Altermagnets are an emerging class of collinear antiferromagnets that exhibit unconventional spin-polarised electronic bands, potentially unlocking new functionalities that do not rely on spin-orbit coupling (SOC). Experimental signatures traditionally associated with spin polarisation, like X-ray magnetic circular dichroism (XMCD), are thus being used as a validation of altermagnetism. However, unlike altermagnetic spin-splitting, these responses require SOC and are not invariant under spin-space rotations. This brings into question the extent to which they can be considered direct signatures of altermagnetism. Here, we exploit the g-wave altermagnet α-Fe_2O_3 to demonstrate that XMCD is governed precisely by the spin-direction-induced symmetry breaking that altermagnetic spin groups are designed to ignore. Strikingly, the XMCD is highly anisotropic and is decoupled from the weak magnetic canting. We show that this anomalous XMCD can be described by on-site Faraday tensors capturing the locally uncompensated spin-orbital anisotropies - a scenario that can be applied to other altermagnets. Leveraging this, we reconstruct complete vectorial maps of nanoscale textures in α-Fe_2O_3 thin films, including domain walls and topological solitons, which are promising for building future spintronics and magnonics devices.
Topological insulators and skyrmion-hosting, chiral magnetic multilayers are two well-explored areas of modern condensed matter physics, each offering unique advantages for spintronics applications. In this paper, we demonstrate the optimization process for the growth of a Bi_2Se_3/buffer/[Pt/CoB/Ru]_× N heterostructure that combines these two material classes: the Bi_2Se_3 epilayer was grown by molecular beam epitaxy before transfer under ultrahigh vacuum to a separate growth chamber where the polycrystalline metallic multilayer was sputter deposited. The structure of the samples was characterized by co-fitted X-ray and polarized neutron reflectometry measurements and scanning transmission electron microscopy. Polarized neutron models and standard magnetometry show that a buffer layer exceeding a critical thickness is required to obtain the desired uniform, perpendicular magnetic anisotropy in every magnetic layer in the multilayer. Samples with both Ta and Mo buffers were used requiring thicknesses of 1.5 and 0.9 nm respectively. In minimizing the Bi_2Se_3 terracing, buffered samples yield well-defined, out-of-plane, magnetic domains suitable for spin-orbit torque induced manipulation as determined by X-ray photoemission electron microscopy.
Excitons are primary elementary excitations in solids that present both fundamental interest and technological importance, showing great potential for photospintronic and quantum transduction applications. The emerging coherent collective excitations in two-dimensional antiferromagnetic semiconductors raise prospects for spin-exciton interactions and multifield control schemes. However, realizing the arbitrary manipulation of excitonic quantum states, while preserving the inherent dynamic and response advantages of antiferromagnetic nature remains challenging. Here we achieve bidirectional modulation of the CrSBr exciton energy via interfacial interaction-modified spin-exciton coupling in a CrSBr/Fe3GaTe2 heterostructure. Compared with pristine CrSBr, the photoluminescence peaks in the heterostructure can exhibit blueshift and redshift corresponding to 6.1% and 8.6% of the total bandwidth, respectively. We reveal that the interfacial charge-transfer-driven magnetic coupling in the heterostructure effectively enhances the magnetic anisotropy and the exchange interaction of CrSBr, thereby stabilizing its antiferromagnetic spin configuration, suppressing interlayer electron-hole recombination, and ultimately leading to an anomalous blueshift of the exciton emission. Our findings demonstrate an approach for bidirectionally modulating exciton energy in two-dimensional antiferromagnetic semiconductors, which provides substantial flexibility in device design and offers an avenue for potential wavelength control in quantum information and optoelectronic technologies.
Rare-earth iron garnet (RE3Fe5O12) films are promising insulating ferrimagnets. They can show low magnetic damping, perpendicular magnetic anisotropy, and ultrafast spin dynamics, which makes them ideal for spin transport applications. In this work, we investigate the interaction between the magnetic sublattices in Er3Fe5O12 thin films grown by pulsed laser deposition on a Gd3Ga5O12 substrate. Structural and magnetic characterization reveals high-quality single-crystal growth, with a compensation temperature close to the reported bulk value (similar to 80 K). Magnetic phase diagrams based on element-specific measurements map out the regions where ferrimagnetic, canted, and aligned phases are stable across the compensation temperature. The micromagnetic dynamics resulting from perpendicular magnetic pulse perturbation of an in-plane magnetized layer was investigated at room temperature and revealed complex configurations. These results are key features for modulating magnetization dynamics through the compensation phenomenon, which is essential for spin-based devices operating in a low-temperature regime.
We describe “RingSim,” a phenomenological agent-based model that allows numerical simulation of magnetic nanowire networks with areas of hundreds of micrometers squared for durations of hundreds of seconds, a practical impossibility for general-purpose micromagnetic simulation tools. In RingSim, domain walls (DWs) are instanced as mobile agents, which respond to external magnetic fields, and their stochastic interactions with pinning sites and other DWs are described via simple phenomenological rules. We first present a detailed description of the model and its algorithmic implementation for simulating the behaviors of arrays of interconnected ring-shaped nanowires, which have previously been proposed as hardware platforms for unconventional computing applications. The model is then validated against a series of experimental measurements of an array’s static and dynamic responses to rotating magnetic fields. The robust agreement between the modeled and experimental data demonstrates that agent-based modeling is a powerful tool for exploring mesoscale magnetic devices, enabling time scales and device sizes that are inaccessible to more conventional magnetic simulation techniques.
Antiferromagnets are promising candidates for ultrafast spintronic applications, leveraging current-induced spin-orbit torques. However, experimentally distinguishing between different switching mechanisms of the staggered magnetization (Néel vector) driven by current pulses remains a challenge. In an exemplary study of the collinear antiferromagnetic compound Mn_2Au, we demonstrate that slower thermomagnetoelastic effects predominantly govern switching over a wide parameter range. In the regime of short current pulses in the nanosecond range, however, we observe fully Néel spin-orbit torque driven switching. We show that this ultrafast mechanism enables the complete directional alignment of the Néel vector by current pulses in device structures.
The elastic degree of freedom is widely exploited to mediate magnetoelectric coupling between ferromagnetic films and ferroelectric substrates. For epitaxial Fe films grown on clean BaTiO3 substrates, shear strain can determine the underlying magnetoelastic coupling. Here, we use PhotoEmission Electron Microscopy of ferroic Fe and BaTiO3 domains, combined with micromagnetic simulations, to directly reveal an inverted interfacial magnetoelastic coupling in the low-dimensional limit. We show that the magnetocrystalline anisotropy competes with the epitaxial shear strain to align the local magnetization of ultrathin Fe films close to the local polarization direction of the ferroelectric BaTiO3 in-plane domains. Poling the BaTiO3 substrate creates c-domains with no shear strain contribution with the local magnetization rotated by ~45°. Tuning shear strain magnetoelastic contributions suggests new routes for designing magnetoelectric devices.
Photoemission electron microscopy (PEEM) offers a potential third modality for large-volume connectomics alongside transmission electron microscopy (TEM) and scanning electron microscopy (SEM). We image osmium stained, ultrathin brain sections on gold coated silicon at synaptic resolution using commercial PEEMs. At coarser resolution, we demonstrate that ultraviolet laser illumination enables gigavoxel-per-second acquisition rates without thermal damage. PEEM combines TEM-like parallel detection with SEM-compatible solid supports into a potentially scalable and cost-effective approach for large-volume connectomes.
In the growing field of spintronic devices incorporating antiferromagnetic materials, control of the domain configuration and Néel axis orientation is critical for technological implementations. Here we show by X-ray magnetic linear dichroism in photoelectron emission microscopy how antiferromagnetic properties of LaFeO3 (LFO) thin films can be tailored through epitaxial strain. LFO films were grown via molecular beam epitaxy with precise stoichiometric control, using substrates that span a range of strain states—from compressive to tensile—and crystal symmetries, including different crystallographic orientations. First, we show that epitaxial strain dictates the Néel axis orientation, shifting it from completely in-plane under compressive strain to completely out-of-plane under tensile strain, regardless of the substrate crystal symmetry. Second, we find that LFO films grown on cubic substrates exhibit a fourfold distribution of antiferromagnetic domains, but can be controlled by varying the substrate miscut, while those on orthorhombic substrates, regardless of strain state, form large-scale monodomains, a highly desirable feature for spintronic applications. Precise control over antiferromagnetic domain configurations and Néel axis orientation is essential for technological advancement of spintronic devices. Here, the authors use epitaxial strain to tailor the magnetic properties of LaFeO3 thin films, demonstrating a crystal engineering approach which may have much wider applicability.
Antiferromagnets (AFs) are characterized by spin structures that are resistant to external magnetic fields, rendering them ideal for persistent information storage but challenging to control. This study demonstrates that a thin ferromagnetic adlayer can serve as a magnetic ‘lever’ to provide a strong handle on the spin texture of an adjacent antiferromagnet. In bilayers composed of NiO(001) and Co, the expected exchange bias effect—a unidirectional shift in the Co hysteresis due to coupling with NiO—is notably absent. Instead, a strong interfacial coupling is observed, causing the NiO to partially follow the magnetization of Co under an applied magnetic field. Using x-ray magnetic linear dichroism, we detect an inversion of dichroism, indicating a reorientation of the Néel vector in NiO. X-ray spectromicroscopy imaging further reveals a direct correlation between ferromagnetic and antiferromagnetic domain structures. These findings are explained using a toy model that distinguishes between stable and unstable AF domains, highlighting the dynamic interplay between NiO and the Co adlayer in the presence of a magnetic field. Published by the American Physical Society 2025
Few-layer flakes of ferromagnetic Fe5-xGeTe2 with x = 0.3 (F5GT) possess a c-axis magnetocrystalline anisotropy that is large enough below ∼200 K to outcompete the easy-plane shape anisotropy, yielding distinctive magnetic microstructures with out-of-plane (OOP) magnetizations. Using photoemission electron microscopy (PEEM) with magnetic contrast from X-ray magnetic circular dichroism (XMCD) to study a thermally demagnetized h-BN-protected nanoflake of F5GT at 110 K, we observe a micron-scale coexistence between domains with OOP magnetizations (∼70% areal fraction) and hitherto unknown domains in which in-plane (IP) magnetization components dominate (∼30% areal fraction). The regions with dominant IP magnetization components do not correlate with small variations of flake thickness (6-10 nm) and instead arise from local changes of magnetocrystalline anisotropy due to a hitherto unidentified chemical inhomogeneity that we suggest to be a higher concentration of Fe vacancies. Our observation of micron-scale inhomogeneity would likely be missed if imaging a single flake orientation and should affect the viability and performance of van der Waals (vdW) spintronic devices with F5GT electrodes.
The van der Waals interaction enables atomically thin layers of exfoliated 2D materials to be interfaced in heterostructures with relaxed epitaxy conditions, however, the ability to exfoliate and freely stack layers without any strain or structural modification is by no means ubiquitous. In this work, the piezoelectricity of the exfoliated van der Waals piezoelectric alpha-In2Se3 is utilized to modify the magnetic properties of exfoliated Fe3GeTe2, a van der Waals ferromagnet, resulting in increased domain wall density, reductions in the transition temperature ranging from 5 to 20 K, and an increase in the magnetic coercivity. Structural modifications at the atomic level are corroborated by a comparison to a graphite/alpha-In2Se3 heterostructure, for which a decrease in the Tuinstra-Koenig ratio is found. Magnetostrictive ferromagnetic domains are also observed, which may contribute to the enhanced magnetic coercivity. Density functional theory calculations and atomistic spin dynamic simulations show that the Fe3GeTe2 layer is compressively strained by 0.4%, reducing the exchange stiffness and magnetic anisotropy. The incorporation of alpha-In2Se3 may be a general strategy to electrostatically strain interfaces within the paradigm of hexagonal boron nitride-encapsulated heterostructures, for which the atomic flatness is both an intrinsic property and paramount requirement for 2D van der Waals heterojunctions. This study focuses on the captivating interplay between the ferromagnetic Fe3GeTe2 and the piezoelectric alpha-In2Se3, both 2D van der Waals (vdW) materials. Strained heterojunctions exhibit several compelling transformations: increased domain density, reduced Curie temperature, and emergent magnetostrictive ferromagnetic domains. Using alpha-In2Se3 is a versatile approach to strain-tune vdW materials, including graphite and Te based vdW chalcogenides. image
The intermetallic compound ZnPd has been found to have desirable characteristics as a catalyst for the steam reforming of methanol. The understanding of the surface structure of ZnPd is important to optimize its catalytic behavior. However, due to the lack of bulk single-crystal samples and the complexity of characterizing surface properties in the available polycrystalline samples using common experimental techniques, all previous surface science studies of this compound have been performed on surface alloy samples formed through thin-film deposition. In this study, we present findings on the chemical and atomic structure of the surfaces of bulk polycrystalline ZnPd studied by a variety of complementary experimental techniques, including scanning tunneling microscopy (STM), x-ray photoelectron spectroscopy (XPS), low energy electron microscopy (LEEM), photoemission electron microscopy (PEEM), and microspot low-energy electron diffraction (mu -LEED). These experimental techniques, combined with density functional theory (DFT)-based thermodynamic calculations of surface free energy and detachment kinetics at the step edges, confirm that surfaces terminated by atomic layers composed of both Zn and Pd atoms are more stable than those terminated by only Zn or Pd layers. DFT calculations also demonstrate that the primary contribution to the tunneling current arises from Pd atoms, in agreement with the STM results. The formation of intermetallics at surfaces may contribute to the superior catalyst properties of ZnPd over Zn or Pd elemental counterparts.
In synthetic antiferromagnets (SAFs), antiferromagnetic (AFM) order and synthesis using conventional sputtering techniques is combined to produce systems that are advantageous for spintronics applications. Here we present the preparation and study of SAF multilayers possessing both perpendicular magnetic anisotropy and the Dzyaloshinskii-Moriya interaction. The multilayers have an antiferromagnetically aligned ground state but can be forced into a full ferromagnetic (FM) alignment by applying an out-of-plane field -100 mT. We study the spin textures in these multilayers in their ground state as well as around the transition point between the AFM and FM states at fields - 40 mT by imaging the spin textures using complementary methods: photoemission electron, magnetic force, and Lorentz transmission electron microscopies. The transformation into a FM state by field proceeds by a nucleation and growth process, where skyrmionic nuclei form and then broaden into regions containing a ferromagnetically aligned labyrinth pattern that eventually occupies the whole film. Remarkably, this process occurs without any significant change in the net magnetic moment of the multilayer. The mix of antiferromagnetically and ferromagnetically aligned regions on the micron scale in the middle of this transition is reminiscent of a first-order phase transition that exhibits phase coexistence. These results are important for guiding the design of spintronic devices whose operation is based on spin textures in perpendicularly magnetized SAFs.
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 magnetization1-4. So far, altermagnetic ordering has been inferred from spatially averaged probes4-19. 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 dichroism12 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 devices3,14,22-24.
Antiferromagnetic materials hold potential for use in spintronic devices with fast operation frequencies and field robustness. Despite the rapid progress in proof-of-principle functionality in recent years, there has been a notable lack of understanding of antiferromagnetic domain formation and manipulation, which translates to either incomplete or non-scalable control of the magnetic order. Here, we demonstrate simple and functional ways of influencing the domain structure in CuMnAs and Mn2Au, two key materials of antiferromagnetic spintronics research, using device patterning and strain engineering. Comparing x-ray microscopy data from two different materials, we reveal the key parameters dictating domain formation in antiferromagnetic devices and show how the non-trivial interaction of magnetostriction, substrate clamping and edge anisotropy leads to specific equilibrium domain configurations. More specifically, we observe that patterned edges have a significant impact on the magnetic anisotropy and domain structure over long distances, and we propose a theoretical model that relates short-range edge anisotropy and long-range magnetoelastic interactions. The principles invoked are of general applicability to the domain formation and engineering in antiferromagnetic thin films at large, which will pave the way towards realizing truly functional antiferromagnetic devices.
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 nuclei out of the insulating state has remained hidden. Here, using operando X-ray nano-imaging, we have captured the early-stages of resistive switching in a V2O3-based device under working conditions. V2O3 is a paradigmatic Mott material, which undergoes a first-order metal-to-insulator transition coupled to a lattice transformation that breaks the threefold rotational symmetry of the rhombohedral metal phase. We reveal a new class of volatile electronic switching triggered by nanoscale topological defects of the lattice order parameter of the insulating phase. Our results pave the way to the use of strain engineering approaches to manipulate topological defects and achieve the full control of the electronic Mott switching. The concept of topology-driven reversible electronic transition is of interest for a broad class of quantum materials, comprising transition metal oxides, chalcogenides and kagome metals, that exhibit first-order electronic transitions coupled to a symmetry-breaking order.
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.
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 (Ovac). These results demonstrate the differences in the reducibility and the reactivity of Co NP size on a Co/TiO2 catalyst and the effect Ovac have on these properties, therefore yielding a better understanding of the physicochemical properties of this popular choice of FTS catalysts.
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.