We employ neutron spherical polarimetry to determine the nature and population of the coexisting antiferromagnetic domains in multiferroic YMn2O5. By applying an electric field, we prove that reversing the electrical polarization results in the population inversion of two types of in-plane domains, related to each other by inversion. Our results are completely consistent with the exchange striction mechanism of ferroelectricity, and support a unified model where cycloidal ordering is induced by coupling to the main magnetic order parameter.
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
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.
Ferroelectric switching in BiFeO$_3$ multiferroic thin films with intrinsic ``stripe-like'' and ``bubble-like'' polydomain configurations was studied by piezoresponse force microscopy. Using the local electric field applied by a scanning probe microscope tip, we observe reversal of both out-of-plane and in-plane components of the polarization, with the final domain state depending on the tip sweeping direction. In ``bubble-like'' samples, complete control of the polarization is achieved, with in-plane polarization change mediated and stabilized by out-of-plane polarization reversal. In ``strip…
Cross-coupling of ordering parameters in multiferroic materials by multiple external stimuli other than electric field and magnetic field is highly desirable from both practical application and fundamental study points of view. Recently, mechanical force has attracted great attention in switching of ferroic ordering parameters via electro-elastic coupling in ferroelectric materials. In this work, mechanical force induced polarization and magnetization switching were investigated in a polycrystalline multiferroic Bi0.9La0.1FeO3 thin film using a scanning probe microscopy system. The piezorespon…
Electric manipulation of magnetic properties is a key problem of materials research. To fulfil the requirements of modern electronics, these processes must be shifted to high frequencies. In multiferroic materials this may be achieved by electric and magnetic control of their fundamental excitations. Here we identify magnetic vibrations in multiferroic iron-borates which are simultaneously sensitive to external electric and magnetic fields. Nearly 100% modulation of the terahertz radiation in an external field is demonstrated for SmFe3(BO3)4. High sensitivity can be explained by a modification…
By performing first-principles calculations, we systematically explore the effect of epitaxial strain on the structure and properties of multiferroic TbMnO3. We show that, although the unstrained bulk TbMnO3 displays a non-collinear antiferromagnetic spin order, TbMnO3 can be ferromagnetic under compressive strain, in agreement with the experimental results on TbMnO3 grown on SrTiO3. By increasing the tensile strain up to 5%, we predict that TbMnO3 transforms into a new multiferroic state with a large ferroelectric polarization,two orders of magnitude larger than that in the unstrained bulk, a…
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…
Unusual domains with curved walls and failure to satisfy the Landau-Lifshitz-Kittel Law are modeled as folding catastrophes (saddle-node bifurcations). This description of ballistic motion in a viscous medium is based upon early work by Dawber et al., Appl. Phys. Lett. 82, 436 (2003). It suggests that ferroelectric films can exhibit folds or vortex patterns but not both.
Highly controllable switching pathways in multiferroic GdMn$_2$O$_5$
Vienna University of Technology（维也纳工业大学）；Istituto Italiano di Tecnologia（意大利理工学院）；University of Science and Technology, Beijing（北京科技大学）；École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；Rutgers University（罗格斯大学）；University of Groningen（格罗宁根大学）
Tuning the lattice degree of freedom in nanoscale functional crystals is critical to exploit the emerging functionalities such as piezoelectricity, shape-memory effect, or piezomagnetism, which are attributed to the intrinsic lattice-polar or lattice-spin coupling. Here it is reported that a mechanical probe can be a dynamic tool to switch the ferroic orders at the nanoscale multiferroic phase boundaries in BiFeO 3 with a phase mixture, where the material can be reversibly transformed between the "soft" tetragonal-like and the "hard" rhombohedrallike structures. The microscopic origin of the n…
The control of the electron spin by external means is a key issue for spintronic devices. Using spin- and angle-resolved photoemission spectroscopy (SARPES) with three-dimensional spin detection, we demonstrate operando electrostatic spin manipulation in ferroelectric GeTe and multiferroic Ge1-xMnxTe. We not only demonstrate for the first time electrostatic spin manipulation in Rashba semiconductors due to ferroelectric polarization reversal, but are also able to follow the switching pathway in detail, and show a gain of the Rashba-splitting strength under external fields. In multiferroic Ge1-…
Deterministic polarization reversal in ferroelectric and multiferroic films is critical for their exploitation in nanoelectronic devices. While ferroelectricity has been studied for nearly a century, major discrepancies in the reported values of coercive fields and saturation polarization persist in literature for many materials. This raises questions about the atomic-scale mechanisms behind polarization reversal. Unconventional ferroelectric switching in $ε$-Fe2O3 films, a material that combines ferrimagnetism and ferroelectricity at room temperature, is reported here. High-resolution in-situ…
Cycloidal spin orders are common in multiferroics. One of the prototypical examples is BiFeO3 (BFO) which shows a large polarization and a cycloidal antiferromagnetic order at room temperature. Here we employ Landau theory and phase-field simulations to analyze the coupled switching dynamics of polarization and cycloidal antiferromagnetic orders in BFO. We are able to identify 14 types of transitional spin structures between two cycloids and 9 electric-field-induced spin switching paths. We demonstrate the electric-field-induced rotation of wave vectors of the cycloidal spins and discover 2 ty…
Spectrum of coupled spin, acoustic, electro-dipole and electromagnetic waves in orthorhombic perovskite multiferroics placed in external electric and magnetic field has been calculated. Frequency and field dependencies of electric, magnetic, and magnetoelectric susceptibilities of multiferroics with cycloidal antiferromagnetic structure in external electric and magnetic fields have been investigated as well. The spectrum of coupled waves has a band structure. Width and frequency ranges of bands depend on external fields. The possibility of control of electrodynamic properties of orthorhombic p…
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 show theoretically with an accurate spin Hamiltonian describing the multiferroic Mn perovskites that the application of the picosecond optical pulse with a terahertz frequency can switch the spin chirality through intensely exciting the electromagnons. There are four states with different spin chiralities, i.e. clockwise and counterclockwise ab/bc-plane spin spirals, and by tuning the strength, shape and length of the pulse, the switching among these states can be controlled at will. Dynamical pattern formation during the switching is also discussed.
Understanding the polarization switching mechanisms at play in ferroelectric materials is crucial for their exploitation in electronic devices. The conventional centrosymmetric reference structure-based mechanism which accounts for ferroelectricity in most of the usual displacive ferroelectric materials is too energy-demanding for some newly diagnosed ferroelectric materials such as the Ga2-xFexO3 (0.8 < x < 1.4) compounds. Some alternative theoretical propositions have been made and need experimental confirmation. A dual-scale electron microscopy study is performed on thin films of the Ga0.6F…
Using the theory of symmetry and the microscopic model we predicted the possibility of a linear roto-antiferromagnetic effect in the perovskites with structural antiferrodistortive and antiferromagnetic long-range ordering and found the necessary conditions of its occurrence. The main physical manifestations of this effect are the smearing of the antiferromagnetic transition and the jump of the specific heat near it. In the absence of external fields linear roto-antiferromagnetic coupling can induce a weak antiferromagnetic ordering above the Neel temperature, but below the temperature of anti…
We demonstrate that the magnetization of a ferromagnet in contact with an antiferromagnetic multiferroic (LuMnO3) can be speedily reversed by electric field pulsing, and the sign of the magnetic exchange bias can switch and recover isothermally. As LuMnO3 is not ferroelastic, our data conclusively show that this switching is not mediated by strain effects but is a unique electric-field driven decoupling of the ferroelectric and ferromagnetic domains walls. Their distinct dynamics are essential for the observed magnetic switching.
Rotating the magnetization of a magnetostrictive nanomagnet with electrically generated mechanical strain dissipates miniscule amount of energy compared to any other rotation method and would have been the ideal method to write bits in nonvolatile magnetic memory, except strain cannot ordinarily rotate the magnetization of magnet by more than 90 degrees and "flip" it. Here, we describe a scheme to achieve complete 180 degree rotation of the magnetization of a nanomagnet with strain that will enable writing of binary bits in non-volatile magnetic memory implemented with magneto-tunneling juncti…
First-principles density functional calculations show that the $\textrm{SrRuO}_{3}/\textrm{PbTiO}_{3}/\textrm{SrRuO}_{3}$ multiferroic junction with asymmetric (RuO$_{2}$/PbO and TiO$_{2}$/SrO) interfaces has a large ferroelectric depolarizing field, whose switching changes the interface transmission probabilities for tunneling electrons, leading to electroresistance modulation over several orders of magnitude. The switching further affects the interface spin density, naturally driving magnetoresistance as well as modulated spin-dependent in-plane resistivity, which may be exploited in field-e…
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…
The electric field effect on magnetism was examined in the multiferroic conical magnet Mn$_2$GeO$_4$, which shows a strong coupling between ferromagnetic and ferroelectric order parameters. The systematic evaluation of the electric polarization in the multiferroic phase below 5.5 K under various field cooling conditions reveals that small magnetic fields of 0.1 T significantly reduce the required electric fields needed to reach saturation. By applying electric fields during magnetic field dependent hysteresis measurements of magnetization M and polarization P an electrically controllable excha…
We report a study of magnetic dynamics in multiferroic hexagonal manganite HoMnO3 by far-infrared spectroscopy. Low-temperature magnetic excitation spectrum of HoMnO3 consists of magnetic-dipole transitions of Ho ions within the crystal-field split J=8 manifold and of the triangular antiferromagnetic resonance of Mn ions. We determine the effective spin Hamiltonian for the Ho ion ground state. The magnetic-field splitting of the Mn antiferromagnetic resonance allows us to measure the magnetic exchange coupling between the rare-earth and Mn ions.
The time dependence of switching multiferroic domains in MnWO$_4$ has been studied by time-resolved polarized neutron diffraction. Inverting an external electric field inverts the chiral magnetic component within rise times ranging between a few and some tens of milliseconds in perfect agreement with macroscopic techniques. There is no evidence for any faster process in the inversion of the chiral magnetic structure. The time dependence is well described by a temperature-dependent rise time suggesting a well-defined process of domain reversion. As expected, the rise times decrease when heating…
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…
Displacive martensitic phase transition is potentially promising in semiconductor based data storage applications with fast switching speed. In addition to traditional phase transition materials, the recently discovered two-dimensional ferroic materials are receiving lots of attention owing to their fast ferroic switching dynamics, which could tremendously boost data storage density and enhance read/write speed. In this study, we propose that a terahertz laser with an intermediate intensity and selected frequency can trigger ferroic order switching in two-dimensional multiferroics, which is a …
The magneto-electrocaloric effect which can be defined as the coupling between magnetocaloric and electrocaloric effects attracts currently considerable attention due to the advantages provided by the caloric effect in designing solid-state refrigeration technologies. The magneto-electrocaloric effect of a multiferroic antiferromagnetic spin system with the Dzyaloshinskii Moriya (DM) interaction is investigated in this paper. The DM interaction is assimilated to a coupling between an external site-dependent electric field and a local electric polarization. The external magnetic is also conside…
In elastically coupled multiferroic heterostructures that exhibit full domain correlations between ferroelectric and ferromagnetic sub-systems, magnetic domain walls are firmly pinned on top of ferroelectric domain boundaries. In this work we investigate the influence of pinned magnetic domain walls on the magnetization reversal process in a Co40Fe40B20 wedge film that is coupled to a ferroelectric BaTiO3 substrate via interface strain transfer. We show that the magnetic field direction can be used to select between two distinct magnetization reversal mechanisms, namely (1) double switching ev…
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.
In the last few years, some ideas of electric manipulations in ferromagnetic heterostructures have been proposed for developing next generation spintronic devices. Among them, the magnetization switching driven by spin-orbit torque (SOT) is being intensely pursued. Especially, how to control the switching current density, which is expected to enrich device functionalities, has aroused much interest among researchers all over the world. In this paper, a novel method to adjust the switching current is proposed, and the BiFeO3 (BFO) based heterostructures with opposite spontaneous polarizations f…
Magnetoelectric coupling in the polycrystalline antiferromagnets CuFe0.95Rh0.05O2 and CuFeO2 has been investigated. For both samples, electric polarization was observed in the absence of an applied external magnetic field demonstrating that for multiferroic research ceramics are worth to be studied. The observed magnetodielectric effect for CuFe0.95Rh0.05O2 in the electrically polar phase supports the existence of a noncollinear antiferromagnetic state. Interestingly, the electric polarization of this sample can be suppressed by a magnetic field. The temperature dependence of the relative magn…
A complex magnetic order of the multiferroic compound Co3TeO6 has been revealed by neutron powder diffraction studies on ceramics and crushed single crystals. The compound adopts a monoclinic structure (s.g. C2/c) in the studied temperature range 2 K - 300 K but exhibits successive antiferromagnetic transitions at low temperature. Incommensurate antiferromagnetic order with the propagation vector k1 = (0, 0.485, 0.055) sets in at 26 K. A transition to a second antiferromagnetic structure with k2 = (0, 0, 0) takes place at 21.1 K. Moreover, a transition to a commensurate antiferromagnetic struc…
We report a comprehensive study of ultrafast carrier dynamics in single crystals of multiferroic BiFeO$_{3}$. Using femtosecond optical pump-probe spectroscopy, we find that the photoexcited electrons relax to the conduction band minimum through electron-phonon coupling with a $\sim$1 picosecond time constant that does not significantly change across the antiferromagnetic transition. Photoexcited electrons subsequently leave the conduction band and primarily decay via radiative recombination, which is supported by photoluminescence measurements. We find that despite the coexisting ferroelectri…
Macroscopic properties of multiferroics, the systems that show simultaneously two types of ordering, could be controlled by the external fields of different nature. We analyze the behavior of multiferroics with antiferro-(AFM) and ferromagnetic (FM) ordering under the action of external magnetic and stress fields. A combination of these two fields makes it possible to achieve macroscopic states with different domain structures. The two-domain state obtained in this way shows a linear dependence of macroscopic strain vs magnetic field which is unusual for AFMs. A small but nonzero stress applie…
We present a 57Fe Mössbauer spectroscopy study of the two incommensurate magnetic phases in the multiferroic material FeVO4. We devise lineshapes appropriate for planar elliptical and collinear modulated magnetic structures and show that they reproduce very well the Mössbauer spectra in FeVO4, in full qualitative agreement with a previous neutron diffraction study. Quantitatively, our spectra provide precise determinations of the characteristics of the elliptical and modulated structures which are in good agreement with the neutron diffraction results. We find that the hyperfine field elliptic…
Over the years attempts have been made to compensate for the inherent weaknesses in the bulk state of the multiferroic BiFeO3, such as high leakage current and the absence of ferromagnetic correlation, and exploit its magnetoelectric potential by forming solid solutions with other perovskites. Studies in the recent few years have shown that alloying of BiFeO3 with BaTiO3, both with and without additives, can induce both ferroelectric and ferromagnetic switching. While the coexistence of both the ferroic orders is encouraging from the view point of technological applications, the origin of ferr…
Electrical manipulation of skyrmions attracts considerable attention for its rich physics and promising applications. To date, such a manipulation is realized mainly via spin-polarized current based on spin-transfer torque or spin-orbital torque effect. However, this scheme is energy-consuming and may produce massive Joule heating. To reduce energy dissipation and risk of heightened temperatures of skyrmion-based devices, an effective solution is to use electric field instead of current as stimulus. Here, we realize an electric-field manipulation of skyrmions in a nanostructured ferromagnetic/…
Multiferroic materials open up the possibility to design novel functionality in electronic devices, with low energy consumption. However, there are very few materials that show multiferroicity at room temperature, which is essential to be practically useful. AlxFe2-xO3 (x-AFO) thin films, belonging to the k-Al2O3 family are interesting because they show room temperature ferrimagnetism and have a polar crystal structure. However, it is difficult to realise its ferroelectric properties at room temperature, due to low resistivity of the films. In this work, we have deposited x-AFO (0.5 <= x <= 1)…
Chirality, i.e., the right- and left-handedness of structure, is one of the key concepts in many fields of science including biology, chemistry and physics, and its manipulation is an issue of vital importance. The electron spins in solids can form chiral configurations. In perovskite manganites RMnO3 (R=Tb, Dy,...etc), the Mn-spins form a cycloidal structure, which induces ferroelectric polarization (P) through the relativistic spin-orbit interaction. This magnetism-induced ferroelectricity (multiferroics) and associated infrared-active spin waves (electromagnons) open a promising route to co…
Multiferroicity can be induced in strontium titanate by applying biaxial strain, resulting in the coexistence of both ferroelectric and antiferrodistortive domains. The magnitude and sign of the strain imposed on the lattice by design can be used to tune the phase transitions and interactions between these two phenomena. Using optical second harmonic generation, we report a transition from centrosymmetric 4/mmm phase to ferroelectric mm2, followed by an antiferrodistortive transition to a coupled ferroelastic-ferroelectric mm2 phase in a strontium titanate thin film strained in biaxial tension…
