Spin-polarized Low-energy Electron Microscopy Research Articles

Super-resolution of magnetic systems using deep learning

We construct a deep neural network to enhance the resolution of spin structure images formed by spontaneous symmetry breaking in the magnetic systems. Through the deep neural network, an image is expanded to a super-resolution image and reduced to the original image size to be fitted with the input feed image. The network does not require ground truth images in the training process. Therefore, it can be applied when low-resolution images are provided as training datasets, while high-resolution images are not obtainable due to the intrinsic limitation of microscope techniques. To show the usefulness of the network, we train the network with two types of simulated magnetic structure images; one is from self-organized maze patterns made of chiral magnetic structures, and the other is from magnetic domains separated by walls that are topological defects of the system. The network successfully generates high-resolution images highly correlated with the exact solutions in both cases. To investigate the effectiveness and the differences between datasets, we study the network’s noise tolerance and compare the networks’ reliabilities. The network is applied with experimental data obtained by magneto-optical Kerr effect microscopy and spin-polarized low-energy electron microscopy.

60∘ and 120∘ domain walls in epitaxial BaTiO3 (111)/Co multiferroic heterostructures

We report on domain pattern transfer from a ferroelectric ${\mathrm{BaTiO}}_{3}$ substrate with a (111) orientation of the surface to an epitaxial Co film grown on a Pd buffer layer. Spatially modulated interfacial strain transfer from ferroelectric/ferroelastic domains and inverse magnetostriction in the ferromagnetic film induce stripe regions with a modulation of the in-plane uniaxial magnetic anisotropy direction. Using spin-polarized low-energy electron microscopy, we observe the formation of two distinct anisotropy configurations between stripe regions, leading to angles of ${60}^{\ensuremath{\circ}}$ or ${120}^{\ensuremath{\circ}}$ between the magnetizations of adjacent domains. Moreover, through application of a magnetic field parallel or perpendicular to these stripes, head-to-head or head-to-tail magnetization configurations are initialized. This results in four distinct magnetic domain-wall types associated with different energies and domain widths, which, in turn, affects whether domain pattern transfer can be achieved.

Competition between exchange and magnetostatic energies in domain pattern transfer from BaTiO3 (111) to a Ni thin film

We use spin-polarized low-energy electron microscopy to investigate domain pattern transfer in a multiferroic heterostructure consisting of a (111)-oriented ${\mathrm{BaTiO}}_{3}$ substrate and an epitaxial Ni film. After in situ thick-film deposition and annealing through the ferroelectric phase transition, interfacial strain transfer from ferroelastic domains in the substrate and inverse magnetostriction in the magnetic thick film introduce a uniaxial in-plane magnetic anisotropy that rotates by ${60}^{\ensuremath{\circ}}$ between alternating stripe regions. We show that two types of magnetic domain wall can be initialized in principle. Combining experimental results with micromagnetic simulations, we show that a competition between the exchange and magnetostatic energies in these domain walls has a strong influence on the magnetic domain configuration.

Stacking influence on the in-plane magnetic anisotropy in a 2D magnetic system.

The magnetization patterns on three atomic layers thick islands of Co on Ru(0001) are studied by spin-polarized low-energy electron microscopy (SPLEEM). In-plane magnetized micrometer wide triangular Co islands are grown on Ru(0001). They present two different orientations correlated with two different stacking sequences which differ only in the last layer position. The stacking sequence determines the type of magnetization pattern observed: the hcp islands present very wide domain walls, while the fcc islands present domains separated by much narrower domain walls. The former is an extremely low in-plane anisotropy system. We estimate the in-plane magnetic anisotropy of the fcc regions to be 1.96 × 104 J m-3 and of the hcp ones to be 2.5 × 102 J m-3.

Ultrasensitive Sub-monolayer Palladium Induced Chirality Switching and Topological Evolution of Skyrmions.

Chiral spin textures are fundamentally interesting, with promise for device applications. Stabilizing chirality is conventionally achieved by introducing Dzyaloshinskii-Moriya interaction (DMI) in asymmetric multilayers, where the thickness of each layer is at least a few monolayers. Here we report an ultrasensitive chirality switching in (Ni/Co)n multilayer induced by capping with only 0.22 monolayer of Pd. Using spin-polarized low-energy electron microscopy, we monitor the gradual evolution of domain walls from left-handed to right-handed Néel walls and quantify the DMI induced by the Pd capping layer. We also observe the chiral evolution of a skyrmion during the DMI switching, where no significant topological protection is found as the skyrmion winding number varies. This corresponds to a minimum energy cost of <1 attojoule during the skyrmion chirality switching. Our results demonstrate the detailed chirality evolution within skyrmions during the DMI sign switching, which is relevant to practical applications of skyrmionic devices.

Tuning Ferromagnetism in a Single Layer of Fe above Room Temperature.

The crystallographic and magnetic properties of an Fe monolayer (ML) grown on 2 ML Au/W(110) substrate are studied with spin-polarized low-energy electron microscopy, density functional theory, and relativistic screened Korringa–Kohn–Rostoker calculations. The single layer of iron atoms possesses hexagonal symmetry and reveals a ferromagnetic order at room temperature. We experimentally demonstrate the possibility of tuning the Curie temperature and the magnitude of magnetization of the Fe monolayer by capping with Au. Taking into account several structural models, the calculation results mostly show ferromagnetic states with enhanced magnetic moments of Fe atoms compared to their bulk value and a further increase in their value after covering with Au. The theoretically calculated Curie temperatures are in fair agreement with those obtained in the experiments. The calculations, furthermore, found evidence for the presence of frustrated isotropic Fe–Fe exchange interactions, and a discussion of the structural effects on the magnetic properties is provided herein.

Chirality-induced zigzag domain wall in in-plane magnetized ultrathin films

The domain structure in in-plane magnetized Fe/Ni/W(110) films is investigated using spin-polarized low-energy electron microscopy. A novel transition of the domain wall shape from a zigzaglike pattern to straight is observed as a function of the film thickness, which is triggered by the transition of the domain wall type from the out-of-plane chiral wall to the in-plane Néel wall. The contribution of the Dzyaloshinskii–Moriya interaction to the wall energy is proposed to explain the transition of the domain wall shape, which is supported by Monte Carlo simulations.

Aberration corrected spin polarized low energy electron microscope

Spin Polarized Low Energy Electron Microscopy (SPLEEM) is a powerful tool to reveal the magnetic structure of ferromagnetic surfaces on the atomic depth scale level[1-3]. With aberration corrected LEEM and a high brightness spin polarized electron gun, high spatial resolution will provide more details for ultra-thin ferromagnetic film studies. This study reports the first realization of aberration corrected SPLEEM (AC-SPLEEM). The performance of the setup was tested on ferromagnetic Fe nanoscale islands on a W(110) single crystal, with spatial resolution of 3.3 nm in spin asymmetry images.

Characteristic magnetic domain size in Fe with exchange-coupled antiferromagnetic NiO underlayer

Characteristic size of magnetic domains in Fe films deposited on NiO layers was measured by spin-polarized low-energy electron microscopy. Our observation results and statistical analysis revealed the increase of magnetic domain sizes with the Fe-thickness increase. Interestingly, the evolution of magnetic domain sizes in Fe showed a strong dependence on the thickness of NiO underneath, or thicker NiO lead the formation of smaller magnetic domains in Fe. This phenomenon can be explained by the increase of the interlayer exchange coupling between Fe and the polycrystalline NiO. It is consistent with the results of recent studies that spin dynamics at a ferromagnet/antiferromagnet interface is affected by the domain structure. Our results suggest a new route to manipulate the micromagnetic structure without the application of external magnetic field.

Fine-tuning of canted magnetization in stepped Fe films through thickness variation, Au capping, and quantum confinement

Author(s): Daobrowski, M; Cinal, M; Schmid, AK; Kirschner, J; Przybylski, M | Abstract: We present a joint experimental and theoretical study that demonstrates how to efficiently control a canted state of magnetization in Fe films grown on Ag(001) vicinal surface and precisely characterize it with the magneto-optical Kerr effect. It is shown that by employing different mechanisms to tune the magnetization tilting angle, any magnetization orientation within the plane perpendicular to the step edges can be achieved. In particular, increasing the Fe film thickness leads to continuous rotation of the magnetization easy axis toward the film surface and the sense of this rotation in uncovered films is opposite to that in films covered with Au. Another tuning mechanism is provided by oscillatory changes of the tilting angle at low temperatures due to formation of quantum well states in Fe films. The observed canting of magnetization is explained within a phenomenological model by an interplay of the shape anisotropy and two magnetocrystalline anisotropy terms, perpendicular and step-induced anisotropies, which results in an effective uniaxial magnetic anisotropy. The fitted thickness dependencies of the anisotropy constants accurately reproduce experimental variations of the tilting angle with both Fe and Au thicknesses as well as transient changes of the magnetization orientation in ultrathin Fe films upon submonolayer Au coverage, observed with spin-polarized low-energy electron microscopy.

Magnetic domain wall contrast under zero domain contrast conditions in spin polarized low energy electron microscopy

Important applications of spin polarized low energy electron microscopy (SPLEEM) employ this technique's vector imaging capability to resolve domain wall (DW) spin textures. Studying several thin film systems including Co/W(110), Co/Cu(001) and (Co/Ni)n/W(110), we show that an additional contrast can appear at magnetic DWs. By imaging the magnetization as a function of electron landing energy, electron energies are selected at which the magnetic domain contrast vanishes. Surprisingly, under such conditions of zero contrast between magnetic domains, we observe the appearance of magnetic contrast outlining the DWs. This DW contrast does not depend on the DW spin texture. Instead, our measurements show that this DW contrast results from a combination of the energy-dependence of the spin reflectivity asymmetry of the magnetic film, the finite energy width of the spin polarized electron source, and the dispersion of the magnetic prism array that separates the illumination and imaging columns of the instrument. Awareness of this DW contrast mechanism is useful to aid correct interpretation of SPLEEM images.

Observation of surface step bunch induced perpendicular magnetic anisotropy using spin-polarized low energy electron microscopy

Using spin-polarized low energy electron microscopy (SPLEEM), we observed surface step bunch induced perpendicular magnetic anisotropy in Fe/Ni bilayers grown on Cu(001) single crystal as well as in Ni/Co/Pd trilayers grown on W(110) crystal. On Cu(100) the formation of step bunches can be stimulated or suppressed by high- or low-temperature annealing cycles, respectively. SPLEEM images resolving the three dimensional magnetization vector in the Fe/Ni films grown on step bunched Cu(100) reveal an additional perpendicular magnetic anisotropy in regions near step bunches. In contrast, no extra perpendicular magnetic anisotropy is observed on low-temperature annealed Cu(100) featuring single-atom height step arrays. Additional investigation of Ni/Co/Pd trilayers on W(110) reveals the influence of step bunch orientation on magnetic anisotropy. Our observations may lead to opportunities for tailoring or patterning anisotropy in magnetic thin-films by controlling film morphology.

Fe on W(001) from continuous films to nanoparticles: Growth and magnetic domain structure

The evolution of the structural and magnetic properties of Fe films during growth on the W(001) surface have been studied with low energy electron diffraction, real-time low energy electron microscopy, and quasi-real-time, spin-polarized low energy electron microscopy in the absence of a magnetic field (virgin state). Depending on the growth temperature, different growth modes are observed: growth of atomically rough and highly strained (10.4% tensile) pseudomorphic films at room temperature, kinetically limited layer-by-layer growth (quasi--Frank-van der Merwe growth mode) of smooth pseudomorphic films up to 4 monolayers at around 500 K and growth of fully relaxed three-dimensional Fe islands on top of a thermodynamically stable 2-monolayer-thick wetting layer (Stranski-Krastanov growth mode) at and above 700 K. Around 500 K, layered growth is terminated by partial (2 monolayers) dewetting of the metastable Fe film and formation of thin, partially relaxed, elongated islands on a thermodynamically stable 2 monolayer film. Ferromagnetic order is first detected during growth at room temperature at 2.35 monolayer Fe film thickness. The magnetization is in-plane with a thickness-dependent direction, rotating from the substrate $\ensuremath{\langle}110\ensuremath{\rangle}$ directions at 3 monolayers toward the $\ensuremath{\langle}100\ensuremath{\rangle}$ directions at 4 monolayers and back again toward the $\ensuremath{\langle}110\ensuremath{\rangle}$ directions at about 8 monolayers. The in-plane spin reorientation that occurs at room temperature is accompanied by significant changes of the magnetic domain structure. In the Frank-van der Merwe growth regime, large magnetic domains are observed in metastable 3 and 4 monolayer films. The isolated three-dimensional Fe islands that form in the Stranski-Krastanov regime have vortex, quasi-single domain ($C$ state), or single magnetic domain structures, depending on their size and shape. The detailed results that are obtained with high thickness, lateral and azimuthal angular resolution with spin-polarized low energy electron microscopy are compared with earlier laterally averaging and laterally resolving magnetic studies, and discrepancies are explained.

Design and commissioning of an aberration-corrected ultrafast spin-polarized low energy electron microscope with multiple electron sources

We describe the design and commissioning of a novel aberration-corrected low energy electron microscope (AC-LEEM). A third magnetic prism array (MPA) is added to the standard AC-LEEM with two prism arrays, allowing the incorporation of an ultrafast spin-polarized electron source alongside the standard cold field emission electron source, without degrading spatial resolution. The high degree of symmetries of the AC-LEEM are utilized while we design the electron optics of the ultrafast spin-polarized electron source, so as to minimize the deleterious effect of time broadening, while maintaining full control of electron spin. A spatial resolution of 2nm and temporal resolution of 10ps (ps) are expected in the future time resolved aberration-corrected spin-polarized LEEM (TR-AC-SPLEEM). The commissioning of the three-prism AC-LEEM has been successfully finished with the cold field emission source, with a spatial resolution below 2nm.

Magnetism of epitaxial Tb films on W(110) studied by spin-polarized low-energy electron microscopy

Thin epitaxial films of Tb metal were grown on a clean W(110) substrate in ultra-high vacuum and studied in-situ by low-energy electron microscopy. Annealed films present magnetic contrast in spin-polarized low-energy electron microscopy. The energy dependence of the electron reflectivity was determined and a maximum value of its spin asymmetry of about 1\% was measured. The magnetization direction of the Tb films is in-plane. Upon raising the temperature, no change in the domain distribution is observed, while the asymmetry in the electron reflectivity decreases when approaching the critical temperature, following a power law $ \sim (1 - T/T_C)^\beta$ with a critical exponent $\beta$ of 0.39.

Controlling magnetic interfaces using ordered surface alloys

We have investigated the growth and magnetic properties of Fe thin films on the clean W(100) surface and W(100)-M c(2 \ifmmode\times\else\texttimes\fi{} 2) ($M=\mathrm{Cu}$, Ag, Au) surface alloy substrates. The influence of the interface on magnetism is assessed experimentally by studying sensitive threshold behavior in magnetic ordering using spin-polarized low-energy electron microscopy. The onset of ferromagnetic order that occurs with increasing film thickness at room temperature due to finite-sized scaling of the Curie temperature varies reproducibly among films on W(100) and the surface alloys. Magnetic moments and exchange coupling constants of the magnetic ground states are also determined theoretically for films with ideal interfaces by first-principles density functional theory calculations. These microscopic quantities are consistently enhanced in Fe films on the noble metal-induced surface alloys compared to their values in films on the clean W(100) surface. We attribute the systematic variation of magnetic onset observed experimentally to the competition between the intrinsically enhanced magnetic coupling and moments on the surface alloy substrates and several extrinsic factors that could suppress magnetic ordering, including intermixing, substrate and film roughness, and surface alloy disorder. Tendencies for intermixing are explored theoretically by determining the energy barrier for noble metal segregation. Despite these possible extrinsic effects, the results suggest that the use of the broad class of ordered surface alloys as alternative substrates may offer greater opportunities for manipulating thin film magnetism.

Magnetic measurements with atomic-plane resolution.

Rapid development of magnetic nanotechnologies calls for experimental techniques capable of providing magnetic information with subnanometre spatial resolution. Available probes of magnetism either detect only surface properties, such as spin-polarized scanning tunnelling microscopy, magnetic force microscopy or spin-polarized low-energy electron microscopy, or they are bulk probes with limited spatial resolution or quantitativeness, such as X-ray magnetic circular dichroism or classical electron magnetic circular dichroism (EMCD). Atomic resolution EMCD methods have been proposed, although not yet experimentally realized. Here, we demonstrate an EMCD technique with an atomic size electron probe utilizing a probe-corrected scanning transmission electron microscope in its standard operation mode. The crucial element of the method is a ramp in the phase of the electron beam wavefunction, introduced by a controlled beam displacement. We detect EMCD signals with atomic-plane resolution, thereby bringing near-atomic resolution magnetic circular dichroism spectroscopy to hundreds of laboratories worldwide.

Canted stripe phase evolution due to a spin reorientation transition in Fe films grown on Ag(001) vicinal surface

The evolution of the domain structure with the thickness of bcc Fe films deposited on the Ag(116) vicinal surface is studied by spin-polarized low-energy electron microscopy. We show that a spin reorientation transition proceeds via two mechanisms: continuous rotation of magnetization within the vertical plane perpendicular to the steps and discontinuous reorientation of the in-plane component of magnetization, leading to splitting of the domains. In contrast to previously investigated systems with stripe domains, we reveal that in the case of a vicinal ferromagnetic surface, the domain width increases while changing the orientation of the magnetization from a canted out-of-plane state into an in-plane state. A theoretical model developed in this work successfully describes the domain structure behavior observed in our experiments and can be equally applied to other ferromagnetic films grown on vicinal surfaces.

Improvement of Quantum Efficiency in Transmission-Type Spin-Polarized Photocathode

We successfully developed a new transmission-type GaAs/GaAsP strained superlattice photocathode with an AlGaAs transparent inter-layer and Si3N4 anti-reflection coating. The electrons emitted from this photocathode showed a high spin polarization of 90% with a quantum efficiency as high as 0.4%. In the application for spin-polarized low energy electron microscope, a high emission current of over 1 µA was observed at 3.6 mW pump laser power. Transmission electron microscopy observation revealed that there were a small disorder and some dislocations in the GaAs/GaAsP superlattice layers. The disordered superlattice layers result in a fluctuation of the superlattice band structure and the dislocations trap the photo-electrons during the diffusion to the surface. Both of the defects influenced the performance of spin-polarized photocathode.

Development of high brightness and high spin-polarized low energy electron microscopy and application to spintronics magnetic thin film materials

Development of high brightness and high spin-polarized low energy electron microscopy and application to spintronics magnetic thin film materials