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Abstract In-materia reservoir computing (RC) leverages the intrinsic physical responses of functional materials to perform complex computational tasks. Magnetic metamaterials are exciting candidates for RC due to their huge state space, nonlinear emergent dynamics, and non-volatile memory. However, to be suitable for a broad range of tasks, the material system is required to exhibit a broad range of properties, and isolating these behaviours experimentally can often prove difficult. By using an electrically accessible device consisting of an array of interconnected magnetic nanorings- a system shown to exhibit complex emergent dynamics- here we show how reconfiguring the reservoir architecture allows exploitation of different aspects the system’s dynamical behaviours. This is evidenced through state-of-the-art performance in diverse benchmark tasks with very different computational requirements, highlighting the additional computational configurability that can be obtained by altering the input/output architecture around the material system.

We demonstrate the reversible current-induced motion of 180° antiferromagnetic domain walls in a CuMnAs device. By controlling the magnitude and direction of the current pulse, the position of a domain wall can be switched between three distinct pinning sites. The domain wall motion is attributed to a field-like spin–orbit torque that induces the same sense of rotation on each magnetic sublattice, owing to the crystal symmetry of CuMnAs. Domain wall motion is observed for current densities down to ≈2.5×1010 A/m2 at room temperature.

Antiferromagnets (AFMs) are prospective for future spintronic devices, owing to their speed and insensitivity to perturbations. Using a combination of electronic and magnetic dichroism measurements, the authors demonstrate reversible current-induced switching of the Néel vector in AFM PtMn.

Key properties of transition metal perovskite oxides are degraded after epitaxial growth on ferroelectric substrates due to lattice-mismatch strain. Here, the authors use epitaxial lift-off and transfer to overcome this problem and demonstrate electric field control of a bulk-like magnetization.

Exchange coupling between ferromagnetic and multiferroic materials is a key to magnetoelectric devices but hard to achieve macroscopically. Here, the authors report room–temperature robust and reproducible magnetoelectric switching in Co/BiFeO3 heterostructures with monodomain properties over the entire sample at room temperature.

Probing the evolution of mixed-phase states in materials offers unique insights into the microscopic mechanism of phase transitions. Here, Mattoni et al. report imaging of nanoscale formation and growth of insulating domains across the metal-insulator transition in NdNiO3thin films, uncovering a rich interplay between structural and electronic degrees of freedom.

For 1 µm-diameter Ni discs on a BaTiO3 substrate, the local magnetization direction is determined by ferroelectric domain orientation as a consequence of growth strain, such that single-domain discs lie on single ferroelectric domains. On applying a voltage across the substrate, ferroelectric domain switching yields non-volatile magnetization rotations of 90°, while piezoelectric effects that are small and continuous yield non-volatile magnetization reversals that are non-deterministic. This demonstration of magnetization reversal without ferroelectric domain switching implies reduced fatigue, and therefore represents a step towards applications. [ABSTRACT FROM AUTHOR]

Using x-ray photoelectron emission microscopy we have observed the coexistence of ferromagnetic and antiferromagnetic phases in a (3 at%)Pd-doped FeRh epilayer. By quantitatively analyzing the resultant images we observe that as the epilayer transforms there is a change in magnetic domain symmetry from predominantly twofold at lower temperatures through to an equally weighted combination of both four and twofold symmetries at higher temperature. It is postulated that the lowered symmetry Ising-like nematic phase resides at the near-surface of the epilayer. This behavior is different to that of undoped FeRh suggesting that the variation in symmetry is driven by the competing structural and electronic interactions in the nanoscale FeRh film coupled with the effect of the chemical doping disorder. [ABSTRACT FROM AUTHOR]

The remanent domain structures of composite element magnetic barcodes have been imaged using photo-emission electron microscopy with contrast from x-ray magnetic circular dichroism (XMCD-PEEM) and analysed with reference to the results of micromagnetic simulations. The magnetisation configuration at the end of wide strips is found to be perpendicular to the majority magnetisation direction. This transitions to an incomplete rotation for nominal strip widths below 300 nm and is found to affect the mechanics of magnetisation reversal for nominal strip widths below 200 nm, owing to a difference in magnetisation orientation when an external magnetic field is applied that is just smaller than the magnetic coercivity of the structures and a corresponding change in reversal dynamics. This change in domain structure as strip width decreases is consistent with both the influence of shape anisotropy and with measurements of magnetic hysteresis. The magnetisation reversal characteristics of composite element structures are found to be dependent on the relative magnetisation configurations of neighbouring strips, which in turn are found to vary stochastically upon the application and removal of a magnetic field along the easy axis of the structure. It is found that the application of a canted field is necessary to ensure sharp, consistent magnetisation reversal of bits when writing a binary code. These results confirm that either improved lithography of narrower strips or non-rectangular elements would be necessary to further increase the number of individually programmable bits in a barcode.

Nanoscale detection and control of the magnetic order underpins a spectrum of condensed-matter research and device functionalities involving magnetism. The key principle involved is the breaking of time-reversal symmetry, which in ferromagnets is generated by an internal magnetization. However, the presence of a net magnetization limits device scalability and compatibility with phases, such as superconductors and topological insulators. Recently, altermagnetism has been proposed as a solution to these restrictions, as it shares the enabling time-reversal-symmetry-breaking characteristic of ferromagnetism, combined with the antiferromagnetic-like vanishing net magnetization 1-4 . So far, altermagnetic ordering has been inferred from spatially averaged probes 4-19 . Here we demonstrate nanoscale imaging of altermagnetic states from 100-nanometre-scale vortices and domain walls to 10-micrometre-scale single-domain states in manganese telluride (MnTe) 2,7,9,14-16,18,20,21 . We combine the time-reversal-symmetry-breaking sensitivity of X-ray magnetic circular dichroism 12 with magnetic linear dichroism and photoemission electron microscopy to achieve maps of the local altermagnetic ordering vector. A variety of spin configurations are imposed using microstructure patterning and thermal cycling in magnetic fields. The demonstrated detection and controlled formation of altermagnetic spin configurations paves the way for future experimental studies across the theoretically predicted research landscape of altermagnetism, including unconventional spin-polarization phenomena, the interplay of altermagnetism with superconducting and topological phases, and highly scalable digital and neuromorphic spintronic devices 3,14,22-24 ., Competing Interests: Competing interests: The authors declare no competing interests., (© 2024. The Author(s).)

Defects are inherent in transition metal dichalcogenides and significantly affect their chemical and physical properties. In this study, surface defect electrochemical nanopatterning is proposed as a promising method to tune in a controlled manner the electronic and functional properties of defective MoS₂ thin films. Using parallel electrochemical nanolithography, MoS₂ thin films are patterned, creating sulphur vacancy-rich active zones alternated with defect-free regions over a centimetre scale area, with sub-micrometre spatial resolution. The patterned films display tailored optical and electronic properties due to the formation of sulphur vacancy-rich areas. Moreover, the effectiveness of defect nanopatterning in tuning functional properties is demonstrated by studying the electrocatalytic activity for the hydrogen evolution reaction., (© 2024 The Author(s). Small Methods published by Wiley‐VCH GmbH.)

Avalanche resistive switching is the fundamental process that triggers the sudden change of the electrical properties in solid-state devices under the action of intense electric fields. Despite its relevance for information processing, ultrafast electronics, neuromorphic devices, resistive memories and brain-inspired computation, the nature of the local stochastic fluctuations that drive the formation of metallic regions within the insulating state has remained hidden. Here, using operando X-ray nano-imaging, we have captured the origin of resistive switching in a V 2 O 3 -based device under working conditions. V 2 O 3 is a paradigmatic Mott material, which undergoes a first-order metal-to-insulator phase transition together with a lattice transformation that breaks the threefold rotational symmetry of the rhombohedral metallic phase. We reveal a new class of volatile electronic switching triggered by nanoscale topological defects appearing in the shear-strain based order parameter that describes the insulating phase. Our results pave the way to the use of strain engineering approaches to manipulate such topological defects and achieve the full dynamical control of the electronic Mott switching. Topology-driven, reversible electronic transitions are relevant across a broad range of quantum materials, comprising transition metal oxides, chalcogenides and kagome metals., (© 2024. The Author(s).)

The nanoparticle (NP) redox state is an important parameter in the performance of cobalt-based Fischer-Tropsch synthesis (FTS) catalysts. Here, the compositional evolution of individual CoNPs (6-24 nm) in terms of the oxide vs metallic state was investigated in situ during CO/syngas treatment using spatially resolved X-ray absorption spectroscopy (XAS)/X-ray photoemission electron microscopy (X-PEEM). It was observed that in the presence of CO, smaller CoNPs (i.e., ≤12 nm in size) remained in the metallic state, whereas NPs ≥ 15 nm became partially oxidized, suggesting that the latter were more readily able to dissociate CO. In contrast, in the presence of syngas, the oxide content of NPs ≥ 15 nm reduced, while it increased in quantity in the smaller NPs; this reoxidation that occurs primarily at the surface proved to be temporary, reforming the reduced state during subsequent UHV annealing. O K-edge measurements revealed that a key parameter mitigating the redox behavior of the CoNPs were proximate oxygen vacancies (O vac ). These results demonstrate the differences in the reducibility and the reactivity of Co NP size on a Co/TiO 2 catalyst and the effect O vac have on these properties, therefore yielding a better understanding of the physicochemical properties of this popular choice of FTS catalysts., Competing Interests: The authors declare the following competing financial interest(s): Andrew M. Beale is a co-owner of Finden Ltd., a contract research organization that performs characterization studies on functional materials., (© 2023 The Authors. Published by American Chemical Society.)

Nanoscale interconnects are an important component of molecular electronics. Here we use X-ray spectromicroscopy techniques as well as scanning probe methods to explore the self-assembled growth of insulated iron nanowires as a potential means of supplying an earth abundant solution. The intrinsic anisotropy of a TiO 2 (110) substrate directs the growth of micron length iron wires at elevated temperatures, with a strong metal-support interaction giving rise to ilmenite (FeTiO 3 ) encapsulation. Iron nanoparticles that decorate the nanowires display magnetic properties that suggest other possible applications.

Devices based on arrays of interconnected magnetic nano-rings with emergent magnetization dynamics have recently been proposed for use in reservoir computing applications, but for them to be computationally useful it must be possible to optimise their dynamical responses. Here, we use a phenomenological model to demonstrate that such reservoirs can be optimised for classification tasks by tuning hyperparameters that control the scaling and input-rate of data into the system using rotating magnetic fields. We use task-independent metrics to assess the rings' computational capabilities at each set of these hyperparameters and show how these metrics correlate directly to performance in spoken and written digit recognition tasks. We then show that these metrics, and performance in tasks, can be further improved by expanding the reservoir's output to include multiple, concurrent measures of the ring arrays' magnetic states., (Creative Commons Attribution license.)

Improving both the extent of metallic Co nanoparticle (Co NP) formation and their stability is necessary to ensure good catalytic performance, particularly for Fischer-Tropsch synthesis (FTS). Here, we observe how the presence of surface oxygen vacancies (O vac ) on TiO 2 can readily reduce individual Co 3 O 4 NPs directly into CoO/Co 0 in the freshly prepared sample by using a combination of X-ray photoemission electron microscopy (X-PEEM) coupled with soft X-ray absorption spectroscopy. The O vac are particularly good at reducing the edge of the NPs as opposed to their center, leading to smaller particles being more reduced than larger ones. We then show how further reduction (and O vac consumption) is achieved during heating in H 2 /syngas (H 2 + CO) and reveal that O vac also prevents total reoxidation of Co NPs in syngas, particularly the smallest (∼8 nm) particles, thus maintaining the presence of metallic Co, potentially improving catalyst performance., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Mott transitions in real materials are first order and almost always associated with lattice distortions, both features promoting the emergence of nanotextured phases. This nanoscale self-organization creates spatially inhomogeneous regions, which can host and protect transient non-thermal electronic and lattice states triggered by light excitation. Here, we combine time-resolved X-ray microscopy with a Landau-Ginzburg functional approach for calculating the strain and electronic real-space configurations. We investigate V 2 O 3 , the archetypal Mott insulator in which nanoscale self-organization already exists in the low-temperature monoclinic phase and strongly affects the transition towards the high-temperature corundum metallic phase. Our joint experimental-theoretical approach uncovers a remarkable out-of-equilibrium phenomenon: the photo-induced stabilisation of the long sought monoclinic metal phase, which is absent at equilibrium and in homogeneous materials, but emerges as a metastable state solely when light excitation is combined with the underlying nanotexture of the monoclinic lattice., (© 2022. The Author(s).)

The interest in understanding scaling limits of magnetic textures such as domain walls spans the entire field of magnetism from its physical fundamentals to applications in information technologies. Here, we explore antiferromagnetic CuMnAs in which imaging by x-ray photoemission reveals the presence of magnetic textures down to nanoscale, reaching the detection limit of this established microscopy in antiferromagnets. We achieve atomic resolution by using differential phase-contrast imaging within aberration-corrected scanning transmission electron microscopy. We identify abrupt domain walls in the antiferromagnetic film corresponding to the Néel order reversal between two neighboring atomic planes. Our work stimulates research of magnetic textures at the ultimate atomic scale and sheds light on electrical and ultrafast optical antiferromagnetic devices with magnetic field-insensitive neuromorphic functionalities.

Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows for the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions among others. We report here on the behavior of chiral DWs at ultrashort timescale after optical pumping in perpendicularly magnetized asymmetric multilayers. The magnetization dynamics is probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously varying spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW texture shortly after the laser pulse as a distortion of the homochiral Néel shape toward a transient mixed Bloch-Néel-Bloch texture along a direction transverse to the DW., (© 2022. The Author(s).)

Efficient manipulation of antiferromagnetic (AF) domains and domain walls has opened up new avenues of research towards ultrafast, high-density spintronic devices. AF domain structures are known to be sensitive to magnetoelastic effects, but the microscopic interplay of crystalline defects, strain and magnetic ordering remains largely unknown. Here, we reveal, using photoemission electron microscopy combined with scanning X-ray diffraction imaging and micromagnetic simulations, that the AF domain structure in CuMnAs thin films is dominated by nanoscale structural twin defects. We demonstrate that microtwin defects, which develop across the entire thickness of the film and terminate on the surface as characteristic lines, determine the location and orientation of 180 ∘ and 90 ∘ domain walls. The results emphasize the crucial role of nanoscale crystalline defects in determining the AF domains and domain walls, and provide a route to optimizing device performance., (© 2022. The Author(s).)

In the quest for post-CMOS (complementary metal-oxide-semiconductor) technologies, driven by the need for improved efficiency and performance, topologically protected ferromagnetic 'whirls' such as skyrmions 1-8 and their anti-particles have shown great promise as solitonic information carriers in racetrack memory-in-logic or neuromorphic devices 1,9-11 . However, the presence of dipolar fields in ferromagnets, which restricts the formation of ultrasmall topological textures 3,6,8,9,12 , and the deleterious skyrmion Hall effect, when skyrmions are driven by spin torques 9,10,12 , have thus far inhibited their practical implementation. Antiferromagnetic analogues, which are predicted to demonstrate relativistic dynamics, fast deflection-free motion and size scaling, have recently become the subject of intense focus 9,13-19 , but they have yet to be experimentally demonstrated in natural antiferromagnetic systems. Here we realize a family of topological antiferromagnetic spin textures in α-Fe 2 O 3 -an Earth-abundant oxide insulator-capped with a platinum overlayer. By exploiting a first-order analogue of the Kibble-Zurek mechanism 20,21 , we stabilize exotic merons and antimerons (half-skyrmions) 8 and their pairs (bimerons) 16,22 , which can be erased by magnetic fields and regenerated by temperature cycling. These structures have characteristic sizes of the order of 100 nanometres and can be chemically controlled via precise tuning of the exchange and anisotropy, with pathways through which further scaling may be achieved. Driven by current-based spin torques from the heavy-metal overlayer, some of these antiferromagnetic textures could emerge as prime candidates for low-energy antiferromagnetic spintronics at room temperature 1,9-11,23 .

Using photoemission electron microscopy (PEEM) to image ferromagnetism in polycrystalline Ni disks, and ferroelectricity in their single-crystal BaTiO 3 substrates, we find that voltage-driven 90° ferroelectric domain switching serves to reversibly annihilate each magnetic vortex via uniaxial compressive strain, and that the orientation of the resulting bi-domain reveals the chirality of the annihilated vortex. Micromagnetic simulations reveal that only 60% of this strain is required for annihilation. Voltage control of magnetic vortices is novel, and should be energetically favourable with respect to the use of a magnetic field or an electrical current. In future, stray field from bi-domains could be exploited to read vortex chirality. Given that core polarity can already be read via stray field, our work represents a step towards four-state low-power memory applications.

A novel method of measuring the core level binding energies of multiple sized nanoparticles on the same substrate is demonstrated using the early stage of Au nanoparticle growth on reduced r-TiO 2 (110). This method employed in situ scanning tunneling microscopy (STM) and microfocused X-ray photoemission spectroscopy. An STM tip-shadowing method was used to synthesize patterned areas of Au nanoparticles on the substrate with different coverages and sizes. Patterns were identified and imaged using a UV photoelectron emission microscope. The Au 4f core level binding energies of the nanoparticles were investigated as a function of Au nanoparticle coverage and size. A combination of initial and final state effects modifies the binding energies of the Au 4f core levels as the nanoparticle size changes. When single Au atoms and Au 3 clusters are present, the Au 4f 7/2 binding energy, 84.42 eV, is similar to that observed at a high coverage (1.8 monolayer equivalent), resulting from a cancellation of initial and final state effects. As the coverage is increased, there is a decrease in binding energy, which then increases at a higher coverage to 84.39 eV. These results are consistent with a Volmer-Weber nucleation-growth model of Au nanoparticles at oxygen vacancies, resulting in electron transfer to the nanoparticles.

We probe the current-induced magnetic switching of insulating antiferromagnet-heavy-metal systems, by electrical spin Hall magnetoresistance measurements and direct imaging, identifying a reversal occurring by domain wall (DW) motion. We observe switching of more than one-third of the antiferromagnetic domains by the application of current pulses. Our data reveal two different magnetic switching mechanisms leading together to an efficient switching, namely, the spin-current induced effective magnetic anisotropy variation and the action of the spin torque on the DWs.

Large changes in the magnetization of ferromagnetic films can be electrically driven by non-180° ferroelectric domain switching in underlying substrates, but the shear components of the strains that mediate these magnetoelectric effects have not been considered so far. Here we reveal the presence of these shear strains in a polycrystalline film of Ni on a 0.68Pb(Mg 1/3 Nb 2/3 )O 3 -0.32PbTiO 3 substrate in the pseudo-cubic (011) pc orientation. Although vibrating sample magnetometry records giant magnetoelectric effects that are consistent with the hitherto expected 90° rotations of a global magnetic easy axis, high-resolution vector maps of magnetization (constructed from photoemission electron microscopy data, with contrast from X-ray magnetic circular dichroism) reveal that the local magnetization typically rotates through smaller angles of 62-84°. This shortfall with respect to 90° is a consequence of the shear strain associated with ferroelectric domain switching. The non-orthogonality represents both a challenge and an opportunity for the development and miniaturization of magnetoelectric devices.

Antiferromagnets have several favourable properties as active elements in spintronic devices, including ultra-fast dynamics, zero stray fields and insensitivity to external magnetic fields 1 . Tetragonal CuMnAs is a testbed system in which the antiferromagnetic order parameter can be switched reversibly at ambient conditions using electrical currents 2 . In previous experiments, orthogonal in-plane current pulses were used to induce 90° rotations of antiferromagnetic domains and demonstrate the operation of all-electrical memory bits in a multi-terminal geometry 3 . Here, we demonstrate that antiferromagnetic domain walls can be manipulated to realize stable and reproducible domain changes using only two electrical contacts. This is achieved by using the polarity of the current to switch the sign of the current-induced effective field acting on the antiferromagnetic sublattices. The resulting reversible domain and domain wall reconfigurations are imaged using X-ray magnetic linear dichroism microscopy, and can also be detected electrically. Switching by domain-wall motion can occur at much lower current densities than those needed for coherent domain switching.

The growth and reactive dewetting of ultrathin films of iron oxides supported on Re(0001) surfaces have been imaged in situ in real time. Initial growth forms a nonmagnetic stable FeO (wüstite like) layer in a commensurate network upon which high aspect ratio nanowires of several microns in length but less than 40 nm in width can be fabricated. The nanowires are closely aligned with the substrate crystallography and imaging by X-ray magnetic circular dichroism shows that each contain a single magnetic domain. The driving force for dewetting appears to be the minimization of strain energy of the Fe 3 O 4 crystallites and follows the Tersoff and Tromp model in which strain is minimized at constant height by extending in one epitaxially matched direction. Such wires are promising in spintronic applications and we predict that the growth will also occur on other hexagonal substrates.

Insertion devices are utilized at synchrotron radiation facilities around the world for their capability to provide a high-brilliance X-ray beam. APPLE-II type undulators are especially important for their capacity to switch between a variety of photon beam polarization states. A high-precision soft X-ray polarimeter has been used to investigate the polarization calibration of an APPLE-II undulator (period length λ u = 64 mm) installed on beamline I06 at Diamond Light Source. Systematic measurement of the beam polarization state at a range of linear arbitrary angles has been compared with the expected result for a given set of undulator gap and row phase parameters calculated from theory. Determination of the corresponding Stokes-Poincaré parameters from the measured data reveals a discrepancy between the two. The limited number of energy/polarization combinations included in the undulator calibration tables necessitates the use of interpolated values for the missing points which is expected to contribute to the discrepancy. However, by modifying the orbit of the electron beam through the undulator by at least 160 µm it has been found that for certain linear polarizations the discrepancies can be corrected. Overall, it is suggested that complete correction of the Stokes-Poincaré parameters for all linear angles would require alteration of both these aspects.

MnAs epitaxial thin films on GaAs(001) single crystalline substrates crystallize at room temperature (RT) in a mixture of two crystalline phases with distinct magnetic properties, organized as stripes along the MnAs [0001] direction. This particular morphology is driven by anisotropic epitaxial strain. We elucidate here the physical mechanisms at the origin of size reduction effect on the MnAs crystalline phase transition. We investigated the structural and magnetic changes in MnAs patterned microstructures (confined geometry) when the lateral dimension is reduced to values close to the periodicity and width of the stripes observed in continuous films. The effects of the microstructure's lateral size, shape and orientation (with respect to the MnAs [Formula: see text] direction) were characterized by local probe synchrotron X-ray diffraction (μ-XRD) using a focused X-ray beam, X-ray Magnetic Circular Dichroïsm - Photo Emission Electron Microscopy (XMCD-PEEM) and Low Energy Electron Microscopy (LEEM). Changes in the transition temperature and the crystalline phase distribution inside the microstructures are evidenced and quantitatively measured. The effect of finite size and strain relaxation on the magnetic domain structure is also discussed. Counter-intuitively, we demonstrate here that below a critical microstructure size, bulk MnAs structural and magnetic properties are restored. To support our observations we developed, tested and validated a model based on the size-dependence of the elastic energy and strain relaxation to explain this phase re-distribution in laterally confined geometry.

Using x-ray magnetic circular and linear dichroism techniques, we demonstrate a collinear exchange coupling between an epitaxial antiferromagnet, tetragonal CuMnAs, and an Fe surface layer. A small uncompensated Mn magnetic moment is observed which is antiparallel to the Fe magnetization. The staggered magnetization of the 5 nm thick CuMnAs layer is rotatable under small magnetic fields, due to the interlayer exchange coupling. This allows us to obtain the x-ray magnetic linear dichroism spectra for different crystalline orientations of CuMnAs in the (001) plane. This is a key parameter for enabling the understanding of domain structures in CuMnAs imaged using x-ray magnetic linear dichroism microscopy techniques.