Search

Reversible ferroelectric domain wall movements beyond the 10 nm range associated with Rayleigh behavior are usually restricted to specific defect-engineered systems. Here, we demonstrate that such long-range movements naturally occur in the improper ferroelectric ErMnO3 during electric-field-cycling. We study the electric-field-driven motion of domain walls, showing that they readily return to their initial position after having travelled distances exceeding 250 nm. By applying switching spectroscopy band-excitation piezoresponse force microscopy, we track the domain wall movement with nanometric spatial precision and analyze the local switching behavior. Phase field simulations show that the reversible long-range motion is intrinsic to the hexagonal manganites, linking it to their improper ferroelectricity and topologically protected structural vortex lines, which serve as anchor point for the ferroelectric domain walls. Our results give new insight into the local dynamics of domain walls in improper ferroelectrics and demonstrate the possibility to reversibly displace domain walls over much larger distances than commonly expected for ferroelectric systems in their pristine state, ensuring predictable device behavior for applications such as tunable capacitors or sensors

The subclass of collinear antiferromagnets where spin Kramers degeneracy is broken -- so that they can display ferromagnetic-like properties -- stimulates a new perspective in magnetism. However, the material base for these so-called altermagnets is still relatively limited. We show that Ruddlesden-Popper and perovskite phases generically host altermagnetic materials. In particular, we analyze prototypical nickel-based systems via first-principles calculations and identify additional materials from their crystal structure and magnetic orders. These materials span both insulating/semiconducting and metallic conduction types and the computed values of the nonrelativistic spin splittings reach 250~meV. Our analysis also indicates some formal inconsistencies that may appear within the traditional classification of magnetically ordered materials, which can easily be resolved from the altermagnetic perspective. In addition, we indicate the possibility of having altermagnetic behavior in systems beyond collinear antiferromagnets with perfectly compensated magnetization., Comment: 7 pages, 5 figures, 1 table

Considering the growing interest in magnetic materials for unconventional computing, data storage, and sensor applications, there is active research not only on material synthesis but also characterisation of their properties. In addition to structural and integral magnetic characterisations, imaging of magnetization patterns, current distributions and magnetic fields at nano- and microscale is of major importance to understand the material responses and qualify them for specific applications. In this roadmap, we aim to cover a broad portfolio of techniques to perform nano- and microscale magnetic imaging using SQUIDs, spin center and Hall effect magnetometries, scanning probe microscopies, x-ray- and electron-based methods as well as magnetooptics and nanoMRI. The roadmap is aimed as a single access point of information for experts in the field as well as the young generation of students outlining prospects of the development of magnetic imaging technologies for the upcoming decade with a focus on physics, materials science, and chemistry of planar, 3D and geometrically curved objects of different material classes including 2D materials, complex oxides, semi-metals, multiferroics, skyrmions, antiferromagnets, frustrated magnets, magnetic molecules/nanoparticles, ionic conductors, superconductors, spintronic and spinorbitronic materials.

Mechanical pressure controls the structural, electric, and magnetic order in solid state systems, allowing to tailor and improve their physical properties. A well-established example is ferroelastic ferroelectrics, where the coupling between pressure and the primary symmetry breaking order parameter enables hysteretic switching of the strain state and ferroelectric domain engineering. Here, we study the pressure-driven response in a non-ferroelastic ferroelectric, ErMnO3, where the classical stress-strain coupling is absent, and the domain formation is governed by creation-annihilation processes of topological defects. By annealing ErMnO3 polycrystals under variable pressures in the MPa-regime, we transform non-ferroelastic vortex-like domains into stripe-like domains. The width of the stripe-like domains is determined by the applied pressure as we confirm by three-dimensional phase field simulations, showing that pressure leads to highly oriented layer-like periodic domains. Our work demonstrates the possibility to utilize mechanical pressure for domain engineering in non-ferroelastic ferroelectrics, providing a processing-accessible lever to control their dielectric, electromechanical, and piezoelectric response.

We report on multiple fundamental qualitative improvements in the growth of improper ferroelectric hexagonal YMnO$_3$ (YMO) thin films and heterostructures by pulsed laser deposition (PLD). By a combination of pre-growth substrate annealing and low-energy-fluence PLD, we obtain a two-dimensional growth mode of the YMO films on yttria-stabilized zirconia (YSZ) with ultralow roughness and devoid of misoriented nanocrystalline inclusions. By inserting a sacrificial manganite layer capped with conducting indium-tin oxide between the substrate and the final film, the latter is grown in a fully lattice-relaxed mode and, thus, without any misfit dislocations while maintaining the extraordinary flatness of the films grown directly on pre-annealed YSZ. This provides a template for the fabrication of heterostructures based on hexagonal manganites as promising class of multiferroics with improper room-temperature ferroelectricity and the implementation of these into technologically relevant epitaxial metal|ferroelectric-type multilayers., Comment: 13 pages, 5 figures

We resolve the domain-wall structure of the model antiferromagnet $\text{Cr}_2\text{O}_3$ using nanoscale scanning diamond magnetometry and second-harmonic-generation microscopy. We find that the 180$^\circ$ domain walls are predominantly Bloch-like, and can co-exist with N\'eel walls in crystals with significant in-plane anisotropy. In the latter case, N\'eel walls that run perpendicular to a magnetic easy axis acquire a well-defined chirality. We further report quantitative measurement of the domain-wall width and surface magnetization. Our results provide fundamental input and an experimental methodology for the understanding of domain walls in pure, intrinsic antiferromagnets, which is relevant to achieve electrical control of domain-wall motion in antiferromagnetic compounds., Comment: 9 pages, 5 figures. Includes 11 pages of supplemental material

Inversion symmetry breaking is a ubiquitous concept in condensed-matter science. On the one hand, it is a prerequisite for many technologically relevant effects such as piezoelectricity, photovoltaic and nonlinear optical properties and spin-transport phenomena. On the other hand, it may determine abstract properties such as the electronic topology in quantum materials. Therefore, the creation of materials where inversion symmetry can be turned on or off by design may be the ultimate route towards controlling parity-related phenomena and functionalities. Here, we engineer the symmetry of ultrathin epitaxial oxide films by sub-unit-cell growth control. We reversibly activate and deactivate inversion symmetry in the layered hexagonal manganites, h-RMnO$_3$ with R = Y, Er, Tb. While an odd number of half-unit-cell layers exhibits a breaking of inversion symmetry through its arrangement of MnO$_5$ bipyramids, an even number of such half-unit-cell layers takes on a centrosymmetric structure. Here we control the resulting symmetry by tracking the growth in situ via optical second-harmonic generation. We furthermore demonstrate that our symmetry engineering works independent of the choice of R and even in heterostructures mixing constituents with different R in a two-dimensional growth mode. Symmetry engineering on the atomic level thus suggests a new platform for the controlled activation and deactivation of symmetry-governed functionalities in oxide-electronic epitaxial thin films., Comment: 5 pages, 4 figures

Materials with long-range order like ferromagnetism or ferroelectricity exhibit uniform, yet differently oriented three-dimensional regions called domains that are separated by two-dimensional topological defects termed domain walls\cite{Tagantsev2010,AlexHubert1998}. A change of the ordered state across a domain wall can lead to local non-bulk properties such as enhanced conductance or the promotion of unusual phases\cite{Seidel2009,Meier2012,Farokhipoor2014}. Although highly desirable, controlled transfer of these exciting properties between the bulk and the walls is usually not possible. Here we demonstrate this crossover from three- to two-dimensions for confining multiferroic Dy$_{0.7}$Tb$_{0.3}$FeO$_3$ domains into multiferroic domain walls at a specified location within a non-multiferroic environment. This process is fully reversible; an applied magnetic or electric field controls the transformation. Aside from the aspect of magnetoelectric functionality, such interconversion can be key to tailoring elusive domain architectures such as in antiferromagnets.

We show, by solving Maxwell's equations, that an electric charge on the surface of a slab of a linear magnetoelectric material generates an image magnetic monopole below the surface provided that the magnetoelectric has a diagonal component in its magnetoelectric response. The image monopole, in turn, generates an ideal monopolar magnetic field outside of the slab. Using realistic values of the electric- and magnetic- field susceptibilties, we calculate the magnitude of the effect for the prototypical magnetoelectric material Cr$_2$O$_3$. We use low energy muon spin rotation to measure the strength of the magnetic field generated by charged muons as a function of their distance from the surface of a Cr$_2$O$_3$ films, and show that the results are consistent with the existence of the monopole. We discuss other possible routes to detecting the monopolar field, and show that, while the predicted monopolar field generated by Cr$_2$O$_3$ is above the detection limit for standard magnetic force microscopy, detection of the field using this technique is prevented by surface charging effects., Comment: 8 pages, 9 figures

Ferroelectric domain walls represent multifunctional 2D-elements with great potential for novel device paradigms at the nanoscale. Improper ferroelectrics display particularly promising types of domain walls, which, due to their unique robustness, are the ideal template for imposing specific electronic behavior. Chemical doping, for instance, induces p- or n-type characteristics and electric fields reversibly switch between resistive and conductive domain-wall states. Here, we demonstrate diode-like conversion of alternating-current (AC) into direct-current (DC) output based on neutral 180$^{\circ}$ domain walls in improper ferroelectric ErMnO$_3$. By combining scanning probe and dielectric spectroscopy, we show that the rectification occurs for frequencies at which the domain walls are fixed to their equilibrium position. The practical frequency regime and magnitude of the output is controlled by the bulk conductivity. Using density functional theory we attribute the transport behavior at the neutral walls to an accumulation of oxygen defects. Our study reveals domain walls acting as 2D half-wave rectifiers, extending domain-wall-based nanoelectronic applications into the realm of AC technology.

Control and detection of spin order in ferromagnets is the main principle allowing storing and reading of magnetic information in nowadays technology. The large class of antiferromagnets, on the other hand, is less utilized, despite its very appealing features for spintronics applications. For instance, the absence of net magnetization and stray fields eliminates crosstalk between neighbouring devices and the absence of a primary macroscopic magnetization makes spin manipulation in antiferromagnets inherently faster than in ferromagnets. However, control of spins in antiferromagnets requires exceedingly high magnetic fields, and antiferromagnetic order cannot be detected with conventional magnetometry. Here we provide an overview and illustrative examples of how electromagnetic radiation can be used for probing and modification of the magnetic order in antiferromagnets. Spin pumping from antiferromagnets, propagation of terahertz spin excitations, and tracing the reversal of the antiferromagnetic and ferroelectric order parameter in multiferroics are anticipated to be among the main topics defining the future of this field., Comment: Part of a collection of reviews on antiferromagnetic spintronics; 26 pages, 7 figures

The spontaneous transformations associated with symmetry-breaking phase transitions generate domain structures and defects that may be topological in nature. The formation of these defects can be described according to the Kibble-Zurek mechanism, which provides a generic relation that applies from cosmological to interatomic lengthscales. Its verification is challenging, however, in particular at the cosmological scale where experiments are impractical. While it has been demonstrated for selected condensed-matter systems, major questions remain regarding e.g. its degree of universality. Here we develop a global Kibble-Zurek picture from the condensed-matter level. We show theoretically that a transition between two fluctuation regimes (Ginzburg and mean-field) can lead to an intermediate region with reversed scaling, and we verify experimentally this behavior for the structural transition in the series of multiferroic hexagonal manganites. Trends across the series allow us to identify additional intrinsic features of the defect formation beyond the original Kibble-Zurek paradigm., Comment: 8 pages, 4 figures

One of the most successful paradigms of many-body physics is the concept of quasiparticles: excitations in strongly interacting matter behaving like weakly interacting particles in free space. Quasiparticles in metals are very robust objects. Yet, when a system's ground state undergoes a qualitative change at a quantum critical point (QCP), the quasiparticles may disintegrate and give way to an exotic quantum-fluid state of matter. The nature of this breakdown is intensely debated, because the emergent quantum fluid dominates the material properties up to high temperature and might even be related to the occurence of superconductivity in some compounds. Here we trace the dynamics of heavy-fermion quasiparticles in CeCu$_{6-x}$Au$_{x}$ and monitor their evolution towards the QCP in time-resolved experiments, supported by many-body calculations. A terahertz pulse disrupts the many-body heavy-fermion state. Under emission of a delayed, phase-coherent terahertz reflex the heavy-fermion state recovers, with a coherence time 100 times longer than typically associated with correlated metals. The quasiparticle weight collapses towards the QCP, yet its formation temperature remains constant -- phenomena believed to be mutually exclusive. Coexistence in the same experiment calls for revisions in our view on quantum criticality., Comment: Published version, including data on CeCu6, CeCu5.9Au0.1, and CeCu5Au1 and extended Supplementary Information. 7 pages, 4 figures, Supplementary Information: 5 pages, 3 figures

We deduce the intrinsic conductivity properties of the ferroelectric domain walls around the topologically protected domain vortex cores in multiferroic YMnO3. This is achieved by performing a careful equivalent-circuit analysis of dielectric spectra measured in single-crystalline samples with different vortex densities. The conductivity contrast between the bulk domains and the less conducting domain boundaries is revealed to reach up to a factor 500 at room temperature, depending on sample preparation. Tunneling of localized defect charge carriers is the dominant charge-transport process in the domain walls that are depleted of mo-bile charge carriers. This work demonstrates that via equivalent-circuit analysis, dielectric spectroscopy can provide valuable information on the intrinsic charge-transport properties of ferroelectric domain walls, which is of high relevance for the design of new domain-wall-based microelectronic devices., Comment: 5 pages, 4 figures + 3 pages, 4 figures in Supplemental Material. Revised version as accepted for publication in Phys. Rev. Lett

We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $\Delta/$ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries., Comment: 26 pages, 7 figures

We demonstrate a concept for post-growth symmetry control in oxide heterostructures. A functional oxide is sandwiched between two ferroelectric layers and inversion symmetry at the position of the oxide constituent is reversibly switched on or off by layer-selective electric-field poling. The functionality of this process is monitored by optical second harmonic generation. The generalization of our approach to other materials and symmetries is considered. We thus establish ferroic trilayer structures as device components in which symmetry-driven charge-, spin-, and strain-related functionalities can be activated and deactivated at will.

The complex interplay between the 3d and 4f moments in hexagonal ErMnO3 is investigated by magnetization, optical second harmonic generation, and neutron-diffraction measurements. We revise the phase diagram and provide a microscopic model for the emergent spin structures with a special focus on the intermediary phase transitions. Our measurements reveal that the 3d exchange between Mn^{3+} ions dominates the magnetic symmetry at 10 K < T < T_N with Mn^3+ order according to the Gamma_4 representation triggering 4f ordering according to the same representation on the Er^{3+}(4b) site. Below 10 K the magnetic order is governed by 4f exchange interactions of Er^{3+} ions on the 2a site. The magnetic Er^{3+}(2a) order according to the representation Gamma_2 induces a magnetic reorientation (Gamma_4 --> Gamma_2) at the Er^{3+}(4b) and the Mn^{3+} sites. Our findings highlight the fundamentally different roles the Mn^{3+}, R^{3+}(2a), and R^{3+}(4b) magnetism play in establishing the magnetic phase diagram of the hexagonal RMnO3 system.

Epitaxial CaMnO3 films grown with 2.3% tensile strain on (001)-oriented LaAlO3 substrates are found to be incipiently ferroelectric below 25 K. Optical second harmonic generation (SHG) was used for the detection of the incipient polarization. The SHG analysis reveals that CaMnO3 crystallites with in-plane orientation of the orthorhombic b axis contribute to an electric polarization oriented along the orthorhombic a (resp.\ c) axis in agreement with the predictions from density functional calculations.

We show that the improper ferroelectric phase transition in the multiferroic hexagonal manganites displays the same symmetry-breaking characteristics as those proposed in early-universe theories. We present an analysis of the Kibble-Zurek theory of topological defect formation applied to the hexagonal manganites, discuss the conditions determining the range of cooling rates in which Kibble-Zurek behavior is expected, and show that recent literature data are consistent with our predictions. We explore experimentally for the first time to our knowledge the cross-over out of the Kibble-Zurek regime and find a surprising "anti-Kibble-Zurek" behavior.

Three independent contributions to the magnetically induced spontaneous polarization of multiferroic TbMn2O5 are uniquely separated by optical second harmonic generation and an analysis in terms of Landau theory. Two of them are related to the magnetic Mn3+/4+ order and are independent of applied fields of up to 7 T. The third contribution is related to the long-range antiferromagnetic Tb3+ order. It shows a drastic decrease upon the application of a magnetic field and mediates the change of sign of the spontaneous electric polarization in TbMn2O5. The close relationship between the rare-earth long-range order and the non-linear optical properties points to isotropic Tb-Tb exchange and oxygen spin polarization as mechanism for this rare-earth induced ferroelectricity., Comment: 8 pages, 5 figures

The magnetic and electrical properties of Co$_3$TeO$_6$ single-crystals with corundum related structure reveal a magnetic-field induced polarization below 21 K. A sharp peak in the specific heat at \approx 18 K indicates a reconstructive-type first-order phase transition. From second-harmonic generation (SHG) measurements breaking of inversion symmetry is evident and the point-group symmetry was determined as m. The temperature and magnetic-field dependence of the magnetic and electrical polarizations are discussed in the light of the SHG results., Comment: 5 pages, 5 figures

By an electrical-pump--optical-probe technique we show that the electric-field-induced reversal of the magnetic order parameter in multiferroic MnWO$_4$ occurs on the time scale of milliseconds and maintains a rigid coupling of the magnetization to the magnetically induced electric polarization. The temporal progression of the spatially resolved domain structure was imaged with nanosecond resolution by optical second harmonic generation and compared to the quasi-static domain reversal. A qualitative model gives an estimate of why the magnetoelectric order-parameter reversal in the magnetically induced ferroelectrics is not inherently ultrafast.

Translation domains differing in the phase but not in the orientation of the corresponding order parameter are resolved in two types of multiferroics. Hexagonal (h-) YMnO$_3$ is a split-order-parameter multiferroic in which commensurate ferroelectric translation domains are resolved by piezoresponse force microscopy whereas MnWO$_4$ is a joint-order-parameter multiferroic in which incommensurate magnetic translation domains are observed by optical second harmonic generation. The pronounced manifestation of the generally rather "hidden" translation domains in these multiferroics and the associated drastic reduction of symmetry emphasize that the presence of translation domains must not be neglected when discussing the physical properties and functionalities of multiferroics.

A comprehensive analysis of optical second harmonic generation (SHG) on an incommensurate (IC) magnetically ordered state is presented using multiferroic MnWO4 as model compound. Two fundamentally different SHG contributions coupling to the primary IC magnetic order or to secondary commensurate projections of the IC state, respectively, are distinguished. Whereas the latter can be described within the formalism of the 122 commensurate magnetic point groups the former involves a breakdown of the conventional macroscopic symmetry analysis because of its sensitivity to the lower symmetry of the local environment in a crystal lattice. Our analysis thus foreshadows the fusion of the hitherto disjunct fields of nonlinear optics and IC order in condensed-matter systems.

Magnetic order of the manganese and rare-earth lattices according to different symmetry representations is observed in multiferroic hexagonal (h-) DyMnO$_3$ by optical second harmonic generation and neutron diffraction. The incompatibility reveals that the 3d-4f coupling in the h-$R$MnO$_3$ system ($R$ = Sc, Y, In, Dy - Lu) is substantially less developed than commonly expected. As a consequence, magnetoelectric coupling effects in this type of split-order parameter multiferroic that were previously assigned to a pronounced 3d-4f coupling have now to be scrutinized with respect to their origin.

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.