Dipolar skyrmions and antiskyrmions of arbitrary topological charge at room temperature.

Magnetic skyrmions are localized, stable topological magnetic textures that can move and interact with each other like ordinary particles when an external stimulus is applied. The efficient control of the motion of spin textures using spin-polarized currents opened an opportunity for skyrmionic devices such as racetrack memory and neuromorphic or reservoir computing. The coexistence of skyrmions with high topological charge in the same system promises further possibilities for efficient technological applications. In this work, we directly observe dipolar skyrmions and antiskyrmions with arbitrary topological charge in Co/Ni multilayers at room temperature. We explore the dipolar-stabilized spin objects with topological charges of up to 10 and characterize their nucleation process, their energy dependence on the topological charge and the effect of the material parameters on their stability. Furthermore, our micromagnetic simulations demonstrate spin-transfer-induced motion of these spin objects, which is important for their potential device application.

Size-dependent bistability of magnetic states in soft magnetic cap arrays.

We have investigated the size dependent energy barrier regarding the transition between magnetic vortex and collinear states in dense arrays of magnetic cap structures hosting magnetic vortices. The cap structures were formed by the deposition of soft magnetic thin films on top of large arrays of densely packed polystyrene spheres. The energy barrier associated with the magnetic field assisted switching from a collinear magnetic state to a non-uniform vortex state (or vice versa) was tuned by tailoring the diameter and thickness of the soft magnetic caps. At a sufficient temperature, known as the bifurcation temperature, the thermal energy overcomes this energy barrier and magnetic bistability with a hysteresis-free switching occurs between the two magnetic states. In magnetic caps with a fixed thickness, the bifurcation temperature decreases with increasing cap diameter. On the other hand, for a fixed diameter, the bifurcation temperature increases with an increase in film thickness of the cap structure. This study demonstrates that the bifurcation temperature can be easily tailored by changing the magnetostatic energy contribution which in turn affects the energy barrier and thus the magnetic bistability.

Temperature Evolution of Magnon Propagation Length in Tm3Fe5O12 Thin Films: Roles of Magnetic Anisotropy and Gilbert Damping.

The magnon propagation length, ⟨ξ⟩, of a ferro-/ferrimagnet (FM) is one of the key factors that controls the generation and propagation of thermally driven magnonic spin current in FM/heavy metal (HM) bilayer based spincaloritronic devices. For the development of a complete physical picture of thermally driven magnon transport in FM/HM bilayers over a wide temperature range, it is of utmost importance to understand the respective roles of temperature-dependent Gilbert damping (α) and effective magnetic anisotropy (Keff) in controlling the temperature evolution of ⟨ξ⟩. Here, we report a comprehensive investigation of the temperature-dependent longitudinal spin Seebeck effect (LSSE), radio frequency transverse susceptibility, and broad-band ferromagnetic resonance measurements on Tm3Fe5O12 (TmIG)/Pt bilayers grown on different substrates. We observe a significant drop in the LSSE voltage below 200 K independent of TmIG film thickness and substrate choice. This is attributed to the noticeable increases in effective magnetic anisotropy field, HKeff (∝Keff) and α that occur within the same temperature range. From the TmIG thickness dependence of the LSSE voltage, we determined the temperature dependence of ⟨ξ⟩ and highlighted its correlation with the temperature-dependent HKeff and α in TmIG/Pt bilayers, which will be beneficial for the development of rare-earth iron garnet based efficient spincaloritronic nanodevices.

Thin-Film Heterostructures Based on Co/Ni Synthetic Antiferromagnets on Polymer Tapes: Toward Sustainable Flexible Spintronics.

Synthetic antiferromagnets with perpendicular magnetic anisotropy (PMA-SAFs) have gained growing attention for both conventional and next-generation spin-based technologies. While the progress of PMA-SAF spintronic devices on rigid substrates has been remarkable, only few examples of flexible thin-film heterostructures are reported in the literature, all containing platinum group metals (PGMs). Systems based on Co/Ni may offer additional advantages with respect to devices containing PGMs, i.e., low damping and high spin polarization. Moreover, limiting the use of PGMs may relieve the demand for critical raw materials and reduce the environmental impact of related technologies, thus contributing to the transition toward a more sustainable future. Here, we discuss for the first time the realization of Co/Ni-based PMA-SAFs on polymer tapes and exploit it to obtain flexible giant magneto-resistive spin valves (GMR-SVs) with perpendicular magnetic anisotropy. Several combinations of buffer and capping layers (i.e., Pt, Pd, and Cu/Ta) are also investigated. High-quality flexible SAFs with a fully compensated antiferromagnetic region and SVs with a sizable GMR ratio (up to 4.4%), in line with the values reported in the literature for similar systems on rigid substrates, were obtained in all cases. However, we demonstrate that PGMs allows achieving the best results when used as a buffer layer, while Cu is the best choice as a capping layer to optimize the properties of the stacks. We justify the role of buffer and capping layers in terms of different interdiffusion mechanisms occurring at the interface between the metallic layers. These results, along with the high robustness of the samples' properties against bending (up to 180°), indicate that complex and bendable Co/Ni-based heterostructures with reduced content of PGMs can be obtained on flexible tapes, allowing for the development of novel flexible and sustainable spintronic devices for applications in many fields including wearable electronics, soft robotics, and biomedicine.

High-Performance Broadband Faraday Rotation Spectroscopy of 2D Materials and Thin Magnetic Films.

A Faraday rotation spectroscopy (FRS) technique is presented for measurements on the micrometer scale. Spectral acquisition speeds of about two orders of magnitude faster than state-of-the-art modulation spectroscopy setups are demonstrated. The experimental method is based on charge-coupled-device detection, avoiding speed-limiting components, such as polarization modulators with lock-in amplifiers. At the same time, FRS spectra are obtained with a sensitivity of 20 µrad ( 0.001 ° \[0.001{\bm{^\circ }}\] ) over a broad spectral range (525-800 nm), which is on par with state-of-the-art polarization-modulation techniques. The new measurement and analysis technique also automatically cancels unwanted Faraday rotation backgrounds. Using the setup, Faraday rotation spectroscopy of excitons is performed in a hexagonal boron nitride-encapsulated atomically thin semiconductor WS2 under magnetic fields of up to 1.4 T at room temperature and liquid helium temperature. An exciton g-factor of -4.4 ± 0.3 is determined at room temperature, and -4.2 ± 0.2 at liquid helium temperature. In addition, FRS and hysteresis loop measurements are performed on a 20 nm thick film of an amorphous magnetic Tb20 Fe80 alloy.

Disclosing the Nature of Asymmetric Interface Magnetism in Co/Pt Multilayers.

Nowadays, a wide number of applications based on magnetic materials rely on the properties arising at the interface between different layers in complex heterostructures engineered at the nanoscale. In ferromagnetic/heavy metal multilayers, such as the [Co/Pt]N and [Co/Pd]N systems, the magnetic proximity effect was demonstrated to be asymmetric, thus inducing a magnetic moment on the Pt (Pd) layer that is typically higher at the top Co/Pt(Pd) interface. In this work, advanced spectroscopic and imaging techniques were combined with theoretical approaches to clarify the origin of this asymmetry both in Co/Pt trilayers and, for the first time, in multilayer systems that are more relevant for practical applications. The different magnetic moment induced at the Co/Pt interfaces was correlated to the microstructural features that are in turn affected by the growth processes that induce a different intermixing during the film deposition, thus influencing the interface magnetic profile.

Influence of magnetic domain walls on all-optical magnetic toggle switching in a ferrimagnetic GdFe film.

We present a microscopic magnetic domain imaging study of single-shot all-optical magnetic toggle switching of a ferrimagnetic Gd26Fe74 film with out-of-plane easy axis of magnetization by X-ray magnetic circular dichroism photoelectron emission microscopy. Individual linearly polarized laser pulses of 800 nm wavelength and 100 fs duration above a certain threshold fluence reverse the sample magnetization, independent of the magnetization direction, the so-called toggle switching. Local deviations from this deterministic behavior close to magnetic domain walls are studied in detail. Reasons for nondeterministic toggle switching are related to extrinsic effects, caused by pulse-to-pulse variations of the exciting laser system, and to intrinsic effects related to the magnetic domain structure of the sample. The latter are, on the one hand, caused by magnetic domain wall elasticity, which leads to a reduction of the domain-wall length at features with sharp tips. These features appear after the optical switching at positions where the line of constant threshold fluence in the Gaussian footprint of the laser pulse comes close to an already existing domain wall. On the other hand, we identify the presence of laser-induced domain-wall motion in the toggle-switching event as a further cause for local deviations from purely deterministic toggle switching.

Highly Tunable Magnetic and Magnetotransport Properties of Exchange Coupled Ferromagnet/Antiferromagnet-Based Heterostructures.

Antiferromagnets (AFMs) with zero net magnetization are proposed as active elements in future spintronic devices. Depending on the critical film thickness and measurement temperature, bimetallic Mn-based alloys and transition-metal oxide-based AFMs can host various coexisting ordered, disordered, and frustrated AFM phases. Such coexisting phases in the exchange coupled ferromagnetic (FM)/AFM-based heterostructures can result in unusual magnetic and magnetotransport phenomena. Here, we integrate chemically disordered AFM γ-IrMn3 thin films with coexisting AFM phases into complex exchange coupled MgO(001)/γ-Ni3Fe/γ-IrMn3/γ-Ni3Fe/CoO heterostructures and study the structural, magnetic, and magnetotransport properties in various magnetic field cooling states. In particular, we unveil the impact of rotating the relative orientation of the thermally disordered and reversible AFM moments with respect to the irreversible AFM moments on the magnetic and magnetotransport properties of the exchange coupled heterostructures. We further reveal that the persistence of thermally disordered and reversible AFM moments is crucial for achieving highly tunable magnetic properties and multilevel magnetoresistance states. We anticipate that the presented approach and the heterostructure architecture can be utilized in future spintronic devices to manipulate the thermally disordered and reversible AFM moments at the nanoscale.

Ultrafast high-harmonic nanoscopy of magnetization dynamics.

Light-induced magnetization changes, such as all-optical switching, skyrmion nucleation, and intersite spin transfer, unfold on temporal and spatial scales down to femtoseconds and nanometers, respectively. Pump-probe spectroscopy and diffraction studies indicate that spatio-temporal dynamics may drastically affect the non-equilibrium magnetic evolution. Yet, direct real-space magnetic imaging on the relevant timescales has remained challenging. Here, we demonstrate ultrafast high-harmonic nanoscopy employing circularly polarized high-harmonic radiation for real-space imaging of femtosecond magnetization dynamics. We map quenched magnetic domains and localized spin structures in Co/Pd multilayers with a sub-wavelength spatial resolution down to 16 nm, and strobosocopically trace the local magnetization dynamics with 40 fs temporal resolution. Our compact experimental setup demonstrates the highest spatio-temporal resolution of magneto-optical imaging to date. Facilitating ultrafast imaging with high sensitivity to chiral and linear dichroism, we envisage a wide range of applications spanning magnetism, phase transitions, and carrier dynamics.

Dipolar-stabilized first and second-order antiskyrmions in ferrimagnetic multilayers.

Skyrmions and antiskyrmions are topologically protected spin structures with opposite vorticities. Particularly in coexisting phases, these two types of magnetic quasi-particles may show fascinating physics and potential for spintronic devices. While skyrmions are observed in a wide range of materials, until now antiskyrmions were exclusive to materials with D2d symmetry. In this work, we show first and second-order antiskyrmions stabilized by magnetic dipole-dipole interaction in Fe/Gd-based multilayers. We modify the magnetic properties of the multilayers by Ir insertion layers. Using Lorentz transmission electron microscopy imaging, we observe coexisting antiskyrmions, Bloch skyrmions, and type-2 bubbles and determine the range of material properties and magnetic fields where the different spin objects form and dissipate. We perform micromagnetic simulations to obtain more insight into the studied system and conclude that the reduction of saturation magnetization and uniaxial magnetic anisotropy leads to the existence of this zoo of different spin objects and that they are primarily stabilized by dipolar interaction.

Control over self-assembled Janus clusters by the strength of magnetic field in [Formula: see text].

Colloidal Janus microparticles can be propelled by controlled chemical reactions on their surfaces. Such microswimmers have been used as model systems for the behavior on the microscale and as carriers for cargo to well-defined positions in hard-to-access areas. Here we demonstrate the propagation motion of clusters of magnetic Janus particles driven by the catalytic decomposition of [Formula: see text] on their metallic caps. The magnetic moments of their caps lead to certain spatial arrangements of Janus particles, which can be influenced by external magnetic fields. We investigate how the arrangement of the particles and caps determines the driven motion of the particle clusters. In addition, we show the influence of confining walls on the cluster motion, which will be encountered in any real-life biological system.

Sensitivity of PS/CoPd Janus particles to an external magnetic field.

The dual nature of Janus particles confers fascinating properties such as a response to multiple stimuli. In this communication, we systematically study the sensitivity to a uniform external magnetic field of isolated Janus rod-shaped and spherical particles in water confined to two dimensions. The Janus asymmetry of the particles is given by magnetic [Co(0.28 nm)/Pd(0.90 nm)]8 multilayer films deposited onto monodisperse polystyrene (PS) nanorods and microspheres, respectively. It is shown that the particles dispersed in water respond to weak magnetic field applied in in-plane direction. Here we demonstrate that a precise control of the in-plane particle orientation can be obtained for magnetic field strengths higher than 0.1 mT for microspheres and 0.4 mT for nanorods.

Micromagnetic Simulations of Submicron Vortex Structures for the Detection of Superparamagnetic Labels.

We present a numerical investigation on the detection of superparamagnetic labels using a giant magnetoresistance (GMR) vortex structure. For this purpose, the Landau-Lifshitz-Gilbert equation was solved numerically applying an external z-field for the activation of the superparamagnetic label. Initially, the free layer's magnetization change due to the stray field of the label is simulated. The electric response of the GMR sensor is calculated by applying a self-consistent spin-diffusion model to the precomputed magnetization configurations. It is shown that the soft-magnetic free layer reacts on the stray field of the label by shifting the magnetic vortex orthogonally to the shift direction of the label. As a consequence, the electric potential of the GMR sensor changes significantly for label shifts parallel or antiparallel to the pinning of the fixed layer. Depending on the label size and its distance to the sensor, the GMR sensor responds, changing the electric potential from 26.6 mV to 28.3 mV.

Microscopic Origin of Magnetization Reversal in Nanoscale Exchange-Coupled Ferri/Ferromagnetic Bilayers: Implications for High Energy Density Permanent Magnets and Spintronic Devices.

Giant exchange bias shifts of several Tesla have been reported in ferrimagnetic/ferromagnetic bilayer systems, which could be highly beneficial for contemporary high energy density permanent magnets and spintronic devices. However, the lack of microscopic studies of the reversal owing to the difficulty of measuring few nanometer-wide magnetic structures in high fields precludes the assessment of the lateral size of the inhomogeneity in relation to the intended application. In this study, the magnetic reversal process of nanoscale exchange-coupled bilayer systems, consisting of a ferrimagnetic TbFeCo alloy layer and a ferromagnetic [Co/Ni/Pt] N multilayer, was investigated. In particular, minor loop measurements, probing solely on the reversal characteristics of the softer ferromagnetic layer, reveal two distinct reversal mechanisms, which depend critically on the thickness of the ferromagnetic layer. For thick layers, irreversible switching of the macroscopic minor loop is observed. The underlying microscopic origin of this reversal process was studied in detail by high-resolution magnetic force microscopy, showing that the reversal is triggered by in-plane domain walls propagating through the ferromagnetic layer. In contrast, thin ferromagnetic layers show a hysteresis-free reversal, which is nucleation-dominated due to grain-to-grain variations in magnetic anisotropy of the Co/Ni/Pt multilayer and an inhomogeneous exchange coupling with the magnetically hard TbFeCo layer, as confirmed by micromagnetic simulations.

Strain-induced perpendicular magnetic anisotropy and Gilbert damping of Tm3Fe5O12 thin films.

In the attempt of implementing iron garnets with perpendicular magnetic anisotropy (PMA) in spintronics, the attention turned towards strain-grown iron garnets. One candidate is Tm3Fe5O12 (TmIG) which possesses an out-of-plane magnetic easy axis when grown under tensile strain. In this study, the effect of film thickness on the structural and magnetic properties of TmIG films including magnetic anisotropy, saturation magnetization, and Gilbert damping is investigated. TmIG films with thicknesses between 20 and 300 nm are epitaxially grown by pulsed laser deposition on substituted-Gd3Ga5O12(111) substrates. Structural characterization shows that films thinner than 200 nm show in-plane tensile strain, thus exhibiting PMA due to strain-induced magnetoelastic anisotropy. However, with increasing film thickness a relaxation of the unit cell is observed resulting in the rotation of the magnetic easy axis towards the sample plane due to the dominant shape anisotropy. Furthermore, the Gilbert damping parameter is found to be in the range of 0.02 ± 0.005.

Field-responsive colloidal assemblies defined by magnetic anisotropy.

Particle dispersions provide a promising tool for the engineering of functional materials that exploit self-assembly of complex structures. Dispersion made from magnetic colloidal particles is a great choice; they are biocompatible and remotely controllable among many other advantages. However, their dominating dipolar interaction typically limits structural complexity to linear arrangements. This paper shows how a magnetostatic equilibrium state with noncollinear arrangement of the magnetic moments, as reported for ferromagnetic Janus particles, enables the controlled self-organization of diverse structures in two dimensions via constant and low-frequency external magnetic fields. Branched clusters of staggered chains, compact clusters, linear chains, and dispersed single particles can be formed and interconverted reversibly in a controlled way. The structural diversity is a consequence of both the inhomogeneity and the spatial extension of the magnetization distribution inside the particles. We draw this conclusion from calculations based on a model of spheres with multiple shifted dipoles. The results demonstrate that fundamentally new possibilities for responsive magnetic materials can arise from interactions between particles with a spatially extended, anisotropic magnetization distribution.

Ion induced ferromagnetism combined with self-assembly for large area magnetic modulation of thin films.

A highly versatile and scalable path to obtain buried magnetic nanostructures within alloy thin films, while maintaining a flat topography, is described. A magnetic pattern of nanoscale periodicity is generated over ∼cm2 areas by employing a B2 → A2 structural transition in the prototype Fe60Al40 thin alloy films. The phase transition was induced in the confined regions via ion-irradiation through self-assembled nanosphere masks. In this way, large area patterns of a hexagonal symmetry of ferromagnetic nanostructures embedded within a paramagnetic Fe60Al40 thin film are realized. The depth and lateral distribution of the induced magnetization was investigated by magnetometry and microscopy methods. Magnetic contrast imaging as well as simulations shows that the obtained magnetic structures are well defined, with the magnetic behavior tunable via the mask geometry.

Nanoscale magnetic imaging using circularly polarized high-harmonic radiation.

This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the exceptional coherence of high harmonics, this approach will facilitate quantitative, element-specific, and spatially resolved studies of ultrafast magnetization dynamics, advancing both fundamental and applied aspects of nanoscale magnetism.

A general approach to obtain soft x-ray transparency for thin films grown on bulk substrates.

We present a general approach to thin bulk samples to transparency for experiments in the soft x-ray and extreme ultraviolet spectral range. The method relies on mechanical grinding followed by focused-ion-beam milling. It results in a uniformly thin area of high surface quality, suitable for nanoscale imaging in transmission. In a proof-of-principle experiment, nanoscale magnetic bits on a commercial hard drive glass disk are imaged with a spatial resolution below 30 nm by soft x-ray spectro-holography. Furthermore, we demonstrate imaging of a lithographically patterned test object via absorption contrast. Our approach is suitable for both amorphous and crystalline substrates and has been tested for a variety of common epitaxy growth substrates. Lateral thinning areas in excess of 100 µm2 and a remaining substrate thickness as thin as 150 nm are easily achievable. Our approach allows preserving a previously grown thin film, and from nanofocus electron diffraction, we find no evidence for morphological changes induced by the process, in agreement with numerical simulations of the ion implantation depth distributon. We expect our method to be widely applicable and especially useful for nanoscale imaging of epitaxial thin films.