Electric-field-induced multiferroic topological solitons.

Topologically protected spin whirls in ferromagnets are foreseen as the cart-horse of solitonic information technologies. Nevertheless, the future of skyrmionics may rely on antiferromagnets due to their immunity to dipolar fields, straight motion along the driving force and ultrafast dynamics. While complex topological objects were recently discovered in intrinsic antiferromagnets, mastering their nucleation, stabilization and manipulation with energy-efficient means remains an outstanding challenge. Designing topological polar states in magnetoelectric antiferromagnetic multiferroics would allow one to electrically write, detect and erase topological antiferromagnetic entities. Here we stabilize ferroelectric centre states using a radial electric field in multiferroic BiFeO3 thin films. We show that such polar textures contain flux closures of antiferromagnetic spin cycloids, with distinct antiferromagnetic entities at their cores depending on the electric field polarity. By tuning the epitaxial strain, quadrants of canted antiferromagnetic domains can also be electrically designed. These results open the path to reconfigurable topological states in multiferroic antiferromagnets.

Onset of Multiferroicity in Prototypical Single-Spin Cycloid BiFeO3 Thin Films.

In the room-temperature magnetoelectric multiferroic BiFeO3, the noncollinear antiferromagnetic state is coupled to the ferroelectric order, opening applications for low-power electric-field-controlled magnetic devices. While several strategies have been explored to simplify the ferroelectric landscape, here we directly stabilize a single-domain ferroelectric and spin cycloid state in epitaxial BiFeO3 (111) thin films grown on orthorhombic DyScO3 (011). Comparing them with films grown on SrTiO3 (111), we identify anisotropic in-plane strain as a powerful handle for tailoring the single antiferromagnetic state. In this single-domain multiferroic state, we establish the thickness limit of the coexisting electric and magnetic orders and directly visualize the suppression of the spin cycloid induced by the magnetoelectric interaction below the ultrathin limit of 1.4 nm. This as-grown single-domain multiferroic configuration in BiFeO3 thin films opens an avenue both for fundamental investigations and for electrically controlled noncollinear antiferromagnetic spintronics.

Room-temperature stabilization of antiferromagnetic skyrmions in synthetic antiferromagnets.

Room-temperature skyrmions in ferromagnetic films and multilayers show promise for encoding information bits in new computing technologies. Despite recent progress, ferromagnetic order generates dipolar fields that prevent ultrasmall skyrmion sizes, and allows a transverse deflection of moving skyrmions that hinders their efficient manipulation. Antiferromagnetic skyrmions shall lift these limitations. Here we demonstrate that room-temperature antiferromagnetic skyrmions can be stabilized in synthetic antiferromagnets (SAFs), in which perpendicular magnetic anisotropy, antiferromagnetic coupling and chiral order can be adjusted concurrently. Utilizing interlayer electronic coupling to an adjacent bias layer, we demonstrate that spin-spiral states obtained in a SAF with vanishing perpendicular magnetic anisotropy can be turned into isolated antiferromagnetic skyrmions. We also provide model-based estimates of skyrmion size and stability, showing that room-temperature antiferromagnetic skyrmions below 10 nm in radius can be anticipated in further optimized SAFs. Antiferromagnetic skyrmions in SAFs may thus solve major issues associated with ferromagnetic skyrmions for low-power spintronic devices.

Imaging and Harnessing Percolation at the Metal-Insulator Transition of NdNiO3 Nanogaps.

Competition between coexisting electronic phases in first-order phase transitions can lead to a sharp change in the resistivity as the material is subjected to small variations in the driving parameter, for example, the temperature. One example of this phenomenon is the metal-insulator transition (MIT) in perovskite rare-earth nickelates. In such systems, reducing the transport measurement area to dimensions comparable to the domain size of insulating and metallic phases around the MIT should strongly influence the shape of the resistance-temperature curve. Here we measure the temperature dependence of the local resistance and the nanoscale domain distribution of NdNiO3 areas between Au contacts gapped by 40-260 nm. We find that a sharp resistance drop appears below the bulk MIT temperature at ∼105 K, with an amplitude inversely scaling with the nanogap width. By using X-ray photoemission electron microscopy, we directly correlate the resistance drop to the emergence and distribution of individual metallic domains at the nanogap. Our observation provides useful insight into percolation at the MIT of rare-earth nickelates.

Chaos in Magnetic Nanocontact Vortex Oscillators.

We present an experimental study of spin-torque driven vortex self-oscillations in magnetic nanocontacts. We find that, above a certain threshold in applied currents, the vortex gyration around the nanocontact is modulated by relaxation oscillations, which involve periodic reversals of the vortex core. This modulation leads to the appearance of commensurate but also, more interestingly here, incommensurate states, which are characterized by devil's staircases in the modulation frequency. We use frequency- and time-domain measurements together with advanced time-series analyses to provide experimental evidence of chaos in incommensurate states of vortex oscillations, in agreement with theoretical predictions.

Direct Mapping of Phase Separation across the Metal-Insulator Transition of NdNiO3.

Perovskite rare-earth nickelates RNiO3 are prototype correlated oxides displaying a metal-insulator transition (MIT) at a temperature tunable by the ionic radius of the rare-earth R. Although its precise origin remains a debated topic, the MIT can be exploited in various types of applications, notably for resistive switching and neuromorphic computation. So far, the MIT has been mostly studied by macroscopic techniques, and insights into its nanoscale mechanisms were only provided recently by X-ray photoemission electron microscopy through absorption line shifts, used as an indirect proxy to the resistive state. Here, we directly image the local resistance of NdNiO3 thin films across their first-order MIT using conductive-atomic force microscopy. Our resistance maps reveal the nucleation of ∼100-300 nm metallic domains in the insulating state that grow and percolate as temperature increases. We discuss the resistance contrast mechanism, analyze the microscopy and transport data within a percolation model, and propose experiments to harness this mesoscopic electronic texture in devices.

Chirality in Magnetic Multilayers Probed by the Symmetry and the Amplitude of Dichroism in X-Ray Resonant Magnetic Scattering.

Chirality in condensed matter has recently become a topic of the utmost importance because of its significant role in the understanding and mastering of a large variety of new fundamental physical mechanisms. Versatile experimental approaches, capable to reveal easily the exact winding of order parameters, are therefore essential. Here we report x-ray resonant magnetic scattering as a straightforward tool to reveal directly the properties of chiral magnetic systems. We show that it can straightforwardly and unambiguously determine the main characteristics of chiral magnetic distributions: i.e., its chiral nature, the quantitative winding sense (clockwise or counterclockwise), and its type, i.e., Néel [cycloidal] or Bloch [helical]. This method is model independent, does not require a priori knowledge of the magnetic parameters, and can be applied to any system with magnetic domains ranging from a few nanometers (wavelength limited) to several microns. By using prototypical multilayers with tailored magnetic chiralities driven by spin-orbit-related effects at Co|Pt interfaces, we illustrate the strength of this method.

Room-Temperature Current-Induced Generation and Motion of sub-100 nm Skyrmions.

Magnetic skyrmions are nanoscale windings of the spin configuration that hold great promise for technology due to their topology-related properties and extremely reduced sizes. After the recent observation at room temperature of sub-100 nm skyrmions stabilized by interfacial chiral interaction in magnetic multilayers, several pending questions remain to be solved, notably about the means to nucleate individual compact skyrmions or the exact nature of their motion. In this study, a method leading to the formation of magnetic skyrmions in a micrometer-sized track using homogeneous current injection is evidenced. Spin-transfer-induced motion of these small electrical-current-generated skyrmions is then demonstrated and the role of the out-of-plane magnetic field in the stabilization of the moving skyrmions is also analyzed. The results of these experimental observations of spin torque induced motion are compared to micromagnetic simulations reproducing a granular type, nonuniform magnetic multilayer in order to address the particularly important role of the magnetic inhomogeneities on the current-induced motion of sub-100 nm skyrmions for which the material grains size is comparable to the skyrmion diameter.

Unidirectional Spin-Dependent Molecule-Ferromagnet Hybridized States Anisotropy in Cobalt Phthalocyanine Based Magnetic Tunnel Junctions.

Organic or molecular spintronics is a rising field of research at the frontier between condensed matter physics and chemistry. It aims to mix spin physics and the richness of chemistry towards designing new properties for spin electronics devices through engineering at the molecular scale. Beyond the expectation of a long spin lifetime, molecules can be also used to tailor the spin polarization of the injected current through the spin-dependent hybridization between molecules and ferromagnetic electrodes. In this Letter, we provide direct evidence of a hybrid interface spin polarization reversal due to the differing hybridization between phthalocyanine molecules and each cobalt electrode in Co/CoPc/Co magnetic tunnel junctions. Tunnel magnetoresistance and anisotropic tunnel magnetoresistance experiments show that interfacial hybridized electronic states have a unidirectional anisotropy that can be controlled by an electric field and that spin hybridization at the bottom and top interfaces differ, leading to an inverse tunnel magnetoresistance.

Voltage-based magnetization switching and reading in magnetoelectric spin-orbit nanodevices.

As CMOS technologies face challenges in dimensional and voltage scaling, the demand for novel logic devices has never been greater, with spin-based devices offering scaling potential, at the cost of significantly high switching energies. Alternatively, magnetoelectric materials are predicted to enable low-power magnetization control, a solution with limited device-level results. Here, we demonstrate voltage-based magnetization switching and reading in nanodevices at room temperature, enabled by exchange coupling between multiferroic BiFeO3 and ferromagnetic CoFe, for writing, and spin-to-charge current conversion between CoFe and Pt, for reading. We show that, upon the electrical switching of the BiFeO3, the magnetization of the CoFe can be reversed, giving rise to different voltage outputs. Through additional microscopy techniques, magnetization reversal is linked with the polarization state and antiferromagnetic cycloid propagation direction in the BiFeO3. This study constitutes the building block for magnetoelectric spin-orbit logic, opening a new avenue for low-power beyond-CMOS technologies.

A ferroelectric memristor.

Memristors are continuously tunable resistors that emulate biological synapses. Conceptualized in the 1970s, they traditionally operate by voltage-induced displacements of matter, although the details of the mechanism remain under debate. Purely electronic memristors based on well-established physical phenomena with albeit modest resistance changes have also emerged. Here we demonstrate that voltage-controlled domain configurations in ferroelectric tunnel barriers yield memristive behaviour with resistance variations exceeding two orders of magnitude and a 10 ns operation speed. Using models of ferroelectric-domain nucleation and growth, we explain the quasi-continuous resistance variations and derive a simple analytical expression for the memristive effect. Our results suggest new opportunities for ferroelectrics as the hardware basis of future neuromorphic computational architectures.

Room temperature electrical manipulation of giant magnetoresistance in spin valves exchange-biased with BiFeO3.

Magnetoelectric multiferroics are attractive materials for the development of low-power electrically controlled spintronic devices. Here we report the optimization of the exchange bias as well as the giant magnetoresistance effect (GMR) of spin valves deposited on top of BiFeO(3)-based heterostructures. We show that the exchange bias can be electrically controlled through a change in the relative proportion of 109° domain walls and propose solutions toward a reversible process.

Atomic and electronic structure of the BaTiO3/Fe interface in multiferroic tunnel junctions.

Artificial multiferroic tunnel junctions combining a ferroelectric tunnel barrier of BaTiO(3) with magnetic electrodes display a tunnel magnetoresistance whose intensity can be controlled by the ferroelectric polarization of the barrier. This effect, called tunnel electromagnetoresistance (TEMR), and the corollary magnetoelectric coupling mechanisms at the BaTiO(3)/Fe interface were recently reported through macroscopic techniques. Here, we use advanced spectromicroscopy techniques by means of aberration-corrected scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS) to probe locally the nanoscale structural and electronic modifications at the ferroelectric/ferromagnetic interface. Atomically resolved real-space spectroscopic techniques reveal the presence of a single FeO layer between BaTiO(3) and Fe. Based on this accurate description of the studied interface, we propose an atomistic model of the ferroelectric/ferromagnetic interface further validated by comparing experimental and simulated STEM images with atomic resolution. Density functional theory calculations allow us to interpret the electronic and magnetic properties of these interfaces and to understand better their key role in the physics of multiferroics nanostructures.

Three-dimensional skyrmionic cocoons in magnetic multilayers.

Three-dimensional spin textures emerge as promising quasi-particles for encoding information in future spintronic devices. The third dimension provides more malleability regarding their properties and more flexibility for potential applications. However, the stabilization and characterization of such quasi-particles in easily implementable systems remain a work in progress. Here we observe a three-dimensional magnetic texture that sits in the interior of magnetic thin films aperiodic multilayers and possesses a characteristic ellipsoidal shape. Interestingly, these objects that we call skyrmionic cocoons can coexist with more standard tubular skyrmions going through all the multilayer as evidenced by the existence of two very different contrasts in room temperature magnetic force microscopy. The presence of these novel skyrmionic textures as well as the understanding of their layer resolved chiral and topological properties have been investigated by micromagnetic simulations. Finally, we show that the skyrmionic cocoons can be electrically detected using magneto-transport measurements.

Almost Perfect Spin Filtering in Graphene-Based Magnetic Tunnel Junctions.

We report on large spin-filtering effects in epitaxial graphene-based spin valves, strongly enhanced in our specific multilayer case. Our results were obtained by the effective association of chemical vapor deposited (CVD) multilayer graphene with a high quality epitaxial Ni(111) ferromagnetic spin source. We highlight that the Ni(111) spin source electrode crystallinity and metallic state are preserved and stabilized by multilayer graphene CVD growth. Complete nanometric spin valve junctions are fabricated using a local probe indentation process, and spin properties are extracted from the graphene-protected ferromagnetic electrode through the use of a reference Al2O3/Co spin analyzer. Strikingly, spin-transport measurements in these structures give rise to large negative tunnel magneto-resistance TMR = -160%, pointing to a particularly large spin polarization for the Ni(111)/Gr interface PNi/Gr, evaluated up to -98%. We then discuss an emerging physical picture of graphene-ferromagnet systems, sustained both by experimental data and ab initio calculations, intimately combining efficient spin filtering effects arising (i) from the bulk band structure of the graphene layers purifying the extracted spin direction, (ii) from the hybridization effects modulating the amplitude of spin polarized scattering states over the first few graphene layers at the interface, and (iii) from the epitaxial interfacial matching of the graphene layers with the spin-polarized Ni surface selecting well-defined spin polarized channels. Importantly, these main spin selection effects are shown to be either cooperating or competing, explaining why our transport results were not observed before. Overall, this study unveils a path to harness the full potential of low Resitance.Area (RA) graphene interfaces in efficient spin-based devices.

Nanoscale electrostatic manipulation of magnetic flux quanta in ferroelectric/superconductor BiFeO3/YBa2Cu3O(7-δ) heterostructures.

Using heterostructures that combine a large-polarization ferroelectric (BiFeO3) and a high-temperature superconductor (YBa2Cu3O(7-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, together with the possibility to reversibly design the ferroelectric domain structure, allows the electrostatic manipulation of magnetic flux quanta.

Tunable Stochasticity in an Artificial Spin Network.

Metamaterials present the possibility of artificially generating advanced functionalities through engineering of their internal structure. Artificial spin networks, in which a large number of nanoscale magnetic elements are coupled together, are promising metamaterial candidates that enable the control of collective magnetic behavior through tuning of the local interaction between elements. In this work, the motion of magnetic domain-walls in an artificial spin network leads to a tunable stochastic response of the metamaterial, which can be tailored through an external magnetic field and local lattice modifications. This type of tunable stochastic network produces a controllable random response exploiting intrinsic stochasticity within magnetic domain-wall motion at the nanoscale. An iconic demonstration used to illustrate the control of randomness is the Galton board. In this system, multiple balls fall into an array of pegs to generate a bell-shaped curve that can be modified via the array spacing or the tilt of the board. A nanoscale recreation of this experiment using an artificial spin network is employed to demonstrate tunable stochasticity. This type of tunable stochastic network opens new paths toward post-Von Neumann computing architectures such as Bayesian sensing or random neural networks, in which stochasticity is harnessed to efficiently perform complex computational tasks.

Imaging non-collinear antiferromagnetic textures via single spin relaxometry.

Antiferromagnetic materials are promising platforms for next-generation spintronics owing to their fast dynamics and high robustness against parasitic magnetic fields. However, nanoscale imaging of the magnetic order in such materials with zero net magnetization remains a major experimental challenge. Here we show that non-collinear antiferromagnetic spin textures can be imaged by probing the magnetic noise they locally produce via thermal populations of magnons. To this end, we perform nanoscale, all-optical relaxometry with a scanning quantum sensor based on a single nitrogen-vacancy (NV) defect in diamond. Magnetic noise is detected through an increase of the spin relaxation rate of the NV defect, which results in an overall reduction of its photoluminescence signal under continuous laser illumination. As a proof-of-concept, the efficiency of the method is demonstrated by imaging various spin textures in synthetic antiferromagnets, including domain walls, spin spirals and antiferromagnetic skyrmions. This imaging procedure could be extended to a large class of intrinsic antiferromagnets and opens up new opportunities for studying the physics of localized spin wave modes for magnonics.

Pattern generation and symbolic dynamics in a nanocontact vortex oscillator.

Harnessing chaos or intrinsic nonlinear behaviours of dynamical systems is a promising avenue toward unconventional information processing technologies. In this light, spintronic devices are promising because of the inherent nonlinearity of magnetization dynamics. Here, we demonstrate experimentally the potential for chaos-based schemes using nanocontact vortex oscillators by unveiling and characterizing their waveform patterns and symbolic dynamics using time-resolved electrical measurements. We dissociate nonlinear deterministic patterns from thermal fluctuations and show that the emergence of chaos results in the unpredictable alternation of well-defined patterns. With phase-space reconstruction techniques, we perform symbolic analyses of the time series and show that the oscillator exhibits maximal entropy and complexity at the centre of its incommensurate region. This suggests that such vortex-based systems are promising nanoscale sources of entropy that could be exploited for information processing.

Band-Structure Spin-Filtering in Vertical Spin Valves Based on Chemical Vapor Deposited WS2.

We report on spin transport in WS2-based 2D-magnetic tunnel junctions (2D-MTJs), unveiling a band structure spin filtering effect specific to the transition metal dichalcogenides (TMDCs) family. WS2 mono-, bi-, and trilayers are derived by a chemical vapor deposition process and further characterized by Raman spectroscopy, atomic force microscopy (AFM), and photoluminescence spectroscopy. The WS2 layers are then integrated in complete Co/Al2O3/WS2/Co MTJ hybrid spin-valve structures. We make use of a tunnel Co/Al2O3 spin analyzer to probe the extracted spin-polarized current from the WS2/Co interface and its evolution as a function of WS2 layer thicknesses. For monolayer WS2, our technological approach enables the extraction of the largest spin signal reported for a TMDC-based spin valve, corresponding to a spin polarization of PCo/WS2 = 12%. Interestingly, for bi- and trilayer WS2, the spin signal is reversed, which indicates a switch in the mechanism of interfacial spin extraction. With the support of ab initio calculations, we propose a model to address the experimentally measured inversion of the spin polarization based on the change in the WS2 band structure while going from monolayer (direct bandgap) to bilayer (indirect bandgap). These experiments illustrate the rich potential of the families of semiconducting 2D materials for the control of spin currents in 2D-MTJs.