Raman Shifts in Two-Dimensional van der Waals Magnets Reveal Magnetic Texture Evolution.

Two-dimensional (2D) van der Waals magnets comprise rich physics that can be exploited for spintronic applications. We investigate the interplay between spin-phonon coupling and spin textures in a 2D van der Waals magnet by combining magneto-Raman spectroscopy with cryogenic Lorentz transmission electron microscopy. We find that when stable skyrmion bubbles are formed in the 2D magnet, a field-dependent Raman shift can be observed, and this shift is absent for the 2D magnet prepared in its ferromagnetic state. Correlating these observations with numerical simulations that take into account field-dependent magnetic textures and spin--phonon coupling in the 2D magnet, we associate the Raman shift to field-induced modulations of the skyrmion bubbles and derive the existence of inhomogeneity in the skyrmion textures over the film thickness.

Néel Skyrmion Bubbles in La0.7Sr0.3Mn1-xRuxO3 Multilayers.

Ferromagnetic La0.7Sr0.3Mn1-xRuxO3 epitaxial multilayers with controlled variation of the Ru/Mn content were synthesized to engineer canted magnetic anisotropy and variable exchange interactions, and to explore the possibility of generating a Dzyaloshinskii-Moriya interaction. The ultimate aim of the multilayer design is to provide the conditions for the formation of domains with nontrivial magnetic topology in an oxide thin film system. Employing magnetic force microscopy and Lorentz transmission electron microscopy in varying perpendicular magnetic fields, magnetic stripe domains separated by Néel-type domain walls as well as Néel skyrmions smaller than 100 nm in diameter were observed. These findings are consistent with micromagnetic modeling, taking into account a sizable Dzyaloshinskii-Moriya interaction arising from the inversion symmetry breaking and possibly from strain effects in the multilayer system.

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices.

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions.

Observation of Magnetic Skyrmion Bubbles in a van der Waals Ferromagnet Fe3GeTe2.

Two-dimensional (2D) van der Waals (vdW) magnetic materials have recently been introduced as a new horizon in materials science, and they enable potential applications for next-generation spintronic devices. Here, in this communication, the observations of stable Bloch-type magnetic skyrmions in single crystals of 2D vdW Fe3GeTe2 (FGT) are reported by using in situ Lorentz transmission electron microscopy (TEM). We find the ground-state magnetic stripe domains in FGT transform into skyrmion bubbles when an external magnetic field is applied perpendicularly to the (001) thin plate with temperatures below the Curie temperature TC. Most interestingly, a hexagonal lattice of skyrmion bubbles is obtained via field-cooling manipulation with magnetic field applied along the [001] direction. Owing to their topological stability, the skyrmion bubble lattices are stable to large field-cooling tilted angles and further reproduced by utilizing the micromagnetic simulations. These observations directly demonstrate that the 2D vdW FGT possesses a rich variety of topological spin textures, being of great promise for future applications in the field of spintronics.

In Situ Electric Field Skyrmion Creation in Magnetoelectric Cu2OSeO3.

Exploiting additional degrees of freedom in solid-state materials may be the most-promising solution when approaching the quantum limit of Moore's law for the conventional electronic industry. Recently discovered topologically nontrivial spin textures, skyrmions, are outstanding among such possibilities. However, the controlled creation of skyrmions, especially by electric means, remains a pivotal challenge in technological applications. Here, we report that skyrmions can be created locally via electric field in the magnetoelectric helimagnet Cu2OSeO3. Using Lorentz transmission electron microscopy, we successfully write skyrmions in situ from a helical-spin background. Our discovery is highly coveted because it implies that skyrmionics can be integrated into modern field effect transistor based electronic technology, in which very low energy dissipation can be achieved and, hence, realize a large step forward toward its practical applications.

Creation of Single Chain of Nanoscale Skyrmion Bubbles with Record-High Temperature Stability in a Geometrically Confined Nanostripe.

Nanoscale topologically nontrivial spin textures, such as magnetic skyrmions, have been identified as promising candidates for the transport and storage of information for spintronic applications, notably magnetic racetrack memory devices. The design and realization of a single skyrmion chain at room temperature (RT) and above in the low-dimensional nanostructures are of great importance for future practical applications. Here, we report the creation of a single skyrmion bubble chain in a geometrically confined Fe3Sn2 nanostripe with a width comparable to the featured size of a skyrmion bubble. Systematic investigations on the thermal stability have revealed that the single chain of skyrmion bubbles can keep stable at temperatures varying from RT up to a record-high temperature of 630 K. This extreme stability can be ascribed to the weak temperature-dependent magnetic anisotropy and the formation of edge states at the boundaries of the nanostripes. The realization of the highly stable skyrmion bubble chain in a geometrically confined nanostructure is a very important step toward the application of skyrmion-based spintronic devices.

Direct Evidence of Topological Defects in Electron Waves through Nanoscale Localized Magnetic Charge.

Topological concepts play an important role in, and provide unique insights into, many physical phenomena. In particular topological defects have become an active area of research due to their relevance to diverse systems including condensed matter and the early universe. These defects arise in systems during phase transitions or symmetry-breaking operations that lead to a specific configuration of the order parameter that is stable against external perturbations. In this work, we experimentally show that excitations or defects carrying magnetic charge in artificial spin ices introduce a topological defect in incident coherent electron waves. This results in the formation of a localized electron vortex beam carrying orbital angular momentum that is directly correlated with the magnetic charge. This work provides unique insight into the interaction of electrons with magnetically charged excitations and the effect on their topology thereby opening new possibilities to explore exotic scattering and quantum effects in nanoscale condensed-matter systems.

Current-Driven Motion of Domain Boundaries between Skyrmion Lattice and Helical Magnetic Structure.

To utilize magnetic skyrmions, nanoscale vortex-like magnetic structures, experimental elucidation of their dynamics against current application in various circumstances such as in confined structure and mixture of different magnetic phases is indispensable. Here, we investigate the current-induced dynamics of the coexistence state of magnetic skyrmions and helical magnetic structure in a thin plate of B20-type helimagnet FeGe in terms of in situ real-space observation using Lorentz transmission electron microscopy. Current pulses with various heights and widths were applied, and the change of the magnetic domain distribution was analyzed using a machine-learning technique. The observed average driving direction of the two-magnetic-state domain boundary is opposite to the applied electric current, indicating ferromagnetic s-d exchange coupling in the spin-transfer torque mechanism. The evaluated driving distance tends to increase with increasing the pulse duration time, current density (>1 × 109 A/m2), and sample temperature, providing valuable information about hitherto unknown current-induced dynamics of the skyrmion-lattice ensemble.

Filming the formation and fluctuation of skyrmion domains by cryo-Lorentz transmission electron microscopy.

Magnetic skyrmions are promising candidates as information carriers in logic or storage devices thanks to their robustness, guaranteed by the topological protection, and their nanometric size. Currently, little is known about the influence of parameters such as disorder, defects, or external stimuli on the long-range spatial distribution and temporal evolution of the skyrmion lattice. Here, using a large (7.3 × 7.3 µm(2)) single-crystal nanoslice (150 nm thick) of Cu2OSeO3, we image up to 70,000 skyrmions by means of cryo-Lorentz transmission electron microscopy as a function of the applied magnetic field. The emergence of the skyrmion lattice from the helimagnetic phase is monitored, revealing the existence of a glassy skyrmion phase at the phase transition field, where patches of an octagonally distorted skyrmion lattice are also discovered. In the skyrmion phase, dislocations are shown to cause the emergence and switching between domains with different lattice orientations, and the temporal fluctuation of these domains is filmed. These results demonstrate the importance of direct-space and real-time imaging of skyrmion domains for addressing both their long-range topology and stability.

Lorentz Transmission Electron Microscopy Image Simulations of Experimental Nano-Chessboard Observations in Co-Pt Alloys.

The magnetization configuration of a novel nano-chessboard structure consisting of L10 and L12 phases in a Co40Pt60 alloy is investigated using Lorentz transmission electron microscopy (LTEM) and micro-magnetic simulations. We show high-resolution LTEM images of nano-size magnetic features acquired through spherical aberration correction in Lorentz Fresnel mode. Phase reconstructions and LTEM image simulations are carried out to fully understand the magnetic microstructure. The experimental Fresnel images of the nano-chessboard structure show zig-zag shaped magnetic domain walls at the inter-phase boundaries between L10 and L12 phases. A circular magnetization distribution with vortex and anti-vortex type arrangement is evident in the phase reconstructed magnetic induction maps as well as simulated maps. The magnetic contrast in experimental LTEM images is interpreted with the help of magnetic induction maps simulated for various relative electron beam-sample orientations inside the TEM.

Deformation of Topologically-Protected Supercooled Skyrmions in a Thin Plate of Chiral Magnet Co8Zn8Mn4.

Magnetic skyrmions in Co8Zn8Mn4 thin plates are observed to deform in a metastable state prepared in a magnetic-field-cooling process by way of the thermal-equilibrium skyrmion phase. In cooling, the disk-shape skyrmions change to bar- or L-shaped elongated form, whereas the skyrmion density is nearly conserved. The deformation of the skyrmions in the supercooled metastable phase is observed irrespective of the crystallographic orientation of the thin plate, whereas the elongation direction nearly aligns along the magnetic easy axis. It is proposed that the deformation should be induced by a large increase in magnetic modulation wavenumber when decreasing the temperature, whereas the topological protection of the skyrmions keeps the averaged skyrmion density constant.

Nanoscale Skyrmions in a Nonchiral Metallic Multiferroic: Ni2MnGa.

Magnetic skyrmions belong to a set of topologically nontrivial spin textures at the nanoscale that have received increased attention due to their emergent behavior and novel potential spintronic applications. Discovering materials systems that can host skyrmions at room temperature in the absence of external magnetic field is of crucial importance not only from a fundamental aspect, but also from a technological point of view. So far, the observations of skyrmions in bulk metallic ferromagnets have been limited to low temperatures and to materials that exhibit strong chiral interactions. Here we show the formation of nanoscale skyrmions in a nonchiral multiferroic material, which is ferromagnetic and ferroelastic, Ni2MnGa at room temperature without the presence of external magnetic fields. By using Lorentz transmission electron microscopy in combination with micromagnetic simulations, we elucidate their formation, behavior, and stability under applied magnetic fields at room temperature. The formation of skyrmions in a multiferroic material with no broken inversion symmetry presents new exciting opportunities for the exploration of the fundamental physics of topologically nontrivial spin textures.

TEM sample preparation of lithographically patterned permalloy nanostructures on silicon nitride membranes.

We have prepared ferromagnetic nanostructures intended for the investigation of high-frequency magnetization dynamics in permalloy (Py) nanodisks using Lorentz transmission electron microscopy (LTEM) and electron holography. Py nanodisks were fabricated on thin silicon nitride (SiN) membranes using three different fabrication methods: lift-off, ion beam etching (IBE), and stencil lithography. They were further analyzed using different instruments, including scanning electron microscopy, LTEM, and electron holography. A bilayer of positive PMMA resist was utilized in the first fabrication method to form an undercut structure that guarantees a clean lift-off procedure. The second approach used dry etching with an Ar beam to etch a thin Py film, while an electron-beam-patterned negative resist mask kept the desired structure. In the third process, nanostencils (shadow masks) with submicrometer apertures were milled on SiN membranes using a focused ion beam. Furthermore, we have developed a new TEM sample preparation method, where we fabricated Py nanostructures on a bulk substrate with a SiN buffer layer and etched the substrate to create a thin SiN membrane under the Py nanostructure. Finally, we observed the vortex dynamics of the Py nanodisk under magnetic fields using LTEM and off-axis electron holography. A correlation between preparation methods and the properties of the Py nanostructures was made.

Bloch Point Quadrupole Constituting Hybrid Topological Strings Revealed with Electron Holographic Vector Field Tomography.

Topological magnetic (anti)skyrmions are robust string-like objects heralded as potential components in next-generation topological spintronics devices due to their low-energy manipulability via stimuli such as magnetic fields, heat, and electric/thermal current. While these 2D topological objects are widely studied, intrinsically 3D electron-spin real-space topology remains less explored despite its prevalence in bulky magnets. 2D-imaging studies reveal peculiar vortex-like contrast in the core regions of spin textures present in antiskyrmion-hosting thin plate magnets with S4 crystal symmetry, suggesting a more complex 3D real-space structure than the 2D model suggests. Here, holographic vector field electron tomography captures the 3D structure of antiskyrmions in a single-crystal, precision-doped (Fe0.63Ni0.3Pd0.07)3P (FNPP) lamellae at room temperature and zero field. These measurements reveal hybrid string-like solitons composed of skyrmions with topological number W = -1 on the lamellae's surfaces and an antiskyrmion (W = + 1) connecting them. High-resolution images uncover a Bloch point quadrupole (four magnetic (anti)monopoles that are undetectable in 2D imaging) which enables the observed lengthwise topological transitions. Numerical calculations corroborate the stability of hybrid strings over their conventional (anti)skyrmion counterparts. Hybrid strings result in topological tuning, a tunable topological Hall effect, and the suppression of skyrmion Hall motion, disrupting existing paradigms within spintronics.

Effect of Surface Oxidation and Crystal Thickness on the Magnetic Properties and Magnetic Domain Structures of Cr2Ge2Te6.

van der Waals (vdW) magnetic materials, such as Cr2Ge2Te6 (CGT), show promise for memory and logic applications. This is due to their broadly tunable magnetic properties and the presence of topological magnetic features such as skyrmionic bubbles. A systematic study of thickness and oxidation effects on magnetic domain structures is important for designing devices and vdW heterostructures for practical applications. Here, we investigate thickness effects on magnetic properties, magnetic domains, and bubbles in oxidation-controlled CGT crystals. We find that CGT exposed to ambient conditions for 5 days forms an oxide layer approximately 5 nm thick. This oxidation leads to a significant increase in the oxidation state of the Cr ions, indicating a change in local magnetic properties. This is supported by real-space magnetic texture imaging through Lorentz transmission electron microscopy. By comparing the thickness-dependent saturation field of oxidized and pristine crystals, we find that oxidation leads to a nonmagnetic surface layer that is thicker than the oxide layer alone. We also find that the stripe domain width and skyrmionic bubble size are strongly affected by the crystal thickness in pristine crystals. These findings underscore the impact of thickness and surface oxidation on the properties of CGT, such as saturation field and domain/skyrmionic bubble size, and suggest a pathway for manipulating magnetic properties through a controlled oxidation process.

Magnetic Skyrmions above Room Temperature in a van der Waals Ferromagnet Fe3GaTe2.

2D van der Waals (vdW) ferromagnetic crystals are a promising platform for innovative spintronic devices based on magnetic skyrmions, thanks to their high flexibility and atomic thickness stability. However, room-temperature skyrmion-hosting vdW materials are scarce, which poses a challenge for practical applications. In this study, a chemical vapor transport (CVT) approach is employed to synthesize Fe3GaTe2 crystals and room-temperature Néel skyrmions are observed in Fe3GaTe2 nanoflakes above 58 nm in thickness through in situ Lorentz transmission electron microscopy (L-TEM). Upon an optimized field cooling procedure, zero-field hexagonal skyrmion lattices are successfully generated in nanoflakes with an extended thickness range (30-180 nm). Significantly, these skyrmion lattices remain stable up to 355 K, setting a new record for the highest temperature at which skyrmions can be hosted. The research establishes Fe3GaTe2 as an emerging above-room-temperature skyrmion-hosting vdW material, holding great promise for future spintronics.

Thickness-Tunable Zoology of Magnetic Spin Textures Observed in Fe5GeTe2.

The family of two-dimensional (2D) van der Waals (vdW) materials provides a playground for tuning structural and magnetic interactions to create a wide variety of spin textures. Of particular interest is the ferromagnetic compound Fe5GeTe2 that we show displays a range of complex spin textures as well as complex crystal structures. Here, using a high-brailliance laboratory X-ray source, we show that the majority (1 × 1) Fe5GeTe2 (FGT5) phase exhibits a structure that was previously considered as being centrosymmetric but rather lacks inversion symmetry. In addition, FGT5 exhibits a minority phase that exhibits a long-range ordered (√3 × âˆš3)-R30° superstructure. This superstructure is highly interesting in that it is innately 2D without any lattice periodicity perpendicular to the vdW layers, and furthermore, the superstructure is a result of ordered Te vacancies in one of the topmost layers of the FGT5 sheets rather than being a result of vertical Fe ordering as earlier suggested. We show, from direct real-space magnetic imaging, evidence for three distinct magnetic ground states in lamellae of FGT5 that are stabilized with increasing lamella thickness, namely, a multidomain state, a stripe phase, and an unusual fractal state. In the stripe phase we also observe unconventional type-I and type-II bubbles where the spin texture in the central region of the bubbles is nonuniform, unlike conventional bubbles. In addition, we find a bobber or a cocoon-like spin texture in thick (∼170 µm) FGT5 that emerges from the fractal state in the presence of a magnetic field. Among all the 2D vdW magnets we have thus demonstrated that FGT5 hosts perhaps the richest variety of magnetic phases that, thereby, make it a highly interesting platform for the subtle tuning of magnetic interactions.

Realization and Current-Driven Dynamics of Fractional Hopfions and Their Ensembles in a Helimagnet FeGe.

3D topological spin textures-hopfions-are predicted in helimagnetic systems but are not experimentally confirmed thus far. By utilizing an external magnetic field and electric current in the present study, 3D topological spin textures are realized, including fractional hopfions with nonzero topological index, in a skyrmion-hosting helimagnet FeGe. Microsecond current pulses are employed to control the dynamics of the expansion and contraction of a bundle composed of a skyrmion and a fractional hopfion, as well as its current-driven Hall motion. This research approach has demonstrated the novel electromagnetic properties of fractional hopfions and their ensembles in helimagnetic systems.

Direct Visualisation of Skyrmion Lattice Defect Alignment at Grain Boundaries.

We present a method to directly visualise a statistical analysis of skyrmion defect alignment at grain boundaries in the skyrmion host [Formula: see text]OSeO3. Using Lorentz transmission electron microscopy, we collected large data sets with several hundreds of frames containing skyrmion lattices with grain boundaries in them. To address the behaviour of strings of dislocations in these grain boundaries, we developed an algorithm to automatically extract and classify strings of dislocations separating the grains. This way we circumvent the problem of having to create configurations with well-defined relative grain orientations by performing a statistical analysis on a dynamically rearranging image sequence. With this statistical method, we are able to experimentally extract the relationship between grain boundary alignment and defect spacing and find an agreement with geometric expectations. The algorithms used can be extended to other types of lattices such as Abrikosov lattices or colloidal systems in optical microscopy.

Doping Control of Magnetic Anisotropy for Stable Antiskyrmion Formation in Schreibersite (Fe,Ni)3 P with S4 symmetry.

Magnetic skyrmions, vortex-like topological spin textures, have attracted much interest in a wide range of research fields from fundamental physics to spintronics applications. Recently, growing attention is also paid to antiskyrmions emerging with opposite topological charge in non-centrosymmetric magnets with D2d or S4 symmetry. In these magnets, complex interplay among anisotropic Dzyaloshinskii-Moriya interaction, uniaxial magnetic anisotropy, and magnetic dipolar interactions generates various magnetic textures. However, the precise role of these magnetic interactions in stabilizing antiskyrmions remains to be elucidated. In this work, the uniaxial magnetic anisotropy of schreibersite (Fe,Ni)3 P with S4 symmetry is controlled by doping and its impact on the stability of antiskyrmions is investigated. The authors' magnetometry study, supported by ferromagnetic resonance spectroscopy, shows that the variation of the Ni content and slight doping with 4d transition metals considerably change the magnetic anisotropy. In particular, doping with Pd induces easy-axis anisotropy, giving rise to formation of antiskyrmions, while a temperature-induced spin reorientation is observed in an Rh-doped compound. In combination with Lorentz transmission electron microscopy and micromagnetic simulations, the stability of antiskyrmion as functions of uniaxial anisotropy and demagnetization energy is quantitatively analyzed, and demonstrated that subtle balance between them is necessary to stabilize the antiskyrmions.