresistance, MR?=?[ρ(H)?-?ρ(0)]/ρ(0), is observed in the vicinity of magnetic transition even up to 2T(N). Similar large magnetoresistance has been observed in the paramagnetic state in some Gd and Eu based alloys and has been attributed to the magneto-polaronic effect.     

Nature of unusual spontaneous and field-induced phase transitions in multiferroics RMn2O5

Complex magnetic, magnetoelectric and magnetoelastic studies of spontaneous and field-induced phase transitions in TmMn₂O₅ were carried out. In the vicinity of spontaneous phase transition temperatures (35 and 25 K) the magnetoelectric and magnetoelastic dependences demonstrated the jumps of polarization and magnetostriction induced by the field ∼150 kOe. These anomalies can be attributed to the influence of magnetic field on the conditions of incommensurate-commensurate phase transition at 35 K and the reverse one at 25 K. In b-axis dependences the magnetic field-induced spin-reorientation phase transition was also observed below 20 K. Finally the magnetoelectric anomaly associated with metamagnetic transition is observed below the temperature of rare-earth subsystem ordering at relatively small critical fields of 5 kOe. This variety of spontaneous and induced phase transitions in RMn₂O₅ stems from the interplay of three magnetic subsystems: Mn³⁺, Mn⁴⁺, R³⁺. The comparison with YMn₂O₅ highlights the role of rare earth in low-temperature region (metamagnetic and spin-reorientation phase transitions), while the phase transition at higher temperatures between incommensurate and commensurate phases should be ascribed to the different temperature dependences of Mn³⁺ and Mn⁴⁺ ions. The strong correlation of magnetoelastic and magnetoelectric properties observed in the whole class of RMn₂O₅ highlights their multiferroic nature.     

Field-dependent diamagnetic transition in magnetic superconductor Sm1.85Ce0.15CuO4-y

The magnetic penetration depth of single crystal Sm(1.85)Ce(0.15)CuO(4-y) was measured down to 0.4 K in dc fields up to 7 kOe. For insulating Sm2CuO4, Sm3+ spins order at the Ne el temperature, T(N)=6 K, independent of the applied field. Superconducting Sm(1.85)Ce(0.15)CuO(4-y) (T(c) approximately 23 K) shows a sharp increase in diamagnetic screening below T(*)(H) which varied from 4.0 K (H=0) to 0.5 K (H=7 kOe) for a field along the c axis. If the field was aligned parallel to the conducting planes, T(*) remained unchanged. The unusual field dependence of T(*) indicates a spin-freezing transition that dramatically increases the superfluid density.     

Giant improper ferroelectricity in the ferroaxial magnet CaMn7O12

In rhombohedral CaMn7O12, an improper ferroelectric polarization of magnitude 2870 μC m(-2) is induced by an incommensurate helical magnetic structure that evolves below T(N1)=90 K. The electric polarization was found to be constrained to the high symmetry threefold rotation axis of the crystal structure, perpendicular to the in-plane rotation of the magnetic moments. The multiferroicity is explained by the ferroaxial coupling mechanism, which in CaMn7O12 gives rise to the largest magnetically induced, electric polarization measured to date.     

Magnetoelectric effect in perovskite quantum paraelectric EuTiO3

On the basis of successful theoretical explanation of the observed large magnetic-field effect (by ∼7% with 1.5 T) on the dielectric constant below the Néel temperature T_N of 5.5 K, we have demonstrated convincingly the magnetoelectric effect in an antiferromagnetic quantum paraelectric EuTiO₃ system. The mutual control of electric and magnetic properties is revealed by the variation of the electric-field-induced polarization with applied magnetic fields as well as the change of the magnetic-field-induced spin moments under the control of electric fields. It is found that the applied electric field (magnetic field) acts like a fictitious magnetic field (electric field) on the EuTiO₃ system. The magnetoelectric susceptibility is deduced to be proportional to the product of the magnetization, electrical polarization, magnetic susceptibility and dielectric susceptibility.     

Polar nanodomains and giant converse magnetoelectric effect in charge-ordered Fe2OBO3

The magnetoelectric coupling and polar nanodomains in the charge-ordered Fe2OBO3 have been extensively studied from room temperature down to 100?K. In?situ TEM investigations demonstrate that the charge-ordering transition characterized by an incommensurate modulation could evidently result in remarkable polar nanodomains at low temperatures. This kind of nanodomain could play a critical role in triggering a high dielectric constant and notable dielectric dispersion as observed in Fe2OBO3. Moreover, measurements of the magnetoelectric coupling under electrical field demonstrate the existence of giant electrically induced changes in magnetization around the magnetic transition.     

Magnetic ordering in semiconducting Tl0.53K0.47Fe1.64Se2 single crystals studied by M?ssbauer spectroscopy

The results of a 57Fe M?ssbauer spectroscopy study between 4.5 and 523.2 K and in external magnetic fields (up to 90 kOe) of semiconducting Tl0.53K0.47Fe1.64Se2 single crystals are reported. Evidence is provided for a possible phase separation into the magnetic majority and minority phases. It is demonstrated that the magnetic moments of the divalent Fe atoms located at the 16i site (space group I4/m) of the majority phase and of the minority phase are antiferromagnetically ordered, with the Néel temperature T(N) = 518.0(3.6) K. The magnetic moments at 5.0 K of 2.09(1) and 2.28(2) μ(B) in these two phases are tilted from the crystallographic c axis by 18(1)° and 32(2)°, respectively. The Debye temperature of Tl0.53K0.47Fe1.64Se2 is found to be 228(4) K.     

Zeeman-driven phase transition within the superconducting state of κ-(BEDT-TTF)2Cu(NCS)2

(13)C nuclear magnetic resonance measurements were performed on κ-(BEDT-TTF)(2)Cu(NCS)(2), with the external field placed parallel to the quasi-2D conducting layers. The absorption spectrum is used to determine the electronic spin polarization M(s) as a function of external field H at a temperature T=0.35 K. A discontinuity in the derivative dM(s)/dH at an applied field of H(s)=213±3 kOe is taken as evidence for a Zeeman-driven transition within the superconducting state and stabilization of inhomogeneous superconductivity.     

Magnetic behavior of Ba3Cu3Sc4O12

The chain-like system Ba(3)Cu(3)Sc(4)O(12) has potentially interesting magnetic properties due to the presence of Cu(2+) and a structure-suggested low dimensionality. We present magnetization M versus magnetic field H and temperature T, T- and H-dependent heat-capacity C(p), (45)Sc nuclear magnetic resonance (NMR), muon spin rotation (μSR), neutron diffraction measurements and electronic structure calculations for Ba(3)Cu(3)Sc(4)O(12). The onset of magnetic long-range antiferromagnetic (AF) order at T(N) ～ 16 K is consistently evidenced from the whole gamut of our data. A significant sensitivity of T(N) to the applied magnetic field H (T(N) ～ 0 K for H = 70 kOe) is also reported. Coupled with a ferromagnetic Curie-Weiss temperature (θ(CW) ～ 65 K) in the susceptibility (from a 100 to 300 K fit), it is indicative of competing ferromagnetic and antiferromagnetic interactions. These indications are corroborated by our density functional theory based electronic structure calculations, where we find the presence of significant ferromagnetic couplings between some copper ions whereas AF couplings were present between some others. Our experimental data, backed by our theoretical calculations, rule out the one-dimensional magnetic behavior suggested by the structure and the observed long-range order is due to the presence of non-negligible magnetic interactions between adjacent as well as next-nearest chains.     

Specificity of magnetoelectric effects in a new GdMnO<Subscript>3</Subscript> magnetic ferroelectric

A complex study of the magnetic, electric, magnetoelectric, and magnetoelastic properties of GdMnO₃ single crystals has been performed in the low-temperature region in strong pulsed magnetic fields up to 200 kOe. An anomaly of the dielectric constant along the a axis of a crystal has been found at 20 K, where a transition from an incommensurate modulated phase to a canted antiferromagnetic phase, as well as electric polarization along the a and b axes of the crystal induced by the magnetic field H‖ b (H_cr ～ 40 kOe), is observed. Upon cooling the crystal in an electric field, the magnetic-field-induced electric polarization changes its sign depending on the sign of the electric field. The occurrence of the electric polarization is accompanied by anisotropic magnetostriction, which points to a correlation between the magnetoelectric and magnetoelastic properties. Based on these results, it has been stated that GdMnO₃ belongs to a new family of magnetoelectric materials with the perovskite structure.     

Magnetic reversal of the ferroelectric polarization in a multiferroic spinel oxide

Ferroelectric transition has been detected in a ferrimagnetic spinel oxide of CoCr2O4 upon the transition to the conical spin order below 25 K. The direction [110] of the spontaneous polarization is normal to both the magnetization easy axis [001] and to the propagation axis [110] of the transverse spiral component, in accord with the prediction based on the spin-current model. The reversal of the spontaneous magnetization by a small magnetic field (approximately 0.1 T) induces the reversal of the spontaneous polarization, indicating the clamping of the ferromagnetic and ferroelectric domain walls.     

Magnetic and structural phase transitions in YMn<Subscript>2</Subscript>O<Subscript>5</Subscript> ferromagnetoelectric crystals induced by a strong magnetic field

Magnetic, magnetoelectric, and magnetoelastic properties of YMn₂O₅ ferromagnetoelectric single-crystals are investigated in strong pulsed magnetic fields of up to 250 kOe and in static magnetic fields of up to 12 kOe. It is found that, in YMn₂O₅ at T < T_N=42 K, a transverse weakly ferromagnetic moment of σ ₀=0.8 G cm³/g exists that is oriented along axis a and is attributed to the magnetoelectric interaction. When a magnetic field is directed along axis b, which is likely to be the axis of antiferromagnetism, a spin-flop transition is observed that is accompanied by jumps in magnetostriction and electric polarization. When a magnetic field is directed along axis a, the temperature of ferroelectric transition shifts from 20 to 25 K at H≈200 kOe. A theoretical analysis of the experimental results is given within phenomenological theory with regard to the fact that a YMn₂O₅ compound belongs to noncollinear antiferromagnetic crystals even in the exchange approximation.     

Dynamic magnetoelectric effect in terbium molybdate

The electric polarization induced in ferroelectric terbium molybdate by a magnetic field linearly varying with time is measured. The measurements are performed in fields up to 19 T at different specified rates of change in the magnetic field at temperatures of 273 and 219 K. The results obtained indicate that there are magnetoelectric effects of two types. One of them is a conventional magnetoelectric effect, which is appropriately referred to as the static magnetoelectric effect. The other effect is characterized by the fact that the electric polarization increases with an increase in the rate of change in the magnetic field and relaxes with time to zero at a fixed nonzero field. This phenomenon is termed the dynamic magnetoelectric effect.     

Evolution of magnetic properties in the normal spinel solid solution Mg(1-x)Cu(x)Cr2O4

We examine the evolution of magnetic properties in the normal spinel oxides Mg(1-x)Cu(x)Cr2O4 using magnetization and heat capacity measurements. The end-member compounds of the solid solution series have been studied in some detail because of their very interesting magnetic behavior. MgCr2O4 is a highly frustrated system that undergoes a first-order structural transition at its antiferromagnetic ordering temperature. CuCr2O4 is tetragonal at room temperature as a result of Jahn-Teller active tetrahedral Cu2+ and undergoes a magnetic transition at 135 K. Substitution of magnetic cations for diamagnetic Mg2+ on the tetrahedral A site in the compositional series Mg(1-x)Cu(x)Cr2O4 dramatically affects magnetic behavior. In the composition range 0 ≤ x ≤ ≈0.3, the compounds are antiferromagnetic. A sharp peak observed at 12.5 K in the heat capacity of MgCr2O4 corresponding to a magnetically driven first-order structural transition is suppressed even for small x. Uncompensated magnetism--with open magnetization loops--develops for samples in the x range ≈0.43 ≤ x ≤ 1. Multiple magnetic ordering temperatures and large coercive fields emerge in the intermediate composition range 0.43 ≤ x ≤ 0.47. The Néel temperature increases with increasing x across the series while the value of the Curie-Weiss Θ(CW) decreases. A magnetic temperature-composition phase diagram of the solid solution series is presented.