Lorentz Transmission Electron Microscopy Research Articles

In situ phase engineering during additive manufacturing enables high-performance soft-magnetic medium-entropy alloys.

Additive manufacturing (AM) shows promise as a method for producing soft-magnetic multicomponent alloys for use in electric motors and sustainable electromobility applications. However, the simultaneous achievement of a high saturation magnetic flux density (Bs) and a low coercivity (Hc) in AM soft-magnetic materials remains challenging. Herein, we present an approach that integrates an elemental powder mixture of Fe45Co30Ni25 with Fe2O3 nano-oxides, which is then subjected to laser powder bed fusion (LPBF) followed by high-temperature annealing to achieve an FCC-structured Fe45Co30Ni25 MEA/FeO composite. The FeO nanoparticles, a byproduct of the reaction between Fe powders and Fe2O3 nano-oxides, serve as nucleation sites for the formation of a single FCC phase in the MEA matrix. The resulting LPBF MEA/FeO composite has a Bs of 2.05 T and an exceedingly low Hc of 115 A m-1, compared to those of the BCC/FCC dual phase MEA and other state-of-the-art additively manufactured soft-magnetic alloys. In situ Lorentz transmission electron microscope (TEM) revealed that the low Hc of the FCC-structured MEA/FeO composite originates from the reduced pinning effect of grain boundaries in the FCC phase on domain wall movement compared with those in the FCC/BCC dual phase.

Chirality Control of Magnetic Vortices in Ferromagnetic Disk–Nanowire System

The results of experimental studies and micromagnetic modeling of magnetic states in a one-dimensional array are presented. The array has the form of a chain of ferromagnetic disks coupled with a ferromagnetic nanowire made of the same material. The disks are located on opposite sides of the nanowire, which makes it possible to obtain distributions when the chiralities of the magnetic vortex shells in neighboring disks alternate, which can find application in vortex spin nanooscillators. Using the application in situ of a magnetic field to an excited objective lens using Lorentz transmission electron microscopy, it is shown that in this system it is possible to control the chiralities of the shells of magnetic vortices, which is realized by magnetization in the sample plane along various azimuthal directions. When wire magnetized along a nanowire, vortex states with opposite chiralities are realized in disks located on opposite sides of it. An antivortex is formed in the nanowire itself at the boundary with the disk, since the local direction of magnetization in the wire and in the disk are anticollinear. When magnetized perpendicular to the nanowire, states with the same chirality are realized in all disks. In this case, two perpendicular domain walls are formed between the disks in the nanowire, and the vortex in the disk is shifted to one of the edges along the nanowire.

Observation of Néel-type magnetic skyrmion in a layered non-centrosymmetric itinerant ferromagnet CrTe1.38

Magnetic skyrmions are nanoscale vortex-like magnetization textures that hold great promise for next-generation memory and spintronic devices. While extensive research has focused on discovering such localized spin textures in bulk magnets and multilayers with heavy metals, there is a growing interest in finding them in two-dimensional (2D) magnetic materials. In this research work, we report two distinct phases of the 2D CrxTey family: non-centrosymmetric CrTe1.38 and centrosymmetric CrTe0.96, with a Curie temperature of around 200 and 300 K, respectively. Detailed magnetic study indicates a prominent out-of-plane magnetic anisotropy in CrTe1.38. In contrast, CrTe0.96 exhibits a weak uniaxial magnetic anisotropy. Lorentz transmission electron microscopy shows that the spontaneous ferromagnetic ground state of CrTe1.38 consists of Néel skyrmions, whereas CrTe0.96 exhibits Bloch domain walls, consistent with their crystalline symmetries. This research expands the quasi-2D CrxTey family and opens up new avenues for exploring non-trivial spin structures and their potential applications in spintronic devices.

Confined antiskyrmion motion driven by electric current excitations

Current-driven dynamics of topological spin textures, such as skyrmions and antiskyrmions, have garnered considerable attention in condensed matter physics and spintronics. As compared with skyrmions, the current-driven dynamics of their antiparticles – antiskyrmions − remain less explored due to the increased complexity of antiskyrmions. Here, we design and employ fabricated microdevices of a prototypical antiskyrmion host, (Fe0.63Ni0.3Pd0.07)3P, to allow in situ current application with Lorentz transmission electron microscopy observations. The experimental results and related micromagnetic simulations demonstrate current-driven antiskyrmion dynamics confined within stripe domains. Under nanosecond-long current pulses, antiskyrmions exhibit directional motion along the stripe regardless of the current direction, while the antiskyrmion velocity is linearly proportional to the current density. Significantly, the antiskyrmion mobility could be enhanced when the current flow is perpendicular to the stripe direction. Our findings provide novel and reliable insights on dynamical antiskyrmions and their potential implications on spintronics.

Room temperature skyrmions in Pt/Co/Gd multilayers and their non-volatile electric-field creation in multiferroic heterostructure

This study delves into the formation and control of magnetic skyrmions within a Pt/Co/Gd multilayer system. By systematically varying the thickness of the Co layer, we observe the emergence of Néel-type skyrmions, characterized by confined magnetization curls with Lorentz transmission electron microscopy. The interplay between magnetic anisotropy, Dzyaloshinskii–Moriya interaction, and antiferromagnetic coupling at material interfaces is investigated to understand the stability and manipulation of these fascinating spin configurations. Additionally, we explore the impact of an external electric field on skyrmion generation, demonstrating a pathway for their controlled creation. The observed electric-field control of skyrmions offers a promising approach to achieving non-volatile magnetic states with low power consumption and negligible Joule heating. These findings hold great potential for advancing spintronics and magneto-electric devices, enabling modulation of skyrmions for information storage and processing applications.

Magnetic Structure-Dependent Spin Texture Lattice in Hexagonal MnFeCoGe Magnets.

Topological spin textures are of great significance in magnetic information storage and spintronics due to their high storage density and low drive current. In this work, the transformation of magnetic configuration from chaotic labyrinth domains to uniform stripe domains was observed in MnFe1-xCoxGe magnets. This change occurs due to the noncollinear magnetic structure switching to a uniaxial ferromagnetic structure with increasing Co content, as identified by neutron diffraction results and Lorentz transmission electron microscopy (L-TEM). Of utmost importance, a hexagonal lattice of high-density robust type-II magnetic bubble lattice was established for x = 0.8 through out-of-plane magnetic field stimulation and field-cooling. The dimensions of the type-II magnetic bubbles were found to be tuned by the sample thickness. Therefore, the stabilization of complex magnetic spin textures, associated with enhanced uniaxial ferromagnetic interaction and magnetic dipole-dipole interaction in MnFe1-xCoxGe through magnetic structure manipulation, as further confirmed by the micromagnetic simulations, will provide a convenient and efficient strategy for designing topological spin textures with potential applications in spintronic devices.

Embedded Skyrmion Bags in Thin Films of Chiral Magnets.

Magnetic skyrmions are topologically nontrivial spin configurations that possess particle-like properties. Earlier research has mainly focused on a specific type of skyrmion with topological charge Q = -1. However, theoretical analyses of 2D chiral magnets have predicted the existence of skyrmion bags-solitons with arbitrary positive or negative topological charge. Although such spin textures are metastable states, recent experimental observations have confirmed the stability of isolated skyrmion bags in a limited range of applied magnetic fields. Here, by utilizing Lorentz transmission electron microscopy, the extraordinary stability of skyrmion bags in thin plates of B20-type FeGe is shown. In particular, it is shown that skyrmion bags embedded within a skyrmion lattice remain stable even in zero or inverted external magnetic fields. A robust protocol for nucleating such embedded skyrmion bags is provided. The results agree perfectly with micromagnetic simulations and establish thin plates of cubic chiral magnets as a powerful platform for exploring a broad spectrum of topological magneticsolitons.

Evolution of magnetization textures in Mn1.4PtSn under magnetic field

We have used Lorentz transmission electron microscopy (LTEM) and the transport of intensity equation (TIE) method to investigate the spin structures in the Mn1.4PtSn magnet, which exhibits D2d symmetry. The evolution of the spin structures under the external magnetic field was observed. In particular, a perpendicular field is able to modulate the striped domain widths and to induce the formation of anti-skyrmions and bubbles. While an in-plane magnetic field can control the state of these structures, the coexistence of different types of skyrmions suggests that the hysteresis properties of the magnet may affect the effectiveness of the field control.

Field-free transformations of topological spin textures in ferrimagnetic TbFeCo films

The generation of topological spin textures under ultrafast laser pulse excitations and field-free manipulation of topological transitions between different spin textures has attracted enormous interest from the perspective of spintronic applications. Here, we utilize ultrafast electron microscopy to showcase the femtosecond laser pulses excitation on magnetic materials and have generated multiple topological spin textures in an amorphous ferrimagnetic TbFeCo film. Furthermore, the following field-free topological transitions between skyrmions and bubbles with diversified topology are identified via in situ heating the sample in Lorentz transmission electron microscopy. The critical role of uniaxial anisotropy variation on changing the magnetic textures during the heating process is confirmed by micromagnetic simulations. Our results provide a perspective on the generation and transformation of topological spin textures.

Simulation-trained machine learning models for Lorentz transmission electron microscopy

Understanding the collective behavior of complex spin textures, such as lattices of magnetic skyrmions, is of fundamental importance for exploring and controlling the emergent ordering of these spin textures and inducing phase transitions. It is also critical to understand the skyrmion–skyrmion interactions for applications such as magnetic skyrmion-enabled reservoir or neuromorphic computing. Magnetic skyrmion lattices can be studied using in situ Lorentz transmission electron microscopy (LTEM), but quantitative and statistically robust analysis of the skyrmion lattices from LTEM images can be difficult. In this work, we show that a convolutional neural network, trained on simulated data, can be applied to perform segmentation of spin textures and to extract quantitative data, such as spin texture size and location, from experimental LTEM images, which cannot be obtained manually. This includes quantitative information about skyrmion size, position, and shape, which can, in turn, be used to calculate skyrmion–skyrmion interactions and lattice ordering. We apply this approach to segmenting images of Néel skyrmion lattices so that we can accurately identify skyrmion size and deformation in both dense and sparse lattices. The model is trained using a large set of micromagnetic simulations as well as simulated LTEM images. This entirely open-source training pipeline can be applied to a wide variety of magnetic features and materials, enabling large-scale statistical studies of spin textures using LTEM.

Geometric phase analysis of magnetic skyrmion lattices in Lorentz transmission electron microscopy images

Magnetic skyrmions are quasi-particles with a swirling spin texture that form two-dimensional lattices. Skyrmion lattices can exhibit defects in response to geometric constraints, variations of temperature or applied magnetic fields. Measuring deformations in skyrmion lattices is important to understand the interplay between the lattice structure and external influences. Geometric phase analysis (GPA) is a Fourier-based image processing method that is used to measure deformation fields in high resolution transmission electron microscopy (TEM) images of crystalline materials. Here, we show that GPA can be applied quantitatively to Lorentz TEM images of two-dimensional skyrmion lattices obtained from a chiral magnet of FeGe. First, GPA is used to map deformation fields around a 5–7 dislocation and the results are compared with the linear theory of elasticity. Second, rotation angles between skyrmion crystal grains are measured and compared with angles calculated from the density of dislocations. Third, an orientational order parameter and the corresponding correlation function are calculated to describe the evolution of the disorder as a function of applied magnetic field. The influence of sources of artifacts such as geometric distortions and large defoci are also discussed.

AI-enabled Lorentz microscopy for quantitative imaging of nanoscale magnetic spin textures

AbstractThe manipulation and control of nanoscale magnetic spin textures are of rising interest as they are potential foundational units in next-generation computing paradigms. Achieving this requires a quantitative understanding of the spin texture behavior under external stimuli using in situ experiments. Lorentz transmission electron microscopy (LTEM) enables real-space imaging of spin textures at the nanoscale, but quantitative characterization of in situ data is extremely challenging. Here, we present an AI-enabled phase-retrieval method based on integrating a generative deep image prior with an image formation forward model for LTEM. Our approach uses a single out-of-focus image for phase retrieval and achieves significantly higher accuracy and robustness to noise compared to existing methods. Furthermore, our method is capable of isolating sample heterogeneities from magnetic contrast, as shown by application to simulated and experimental data. This approach allows quantitative phase reconstruction of in situ data and can also enable near real-time quantitative magnetic imaging.

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.

Multilayer Metamaterials with Ferromagnetic Domains Separated by Antiferromagnetic Domain Walls

AbstractMagnetic nano‐objects possess great potential for more efficient data processing, storage, and neuromorphic‐type applications. Using high perpendicular magnetic anisotropy synthetic antiferromagnets in the form of multilayer‐based metamaterials, the antiferromagnetic interlayer exchange energy is purposefully reduced below the out‐of‐plane demagnetization energy, which controls magnetic domain formation. In this unusual magnetic energy regime, as demonstrated via macroscopic magnetometry and microscopic Lorentz transmission electron microscopy, it becomes possible to stabilize nanometer‐scale stripe and bubble textures consisting of ferromagnetic out‐of‐plane domain cores separated by antiferromagnetic in‐plane Bloch‐type domain walls. This unique coexistence of mixed ferromagnetic/antiferromagnetic order on the nanometer scale opens so far unexplored perspectives in the architecture of magnetic domain landscapes as well as the design and functionality of individual magnetic textures, such as bubble domains with depth‐wise alternating chirality.

Comparison of differential phase Contrast, Lorentz and non-Lorentz transmission electron microscopy for microstructural and magnetic imaging of alnico magnet

In this work, non-Lorentz, Lorentz transmission electron microscopy (LTEM) and differential phase contrast (DPC) methods were used to observe the phase and magnetic structure of the alnico magnet. All observations were performed on alnico-5 in transverse orientation. The results showed the magnetic contrast of the domain walls in the conventional TEM images despite the effects of the lens magnetic field, which was verified and explained using DPC. Experimental methodology and sample results are summarized with advice for further research.

Room-temperature skyrmions in the van der Waals ferromagnet Fe3GaTe2

The recently emerged van der Waals ferromagnet Fe3GaTe2 has an above-room-temperature TC of ∼350 K. By measuring the magneto-optical Kerr effect microscopy and Lorentz transmission electron microscopy on high quality Fe3GaTe2 crystals at room temperature, we visualized that the magnetic field applied perpendicularly to the (001) plane of the bulk crystal below TC can turn the ground-state labyrinth-stripe magnetic domain into Néel-type skyrmions. The result is also supported by the measured topological Hall effect. Furthermore, we identified that the reduction in crystal thickness can influence the density of skyrmions. The observation paves the way to use this van der Waals ferromagnet in next-generation low-power magnetoelectronic and spintronic devices that can work at room temperature.

Laser‐Induced Real‐Space Topology Control of Spin Wave Resonances

AbstractFemtosecond laser excitation of materials exhibiting magnetic spin textures promises advanced magnetic control via the generation of non‐equilibrium spin dynamics. Ferrimagnetic [Fe(0.35 nm)/Gd(0.40 nm)]160 multilayers are used to explore this approach, as they host a rich diversity of magnetic textures from stripe domains at low magnetic fields, a dense bubble/skyrmion lattice at intermediate fields, and a single domain state for high magnetic fields. Using femtosecond magneto‐optics, distinct coherent spin wave dynamics are observed in this material in response to a weak laser excitation, enabling an unambiguous identification of the different magnetic spin textures. Moreover, employing strong laser excitation, versatile control of the coherent spin dynamics via non‐equilibrium transformation of magnetic spin textures becomes possible by both creating and annihilating bubbles/skyrmions. Micromagnetic simulations and Lorentz transmission electron microscopy with in situ optical excitation corroborate these findings.

Spontaneous Small Biskyrmions in a Centrosymmetric Rare-Earth Kagome Ferrimagnet

Magnetic skyrmions with nontrivial topologies have great potential to serve as memory cells in novel spintronic devices. Small skyrmions were theoretically and experimentally confirmed to be generated under the influence of external fields in ferrimagnetic films via Dzyaloshinskii–Moriya interactions (DMIs). However, this topological state has yet to be verified in ferrimagnetic crystals, especially in the absence of external fields and DMIs. Here, spontaneous biskyrmions were directly observed in the Tb0.2Gd0.8Co2 ferrimagnetic crystal with a Kagome lattice using Lorentz transmission electron microscopy. The high-density biskyrmions exhibited a small size (approximately 50 nm) over a wide temperature range, were closely related to subtle magnetic interaction competition, and coexisted with some broken stripes that could be easily converted into zero-field biskyrmions by utilizing proper field-cooling manipulation. These results can be used to establish a platform for investigating functional sub-50-nm skyrmions in ferrimagnetic crystals and to facilitate advanced applications in magnetic devices.

Exotic Topological Magnetic States in Thin Co/Pd Ferromagnetic Films

AbstractThin ferromagnet/heavy metal multilayer films are considered as prospective media for a magnetic recording and Co/Pd films are a good example of such materials. In this work, the magnetic properties and micromagnetic structure of Co/Pd multilayer films are studied with different bilayer thicknesses ([Co(0.3 × t nm)/Pd(0.5 × t nm)]10), but with the same ratio Co versus Pd. Transmission electron microscope and X‐ray diffraction studies allow authors to suppose that the investigated films are highly mixed alloys. Magnetic force microscopy and Lorentz transmission electron microscopy showed the presence of various micromagnetic features in the films. Along with skyrmions that are well‐known magnetic topological artifacts some new features are revealed, which are interpreted as 360° domain walls, skyrmioniums and the combination of the above two. It is found that the type and density of micromagnetic features strongly depend on the bilayer thickness parameter (t). The effect is associated with the peculiarities of interfacial magnetic interactions in the samples with highly mixed interfaces. The tooling coefficient represents a useful tool of the electron beam evaporation technique enabling wide manipulation of micromagnetic particles, in particular, skyrmioniums that are currently considered a prospective media for current driven magnetic recording.

Vortex-based soft magnetic composite with ultrastable permeability up to gigahertz frequencies

Soft magnetic materials with stable permeability up to hundreds of megahertz (MHz) are urgently needed for integrated transformers and inductors, which are crucial in the more-than-Moore era. However, traditional frequency-stable soft magnetic ferrites suffer from low saturation magnetization and temperature instability, making them unsuitable for integrated circuits. Herein, we fabricate a frequency-stable soft magnetic composite featuring a magnetic vortex structure via cold-sintering, where ultrafine FeSiAl particles are magnetically isolated and covalently bonded by Al2SiO5/SiO2/Fe2(MoO4)3 multilayered heterostructure. This construction results in an ultrastable permeability of 13 up to 1 gigahertz (GHz), relatively large saturation magnetization of 105 Am2/kg and low coercivity of 48 A/m, which we ascribe to the elimination of domain walls associated with almost uniform single-vortex structures, as observed by Lorentz transmission electron microscopy and reconstructed by micromagnetic simulation. Moreover, the ultimate compressive strength has been simultaneously increased up to 337.1 MPa attributed to the epitaxially grown interfaces between particles. This study deepens our understanding on the characteristics of magnetic vortices and provides alternative concept for designing integrated magnetic devices.