An investigation of the spatially resolved distribution of domains in the multiferroic phase of MnWO$_4$ reveals that characteristic features of magnetic and ferroelectric domains are inseparably entangled. Consequently, the concept of "multiferroic hybrid domains" is introduced for compounds in which ferroelectricity is induced by magnetic order. The three-dimensional structure of the domains is resolved. Annealing cycles reveal a topological memory effect that goes beyond previously reported memory effects and allows one to reconstruct the entire multiferroic multidomain structure subsequent to quenching it.
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…
We report the discovery of a complete suppression of ferroelectricity in $MnWO_4$ by 10 % iron substitution and its restoration in external magnetic fields. The spontaneous polarization in $Mn_{0.9}Fe_{0.1}WO_4$ arises below 12 K in external fields above 4 T. The magnetic/ferroelectric phase diagram is constructed from the anomalies of the dielectric constant, polarization, magnetization, and heat capacity. The observations are qualitatively described by a mean field model with competing interactions and strong anisotropy. We propose that the magnetic field induces a non-collinear inversion sy…
High resolution inelastic neutron scattering reveals that the elementary magnetic excitations in multiferroic MnWO4 consist of low energy dispersive electromagnons in addition to the well-known spin-wave excitations. The latter can well be modeled by a Heisenberg Hamiltonian with magnetic exchange coupling extending to the 12th nearest neighbor. They exhibit a spin-wave gap of 0.61(1) meV. Two electromagnon branches appear at lower energies of 0.07(1) meV and 0.45(1) meV at the zone center. They reflect the dynamic magnetoelectric coupling and persist in both, the collinear magnetic and parael…
The spin-wave excitations of the multiferroic $\rm MnWO_4$ have been measured in its low-temperature collinear commensurate phase using high-resolution inelastic neutron scattering. These excitations can be well described by a Heisenberg model with competing long-range exchange interactions and a single-ion anisotropy term. The magnetic interactions are strongly frustrated within the zigzag spin chain along c axis and between chains along the a axis, while the coupling between spin along the b axis is much weaker. The balance of these interactions results in the noncollinear incommensurate spi…
The electric-field dependence of the magnetic structure of multiferroic MnWO4 has been investigated using spherical neutron polarimetry as a function of temperature. The application of an electric field drives the magnetic structure to a single chiral domain. The magnitude of the field required to do this is shown to increase with temperature. The link between the magnetic order and electric polarization is further demonstrated.
Different methods of texturing polycrystalline materials are developed over years to use/probe anisotropic material properties with relative ease, where complicated and expensive single crystal growth processes could be avoided. In this paper, particle morphology assisted texturing in multiferroic MnWO$_4$ has been discussed. Detailed powder x-ray diffraction vis-a-vis scanning electron microscopic studies on differently annealed and processed samples have been employed to probe the giant texturing effect in powdered MnWO$_4$. A quantitative measure of the texturing has been carried out by mea…
Dielectric, magnetic and lattice dynamics properties of double perovskite (Ca0.5Mn1.5)MnWO6
Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Faculty of Nuclear Sciences and Physical Engineering, Czech Technical University in Prague（布拉格捷克技术大学核科学与物理工程学院）；Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS)（国家材料科学研究所材料纳米构造研究中心）；Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院凝聚态物理系）
Tungstates $A$WO$_4$ with the wolframite structure characterized by the $A$O$_6$ octahedral zigzag chains along the $c$-axis, can be magnetic if $A$=Mn, Fe, Co, Cu, Ni. Among them, MnWO$_4$ is a unique member with a cycloid Mn$^{2+}$ spin order developed at low temperature, leading to an interesting type-II multiferroic behavior. However, so far no other multiferroic material in the tungstate family has been found. In this work, we present the synthesis and the systematic study of the double tungstate LiFe(WO$_4$)$_2$. Experimental characterizations including structural, thermodynamic, magneti…
We report the remarkably robust ferroelectric state in the multiferroic compound Mn$_{1-x}$Zn$_x$WO$_4$. The substitution of the magnetic Mn$^{2+}$ with nonmagnetic Zn$^{2+}$ reduces the magnetic exchange and provides control of the various magnetic and multiferroic states of MnWO$_4$. Only 5 % of Zn substitution results in a complete suppression of the frustrated collinear (paraelectric) low temperature phase. The helical magnetic and ferroelectric phase develops as the ground state. The multiferroic state is stable up to a high level of substitution of more than 50 %. The magnetic, thermodyn…
We propose a microscopic theory for magnetic switching of electric polarization (P) in the spin-spiral multiferroics by taking TbMnO3 and DyMnO3 as examples. We reproduce their phase diagrams under a magnetic field H_ex by Monte-Carlo simulation of an accurate spin model and reveal that competition among the Dzyaloshinskii-Moriya interaction, spin anisotropy, and spin exchange is controlled by the applied H_ex, resulting in magnetic transitions accompanied by reorientation or vanishing of P. We also discuss the relevance of the proposed mechanisms to many other multiferroics such as LiCu2O2, M…
The complete magnetic and multiferroic phase diagram of Mn$_{1-x}$Co$_{x}$WO$_4$ single crystals is investigated by means of magnetic, heat capacity, and polarization experiments. We show that the ferroelectric polarization $\overrightarrow{P}$ in the multiferroic state abruptly changes its direction twice upon increasing Co content, x. At x$_{c1}$=0.075, $\overrightarrow{P}$ rotates from the $b-$axis into the $a-c$ plane and at x$_{c2}$=0.15 it flips back to the $b-$axis. The origin of the multiple polarization flops is identified as an effect of the Co anisotropy on the orientation and shape…
We present a comprehensive single crystal neutron diffraction investigation of the $\rm Mn_{1-x}Co_{x}WO_4$ with $0.02\leq x \leq0.30$. At lower concentration $x \leq 0.05$, the system is quickly driven into the multiferroic phase with spin structure forming an elliptical spiral order similar to the parent compound. The reduction of electric polarization is ascribed to the tilting of the spiral plane. For $x\sim 0.075$, the magnetic structure undergoes a spin flop transition that is characterized by a sudden rotation of the spin helix envelope into the $ac$ plane. This spin structure persists …
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-…
The interplay between electronic eigenstates, spin, and orbital degrees of freedom, combined with fundamental breaking of symmetries is currently one of the most exciting fields of research. Multiferroics such as (GeMn)Te fulfill these requirements providing unusual physical properties due to the coexistence and coupling between ferromagnetic and ferroelectric order in one and the same system. Here we show that multiferroic (GeMn)Te inherits from its parent ferroelectric α-GeTe compound a giant Rashba splitting of three-dimensional bulk states which competes with the Zeeman spin splitting indu…
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…
By applying Berry-phase theory for the effective half-filled Hubbard model, we derive an analytical expression for the electronic polarization driven by the relativistic spin-orbit (SO) coupling. The model itself is constructed in the Wannier basis, using the input from the first-principles electronic structure calculations in the local-density approximation, and then treated in the spirit of the superexchange theory. The obtained polarization has the following form: ${\bf P}_{ij} = \boldsymbolε_{ji} \boldsymbol{\cal P}_{ij} \cdot [\boldsymbol{e}_i \times \boldsymbol{e}_j]$, where $\boldsymbol…
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…
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/…
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…
The electric-field control of $d$-electron magnetism in multiferroic transition metal oxides is attracting widespread interest for the underlying fundamental physics and for next generation spintronic devices. Here, we report an extensive study of the $3d$ magnetism in magnetoelectric Ga$_{0.6}$Fe$_{1.4}$O$_3$ (GFO) epitaxial films by polarization dependent x-ray absorption spectroscopy. We found a non-zero integral of the x-ray magnetic circular dichroism, with a sign depending upon the relative orientation between the external magnetic field and the crystallographic axes. %By reliably enlarg…
Realizing effective manipulation and explicit identification of topological spin textures are two crucial ingredients to make them as information carrier in spintronic devices with high storage density, high data handling speed and low energy consumption. Electric-field manipulation of magnetism has been achieved as a dissipationless method compared with traditional regulations. However, the magnetization is normally insensitive to the electric field since it does not break time-reversal symmetry directly, and distribution of topological magnetic quasiparticles is difficult to maintain due to …
A rapidly developing field of spintronics is based on the premise that substituting charge with spin as a carrier of information can lead to new devices with lower power consumption, non-volatility and high operational speed. Despite efficient magnetization detection, magnetization manipulation is primarily performed by current-generated local magnetic fields and is very inefficient. Here we report a novel non-volatile hybrid multiferroic memory cell with electrostatic control of magnetization based on strain-coupled GaMnAs ferromagnetic semiconductor and a piezoelectric material. We use the c…
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…
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…
Germanium telluride features special spin-electric effects originating from spin-orbit coupling and symmetry breaking by the ferroelectric lattice polarization, which opens up many prospectives for electrically tunable and switchable spin electronic devices. By Mn doping of the α-GeTe host lattice, the system becomes a multiferroic semiconductor possessing magnetoelectric properties in which the electric polarization, magnetization and spin texture are coupled to each other. Employing spin- and angle-resolved photoemission spectroscopy in bulk- and surface-sensitive energy ranges and by varyin…
Laser-Induced Rashba Spin-Orbit Torques in Multiferroic Semiconductor (Ge,Mn)Te
Charles University（查理大学）；Institute of Physics ASCR, v.v.i.（捷克科学院物理研究所）；Johannes Kepler Universität（约翰内斯·开普勒大学）；École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；Paul Scherrer Institut（保罗谢尔研究所）
Two-dimensional (2D) van der Waals ferroelectrics provide an unprecedented architectural freedom for the creation of artificial multiferroics and non-volatile electronic devices based on vertical and co-planar heterojunctions of 2D ferroic materials. Nevertheless, controlled microscopic manipulation of ferroelectric domains is still rare in monolayer-thick 2D ferroelectrics with in-plane polarization. Here we report the discovery of robust ferroelectricity with a critical temperature close to 400 K in SnSe monolayer plates grown on graphene, and the demonstration of controlled room temperature…
The coupling between antiferrodistortion (AFD) and ferroelectric (FE) polarization, universal for all tilted perovskite multiferroics, is known to strongly correlate with domain wall functionalities in the materials. The intrinsic mechanisms of domain wall phenomena, especially AFD-FE coupling-induced phenomena at the domain walls, have continued to intrigue the scientific and technological communities because of the need to develop the future nano-scale electronic devices. Over the past years, theoretical studies often show controversial results, owing to the fact that they are neither suffic…
Multiferroics have received intense attention due to their great application potential in multi-state information storage devices and new types of sensors. Coupling among ferroic orders such as ferroelectricity, (anti-)ferromagnetism, ferroelasticity, etc. will enable dynamic interaction between these ordering parameters. Direct visualization of such coupling behaviour in single phase multiferroic materials is highly desirable for both applications and fundamental study. Manipulation of both ferroelectric and magnetic domains of Bi5Ti3FeO15 thin film using electric field and external mechanica…
In numerous functional materials, such as steels, ferroelectrics and magnets, new functionalities can be achieved through the engineering of the domain structures, which are associated with the ordering of certain parameters within the material. The recent progress in imaging techniques with atomic-scale spatial resolution transformed our understanding of domain topology revealing that, along with simple stripe-like or irregularly shaped domains, intriguing vortex-type topological domain configurations also exist. In this Review, we present a new classification scheme of "ZmxZn domains with Zl…
We present a model artificial multiferroic system consisting of a (011)-oriented ferroelectric Pb(Mg,Nb,Ti)O$_3$ substrate intimately coupled to a ferromagnetic (La,Sr)MnO$_3$ film through epitaxial strain and converse piezoelectric effects. Electric field pulse sequences of less than 6 kV/cm were shown to induce large reversible and bistable remanent strains in the manganite film. Magnetic hysteresis loops demonstrate that the changes in strain states result in significant changes in magnetic anisotropy from a highly anisotropic two-fold magnetic symmetry to a more isotropic one. Such changes…
