Specific heat, magnetic torque, and magnetization studies of LiCoPO4 olivine are presented. They show that an unique set of physical properties of LiCoPO4 leads to the appearance of features characteristic of 2D Ising systems near the Neel temperature, T_N =21.6 K, and to the appearance of an uncommon effect of influence of magnetic field on the magnetocrystalline anisotropy. The latter effect manifests itself as a first-order transition, discovered at ~9 K, induced by magnetic field of 8 T. Physical nature of this transition was explained and a model describing experimental dependences satisfactorily was proposed.
MnCr2O4 that exhibits spin frustration and complex spiral spin order is of great interest from both fundamental as well as application-oriented perspectives. Unlike CoCr2O4 whose ground state presents the coexistence of commensurate spiral spin order (CSSO) and ferroelectric order, MnCr2O4 shows no multiferroicity. One reason is that the spiral spin order is highly sensitive to the oxygen concentration in MnCr2O4. Here, we have successfully grown high-quality single-crystalline MnCr2O4 by the chemical vapor transport method. We observe a new first-order magnetic transition from the incommensur…
The orbital motion of electrons in a three-dimensional solid can generate a pseudoscalar magnetoelectric coupling $θ$, a fact we derive for the single-particle case using a recent theory of polarization in weakly inhomogeneous materials. This polarizability $θ$ is the same parameter that appears in the "axion electrodynamics" Lagrangian $Δ{\cal L}_{EM} = (θe^2 / 2 πh) {\bf E} \cdot {\bf B}$, which is known to describe the unusual magnetoelectric properties of the three-dimensional topological insulator ($θ=π$). We compute $θ$ for a simple model that accesses the topological insulator and discu…
Below its Néel temperature, the frustrated magnet CdCr$_2$O$_4$ exhibits an antiferromagnetic spin-spiral ground state. Such states can give rise to a sizable magnetoelectric coupling. In this report, we measure the electric polarization induced in single-crystalline CdCr$_2$O$_4$ by a large applied magnetic field. Because the detection of a macroscopic polarization is hindered by the structural domains in the tetragonal spin-spiral phase, we have pioneered an alternative method of measuring polarization induced by high magnetic fields, using electrostatic force microscopy. This method enables…
It is shown theoretically that a giant magnetoelectric susceptibility exceeding 10^-6 s/m may be achieved in the ferromagnetic/ferroelectric epitaxial systems via the magnetization rotation induced by an electric field applied to the substrate. The predicted magnetoelectric anomaly results from the strain-driven spin-reorientation transitions in ferromagnetic films, which take place at experimentally accessible misfit strains in CoFe2O4 and Ni films.
The search for materials displaying a large magnetoelectric effect has occupied researchers for many decades. The rewards could include not only advanced electronics technologies, but also fundamental insights concerning the dielectric and magnetic properties of condensed matter. In this article, we focus on the magnetoelectric effect in transition metal oxides and review the manner in which first-principles calculations have helped guide the search for (and increasingly, predicted) new materials and shed light on the microscopic mechanisms responsible for magnetoelectric phenomena.
We report a giant linear magnetoelectric coupling in strained BiMnO3 thin films in which the disorder associated with an islanded morphology gives rise to extrinsic relaxor ferroelectricity that is not present in bulk centrosymmetric ferromagnetic crystalline BiMnO3. Strain associated with the disorder is treated as a local variable which couples to the two ferroic order parameters, magnetization M and polarization P. A straightforward "gas under a piston" thermodynamic treatment explains the observed correlated temperature dependencies of the product of susceptibilities and the magnetoelectri…
Electrical control of magnetization or magnetic control of polarization offers an extra degree of freedom in materials possessing both electric and magnetic dipole moments viz., magnetoelectric multiferroics. Microstructure with polycrystalline configurations that enhances the overall polarization/magnetization and that outperform single crystalline configurations are identified. The characterization of local fields corresponding to the polycrystal configuration underlines nontrivial role played by randomness in better cross-coupling mediated by anisotropic and asymmetric strains.
Apart from being so far the only known binary multiferroic compound, CuO has a much higher transition temperature into the multiferroic state, 230 K, than any other known material in which the electric polarization is induced by spontaneous magnetic order, typically lower than 100 K. Although the magnetically induced ferroelectricity of CuO is firmly established, no magnetoelectric effect has been observed so far as direct crosstalk between bulk magnetization and electric polarization counterparts. Here we demonstrate that high magnetic fields of about 50 T are able to suppress the helical mod…
Insulating helimagnetic Cu2OSeO3 shows sizeable magnetoelectric effects in its skyrmion phase. Using magnetization measurements, magneto-current analysis and dielectric spectroscopy, we provide a thorough investigation of magnetoelectric coupling, polarization and dielectric constants of the ordered magnetic and polar phases of single-crystalline Cu2OSeO3 in external magnetic fields up to 150 mT and at temperatures below 60 K. From these measurements we construct a detailed phase diagram. Especially, the skyrmion phase and the metamagnetic transition of helical to conical spin order are charac…
We have investigated the magnetoelectric (ME) effect in layered composite rings subjected to circumferential AC magnetic fields and DC magnetic fields in radial, axial or circumferential directions. Bilayer samples were obtained combining different grades of commercial Mn-Zn ferrites or Ni-Zn ferrites with commercial lead zirconate titanate (PZT). Mn-Zn ferrites with low magnetostriction saturation () and low magneto-crystalline anisotropy constants show high ME capabilities when associated with PZT in ring structures. In certain conditions, these ME effects are higher than those obtained with…
Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice chang…
Thin FeRh film was extensively studied recently, and an emergent substrate- and capping-dependent interfacial ferromagnetism (FM) was widely observed in experiments. However, the voltage modulation of this interfacial ferromagnetism is barely studied, which would have profound applications in antiferromagnetic (AFM) FeRh-based magnetoelectric-random access memory (MeRAM). Using ab initio techniques, we comparatively study the interfacial ferromagnetic properties and magnetoelectric responses of ultrathin FeRh films capped by heavy transition metal Ta. We find that Ta capping reverses the phase…
The effect of Cr doping with nominal compositions Mn2-xCrxO3 (0 less than equal to x less than equal to 0.10) has been undertaken to investigate its effect on structural, magnetic, dielectric and magnetoelectric properties. The Cr doping transformed the room temperature crystal structure from orthorhombic to cubic symmetry. Similar to alpha-Mn2O3, two magnetic transitions have been observed in the Cr doped samples. The effect of Cr doping is significant on the low temperature transition i.e. the lower magnetic transition shifted towards higher temperature (25 K for pristine to 40 K for x=0.10)…
Our measured dielectric constant and mechanical response of multiferroic BiFeO3 indicate four phase transitions below room temperature. Features correlate with those reported at 50K (from a peak in the zero-field-cooled magnetic susceptibility) and 230K (from splitting between field-cooled and zero-field-cooled magnetic data[1], and 200K (from magnon light scattering cross sections[2]). The primary order parameter is not the polarization in any of the low-T transitions. Instead, the transition near 230 K shows strong elastic coupling, while that at 50K is fundamentally magnetic, but magnetostr…
Terahertz optical activity near crystal field transitions of Tm3+ ions in magnetoelectric alumoborates
Prokhorov General Physics Institute of the Russian Academy of Sciences（俄罗斯科学院普尔科沃普通物理研究所）；Vienna University of Technology（维也纳工业大学）；Institute of Spectroscopy of the Russian Academy of Sciences（俄罗斯科学院光谱研究所）；Kirensky Institute of Physics, Siberian Branch of the Russian Academy of Sciences（俄罗斯科学院西伯利亚分院基连斯基物理研究所）
Magnetoelectric materials are attractive for several applications, including actuators, switches, and magnetic field sensors. Typical mechanisms for achieving a strong magnetoelectric coupling are rooted in transition metal magnetism. In sharp contrast, here we identify CsEr(MoO4)2 as a magnetoelectric material without magnetic transition metal ions, thus ensuring that the Er ions play a key role in achieving this interesting property. Our detailed study includes measurements of the structural, magnetic, and electric properties of this material. Bulk characterization and neutron powder diffrac…
Hexagonal ferrites (h-RFeO$_3$, R=Y, Dy-Lu) have recently been identified as a new family of multiferroic complex oxides. The coexisting spontaneous electric and magnetic polarizations make h-RFeO$_3$ rare-case ferroelectric ferromagnets at low temperature. Plus the room-temperature multiferroicity and predicted magnetoelectric effect, h-RFeO$_3$ are promising materials for multiferroic applications. Here we review the structural, ferroelectric, magnetic, and magnetoelectric properties of h-RFeO$_3$. The thin film growth is also discussed because it is critical in making high quality single cr…
We present a unique example of giant magnetoelectric effect in a conventional multiferroic HoMnO3, where polarization is very large (~56 mC/m2) and the ferroelectric transition temperature is higher than the magnetic ordering temperature by an order. We attribute the uniqueness of the giant magnetoelectric effect to the ferroelectricity induced entirely by the off-center displacement of rare earth ions with large magnetic moments. This finding suggests a new avenue to design multiferroics with large polarization and higher ferroelectric transition temperature as well as large magnetoelectric e…
The general approach for the consideration of the magnetoelectric effects in ferroic nanorods is proposed in the framework of the phenomenological theory. The intrinsic surface stress, magneto- and electrostriction as well as piezoelectric and piezomagnetic effects are included into the free energy. The intrinsic surface stress under the curved nanoparticle surface is shown to play an important role in the shift of ferroelectric and ferromagnetic transition temperatures and built-in magnetic and electric fields appearance, which are inversely proportional to the nanorod radius. We consider the…
We present the results of detailed dielectric investigations of the relaxation dynamics in DyMnO$_3$ multiferroic manganite. Strong low-frequency relaxation process near the paraelectric-ferroelectric phase transition is observed. The high frequency mode is directly to the relaxational motion of multiferroic domain walls. We provide an experimental evidence that this relaxation mode corresponds to a chirality switching of the spin cycloid in DyMnO$_3$. We demonstrate that the relaxation dynamics in DyMnO$_3$ is typical for an order-disorder phase transition and may be understood within a simpl…
In order to establish the correlation between the magnetoelectric coupling and magnetic instability, we have studied the structural, magnetic, and ferroelectric properties of \textit{x}BaTiO${_3}$-(1-\textit{x})BiCoO${_3}$ as a function of BaTiO$_3$ concentration ($x$) and volume.The $G-$type antiferromagnetic ordering is found to be energetically favorable for $x<$ 0.45 and higher concentrations stabilize with nonmagnetic states. We observe metamagnetic spin state transitions associated with paraelectric to ferrolectric transitions as a function of volume and $x$ using synchrotron diffraction…
Few materials undergo cooperative Jahn-Teller (JT) transitions at low temperatures, but zircon-type oxides are one class that includes DyVO$_4$, which transforms from a tetragonal to an orthorhombic structure at around 13.6 K, with a narrow transition temperature range within 0.5 K. Since many rare-earth ions can be accommodated in the structure, there should be ample routes to vary the transition temperature and structural effects of the transition. We have synthesized pure DyVO$_4$ and solid solutions Dy$_{1-x}$Tm$_x$VO$_4$ ($x$ = 0.05, 0.1, 0.15, 0.2, and 0.5) and Dy$_{1-y}$Pr$_y$VO$_4$ ($y…
In-plane temperature dependent dielectric behavior of BiFeO3 (BFO) as-grown thin films show diffuse but prominent phase transitions near 450 (+/-10) K and 550 K with dielectric loss temperature dependences that suggest skin layer effects. The 450 K anomalies are near the "transition" first reported by Polomska et al. [Phys. Stat. Sol. 23, 567 (1974)]. The 550 K anomalies coincide with the surface phase transition recently reported [Xavi et al. PRL 106, 236101 (2011)]. In addition, anomalies are found at low temperatures: After several experimental cycles the dielectric loss shows a clear relax…
Magnetoelectric effect is a fundamental physics phenomenon that synergizes electric and magnetic degrees of freedom to generate distinct material responses like electrically tuned magnetism, which serves as a key foundation of the emerging field of spintronics. Here, we show by first-principles studies that ferroelectric (FE) polarization of an In2Se3 monolayer can modulate the magnetism of an adjacent transition-metal (TM) decorated graphene layer via an FE induced electronic transition. The TM nonbonding d-orbital shifts downward and hybridizes with carbon p states near the Fermi level, supp…
In this work, we have designed obtained a novel multiferroic nanocomposite using the high-pressure torsion (HPT) method. The crystal structure, phase composition, morphology, ferromagnetic (FM) and ferroelectric (FE) properties of the initial powders and "multiferroic-ferromagnetic" nanocomposites have been studied comprehensively. The initial powders and their composites show the perovskite and spinel crystalline phases for the FE and FM fractions, respectively. After HPT, the particle sizes of the initial powders are decreased significantly. It is shown that the novel nanocomposite consists …
A general formula for the average vector potential of bulk periodic systems is proposed and shown to set the boundary conditions at magnetic interfaces. For antiferromagnetic materials, the study reveals a unique relation between the macroscopic potential and the orientation-dependent magnetic quadrupole, as a result of the different crystalline and magnetic symmetries. In particular, at surfaces and interfaces of a truncated bulk without inversion and time-reversal symmetries, the average vector potential exhibits a discontinuity, which results in an interfacial magnetic field. In general, ho…
A detailed high pressure investigation is carried out on $Fe_4Nb_2O_9$ using angle resolved x-ray diffraction and Raman spectroscopy measurements. We find a structural transition from the ambient trigonal phase to a monoclinic phase above 8.8 GPa. The structural transition is assumed to be driven by a large distortion of $Nb-O_6$ octahedra as seen from x-ray diffraction analysis and a large pressure dependence of $Nb-O_6$ octahedra breathing Raman mode. Anomalous behaviour of Raman modes and increase in the phonon life time at the phase transition pressure indicate a trigonal paramagnetic phas…
We have observed the magnetoelectric response at room temperature and above in high-resistive ceramics made of multiferroic Pb(Fe1/2Nb1/2)O3 (PFN) and PFN-based solid solution 0.91PFN-0.09PbTiO3 (PFN-PT). The value of the paramagnetoelectric (PME) coefficient shows a pronounced maximum near the ferroelectric-to-paraelectric phase transition temperature, T_C, and then decreases sharply to zero for T>T_C. The maximal PME coefficient in PFN is about 4x10(-18) s/A. The theoretical description of the PME effect, within the framework of a Landau theory of phase transitions allowing for realistic tem…
Although the magnetoelectric effects - the mutual control of electric polarization by magnetic fields and magnetism by electric fields, have been intensively studied in a large number of inorganic compounds and heterostructures, they have been rarely observed in organic materials. Here we demonstrate magnetoelectric coupling in a metal-organic framework [(CH3)2NH2]Mn(HCOO)3 which exhibits an order-disorder type of ferroelectricity below 185 K. The magnetic susceptibility starts to deviate from the Curie-Weiss law at the paraelectric-ferroelectric transition temperature, suggesting an enhanceme…
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 f…
We incorporate single crystal Fe$_3$O$_4$ thin films into a gated device structure and demonstrate the ability to control the Verwey transition with static electric fields. The Verwey transition temperature ($T_V$) increases for both polarities of the electric field, indicating the effect is not driven by changes in carrier concentration. Energetics of induced electric polarization and/or strain within the Fe$_3$O$_4$ film provide a possible explanation for this behavior. Electric field control of the Verwey transition leads directly to a large magnetoelectric effect with coefficient of 585 pT…
We observe a seemingly complex magnetic field dependence of dielectric constant of hexagonal YbMnO3 near the spin ordering temperature. After rescaling, the data taken at different temperatures and magnetic fields collapse on a single curve describing the sharp anomaly in nonlinear magnetoelectric response at the magnetic transition. We show that this anomaly is a result of the competition between two magnetic phases. The scaling and the shape of the anomaly are explained using the phenomenological Landau description of the competing phases in hexagonal manganites.
A theoretical description of the sequence of magnetic phases in Co3TeO6 is presented. The strongly first-order character of the transition to the commensurate multiferroic ground state, induced by coupled order parameters corresponding to different wavevectors, is related to a large magnetoelastic effect with an exchange energy critically sensitive to the interatomic spacing. The monoclinic magnetic symmetry C2' of the multiferroic phase permits spontaneous polarization and magnetization as well as the linear magnetoelectric effect. The existence of weakly ferromagnetic domains is verified exp…
Magnetic phase transitions in multiferroic bismuth ferrite (BiFeO3) induced by magnetic field, epitaxial strain, and composition modification are considered. These transitions from a spatially modulated spin spiral state to a homogenous antiferromagnetic one are accompanied by the release of latent magnetization and a linear magnetoelectric effect that makes BiFeO3-based materials efficient room-temperature single phase multiferroics.
Ferroelectricity in the incommensurate helical magnetic phase (below TN, 43K) of alpha CaCr2O4 has been confirmed by pyroelectric measurements. Magnetoelectric and magnetodielectric coupling exist below TN and are proportional to the square of magnetic field. From symmetry analysis, we suggest that the presence of an external electric field destabilizes the symmetrical 2221' phase and stabilizes 21' symmetry. This provides a unique system in which polarization varies as the fourth-degree of the order-parameter amplitude and exhibit a vanishingly small value below the first-order transition at …
Nonreciprocal devices that allow the light propagation in only one direction are indispensable in photonic circuits and emerging quantum technologies. Contemporary optical isolators and circulators, however, require large size or strong magnetic fields because of the general weakness of magnetic light-matter interactions, which hinders their integration into photonic circuits. Aiming at stronger magneto-optical couplings, a promising approach is to utilize nonlinear optical processes. Here, we demonstrate nonreciprocal magnetoelectric second harmonic generation (SHG) in CuB2O4. SHG transmissio…
We report the discovery of a metamagnetic phase transition in a polar antiferromagnet Ni$_3$TeO$_6$ that occurs at 52 T. The new phase transition accompanies a colossal magnetoelectric effect, with a magnetic-field-induced polarization change of 0.3 $μ$C/cm$^2$, a value that is 4 times larger than for the spin-flop transition at 9 T in the same material, and also comparable to the largest magnetically-induced polarization changes observed to date. Via density-functional calculations we construct a full microscopic model that describes the data. We model the spin structures in all fields and cl…
We report a detailed single crystal investigation of a magnetoelectric ferrimagnet Cu2OSeO3 using dc magnetization and ac susceptibility along the three principal directions [100], [110] and [111]. We have observed that in small magnetic fields two magnetic transitions occur, one at Tc = 57 K and the second one at TN = 58 K. At Tc the non-linear susceptibility reveals the emergence of the ferromagnetic component and below Tc the magnetization measurements show the splitting between field-cooled and zero-field-cooled regimes. Above 1000 Oe the magnetization saturates and the system is in a sing…
The properties of antiferromagnetic materials with violated space-time parity are considered. Particular attention is given to the bismuth ferrite BiFeO3 ferroelectric magnet. This material is distinguished from other antiferromagnets in that the inversion center is absent in its crystal and magnetic structures. This circumstance gives rise to the diversified and unusual properties, namely, to the appearance of a spatially modulated spin structure and to the unique possibility of the linear magnetoelectric effect coexisting with a weak ferromagnetic moment. The magnetic-induced phase transitio…
Electric and magnetic properties of multiferroic GdMn2O5 in external magnetic fields were investigated to map out the magnetoelectric phases in this material. Due to strong magnetoelectric coupling, the dielectric permittivity is highly sensitive to phase boundaries in GdMn2O5, which allowed to construct the field-temperature phase diagrams. Several phase transitions are observed which are strongly field-dependent with respect to field orientation and strength. The phase diagram for a magnetic field along the crystallographic a-axis corresponds well to a polarization step, as induced by 90 deg…
We demonstrate room temperature ferroelectricity in the epitaxial thin films of magnetoelectric GaFeO3. Piezo-force measurements show a 180o phase shift of piezoresponse upon switching the electric field indicating nanoscale ferroelectricity in epitaxial thin films of gallium ferrite. Further, temperature dependent impedance analysis with and without the presence of an external magnetic field clearly reveals a pronounced magneto-dielectric effect across the magnetic transition temperature. In addition, our first principles calculations show that Fe ions are not only responsible for ferrimagnet…
In this article, we perform the symmetry analysis of perovskite-based multiferroics: bismuth ferrite (BiFeO3)-like, orthochromites (RCrO3), and Ruddlesden-Popper perovskites (Ca3Mn2O7-like), being the typical representatives of multiferroics of the trigonal, rhombic, and tetragonal crystal families and explore the effect of crystallographic distortions on magnetoelectric properties. We determine the principal order parameters for each of the considered structures and obtain their invariant combinations consistent with the particular symmetry. This approach allowed us to analyze the features of…
Nanoparticles of the ferrimagnetic epsilon-Fe2O3 oxide have been synthesized by sol-gel method. Here, we report on the measurements of the dielectric permittivity as a function of temperature, frequency and magnetic field. It is found that, coinciding with the transition from collinear ferrimagnetic ordering to an incommensurate magnetic state occurring at about 100 K, there is an abrupt change (about 30 %) of permittivity suggesting the existence of a magnetoelectric coupling in this material. Indeed, magnetic field dependent measurements at 100 K have revealed an increase of the permittivity…
The intrinsic noncollinear spin patterns in rare-earth pyrochlore are physically interesting, hosting many emergent properties, e.g. spin ice and monopole-type excitation. Recently, the magnetic monopole excitation of spin ice systems was predicted to be magnetoelectric active, while rare experimental works have directly confirmed this scenario. In this work, we performed systematic experimental investigation on the magnetoelectricity of Dy$_2$Ti$_2$O$_7$ by probing the ferroelectricity, spin dynamics, and dielectric behaviors. Two ferroelectric transitions at $T_{c1}$=25 K and $T_{c2}$=13 K h…
We show that 1:1 ordering of A$'$ and A$''$ cations in A$'_{1/2}$A$''_{1/2}$B$_2$X$_4$ magnetic spinels results in appearance of magnetoelectric properties. Possible value of magnetically induced electric polarization is calculated using the recently proposed microscopic model, which takes into account spin-dependent electric dipole moments of magnetic ions located in noncentrosymmetric crystallographic positions. We build phenomenological models of magnetic phase transitions in cation-ordered spinels, which describe ferromagnetic and antiferromagnetic ordering patterns of B cation spins, and …
Two kinds of specimens, with the major phase of Sr3Co2Fe24O41 (Sr3Co2Z) and SrCo2Fe16O27 (SrCo2W) hexaferrites respectively, were fabricated through solid-state reaction. The phase composition, magnetic and dielectric properties, magnetodielectric (MD) effect, magnetoelectric (ME) effect and pyroelectric properties were studied. Results show that magnetic and dielectric anomalies are induced by the magnetocrystalline anisotropy (MCA) transition. They can be considered as characteristic properties (e.g., Sr3Co2Z at 370 K) but are not a sufficient condition for the MD and ME coupling. The T-bloc…
We report coupling between magnetic and electric orders for antiferromagnetic polycrystalline FeVO4 in which magnetism-induced polarization has been recently found in noncollinear antiferromagnetic state below the second antiferromagnetic phase transition at TN2=15.7K. In this low symmetry phase space group P-1, the magnetic field dependence of electric polarization evidences a clear magnetoelectric coupling in the noncollinear spin-configured antiferromagnetic phase. The discontinuity of magnetodielectric effect observed at the vicinity of the polar to nonpolar transition evidences competitio…
Co4Nb2O9 (CNO) having α-Al2O3 crystal structure with Co chains along c-direction shows gigantic magnetoelelctric coupling below antiferromagnetic ordering temperature of 27 K but above a spin flop field of 1.6 T. We have investigated structural, magnetic and magnetoelectric properties of Fe substituted (10% and 20%) samples and compared with the parent one. In fact magnetic and specific heat measurements have revealed an additional magnetic transition below 10 K and presence of short range magnetic ordering above ~ 50 K in parent as well as in Fe substituted samples. Linear magnetoelelctric an…
High-resolution neutron diffraction determination of noncollinear antiferromagnetic order in the honeycomb magnetoelectric Fe$_{4}$Nb$_{2}$O$_{9}$
Institute for Basic Science (IBS)（韩国基础科学研究院）；Yonsei University（延世大学）；Chonnam National University（全南国立大学）；Center for Integrated Nanostructure Physics, Institute for Basic Science (IBS)（韩国基础科学研究院集成纳米物理中心）；Sungkyunkwan University（成均馆大学）；Rutgers University（罗格斯大学）
We report the magnetic, dielectric and ferroelectric properties of polycrystalline iron vanadate(FeVO4), which has been recently found to exhibit multiferroicity in low temperature with noncollinear magnetic orderings. The influence of external magnetic field up to 9T on these properties is systematically investigated. Besides the suppressing effect on the original ferroelectric transition, the strong magnetic field seems to induce a secondary ferroelectric transition at a slight lower temperature. And the corresponding magnetization measurement reveals a field-induced metamagnetic transition …
By combining single crystal x-ray and neutron diffraction, and the magnetodielectric measurements on single crystal Fe4Nb2O9, we present the magnetic structure and the symmetry-allowed magnetoelectric coupling in Fe4Nb2O9. It undergoes an antiferromagnetic transition at TN=93 K, followed by a displacive transition at TS=70 K. The temperature-dependent dielectric constant of Fe4Nb2O9 is strongly anisotropic with the first anomaly at 93 K due to the exchange striction as a result of the long range spin order, and the second one at 70 K emanating from the structural phase transition primarily dri…
We present a thorough $^{77}$Se NMR study of a single crystal of the magnetoelectric compound Cu$_2$OSeO$_3$. The temperature dependence of the local electronic moments extracted from the NMR data is fully consistent with a magnetic phase transition from the high-T paramagnetic phase to a low-T ferrimagnetic state with 3/4 of the Cu$^{2+}$ ions aligned parallel and 1/4 aligned antiparallel to the applied field of 14.09 T. The transition to this 3up-1down magnetic state is not accompanied by any splitting of the NMR lines or any abrupt modification in their broadening, hence there is no observa…
The nature and symmetry of the transition mechanisms in the spin-spiral copper halides CuCl$_2$ and CuBr$_2$ are analyzed theoretically. The magnetoelectric effects observed in the two multiferroic compounds are described and their phase diagram at zero and applied magnetic fields are worked out. The emergence of the electric polarization at zero field below the paramagnetic phase is shown to result from the coupling of two distinct spin-density waves and to be only partly related to the Dzialoshinskii-Moriya interactions. Applying a magnetic field along the two-fold monoclinic axis of CuCl$_2…
In this work, we analysed GdMnO3 magnetoelectric thin films prepared by a general sol-gel method. The film formation temperature is analysed by termogravimetric analysis, while the lattice parameters of the Pbnm orthorhombic films are determined from the analysis of the x-ray spectra. The x-ray results also reveal that GdMnO3 films are under compression along the b axis. The lattice dynamic analysis carried out by Raman spectroscopy confirms the formation of films with a Pbnm orthorhombic structure. Moreover, the analysis of the Raman spectra suggests that besides film-substrate interaction, t…
The magnetoelectric (ME) effects are investigated in a cubic compound SrCuTe2O6, in which uniform Cu2+ (S=1/2) spin chains with considerable spin frustration exhibit a concomitant antiferromagnetic transition and dielectric constant peak at TN=5.5 K. Pyroelectric Jp(T) and magnetoelectric current JME(H) measurements in the presence of a bias electric field are used to reveal that SrCuTe2O6 shows clear variations of Jp(T) across TN at constant magnetic fields. Furthermore, isothermal measurements of JME(H) also develop clear peaks at finite magnetic fields, of which traces are consistent with t…
For disordered Heisenberg systems with small single ion anisotropy, two spin glass transitions below the long range ordered phase transition temperature has been predicted theoretically for compositions close to the percolation threshold. Experimental verification of these predictions is still controversial for conventional spin glasses. We show that multiferroic spin glass systems can provide a unique platform for verifying these theoretical predictions via a study of change in magnetoelastic and magnetoelectric couplings, obtained from an analysis of diffraction data, at the spin glass trans…
By means of symmetry analysis, density functional theory calculations, and Monte Carlo simulations we show that goethite, $α$-FeOOH, is a linear magnetoelectric below its Néel temperature $T_{\rm N}=400$ K. The experimentally observed magnetic field induced spin-flop phase transition results in either change of direction of electric polarization or its suppression. Calculated value of magnetoelectric coefficient is 0.24 $μ$C m$^{-2}$ T$^{-1}$. The abundance of goethite in nature makes it arguably the most widespread magnetoelectric material.
Magnetic-field effect on the magnetic and electric properties in a chiral polar ordered corundum Ni$_2$InSbO$_6$ has been investigated. Single-crystal soft x-ray and neutron diffraction measurements confirm long-wavelength magnetic modulation. The modulation direction tends to align along the magnetic field applied perpendicular to the polar axis, suggesting that the nearly proper-screw type helicoid should be formed below 77\,K. The application of a high magnetic field causes a metamagnetic transition. In a magnetic field applied perpendicular to the polar axis, a helix-to-canted antiferromag…
