Analytical expressions for the magnetoelastic anisotropy constants of cubic magnetic systems are derived for rectangular and oblique distortions originating from epitaxial growth on substrates with lower crystal symmetry. In particular, the temperature variation of the magnetic properties of magnetic films grown on barium titanate (BaTiO3) substrates are explained in terms of strain-induced magnetic anisotropies caused by the temperature dependent phase transitions of BaTiO3. Our results quantify the experimental observations in ferromagnet/\bto-based structures, which have been proposed as templates for magnetoelectric composite heterostructures.
Extrinsic multiferroic hybrid structures consisting of ferromagnetic and ferroelectric layers elastically coupled to each other are promising due to their robust magnetoelectric effects even at room temperature. For a quantitative analysis of these magnetoelectric effects, a detailed knowledge of the piezoelectric and magnetoelastic behavior of both constituents as well as their mutual elastic coupling is mandatory. We here report on a theoretical and experimental study of the magnetic behavior of BaTiO3-based extrinsic multiferroic structures. An excellent agreement between molecular dynamics…
Multiferroics where at least two primary ferroic orders are present and coupled in a single system constitute an important class of materials. They attracted special consideration as they present both intriguing fundamental physics problems and technological importance for potential multifunctional devices. Here, we present the evidence of multiferroicity and magnetoelectric (ME) coupling in alpha-Mn2O3; a unique binary perovskite. Corresponding to the antiferromagnetic (AFM) ordering around 80K, a clear frequency independent transition is observed in the dielectric permittivity. We showed tha…
Complex experimental and theoretical study 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 much larger (above 3 10^(-4) C/m^2) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (~50 …
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…
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…
Magnetoelastic and magnetoelectric coupling in the artificial multiferroic heterostructures facilitate valuable features for device applications such as magnetic field sensors and electric write magnetic-read memory devices. In a ferromagnetic/ferroelectric heterostructures, the strain mediated coupling exploits piezoelectricity/electrostriction in ferroelectric phase and magnetostriction/piezomagnetism in ferromagnetic phase. Such verity of these combined effect can be manipulated by an external perturbation, such as electric field, temperature or magnetic field. Here, we demonstrate the remo…
The magnetoelastic coupling in multiferroic $DyMn_2O_5$ is investigated by magnetostriction measurements along the three crystallographic orientations. Strong lattice anomalies as a function of the magnetic field are detected at the low temperature magnetic and ferroelectric phase transitions. The sign and magnitude of the magnetostrictive coefficient as well as the lattice anomalies at the transitions are correlated with the Dy moment order and with the sharp changes of the dielectric constant and the ferroelectric polarization. With the magnetic field applied along the c-axis a new high-fiel…
We have investigated magnetoelastic effects in multiferroic YMnO$_3$ below the antiferromagnetic phase transition, $T_N \approx 70$ K, using neutron powder diffraction. The $a$ lattice parameter of the hexagonal unit cell of YMnO$_3$ decreases normally above $T_N$, but decreases anomalously below T$_N$, whereas the $c$ lattice parameter increases with decreasing temperature and then increases anomalously below T$_N$. The unit cell volume also undergoes an anomalous contraction below $T_N$. By fitting the background thermal expansion for a non-magnetic lattice with the Einstein-Grüneisen equati…
Using THz spectroscopy, we show that the spin-wave spectrum of multiferroic BiFeO$_3$ in its high-field canted antiferromagnetic state is well described by a spin model that violates rhombohedral symmetry. We demonstrate that the monoclinic distortion of the canted antiferromagnetic state is induced by the single-ion magnetoelastic coupling between the lattice and the two nearly anti-parallel spins. The revised spin model for BiFeO$_3$ contains two new single-ion anisotropy terms that violate rhombohedral symmetry and depend on the direction of the magnetic field.
Using a magneto-optical pump-probe technique with micrometer spatial resolution we show that magnetization precession can be launched in individual magnetic domains imprinted in a Co$_{40}$Fe$_{40}$B$_{20}$ (CoFeB) layer by elastic coupling to ferroelectric domains in a BaTiO$_{3}$ substrate. The dependence of the precession parameters on external magnetic field strength and orientation reveal that by laser-induced ultrafast partial quenching of the magnetoelastic coupling parameter of CoFeB by $\approx$27% along with 10% ultrafast demagnetization trigger the magnetization precession. The rela…
Hexagonal YMnO_3 with space group P63cm is one of the rare examples of multiferroic materials that exhibit co-dependence of a robust ferroelectric phase along with antiferromagnetic ordering. This is primarily ascribed to tilting of the MnO_5 polyhedra driven by magnetoelectric coupling. We report on the effect of magnetic field at the atomic level in YMnO_3 by utilizing magnetic field and temperature dependent neutron diffraction measurements. We show that near the Néel temperature the lattice parameters, effective magnetic moment per site, Mn-O bond lengths and O-Mn-O bond angles show large …
Magnetoelastic coupling, i.e., the change of crystal lattice induced by a spin order, is not only scientifically interesting, but also technically important. In this work, we propose a general microscopic model from first-principles calculations to describe the magnetoelastic coupling and provide a way to construct the microscopic model from density functional theory calculations. Based on this model, we reveal that there exists a previously unexpected contribution to the electric polarization induced by the spin-order in multiferroics due to the combined effects of magnetoelastic coupling and…
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…
Evidence for a strong spin-lattice coupling in multiferroic HoMnO_3 is derived from thermal expansion measurements along a- and c-axis. The magnetoelastic effect results in sizable anomalies of the thermal expansivities at the antiferromagnetic (T_N) and the spin rotation (T_{SR}) transition temperatures as well as in a negative c-axis expansivity below room temperature. The coupling between magnetic orders and dielectric properties below T_N is explained by the lattice strain induced by the magnetoelastic effect. At T_{SR} various physical quantities show discontinuities that are thermodynami…
Many technological applications of multiferroics are based on their ability to reconstruct the domain structure (DS) under the action of small external fields. In the present paper we analyze the different scenarios of the DS behavior in a multiferroic that shows simultaneously ferro- and antiferromagnetic ordering on the different systems of magnetic ions. We consider the way to control a composition of the DS and macroscopic properties of the sample by an appropriate field treatment. We found out that sensitivity of the DS to the external magnetic field and the magnetic susceptibility in a l…
In this work, we consider the possibility of using synthetic multiferroics comprising piezoelectric and magnetostrictive materials as an interconnect for nano magnetic logic circuits. The proposed interconnect resembles a parallel plate capacitor filled with a piezoelectric, where one of the plates is made of a magnetoelastic material. The operation of the interconnect is based on the effect of stress-mediated anisotropy modulation, where an electric field applied across the piezoelectric material produces stress, which, in turn, affects the anisotropy field in the magnetostrictive material. W…
The multiferroic properties of EuTiO3 are greatly enhanced when a sample is strained, signifying that coupling between strain and structural, magnetic or ferroelectric order parameters is extremely important. Here resonant ultrasound spectroscopy has been used to investigate strain coupling effects, as well as possible additional phase transitions, through their influence on elastic and anelastic relaxations that occur as a function of temperature between 2 and 300 K and with applied magnetic field up to 14 T. Antiferromagnetic ordering is accompanied by acoustic loss and softening, and a weak…
We investigate theoretically the magnetic dynamics in a ferroelectric/ferromagnetic heterostructure coupled via strain-mediated magnetoelectric interaction. We predict an electric field-induced magnetic switching in the plane perpendicular to the magneto-crystalline easy axis, and trace this effect back to the piezoelectric control of the magnetoelastic coupling. We also investigate the magnetic remanence and the electric coercivity.
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…
Here we demonstrate that MnTe epitaxial films with zinc-blend structure and MnTe/ZnTe multilayers should show ferroelectric polarization in antiferromagnetically (AFM) ordered state and thus belong to multiferroics. Spontaneous ferroelectric polarization results from the bending of highly ionic Mn-Te-Mn bonds induced by magnetostrictive shear strain. Orientation of ferroelectric polarization is coupled with orientation of AFM vector and thus can be controlled by application of the external magnetic field. Due to the clamping of electric and magnetic order parameters, domain structure in MnTe i…
A method is developed which allows to determine the first-order and the second-order magnetoelastic coefficients of a magnetic bulk material from the ab-initio calculation of the magnetocrystalline anisotropy energy as function of a prestrain. Excplicit results are given for bcc Fe, and they agree well with experimental data obtained from the magnetostrictive stress measurements for epitaxial Fe films.
We have studied the magnetodielectric and magnetoelastic coupling in TbFe3(BO3)4 single crystals by means of capacitance, magnetostriction and Raman spectroscopy measurements. The data reveal strong magnetic field effects on the dielectric constant and on the macroscopic sample length which are associated to long range magnetic ordering and a field-driven metamagnetic transition. We discuss the coupling of the dielectric, structural, and magnetic order parameters and attribute the origin of the magnetodielectric coupling to phonon mode shifts according to the Lyddane-Sachs-Teller (LST) relatio…
We present a laterally resolved X-ray magnetic dichroism study of the magnetic proximity effect in a highly ordered oxide system, i.e. NiO films on Fe3O4(110). We found that the magnetic interface shows an ultrasharp electronic, magnetic and structural transition from the ferrimagnet to the antiferromagnet. The monolayer which forms the interface reconstructs to NiFe2O4 and exhibits an enhanced Fe and Ni orbital moment, possibly caused by bonding anisotropy or electronic interaction between Fe and Ni cations. The absence of spin-flop coupling for this crystallographic orientation can be explai…
The realization of intertwined ferroelasticity and ferromagnetism in two-dimensional (2D) lattices is of great interest for broad nanoscale applications, but still remains a remarkable challenge. Here, we propose an alternative approach to realize the strongly coupled ferromagnetism and ferroelasticity by carrier doping. We demonstrate that prototypical 2D \b{eta}-PbO is dynamically, thermally and mechanically stable. Under hole doping, 2D \b{eta}-PbO possesses ferromagnetism and ferroelasticity simultaneously. Moreover, the robustness of ferromagnetic and ferroelastic orders are doping tunabl…
We show that the magnetoelastic coupling between the magnetization and the amplitude of a short wavelength phonon enables the existence of a first order premartensitic transition from a bcc to a micromodulated phase in $Ni_{2}MnGa$. Such a magnetoelastic coupling has been experimentally evidenced by AC susceptibility and ultrasonic measurements under applied magnetic field. A latent heat around 9 J/mol has been measured using a highly sensitive calorimeter. This value is in very good agreement with the value predicted by a proposed model.
We report measurements of the in-plane magnetoelastic coupling in ultra-thin Ta|CoFeB|MgO layers as a function of uniaxial strain, conducted using a four-point bending apparatus. For annealed samples, we observe a strong dependence on the thickness of the CoFeB layer in the range 1.3-2.0 nm, which can be modeled as arising from a combination of effective surface and volume contributions to the magnetoelastic coupling. We point out that if similar thickness dependence exists for magnetoelastic coupling in response to biaxial strain, then the standard Néel model for the magnetic anisotropy energ…
Chiral Phonons Enable Ultrafast Magnetization Switching via Magnetoelastic Coupling
Nanjing University of Aeronautics and Astronautics (NUAA)（南京航空航天大学）；Instituto de Ciencia de Materiales de Madrid (ICMM), CSIC（马德里材料科学研究所，西班牙国家科学研究委员会）；The University of Manchester（曼彻斯特大学）；University of York（约克大学）
The existence of a magnetodielectric (magnetocapacitance) effect is often used as a test for multiferroic behavior in new material systems. However, strong magnetodielectric effects can also be achieved through a combination of magnetoresistance and the Maxwell-Wagner effect, unrelated to multiferroic coupling. The fact that this resistive magnetocapacitance does not require multiferroic materials may be advantageous for some practical applications. Conversely, it also implies that magnetocapacitance per se is not sufficient to establish multiferroic coupling.
Exchange interactions in α- and γ-Fe are investigated within an ab-initio spin spiral approach. We have performed total energy calculations for different magnetic structures as a function of lattice distortions, related with various cell volumes and the Bain tetragonal deformations. The effective exchange parameters in γ-Fe are very sensitive to the lattice distortions, leading to the ferromagnetic ground state for the tetragonal deformation or increase of the volume cell. At the same time, the magnetic-structure-independent part of the total energy changes very slowly with the tetragonal defo…
Pressure-induced thermal expansion anomalies in dhcp iron hydride associated with magnetoelastic coupling
The University of Tokyo（东京大学）；Yale University（耶鲁大学）；Flatiron Institute（平顿研究所）；Center for High Pressure Science and Technology Advanced Research（高压科学与技术先进研究中心）；Pohang University of Science and Technology（浦项科技大学）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究所）
Dynamical properties of the lattice structure was studied by optical spectroscopy in ACr2O4 chromium spinel oxide magnetic semiconductors over a broad temperature region of T=10-335K. The systematic change of the A-site ions (A=Mn, Fe, Co, Ni and Cu) showed that the occupancy of 3d orbitals on the A-site, has strong impact on the lattice dynamics. For compounds with orbital degeneracy (FeCr2O4, NiCr2O4 and CuCr2O4), clear splitting of infrared-active phonon modes and/or activation of silent vibrational modes have been observed upon the Jahn-Teller transition and at the onset of the subsequent …
We proved the existence of a universal flexo-antiferrodistortive coupling as a necessary complement to the well-known flexoelectric coupling. The coupling is universal for all antiferrodistortive systems and can lead to the formation of incommensurate, spatially-modulated phases in multiferroics. Our analysis can provide a self-consistent mesoscopic explanation for a broad range of modulated domain structures observed experimentally in multiferroics.
Multiferroics offer exciting opportunities for electric-field control of magnetism. Unfortunately, single-phase multiferroics suitable for such applications at room temperature has not been discovered. Here, we propose the concept of a new type of multiferroics, namely, "asymmetric multiferroic". In asymmetric multiferroics, two locally stable ferroelectric states are not symmetrically equivalent, leading to different magnetic properties between these two states. Furthermore, we predict from first-principles that a Fe-Cr-Mo superlattice with the LiNbO3-type structure is such an asymmetric mult…
Temperature dependent X-ray diffraction and Raman spectroscopic studies were carried out on the flux grown single crystals of gallium ferrite with Ga:Fe ratio of 0.9:1.1. Site occupancy calculations from the Rietveld refinement of the X-ray data led to the estimated magnetic moment of ~0.60 \muB /f.u. which was in good agreement with the experimental data. Combination of these two measurements indicates that there is no structural phase transition in the material between 18 K to 700 K. A detailed line shape analysis of the Raman mode at ~375 cm^-1 revealed a discontinuity in the peak position …
We report local probe investigations of the magnetic interaction between BiFeO3 films and a ferromagnetic Co0.9Fe0.1 layer. Within the constraints of intralayer exchange coupling in the Co0.9Fe0.1, the multiferroic imprint in the ferromagnet results in a collinear arrangement of the local magnetization and the in-plane BiFeO3 ferroelectric polarization. The magnetic anisotropy is uniaxial, and an in-plane effective coupling field of order 10 mT is derived. Measurements as a function of multiferroic layer thickness show that the influence of the multiferroic layer on the magnetic layer becomes …
Two-dimensional (2D) semiconducting multiferroics that can effectively couple magnetic and polarization (P) orders have great interest for both fundamental research and technological applications in nanoscale, which are, however, rare in nature. In this study, we propose a general mechanism to realize semiconducting 2D multiferroics via vdW heterojunction engineering, as demonstrated in a typical heterostructure consisting of magnetic bilayer CrI3 (bi-CrI3) and ferroelectric monolayer In2Se3. Interestingly, the novel indirect orbital coupling between Se 4p and Cr 3d orbitals, intermediated by …
We report the first magnetic-field-dependent Raman scattering studies on Pb(Zr,Ti)O3-CoFe2O4 bilayer multiferroic system. The phonon frequencies of the nano-bilayers obviously change with magnetic field, which is absent in the single Pb(Zr,Ti)O3 films. The magnetostriction of the CoFe2O4 layer generates stress mechanically transferred to the Pb(Zr,Ti)O3 layer, resulting in the mode changes. The observed magnetic-field-induced softening of the soft mode in the Pb(Zr,Ti)O3 layer bears a striking resemblance to direct magnetoelectric output in the bilayers, providing evidence for stress-mediated …
We study theoretically the multiferroic dynamics in a composite one-dimensional system consisting of BaTiO3 multiferroically coupled to an iron chain. The method treats the magnetization and the polarization as thermodynamic quantities describable via a combination of the Landau-Lifshits- Gilbert and the Ginzburg-Landau dynamics coupled via an additional term in the total free energy density. This term stems from the multiferroic interaction at the interface. For a wide range of strengths of this coupling we predict the possibility of obtaining a well-developed hysteresis in the ferromagnetic …
The electric and magnetic properties of (BaTiO$_3$)$_n$/(CaMnO$_3$)$_n$ short-period superlattices are studied by the first-principles calculations. The local electric polarizations in the CaMnO$_3$ layers are significant, comparable to that in the BaTiO$_3$ layers. Remarkably, the electric polarization is almost doubled when the spin configuration changes from antiferromagnetic to ferromagnetic in the superlattices, indicating a giant magnetoelectric coupling. This enhancement of the magnetoelectric coupling is due to the suppression of the antiferrodistortive mode in the CaMnO$_3$ layers at …
We investigate polarization memory effects in single-crystal CuFeO2, which has a magnetically-induced ferroelectric phase at low temperatures and applied B fields between 7.5 and 13 T. Following electrical poling of the ferroelectric phase, we find that the nonpolar collinear antiferromagnetic ground state at B = 0 T retains a strong memory of the polarization magnitude and direction, such that upon re-entering the ferroelectric phase a net polarization of comparable magnitude to the initial polarization is recovered in the absence of external bias. This memory effect is very robust: in pulsed…
The influence of epitaxial strain on uniaxial magnetic anisotropy of Co$_{2}$FeSi (CFS) and Co$_{2}$MnSi (CMS) Heusler alloy thin films grown on (001) SrTiO$_3$ (STO) and MgO is reported. The in-plane biaxial strain is susceptible to tune by varying the thickness of the films on STO, while on MgO the films show in-plane easy axis for magnetization (\overrightarrow{M}) irrespective of their thickness. A variational analysis of magnetic free energy functional within the Stoner-Wohlfarth coherent rotation model with out-of-plane uniaxial anisotropy for the films on STO showed the presence of magn…
We theoretically investigate the magnetoelastic coupling (MEC) and its effect on magnon transport in two-dimensional antiferromagnets with a honeycomb lattice. MEC coeffcient along with magnetic exchange parameters and spring constants are computed for monolayers of transition metal trichalcogenides with Néel order ($\text{MnPS}_3$ and $\text{VPS}_3$) and zigzag order ($\text{CrSiTe}_3$, $\text{NiPS}_3$ and $\text{NiPSe}_3$) by $ab$ $initio$ calculations. Using these parameters, we predict that the spin-Nernst coefficient is significantly enhanced due to magnetoelastic coupling. Our study show…
The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated mag…
We report observation of magneto-electric and magneto-dielectric couplings in ceramic Co3TeO6. Temperature dependent DC magnetization and dielectric constant measurements together indicate coupling between magnetic order and electronic polarization. Strong anomaly in dielectric constant at ~ 18K in zero magnetic field indicates presence of spontaneous polarization. Observations like weak ferromagnetic order at lower temperature, field and temperature dependences of the ferroelectric transition provide experimental verification of the recent theoretical proposal by P. Toledano et al., Phys. Rev…
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 …
Organic-inorganic multiferroics are promising for the next generation of electronic devices. To date, dozens of organic-inorganic multiferroics have been reported; however, most of them show magnetic Curie temperature much lower than room temperature, which drastically hampers their application. Here, by performing first-principle calculations and building effective model Hamiltonians, we reveal a molecular orbital-mediated magnetic coupling mechanism in two-dimensional Cr(pyz)2 (pyz=pyrazine), and the role that the valence state of the molecule plays in determining the magnetic coupling type …
The list of materials systems displaying both electric and magnetic long range order is short. Oxides, however, concentrate numerous examples of multiferroicity with, in some cases, a large magnetoelectric coupling. As a result, a fruitful research field has emerged contemporaneously with the consolidation of spintronic. The synergy between multiferroics and spintronics was meant to be inevitable and hence the characterization of spintronic functionalities in multiferroic materials is rather abundant. The aim of the present chapter is to review the oxide heterostructures where magnetoelectric …
Microscopic spin interactions on a deformed Kagomé lattice of volborthite are investigated through magnetoelastic couplings. A negative longitudinal magnetostriction $ΔL<0$ in the $b$ axis is observed, which depends on the magnetization $M$ with a peculiar relation of $ΔL/L \propto M^{1.3}$. Based on the exchange striction model, it is argued that the negative magnetostriction originates from a pantograph-like lattice change of the Cu-O-Cu chain in the $b$ axis, and that the peculiar dependence arises from the local spin correlation. This idea is supported by DFT+$U$ calculations simulating th…
Double perovskites provide a unique opportunity to induce and control multiferroic behaviors in oxide systems. The appealing possibility to design materials with a strong coupling between the magnetization and the polarization fields may be achieved in this family since these magnetic insulators can present structural self-ordering in the appropriate growth conditions. We have studied the functional properties of La2CoMnO6 and Bi2CoMnO6 epitaxial thin films grown by pulsed laser deposition. Cation-ordered La2CoMnO6 films display a magnetic Curie temperature of 250 K while cation-disordered Bi2…
