We report an X-ray Magnetic Circular Dichroism (XMCD) study of nanostructured FeCo films prepared by depositing 2.1 nm Co gas phase nanoparticles in conjunction with atomic Fe matrices at different Co concentrations to measure the spin and orbital magnetic moments of the constituents. These films have been shown in previous studies to have a very high saturation magnetisation that exceeds the Slater-Pauling limit of 2.45 µB/atom. We show that, at the optimum concentration, the Fe atoms have a total magnetic moment of, at least, 2.64 mB/atom, while the Co atoms show a value of 2.7 mB/atom. From these quantities, the average magnetic moment per atom of the film is shown to agree with the previously reported high values determined by magnetometry. Relative to the bulk values the enhancement of the Co moment is the greatest and the Co spin moment reaches 2.31 µB/atom, which is 77% of the spin polarisation in the free atom. We also show that the enhancement of the orbital magnetic moment of Fe and Co plays a major role in the magnetisation of the samples, these being as high as 0.178 mB/atom. and 0.388 mB/atom. respectively, i.e., twice their bulk values. This work thus confirms the origin of these films’ exceptionally high saturation magnetisation, whose optimum magnetic moments per atom occur at a Co concentration close to the percolation threshold, where there is a maximum proportion of Fe/Co interface.
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
Nanostructured FeCo films comprising small (2.1 nm mean diameter) Co nanoparticles deposited into an Fe matrix are investigated by magnetometry, transmission electron microscopy and X-ray Magnetic Circular Dichroism (XMCD). Similar films were previously reported to possess a saturation magnetisation of up to 3 mu B/ atom, thus exceeding the Slater-Pauling limit by a significant margin. The present work confirms the previous findings by magnetometry and demonstrates that the Co nanoparticles maintain their particulate identity within the film while adopting the crystallographic structure of the Fe matrix. The films show no evidence for voids or porosity (they exhibit the bulk density). An important factor in the high magnetisation in the films is an enhanced magnetic moment on the Co atoms, which XMCD indicates to be at least 2.21 mu B, i.e., 30 % larger than the bulk value for metallic cobalt.
Altermagnetism is a recently identified magnetic symmetry class combining characteristics of conventional collinear ferromagnets and antiferromagnets, that were regarded as mutually exclusive, and enabling phenomena and functionalities unparalleled in either of the two traditional elementary magnetic classes. In this work we use symmetry, ab initio theory, and experiments to explore x-ray magnetic circular dichroism (XMCD) in the altermagnetic class. As a representative material for our XMCD study we choose α-MnTe with compensated antiparallel magnetic order in which an anomalous Hall effect has been already demonstrated. We predict and experimentally confirm a characteristic XMCD line shape for compensated moments lying in a plane perpendicular to the light propagation vector. Our results highlight the distinct phenomenology in altermagnets of this time-reversal symmetry breaking response, and its potential utility for element-specific spectroscopy and microscopy.
We present a spectroscopic study of the magnetic properties ofFe3-δGeTe2single crystals with varying Fe content, achieved by tuning the stoichiometry of the crystals. We carried out x-ray absorption spectroscopy and analyzed the x-ray circular magnetic dichroism spectra using the sum rules, to determine the orbital and spin magnetic moments of the materials. We find a clear reduction of the spin and orbital magnetic moment with increasing Fe deficiency. Magnetic susceptibility measurements show that the reduction in magnetization is accompanied by a reduced Curie temperature. Multiplet calculations reveal that the Fe2+state increasingly mixes with a higher valence state when the Fe deficiency is increased. This effect is correlated with the weakening of the magnetic moment. As single crystals are the base material for exfoliation processes, our results are relevant for the assembly of 2D magnetic heterostructures.
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.
The electron spin polarization on half-metallic double perovskites is usually conditioned to the ordered rock-salt arrangement of the transition-metal ions along the lattice. In this work, we investigate a polycrystalline sample of the Ca1.5La0.5MnRuO6 1 . 5 La 0 . 5 MnRuO 6 compound by employing x-ray powder diffraction, high-resolution transmission electron microscopy, x-ray absorption and magnetic circular dichroism at the Mn L 2 , 3 and Ru M 2 , 3 edges, magnetometry, electrical transport, and first-principles calculations in order to show that this is a fully disordered material exhibiting near-room-temperature ferrimagnetism and half-metallic conductivity, with significant intergrain tunneling magnetoresistance. These unprecedented results are compared to those of archetypical ordered double perovskites, and discussed in terms of the Mn and Ru valences and their orbital hybridization.
Eu$_5$In$_2$Sb$_6$ is a member of a family of orthorhombic nonsymmorphic rare-earth intermetallics that combines large localized magnetic moments and itinerant exchange with a low carrier density and perpendicular glide planes. This may result in special topological crystalline (wallpaper fermion) or axion insulating phases. Recent studies of Eu$_5$In$_2$Sb$_6$ single crystals have revealed colossal negative magnetoresistance and multiple magnetic phase transitions. Here, we clarify this ordering process using neutron scattering, resonant elastic X-ray scattering, muon spin-rotation, and magnetometry. The nonsymmorphic and multisite character of Eu$_5$In$_2$Sb$_6$ results in coplanar noncollinear magnetic structure with an Ising-like net magnetization along the $a$ axis. A reordering transition, attributable to competing ferro- and antiferromagnetic couplings, manifests as the onset of a second commensurate Fourier component. In the absence of spatially resolved probes, the experimental evidence for this low-temperature state can be interpreted either as an unusual double-$q$ structure or in a phase separation scenario. The net magnetization produces variable anisotropic hysteretic effects which also couple to charge transport. The implied potential for functional domain physics and topological transport suggests that this structural family may be a promising platform to implement concepts of topological antiferromagnetic spintronics.
Antiferromagnets (AFMs) are promising for future spintronic applications because of their fast dynamics and lack of stray fields. For the required switching of the Néel vector (staggered magnetization), a current induced bulk Néel spin-orbit torque (NSOT) is most promising. Here we demonstrate current pulse induced complete, remanent, and reversible Néel vector switching of epitaxial Mn2Au(001) thin films. A current polarity dependence demonstrates an NSOT acting on AFM domain walls. We correlate direct imaging of the Néel vector reorientation by x-ray photoemission electron microscopy with measurements of the associated anisotropic magnetoresistance [1].
Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO6 octahedral rotations throughout LaCoO3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO3 films while suggesting potential applications toward low-power spintronic devices.
Here, we report on the structural, electronic, and magnetic properties of a polycrystalline sample of the LaCaCoIrO6 double-perovskite investigated by means of synchrotron x-ray powder diffraction, x-ray absorption spectroscopy, and x-ray magnetic circular dichroism at the Co and Ir L23 edges, magnetometry, and electrical transport. Our results indicate a configuration of nearly Co2+/Ir5+ configuration for the transition-metal ions, with spin canting within the Co antiferromagnetic superstructure responsible for the ferromagnetic-like behavior observed below 100 K. The highly insulating character of LaCaCoIrO6 and its positive magnetoresistance further suggest that this antiferromagnetic superexchange interaction occurs through an indirect hybridization between the Co eg orbitals.
The recent prediction that honeycomb lattices of Co2+ (3d7) ions could host dominant Kitaev interactions provides an exciting direction for exploration of new routes to stabilizing Kitaev's quantum spin liquid in real materials. Na3Co2SbO6 has been singled out as a potential material candidate provided that spin and orbital moments couple into a Jeff = 12 ground state, and that the relative strength of trigonal crystal field and spin-orbit coupling acting on Co ions can be tailored. Using x-ray linear dichroism (XLD) and x-ray magnetic circular dichroism (XMCD) experiments, alongside configuration interaction calculations, we confirm the counterintuitive positive sign of the trigonal crystal field acting on Co2+ ions and test the validity of the Jeff = 12 description of the electronic ground state. The results lend experimental support to recent theoretical predictions that a compression (elongation) of CoO6 octahedra along (perpendicular to) the trigonal axis would drive this cobaltate toward the Kitaev limit, assuming the Jeff = 12 character of the electronic ground state is preserved.
Current pulse driven Néel vector rotation in metallic antiferromagnets is one of the most promising concepts in antiferromagnetic spintronics. We show microscopically that the Néel vector of epitaxial thin films of the prototypical compound Mn 2 Au can be reoriented reversibly in the complete area of cross shaped device structures using single current pulses. The resulting domain pattern with aligned staggered magnetization is long term stable enabling memory applications. We achieve this switching with low heating of ≈20 K, which is promising regarding fast and efficient devices without the need for thermal activation. Current polarity dependent reversible domain wall motion demonstrates a Néel spin-orbit torque acting on the domain walls.
The layered-ruthenate family of materials possess an intricate interplay of structural, electronic and magnetic degrees of freedom that yields a plethora of delicately balanced ground states. This is exemplified by Ca3Ru2O7, which hosts a coupled transition in which the lattice parameters jump, the Fermi surface partially gaps and the spins undergo a 90∘ in-plane reorientation. Here, we show how the transition is driven by a lattice strain that tunes the electronic bandwidth. We apply uniaxial stress to single crystals of Ca3Ru2O7, using neutron and resonant x-ray scattering to simultaneously probe the structural and magnetic responses. These measurements demonstrate that the transition can be driven by externally induced strain, stimulating the development of a theoretical model in which an internal strain is generated self-consistently to lower the electronic energy. We understand the strain to act by modifying tilts and rotations of the RuO6 octahedra, which directly influences the nearest-neighbour hopping. Our results offer a blueprint for uncovering the driving force behind coupled phase transitions, as well as a route to controlling them.
Here we present a detailed investigation of the Co and Ir local electronic structures in La1.5A0.5CoIrO6 (A = Ba, Ca) compounds in order to unravel the orbital hybridization mechanism in these CoIr-based double perovskites. Our results of x-ray powder diffraction, ac and dc magnetization, Co and Ir L2,3-edge and Co K-edge x-ray absorption spectroscopy and x-ray magnetic circular dichroism suggest a competition between magnetic interactions. A dominant antiferromagnetic coupling is found to be responsible for the ferrimagnetic behavior observed for A = Ca below & SIM;96 K, the competing magnetic phases, and the cationic disorder in this compound giving rise to a spin-glass state at low temperatures. For the A = Ba, on the other hand, there is no evidence of long-range order down to its spin-glass transition temperature. The remarkably different magnetic properties observed between these two compounds are discussed in terms of the structural distortion that alters the strength of the Co-Ir couplings, with a relevant role played by the Co 3d eg-Ir 5d jeff = 1/2 hybridization.
Using the element and orbital selectivity of x-ray absorption spectroscopy at Eu and Pt L-3 edges we investigate the effects of the lattice contraction, induced by temperature and external pressure, on the magnetic and electronic properties of the EuPt2Si2 system. Our findings point to a clear relationship between the volume and the Eu valence in this material. From XANES experiments as a function of pressure we show that the Europium valence tends to stabilize at 3+ for pressures up to 27 GPa. The XMCD results demonstrate that pressure induced valence change of the Europium ion leads to a suppression of the magnetic ordering of the material. Altogether our results provide direct evidence that Eu-4f/5d electronic hybridization effects underlie the mechanism that regulates the valence and magnetic ordering in this material.
Strain engineering of epitaxial transition metal oxide heterostructures offers an intriguing opportunity to control electronic structures by modifying the interplay between spin, charge, orbital, and lattice degrees of freedom. Here, we demonstrate that the electronic structure, magnetic and transport properties of La0.9Ba0.1MnO3 thin films can be effectively controlled by epitaxial strain. Spectroscopic studies and first-principles calculations reveal that the orbital occupancy in Mn e(g) orbitals can be switched from the d(3z2-r2) orbital to the d(x2-y2) orbital by varying the strain from compressive to tensile. The change of orbital occupancy associated with Mn 3d-O 2p hybridization leads to dramatic modulation of the magnetic and electronic properties of strained La0.9Ba0.1MnO3 thin films. Under moderate tensile strain, an emergent ferromagnetic insulating state with an enhanced ferromagnetic Curie temperature of 215 K is achieved. These findings not only deepen our understanding of electronic structures, magnetic and transport properties in the La0.9Ba0.1MnO3 system, but also demonstrate the use of epitaxial strain as an effective knob to tune the electronic structures and related physical properties for potential spintronic device applications.
Transparent conducting oxides have become ubiquitous in modern optoelectronics. However, the number of oxides that are transparent to visible light and have the metallic-like conductivity necessary for applications is limited to a handful of systems that have been known for the past 40 years. In this work, we use hybrid density functional theory and defect chemistry analysis to demonstrate that tri-rutile zinc antimonate, ZnSb2O6, is an ideal transparent conducting oxide and to identify gallium as the optimal dopant to yield high conductivity and transparency. To validate our computational predictions, we have synthesized both powder samples and single crystals of Ga-doped ZnSb2O6 which conclusively show behavior consistent with a degenerate transparent conducting oxide. This study demonstrates the possibility of a family of Sb(V)-containing oxides for transparent conducting oxide and power electronics applications.
Crystal geometry can greatly influence the emergent properties of quantum materials. As an example, the kagome lattice is an ideal platform to study the rich interplay between topology, magnetism, and electronic correlation. In this work, combining high-resolution angle-resolved photoemission spectroscopy and ab-initio calculation, we systematically investigate the electronic structure of XMn6Sn6 (X = Dy, Tb, Gd, Y) family compounds. We observe the Dirac fermion and the flat band arising from the magnetic kagome lattice of Mn atoms. Interestingly, the flat band locates in the same energy region in all compounds studied, regardless of their different magnetic ground states and 4f electronic configurations. These observations suggest a robust Mn magnetic kagome lattice across the XMn6Sn6 family, thus providing an ideal platform for the search and investigation on new emergent phenomena in magnetic topological materials.
C. D. Dashwood , A. Geondzhian, J. G. Vale, A. C. Pakpour-Tabrizi, C. A. Howard , Q. Faure, L. S. I. Veiga, D. Meyers, S. G. Chiuzbăian , A. Nicolaou , N. Jaouen , R. B. Jackman , A. Nag , M. García-Fernández, Ke-Jin Zhou, A. C. Walters , K. Gilmore , D. F. McMorrow, and M. P. M. Dean 5,† London Centre for Nanotechnology and Department of Physics and Astronomy, University College London, London, WC1E 6BT, United Kingdom Max Planck POSTECH/KOREA Research Initiative, 37673 Pohang, South Korea Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany London Centre for Nanotechnology and Department of Electronic and Electrical Engineering, University College London, London, WC1E 6BT, United Kingdom Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory, Upton, New York 11973, USA Department of Physics, Oklahoma State University, Stillwater, Oklahoma 74078, USA Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, B.P. 48, 91192 Gif-sur-Yvette, France Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matiére et Rayonnement, UMR 7614, 4 place Jussieu, 75252 Paris Cedex 05, France Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, United Kingdom Physics Department and IRIS Adlershof, Humboldt-Universität zu Berlin, Zum Großen Windkanal 2, 12489 Berlin, Germany European Theoretical Spectroscopy Facility (ETSF)