Antiferromagnetic nanoscale bit arrays of magnetoelectric Cr$_2$O$_3$ thin films
Peter Rickhaus, Oleksandr V. Pylypovskyi, Gediminas Seniutinas, Vicent Borras, Paul Lehmann, Kai Wagner, Liza Žaper, Paulina J. Prusik, Pavlo Makushko, Igor Ver… 展开作者
Peter Rickhaus, Oleksandr V. Pylypovskyi, Gediminas Seniutinas, Vicent Borras, Paul Lehmann, Kai Wagner, Liza Žaper, Paulina J. Prusik, Pavlo Makushko, Igor Veremchuk, Tobias Kosub, René Hübner, Denis D. Sheka, Patrick Maletinsky, Denys Makarov
Magnetism of oxide antiferromagnets (AFMs) has been studied in single crystals and extended thin films. The properties of AFM nanostructures still remain underexplored. Here, we report on the fabrication and magnetic imaging of granular 100-nm-thick magnetoelectric Cr$_2$O$_3$ films patterned in circular bits with diameters ranging from 500 down to 100 nm. With the change of the lateral size, the domain structure evolves from a multidomain state for larger bits to a single domain state for the smallest bits. Based on spin-lattice simulations, we show that the physics of the domain pattern formation in granular AFM bits is primarily determined by the energy dissipation upon cooling, which results in motion and expelling of AFM domain walls of the bit. Our results provide a way towards the fabrication of single domain AFM-bit-patterned memory devices and the exploration of the interplay between AFM nanostructures and their geometric shape.
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…
Intrinsic magnetic topological insulator ${\mathrm{MnBi}}_{2}{\mathrm{Te}}_{4}$ is believed to be an axion insulator in its antiferromagnetic ground state. However, direct identification of axion insulators remains experimentally elusive because the observed vanishing Hall resistance, while indicating the onset of the axion field, is inadequate to distinguish the system from a trivial normal insulator. Using numerical Green's functions, we theoretically demonstrate the quantized magnetoelectric current in a tunnel junction of atomically thin ${\mathrm{MnBi}}_{2}{\mathrm{Te}}_{4}$ sandwiched be…
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…
We report the discovery of linear magnetoelectric effect in the well-known green phase compound, Sm2BaCuO5, which crystallizes in the centrosymmetric orthorhombic (Pnma) structure. Magnetization and specific heat measurements reveal the long-range antiferromagnetic ordering of Cu2+ and Sm3+-ions moments at TN1 = 23 K and TN2 = 5 K, respectively. Applied magnetic field induces dielectric anomaly at TN1 whose magnitude increases with field, which results in significant (1.7%) magnetocapacitance effect. On the other hand, the dielectric anomaly observed in zero-applied magnetic field at TN2 shows…
We report the results of direct measurement of remanent hysteresis loops on nanochains of BiFeO$_3$ at room temperature under zero and $\sim$20 kOe magnetic field. We noticed a suppression of remanent polarization by nearly $\sim$40\% under the magnetic field. The powder neutron diffraction data reveal significant ion displacements under a magnetic field which seems to be the origin of the suppression of polarization. The isolated nanoparticles, comprising the chains, exhibit evolution of ferroelectric domains under dc electric field and complete 180$^o$ switching in switching-spectroscopy pie…
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
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）
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…
Imaging antiferromagnetic domains in LiCoPO$_4$ via the optical magnetoelectric effect
Budapest University of Technology and Economics（布达佩斯技术与经济大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所新兴物质科学中心）；Leibniz IFW Dresden（莱布尼茨德累斯顿固体研究所）；University of Tokyo（东京大学）；Tokyo College, University of Tokyo（东京大学东京学院）；HUN-REN–BME Condensed Matter Physics Research Group, Budapest University of Technology and Economics（匈牙利研究与教育网络-布达佩斯技术与经济大学凝聚态物理研究组）；University of Augsburg（奥格斯堡大学）
In the present study, we investigated magnetodielectric, magnetoelectric (ME), and angular-dependent polarization in single-crystal Fe4Nb2O9. The magnetodielectric effects in epsilon(x) (x//[100]), epsilon(y) (y//[120]), and epsilon(z) (z//[001]) are found to be significant only around T-N approximate to 95 K when magnetic fields are applied along three orthogonal x-, y- (y//[120]), and z directions. The finite polarization P-x, P-y, and P-z of 70, 100, and 30 mu C/m(2), respectively, can be induced in the antiferromagnetic phase when a finite magnetic field up to 9 T is applied along the thre…
The space and time symmetry breaking at magnetic phase transitions in multiferroics results in a number of strongly pronounced optical effects. Our high-resolution spectroscopic study of 3d- excitons in a complex multi-sublattice magnetoelectric CuB2O4 demonstrates that, among those, a large antiferromagnetic linear dichroism is observed which is highly sublattice-sensitive to subtle changes in the spin subsystems. We prove that the discovered linear dichroism is related microscopically to the magnetic Davydov splitting of the exciton states. We announce a novel magnetic phase transition and a…
Thermomechanical cycles with a ferroelectric working substance convert heat to electrical energy. As shown here, magnetoelectrically coupled ferroelectric/ferromangtic composites (also called multiferroics) add new functionalities and allow for an efficient thermal energy harvesting at room temperature by exploiting the pyroelectric effect. By virtue of the magnetoelectric coupling, external electric and magnetic fields can steer the operation of these heat engines. Our theoretical predictions are based on a combination of Landau-Khalatnikov-Tani approach (with a Ginzburg-Landau-Devonshire pot…
All-optical control of antiferromagnetic domains via an inverse optical magnetoelectric effect
RIKEN Center for Emergent Matter Science (CEMS)（RIKEN 新兴物质科学中心）；Institut für Festkörperforschung（固体研究所）；Department of Advanced Materials Science, The University of Tokyo（东京大学先进材料科学系）；Center for Electronic Correlations and Magnetism, University of Augsburg（奥格斯堡大学电子关联与磁性中心）；Tokyo College and department of Applied Physics, The University of Tokyo（东京大学东京学院与应用物理系）
The antiferromagnetic domain structure of a multiferroic has been investigated in the presence of a ferroelectric domain structure. It has been demonstrated that an inhomogeneous magnetoelectric (flexomagnetoelectric) interaction leads to pinning of antiferromagnetic domain walls at the walls of the ferroelectric domains and to a change in the structure of antiferromagnetic domain walls.
Magnetoelectric, dielectric and magnetic susceptibility tensors of multiferroic TbMnO3 with cycloidal antiferromagnetic structure in external electric and magnetic fields have been investigated with taking into account dynamics of spin, electro-dipole and acoustic subsystems. All components of tensors depend on values of external electric and magnetic fields. The possibility of control of electrodynamic properties of multiferroic TbMnO3 with cycloidal antiferromagnetic structure by external electric and magnetic fields has been shown. The resonant interaction of spin, electro-dipole, electroma…
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…
Symmetry arguments are used to show that a boundary of a magnetoelectric antiferromagnet has an equilibrium magnetization. This magnetization is coupled to the bulk antiferromagnetic order parameter and can be switched along with it by a combination of E and B fields. As a result, the antiferromagnetic domain state of a magnetoelectric can be used as a non-volatile switchable state variable in nanoelectronic device applications. Mechanisms affecting the boundary magnetization and its temperature dependence are classified. The boundary magnetization can be especially large if the boundary break…
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…
We study theoretically a three-dimensional correlated and spin-orbit coupled system, the half-filled extended Fu-Kane-Mele-Hubbard model on a diamond lattice, focusing on the topological magnetoelectric response of the antiferromagnetic insulator phase. In the antiferromagnetic insulator phase, the Dirac-like low-energy effective Hamiltonian is obtained. Then the theta term, which results in the magnetoelectric response, is derived as a consequence of the chiral anomaly. The realization of the dynamical axion field in our model is discussed. The relation with a symmetry broken phase induced by…
Antiferromagnetic and magnetoelectric Cr2O3-surfaces strongly affect the electronic properties in half metallic CrO2. We show the presence of a Cr2O3 surface layer on CrO3 grains by high-resolution transmission electron microscopy. The effect of these surface layers is demonstrated by measurements of the temperature variation of the magnetoelectric susceptibility. A major observation is a sign change at about 100 K followed by a monotonic rise as a function of temperature. These electric field induced moments in CrO3 are correlated with the magnetoelectric susceptibility of pure Cr2O3. This st…
Twisting in bilayers introduces structural chirality with two enantiomers, i.e., left- and right-hand bilayers, depending on the oriented twist angle. The interplay between this global chirality and additional degrees of freedom, such as magnetic ordering and the local octahedral chirality arising from the geometry of the bonds, can yield striking phenomena. In this work, we focus on collinear antiferromagnetic CrI$_3$ twisted homo-bilayers, which are characterized by a staggered octahedral chirality in each monolayer. Using symmetry analysis, density functional theory and tight-binding model …
In the first part of this work we calculate the high frequency magnetoelectric susceptibility of a simultaneously ferroelectric and canted antiferromagnetic (also know as weak ferromagnetic) thin film with magnetostrictive magnetoelectric coupling. We show that a dynamic coupling exists between the ferroelectric and optic antiferromagnetic excitations. In the second part of the paper, we calculate using an effective medium method the susceptibility of a heterostructure comprising alternating thin films of such a material together with a ferromagnet. Dipolar magnetic fields serve to couple the …
We show that misfit strain originated from the film-substrate lattice mismatch strongly increases the value of the quadratic magnetoelectric coupling. The giant magnetoelectric coupling, size effects and misfit strain cause strong changes of ferroic films phase diagrams at zero external magnetic and electric fields, in particular, the transformation of antiferromagnetic phase into ferromagnetic or ferrimagnetic ones for compressive or tensile misfit strains correspondingly as well as thickness induced paramagnetic or/and paraelectric phases appearance. Ferromagnetism appearance and magnetoelec…
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…
Antiferromagnets (AFMs) are presently considered as promising materials for applications in spintronics and random access memories due to the robustness of information stored in AFM state against perturbing magnetic fields (P. Wadley et al., Science 351, 587 (2016)). In this respect, AFM multiferroics maybe attractive alternatives for conventional AFMs as the coupling of magnetism with ferroelectricity (magnetoelectric effect) offers an elegant possibility of electric field control and switching of AFM domains. Here we report the results of comprehensive experimental and theoretical investigat…
Antiferromagnets offer remarkable promise for future spintronics devices, where antiferromagnetic order is exploited to encode information. The control and understanding of antiferromagnetic domain walls (DWs) - the interfaces between domains with differing order parameter orientations - is a key ingredient for advancing such antiferromagnetic spintronics technologies. However, studies of the intrinsic mechanics of individual antiferromagnetic DWs remain elusive since they require sufficiently pure materials and suitable experimental approaches to address DWs on the nanoscale. Here we nucleate…
Using heterostructures that combine a large-polarization ferroelectric (BiFeO3) and a high-temperature superconductor (YBa2Cu3O7-δ), we demonstrate the modulation of the superconducting condensate at the nanoscale via ferroelectric field effects. Through this mechanism, a nanoscale pattern of normal regions that mimics the ferroelectric domain structure can be created in the superconductor. This yields an energy landscape for magnetic flux quanta and, in turn, couples the local ferroelectric polarization to the local magnetic induction. We show that this form of magnetoelectric coupling, toget…
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.
We use symmetry analysis to show that the G, C and A-type antiferromagnetic Pnma perovskites can exhibit magnetoelectric (ME) responses when a ferroelectric instability is induced with epitaxial strain. Using first-principles calculations we compute the values of the allowed ME response in strained CaMnO3 as a model system. Our results show that large linear and non-linear ME responses are present and can diverge when close to the ferroelectric phase transition. By decomposing the electronic and ionic contributions, we explore the detailed mechanism of the ME response.
We have recently reported that the Haldane spin-chain system, Er2BaNiO5, undergoing antiferromagnetic order below 32 K, is characterized by the onset of ferroelectricity near 60K due to magnetoelectric coupling induced by short-range magnetic-order within spin-chains. We have carried out additional magnetic and dielectric studies to understand the properties well below antiferromagnetic ordering temperature. We emphasize here on the following: (i) A strong frequency dependent behaviors of ac magnetic susceptibility and complex dielectric properties have been observed at much lower temperatures…
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…
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 dynamical axion field is a new state of quantum matter where the magnetoelectric response couples strongly to its low-energy magnetic fluctuations. It is fundamentally different from an axion insulator with a static quantized magnetoelectric response. The dynamical axion field exhibits many exotic phenomena such as axionic polariton and axion instability. However, these effects have not been experimentally confirmed due to the lack of proper topological magnetic materials. Here by combining analytic models and first-principles calculations, we predict a series of van der Waal layered Mn$_2…
We report direct imaging of boundary magnetization associated with antiferromagnetic domains in magnetoelectric epitaxial Cr2O3 thin films using diamond nitrogen vacancy microscopy. We found a correlation between magnetic domain size and structural grain size which we associate with the domain formation process. We performed field cooling, i.e., cooling from above to below the Néel temperature in the presence of magnetic field, which resulted in the selection of one of the two otherwise degenerate 180 degree domains. Lifting of such a degeneracy is achievable with a magnetic field alone due to…
We report a comprehensive muon spin rotation ($μ$SR) study of the prototypical magnetoelectric antiferromagnet Cr$_2$O$_3$. We find the positively charged muon ($μ^+$) occupies several distinct interstitial sites, and displays a rich dynamic behavior involving local hopping, thermally activated site transitions and the formation of a charge-neutral complex composed of a muon and an electron polaron. The discovery of such a complex has implications for the interpretation of $μ$SR spectra in a wide range of magnetic oxides, and opens a route to study the dopant characteristics of interstitial hy…
Single-crystal growth and magnetic, magnetoelectric, and optical properties of ferroaxial-type SrMn$_2$Ni$_6$Te$_3$O$_{18}$
Osaka Metropolitan University（大阪公立大学）；The University of Tokyo（东京大学）；Kyoto University（京都大学）；High Energy Accelerator Research Organization（高能加速器研究机构）；The University of Osaka（大阪大学）
The correlation between antiferromagnetic and ferroelectric domain structures in multiferroics has been studied. The role of magnetoelectric interactions in a formation of antiferromagnetic domain structure has been analysed. It has been shown the major physical mechanism binding antiferromagnetic domains to ferroelectrics ones is inhomogeneous flexomagnetoelectric interaction of the Pz((lgrad)lz-lz(divl)) type. The dependences illustrating rearrangement of antiferromagnetic domain pattern together with change of ferroelectric domains thickness has been performed.
The polar magnet CaBaCo$_{4}$O$_{7}$ is known to exhibit the largest magnetic-field-driven electric polarization change ($ΔP$) associated with an antiferromagnetic (AFM)-ferrimagnetic (FIM) transition in a narrow temperature range between 62 and 69 K. In this work, we investigate the effect of Ni doping on its multiferroic properties, by means of magnetization, electric polarization, dielectric constant, and magnetostriction measurements on single crystals of CaBaCo$_{3.9}$Ni$_{0.1}$O$_{7}$ up to 50 T. In the doped material, two kinds of AFM phases appear below 78 K, accompanying negative $ΔP$…
Cr$_2$O$_3$ is the archetypal magnetoelectric (ME) material, which has a linear coupling between electric and magnetic polarizations. Quadratic ME effects are forbidden for the magnetic point group of Cr$_2$O$_3$, due to space-time inversion symmetry. In Cr$_2$O$_3$ films grown by sputtering, we find a signature of a quadratic ME effect that is not found in bulk single crystals. We use Raman spectroscopy and magetization measurements to deduce the removal of space-time symmetry, and corroborate the emergence of the quadratic ME effect. We propose that meta-stable site-selective trace dopants r…
Sign-resolved nanoscale readout and control of hidden antiferromagnetic spin order
University of Regensburg（雷根斯堡大学）；Physikalisch-Technische Bundesanstalt（德国联邦物理技术研究院）；RWTH Aachen University（亚琛工业大学）；Charles University（查理大学）；University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校）；Czech Academy of Sciences（捷克科学院）；Bundesanstalt für Materialforschung und -prüfung (BAM)（德国联邦材料研究与测试研究所）
Magnetic solitons offer functionalities as information carriers in multiple spintronic and magnonic applications. However, their potential for nanoscale energy transport has not been revealed. Here we demonstrate that antiferromagnetic solitons, e.g. domain walls, can uptake, transport and release energy. The key for this functionality resides in their relativistic kinematics; their self-energy increases with velocity due to Lorentz contraction of the soliton and their dynamics can be accelerated up to the effective speed of light of the magnetic medium. Furthermore, their classification in ro…
We report the epitaxial growth of BiFeO3 by pulsed electron deposition and the resulting crystal quality, magnetic and nanoscale switching properties. X-ray diffraction shows high quality single phase, epitaxial (001) oriented films grown on SrTiO3 (001) substrates. Both field and temperature dependent magnetic properties reveal an antiferromagnetic behavior of the films. For the film with a SrRuO3 bottom electrode, an exchange-enhancement effect between antiferromagnetic BiFeO3 and ferromagnetic SrRuO3 was observed at low temperature. The piezoelectric force microscopy and switching spectrosc…
