Magnetic axis rotation (MAR) in ferromagnetic (FM) layers is crucial for strain-mediated converse magnetoelectric coupling. Employing the density functional theory (DFT), we computationally study the magnetic anisotropy of selected deformed FM materials such as body-centered iron. The results show that the short axis is more energy-favorable at high in-plane strain difference than previously predicted phenomenologically. This anomalous trend and the complex energy behaviors at different strain conditions explain why spin-lattice dynamics (SLD) simulation does not produce in-plane MAR and imply couplings between different energy terms together with high order coefficient contributions.
We present a first-principles scheme for the computation of the magnetoelectric response of magnetic insulators. The method focuses on the lattice-mediated part of the magnetic response to an electric field, which we argue can be expected to be the dominant contribution in materials displaying a strong magnetoelectric coupling. We apply our method to Cr2O3, a relatively simple and experimentally well studied magnetoelectric compound.
Experiments have been performed to measure magnetoelectric properties of room temperature spirally ordered Sr3Co2Fe24O41 hexaferrite slabs. The measured properties include the magnetic permeability, the magnetization and the strain all as a function of the electric field E and the magnetic intensity H. The material hexaferrite Sr3Co2Fe24O41 exhibits broken symmetries for both time reversal and parity. The product of the two symmetries remains unbroken. This is the central feature of these magnetoelectric materials. A simple physical model is proposed to explain the magnetoelectric effect in th…
The quantitative understanding of converse magnetoelectric effects, i.e., the variation of the magnetization as a function of an applied electric field, in extrinsic multiferroic hybrids is a key prerequisite for the development of future spintronic devices. We present a detailed study of the strain-mediated converse magnetoelectric effect in ferrimagnetic Fe3O4 thin films on ferroelectric BaTiO3 substrates at room temperature. The experimental results are in excellent agreement with numerical simulation based on a two-region model. This demonstrates that the electric field induced changes of …
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 …
While tremendous success has been achieved to date in creating both single phase and composite magnetoelectric materials, the quintessential electric-field control of magnetism remains elusive. In this work, we demonstrate a linear magnetoelectric effect which arises from a novel carrier-mediated mechanism, and is a universal feature of the interface between a dielectric and a spin-polarized metal. Using first-principles density functional calculations, we illustrate this effect at the SrRuO$_3$/SrTiO$_3$ interface and describe its origin. To formally quantify the magnetic response of such an …
Magnetoelectric coupling between magnetic and electric dipoles is one of the cornerstones of modern physics towards developing the most energy-efficient magnetic data storage. Conventionally, magnetoelectric coupling is achieved in single-phase multiferroics or in magnetoelectric composite nanostructures consisting of ferromagnetic and ferroelectric/piezoelectric materials. Here, we demonstrate an electric-field-induced strain-mediated magnetoelectric effect in ultrathin CoFeB/MgO magnetic tunnel junction employing non-piezoelectric material, which is a vitally important structure for spintron…
We present a phenomenological scheme to study the size-dependent electric voltage-controlled magnetic anisotropy in ferromagnetic (FM)/ferroelectric (FE) heterostructures. The FM layers are either metallic Fe(001), Ni(001), Co(0001), or half-metallic (La, Sr)MnO3 films. Two magnetoelectric mechanisms, i.e., interface-charge and strain-mediated couplings, are considered. We show that the interface-charge mediated coupling is the main mechanism for the magnetoelectic coupling when the FM film thickness is below a certain transition thickness dtr while the strain-mediated coupling dominates above…
Electromechanical and magnetoelectric properties of Metglas/LiNbO3/Metglas trilayers have been studied in the frequency range from 20 Hz to 0.4 MHz. A trilayer of Metglas/PMN-PT/Metglas prepared in the same way was used as a reference. Though PMN-PT has much larger charge piezocoefficients than LiNbO3 (LNO), the direct magnetoelectric voltage coefficient is found to be comparable in both trilayers due to the much lower dielectric permittivity of LNO. The magnitude of the direct magnetoelectric effect in the LNO trilayers is about 0.4 V/cm*Oe in the quasistatic regime and about 90 V/cm*Oe at el…
Magnetoelectric coupling terms are derived in piezoelectric/magnetostrictive (multiferroic) thin film heterostructures using Landau-Ginzburg free energy expansions in terms of strain and by considering strain boundary conditions between the two materials. Then, a general effective medium method for solving for the complete electromagnetic susceptibility tensor of such heterostructures is used to calculate the ferromagnetic resonance frequency in a BaTiO$_3$/NiFe$_2$O$_4$ superlattice. This method differs from existing methods for treating magnetoelectric heterostructures since the magnetic and…
Magnetoelectric (ME) effect has been studied in a structure of a magnetostrictive TbFe2 alloy, two piezoelectric Pb(Zr,Ti)O3 (PZT) ceramics, and two nonmagnetic flakes. The ME coupling originates from the magnetic-mechanical-electric transform of the magnetostrictive effect in TbFe2 and the piezoelectric effect in PZT by end bonding, instead of interface bonding. Large ME coefficients of 10.5 and 9.9 Vcm-1Oe-1 were obtained at the first planar acoustic and third bending resonance frequencies, which are larger than that of conventional layered TbFe2/PZT composites. The results show that the lar…
We show that the presence of free carriers in a substance can generate the multiferroic behavior. Namely, if the substance has mixed-valence ions, which can supply free carriers and have electric dipole and spin moments, all three types of long-range order (ferromagnetic, ferroelectric and magnetoelectric (ME)) can occur at low temperature. The physical origin of the effect is that charge carriers can mediate the multiferroic behavior via spin - spin (RKKY), dipole-dipole and dipole - spin interactions. Our estimate of the interaction magnitude shows that there exist an optimal carrier concent…
We demonstrate that the electronic contribution to the linear magnetoelectric response, usually omitted in first-principles studies, can be comparable in magnitude to that mediated by lattice distortions, even for materials in which responses are strong. Using a self-consistent Zeeman response to an applied magnetic field for noncollinear electron spins, we show how electric polarization emerges in linear magnetoelectrics through both electronic- and lattice-mediated components -- in analogy with the high- and low-frequency dielectric response to an electric field. The approach we use is conce…
Electric-field control of magnetism without electric currents potentially revolutionizes spintronics towards ultralow power. Here by using mechanically coupled phase field simulations, we computationally demonstrate the application of the strain-mediated magnetoelectric effect for the electric-field control of magnetic states in heterostructure. In the model heterostructure constituted of the soft nanomagnet Co and the piezoelectric substrate PMN-PT, both the volatility of magnetic states and the magnetization switching dynamics excited by the electric field are explored. It is found that an e…
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.
Development and Application of a Magnetoelectric Coupling Measurement System for Strain-Mediated Effects
UGC-DAE Consortium for Scientific Research（UGC-DAE 科学研究联盟）；Maharaja Institute of Technology Mysore（迈索尔 Maharaja 理工学院）；Institute of Sciences, SAGE University（SAGE 大学理学院）；Raja Ramanna Centre for Advanced Technology（Raja Ramanna 先进技术中心）
The self-polarization of PbZr0.52Ti0.48O3 thin film is switched by changing film thickness through the competition between the strain relaxation-induced flexoelectric fields and the interfacial effects. Without an applied electric field, this reversal of self-polarization is exploited to control the magnetic properties of La0.67Sr0.33MnO3 by the competition/cooperation between the charge-mediated and the strain-mediated effects. Scanning transmission electron microscopy, polarized near edge x-ray absorption spectroscopy, and half-integer diffraction measurements are employed to decode this int…
We introduce the notion of inverse effect of magnetostriction for magnetostrictive/piezoelectric heterostructures and study this effect theoretically and experimentally. It is shown that the inverse effect of magnetostriction may crucially contribute to the mechanism of magnetoelectric coupling. It is shown that the studied effect essentially modifies the saturation magnetostriction of the whole structure as compared to its magnetic phase bulk and also induces an additional magnetic anisotropy. Our consideration provides useful insight into the fundamental issue of strain-mediated magnetoelect…
The direct magnetoelectric (ME) effect mediated by lattice strains induced in a ferroelectric film by a ferromagnetic substrate is evaluated using first-principles-based calculations. To that end, the strain sensitivity of ferroelectric polarization and the film permittivity are calculated as a function of the in-plane biaxial strain for Pb(Zr0.52Ti0.48)O3 films under various depolarizing fields. It is found that the ME voltage coefficient varies nonmonotonically with this strain and may reach giant values exceeding 100 Vcm-1 Oe-1 over a strain range that can be controlled through the electric…
Controlling magnetism using voltage is highly desired for applications, but remains challenging due to fundamental contradiction between polarity and magnetism. Here we propose a mechanism to manipulate magnetic domain walls in ferrimagnetic or ferromagnetic multiferroics using electric field. Different from those studies based on static domain-level couplings, here the magnetoelectric coupling relies on the collaborative spin dynamics around domain walls. Accompanying the reversal of spin chirality driven by polarization switching, a "rolling-downhill"-like motion of domain wall is achieved a…
Although several multiferroic materials/heterostructures have been extensively studied, finding strong magnetoelectric couplings for the electric field control of the magnetization remains challenging. Here, a novel interfacial magnetoelectric coupling based on three components (ferroelectric dipole, magnetic moment, and antiferromagnetic order) is analytically formulated. As an extension of carrier-mediated magnetoelectricity, the new coupling is shown to induce an electric-magnetic hysteresis loop. Realizations employing BiFeO$_3$ bilayers grown along the [$111$] axis are proposed. Without i…
Magnetoelectric interactions in bilayers of magnetostrictive and piezoelectric phases are mediated by mechanical deformation. Here we discuss the theory and companion data for magnetoelectric (ME) coupling at electromechanical resonance (EMR) in a ferrite-lead zirconate titanate (PZT) bilayer. Estimated ME voltage coefficient versus frequency profiles for nickel, cobalt, or lithium ferrite and PZT reveal a giant ME effect at EMR with the highest coupling expected for cobalt ferrite-PZT. Measurements of resonance ME coupling have been carried out on layered and bulk composites of nickel ferrite…
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…
Magnetoelectric (ME) interactions in layered structures of magnetostrictive and piezoelectric phases are mediated by mechanical deformation. Here we discuss the frequency dependence of ME coupling in bilayers and trilayers of Permendur, a ferromagnetic alloy, and lead zirconate titanate. Data on ME voltage coefficient versus frequency profiles reveal a giant ME coupling at electromechanical resonance. The maximum voltage coefficient of 90 V/cm Oe is three orders of magnitude higher than low-frequency values. The ME interactions for transverse fields is an order of magnitude stronger than for l…
Large magnetoelectric response in thin films is highly desired for high-throughput and high-density microelectronic applications. However, the d0 rule in single-phase compounds usually results in a weak interaction between ferroelectric and magnetic orders; the magnetoelectric coupling via elastic resonance in composites restricts their thin-film integration in broadband. Here, we effectuate a concurrence of ferroelectric-like and antiferromagnetic phase transitions in Sr2IrO4/SrTiO3 superlattices by artificial design periodically non-equivalent interfaces, where a maximum magnetoelectric coef…
Strain-mediated magnetoelectric (ME) coupling in ferroelectric (FE) / ferromagnetic (FM) heterostructures offers a unique opportunity for both fundamental scientific research and low power multifunctional devices. Relaxor-ferroelectrics, like (1-x)Pb(Mg1/3Nb2/3)O3-(x)PbTiO3 (PMN-xPT), are ideal FE layer candidates due to their giant piezoelectricity. But thin films of PMN-PT suffer from substrate clamping which substantially reduces piezoelectric in-plane strains. Here we present the first demonstration of low voltage ME coupling in an all-thin-film heterostructure which utilizes the anisotrop…
We report magnetization measurements and magnetic resonance data for SrTiO3 doped by manganese. We show that the recently reported coexistent spin and dipole glass (multiglass) behaviours are strongly affected by the distribution of Mn ions between the Sr and Ti sites. Motivated by this finding we calculate the magnetic interactions between Mn impurities of different kinds. Both LSDA+U and many-body perturbation theory evidence that magnetic and magnetoelectric interactions are mediated by Mn$_B^{4+}$ ions substituting for Ti. We propose two microscopic magnetoelectric coupling mechanisms, whi…
Magnetoelectric (ME) materials are of fundamental interest and have been investigated for their broad potential for technological applications. The search for, and eventually the theoretical design of, materials with large ME couplings present challenging issues. First-principles methods have only recently been developed to calculate the full ME response tensor $α$ including both electronic and ionic (i.e., lattice-mediated) contributions. The latter is proportional to both the Born dynamical electric charge $Z^{\rm e}$ and its analogue, the dynamical magnetic charge $Z^{\rm m}$. Here we prese…
Magnetoelectric composites are an important class of multiferroic materials that pave the way towards a new generation of multifunctional devices directly integrable in data storage technology and spintronics. This study focuses on strain-mediated electrical manipulation of magnetization in an extrinsic multiferroic. The composite includes 5 nm or 60 nm Fe$_{81}$Ga$_{19}$ thin films coupled to a piezoelectric (011)-PMN-PZT. The magnetization reversal study reveals a converse magnetoelectric coefficient $α_\mathrm{CME,max} \approx 2.7 \times {10^{-6}}$ s.m$^{-1}$ at room temperature. This repor…
Magnetic skyrmions, vortex-like swirling spin textures characterized by a quantized topological invariant, realized in chiral-lattice magnets are currently attracting intense research interest. In particular, their dynamics under external fields is an issue of vital importance both for fundamental science and for technical application. Whereas observations of magnetic skyrmions had been limited to metallic magnets so far, their realization was discovered also in a chiral-lattice insulating magnet Cu2OSeO3 in 2012. Skyrmions in the insulator turned out to exhibit multiferroic nature with spin-i…
Magnetoelectric coupling permits a magnetic order parameter to be addressed electrically or vice versa, and could find use in data storage, field sensors and actuators. Coupling constants for single phase materials such as chromium dioxide, boracites and manganites are typically as low as 10^{-12} - 10^{-9} s/m, e.g. because the polarisations and magnetisations are small. Two phase multiferroics with strain mediated coupling, such as laminates, composites and epitaxial nanostructures, are more promising because each phase may be independently optimised. The resulting magnetoelectric switching …
The strain dependent functional properties of epitaxial transition metal oxide films can be significantly modified via substrate selection. However, large lattice mismatches preclude dislocation-free epitaxial growth on ferroelectric substrates, whose strain states are modified by applied electric fields. Here we overcome this mismatch problem by depositing an epitaxial film of ferromagnetic La0.7Sr0.3MnO3 on a single crystal substrate of well lattice matched SrTiO3 via a film of SrRuO3 that we subsequently dissolved, permitting the transfer of unstrained La0.7Sr0.3MnO3 to a ferroelectric subs…
Theoretical investigation demonstrates that the composite bilayer (i.e., chiral-magnetic/ferroelectric bilayer) offers the possibility of electric-induced magnetic Skyrmions [Phys. Rev. B \textbf{94}, 014311 (2016)]. In this Article, we propose a micromagnetic model to physically manipulate magnetic Bloch Skyrmions propagating in a chiral-magnetic thin film with a polarized ferroelectric essential to drive the system through the converse magnetoelectric effect. Effects caused by different velocities of the propagation, sizes of the thin film, and strength of the magnetoelectric couplings stron…
During the last fifteen years, multiferroic (MF) research communities have been searching for an alternative room temperature MF material with large magnetoelectric (ME) coupling for possible applications in high density electronic components, low heat dissipation memory and logic devices. We have studied Pb(Zr0.20Ti0.80)0.70Pd0.30O3-δ (PZTP30) system with an unusually large (30%) palladium occupancy in B site of PZT. This material exhibited a giant ME coupling coefficient ~0.36 mV/cm.Oe. Interestingly, this is the first time any room temperature single phase compound that showed ME trends, an…
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…
Ferromagnetic-ferroelectric nanocomposites are of interest for realizing strong strain mediated coupling between electric and magnetic subsystems due to high surface area-to-volume ratio. This report is on the synthesis of nickel ferrite (NFO) -barium titanate (BTO) core-shell nano-fibers, magnetic field assisted assembly into superstructures, and studies on magneto-electric (ME) interactions. Electrospinning techniques were used to prepare coaxial fibers of 0.5-1.5 micron in diameter. The core-shell structure of annealed fibers was confirmed by electron microscopy and scanning probe microscop…
The coupling between magnetic order and ferroelectricity has been under intense investigation in a wide range of transition-metal oxides. The strongest coupling is obtained in so-called magnetically-induced multiferroics where ferroelectricity arises directly from magnetic order that breaks inversion symmetry. However, it has been difficult to find non-oxide based materials in which these effects occur. Here we present a study of copper dimethyl sulfoxide dichloride (CDC), an organo-metallic quantum magnet containing $S = 1/2$ Cu spins, in which electric polarization arises from non-collinear …
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.
Structural and magnetic properties of the doped terbium manganites (Tb,A)MnO3 (A = Gd, Dy and Ho) have been investigated using first-principles calculations and further confirmed by subse- quent experimental studies. Both computational and experimental studies suggest that compared to the parent material, namely, TbMnO3 (with a magnetic moment of 9.7 /muB for Tb3+) Dy- and Ho- ion substituted TbMnO3 results in an increase in the magnetic moment (< 10.6/muB for Dy3+ and Ho3+). The observed spiral-spin AFM order in TbMnO3 is stable with respect to the dopant substitutions, which modify the Mn-O-…
We consider the anomalous thermoelectric transport in gapped single and bilayer graphene where the gap may be due to broken inversion symmetry. In the presence of the gap, non-trivial Berry phase effects can be shown to mediate a transverse thermoelectric voltage in response to an applied temperature gradient even in the absence of a perpendicular magnetic field. This spontaneous, anomalous Nernst effect is nonzero for non-uniform chemical potential in the two inequivalent valleys in the graphene band structure. Conversely, the Nernst response can be used to create a valley-index polarization …
Identifying intrinsic low-dimensional ferromagnets with high transition temperature and electrically tunable magnetism is crucial for the development of miniaturized spintronics and magnetoelectrics. Recently long-range 2D ferromagnetism was observed in van der Waals crystals CrI$_3$ and Cr$_2$Ge$_2$Te$_6$, however their Curie temperature is significantly lowered when reducing down to monolayer/few layers. Herein, using renormalized spin-wave theory and first-principles electronic structure theory, we present a theoretical study of electrically tunable 2D ferromagnetism in van der Waals layere…
We study the coexistence of strain- and charge-mediated magnetoelectric coupling in a cobalt (0-7 nm) wedge on ferroelectric [Pb(Mg$_{1/3}$/Nb$_{2/3}$)O$_{3}$]$_{0.68}$-[PbTiO$_{3}$]$_{0.32}$ (011) using surface-sensitive x-ray magnetic circular dichroism spectroscopy at the Co L$_{3,2}$ edges. Three distinct electric field driven remanent magnetization states can be set in the Co film at room temperature. Ab-initio density functional theory calculations unravel the relative contributions of both strain and charge to the observed magnetic anisotropy changes illustrating magnetoelectro-elastic …
Perpendicular exchange bias (EB), which combines the perpendicular magnetic anisotropy and the ferromagnetic (FM) - antiferromagnetic (AFM) exchange coupling, is extremely important in the high-density AFM spintronics. However, the effective modulation of EB remains challenging, since the alternant spins at the AFM/FM interface are strongly pinned by the AFM layer. Voltage tuning of EB through the magnetoelectric coupling provides a potential way to achieve a rapid magnetization switching in an energy-efficient manner. Nevertheless, the interfacial strain mediation of perpendicular EB induced …
We find the realization of large converse magnetoelectric (ME) effects at room temperature in a multiferroic hexaferrite Ba$_{0.52}$Sr$_{2.48}$Co$_{2}$Fe$_{24}$O$_{41}$ single crystal, in which rapid change of electric polarization in low magnetic fields (about 5 mT) is coined to a large ME susceptibility of 3200 ps/m. The modulation of magnetization then reaches up to 0.62 $μ$$_{B}$/f.u. in an electric field of 1.14 MV/m. We find further that four ME states induced by different ME poling exhibit unique, nonvolatile magnetization versus electric field curves, which can be approximately describ…
Ferroelasticity in Two-Dimensional Hybrid Ruddlesden$-$Popper Perovskites Mediated by Cross-Plane Intermolecular Coupling and Metastable Funnel-Like Phases
该研究结合第一性原理与元动力学，揭示单层八面体 (BA)$_2$PbI$_4$ 的铁弹性切换由跨平面耦合及亚稳漏斗状 PE 相调控，并阐明温度与 Br 混合对势垒和相浓度的影响。
We present a study of the control of electric field induced strain on the magnetic and electrical transport properties in a magneto-elastically coupled artificial multiferroic Fe3O4/BaTiO3 heterostructure. In this Fe3O4/BaTiO3 heterostructure, the Fe3O4 thin film is epitaxially grown in the form of bilateral domains, analogous to a-c stripe domains of the underlying BaTiO3(001) substrate. By in-situ electric field dependent magnetization measurements, we demonstrate the extrinsic control of the magnetic anisotropy and the characteristic Verwey metal-insulator transition of the epitaxial Fe3O4 …
Light-modulated exchange bias in multiferroic heterostructures
Universitat Autònoma de Barcelona（巴塞罗那自治大学）；Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST（加泰罗尼亚纳米科学和纳米技术研究所（ICN2，CSIC和BIST））；Univ. Brest, Laboratoire d’Optique et de Magnétisme (OPTIMAG)（布雷斯特大学，光学与磁性实验室（OPTIMAG））；Institució Catalana de Recerca i Estudis Avançats (ICREA)（加泰罗尼亚高级研究制度（ICREA））
