Nonmagnetic framboid and associated iron nanoparticles with a space-weathered feature from asteroid Ryugu.

Extraterrestrial minerals on the surface of airless Solar System bodies undergo gradual alteration processes known as space weathering over long periods of time. The signatures of space weathering help us understand the phenomena occurring in the Solar System. However, meteorites rarely retain the signatures, making it impossible to study the space weathering processes precisely. Here, we examine samples retrieved from the asteroid Ryugu by the Hayabusa2 spacecraft and discover the presence of nonmagnetic framboids through electron holography measurements that can visualize magnetic flux. Magnetite particles, which normally provide a record of the nebular magnetic field, have lost their magnetic properties by reduction via a high-velocity (>5 km s-1) impact of a micrometeoroid with a diameter ranging from 2 to 20 µm after destruction of the parent body of Ryugu. Around these particles, thousands of metallic-iron nanoparticles with a vortex magnetic domain structure, which could have recorded a magnetic field in the impact event, are found. Through measuring the remanent magnetization of the iron nanoparticles, future studies are expected to elucidate the nature of the nebular/interplanetary magnetic fields after the termination of aqueous alteration in an asteroid.

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.

Visualization of nanoscale magnetic domain states in the asteroid Ryugu.

In the samples collected from the asteroid Ryugu, magnetite displays natural remanent magnetization due to nebular magnetic field, whereas contemporaneously grown iron sulfide does not display stable remanent magnetization. To clarify this counterintuitive feature, we observed their nanoscale magnetic domain structures using electron holography and found that framboidal magnetites have an external magnetic field of 300 A m-1, similar to the bulk value, and its magnetic stability was enhanced by interactions with neighboring magnetites, permitting a disk magnetic field to be recorded. Micrometer-sized pyrrhotite showed a multidomain magnetic structure that was unable to retain natural remanent magnetization over a long time due to short relaxation time of magnetic-domain-wall movement, whereas submicron-sized sulfides formed a nonmagnetic phase. These results show that both magnetite and sulfide could have formed simultaneously during the aqueous alteration in the parent body of the asteroid Ryugu.

Removal of phase residues in electron holography.

Electron holography provides quantitative phase information regarding the electromagnetic fields and the morphology of micro- to nano-scale samples. A phase image reconstructed numerically from an electron hologram sometimes includes phase residues, i.e. origins of unremovable phase discontinuities, which make it much more difficult to quantitatively analyze local phase values. We developed a method to remove the residues in a phase image by a combination of patching local areas of a hologram and denoising based on machine learning. The small patches for a hologram, which were generated using the spatial frequency information of the own fringe patterns, were pasted at each residue point by an algorithm based on sparse modeling. After successive phase reconstruction, the phase components with no dependency on the vicinity were filtered out by Gaussian process regression. We determined that the phase discontinuities that appeared around phase residues were removed and the phase distributions of an atomic resolution phase image of a Pt nanoparticle were sufficiently restored.

Direct identification of the charge state in a single platinum nanoparticle on titanium oxide.

A goal in the characterization of supported metal catalysts is to achieve particle-by-particle analysis of the charge state strongly correlated with the catalytic activity. Here, we demonstrate the direct identification of the charge state of individual platinum nanoparticles (NPs) supported on titanium dioxide using ultrahigh sensitivity and precision electron holography. Sophisticated phase-shift analysis for the part of the NPs protruding into the vacuum visualized slight potential changes around individual platinum NPs. The analysis revealed the number (only one to six electrons) and sense (positive or negative) of the charge per platinum NP. The underlying mechanism of platinum charging is explained by the work function differences between platinum and titanium dioxide (depending on the orientation relationship and lattice distortion) and by first-principles calculations in terms of the charge transfer processes.

Higher-order structure of barley chromosomes observed by electron tomography.

The higher order structure of the metaphase chromosome has been an enigma for over a century and several different models have been presented based on results obtained by a variety of techniques. Some disagreements in the results between methods have possibly arisen from artifacts caused during sample preparation such as staining and dehydration. Therefore, we treated barley chromosomes with ionic liquid to minimize the effects of dehydration. We also observed chromosomes on a film with holes to keep pristine chromosome structure from being flattened as seen when placed on a continuous support film. A chromosome placed over a hole in a thin carbon film was mounted on a tomography holder, and its structure was observed in three dimensions (3D) using electron tomography. We found that there are periodic structures with 300-400 nm pitch along the axis in barley chromosomes. The pitch sizes are larger than those observed in human chromosomes.

Analysis of spatial point patterns in electron-counting images.

In this study, the spatial counting statistics of free electron beams, which were released via field emission from cold metal and propagated through a vacuum region, were investigated to examine the normal functioning of the counting equipment for electron correlation spectroscopy. The beam electrons were recorded separately according to the locations of individual events as they reached the direct detection transmission Complementary Metal Oxide Semiconductor (CMOS) sensor. We examined the spatial point patterns arising from the locations of the individual events of each primary electron being detected in the case of electrons in a state in which the wave function is constant on the sensor. The quadrat method, which compares the observed frequencies of the number of electron counts in the subsets of the study region with the predicted frequencies from a Poisson distribution, indicates a clustering-type departure from complete spatial randomness. To explore some of the basic principles governing the location of coherent electrons being counted, Ripley's K-function and the corresponding L-function of a stationary spatial point process were used to test the complete spatial randomness from the data. The maximum peak in the average of the L-functions was sensitive only to the mean counts per frame. Thus, clustering of spatial point patterns may result from abnormalities in the direct detection camera. When the interaction of the beam electrons with the sensor is included in the simulation, there is a reasonable match between the average of the L-functions and the experimental curves with the theoretically simulated curves.

Improved efficiency in automated acquisition of ultra-high-resolution electron holograms using automated target detection.

An automated hologram acquisition system for big-data analysis and for improving the statistical precision of phase analysis has been upgraded with automated particle detection technology. The coordinates of objects in low-magnification images are automatically detected using zero-mean normalized cross-correlation with preselected reference images. In contrast with the conventional scanning acquisitions from the whole area of a microgrid and/or a thin specimen, the new method allows efficient data collections only from the desired fields of view including the particles. The acquisition time of the cubic/triangular nanoparticles that were observed was shortened by about one-fifty eighth that of the conventional scanning acquisition method because of efficient data collections. The developed technology can improve statistical precision in electron holography with shorter acquisition time and is applicable to the analysis of electromagnetic fields for various kinds of nanoparticles.

Higher-Order Structure of Human Chromosomes Observed by Electron Diffraction and Electron Tomography.

It is well known that two DNA molecules are wrapped around histone octamers and folded together to form a single chromosome. However, the nucleosome fiber folding within a chromosome remains an enigma, and the higher-order structure of chromosomes also is not understood. In this study, we employed electron diffraction which provides a noninvasive analysis to characterize the internal structure of chromosomes. The results revealed the presence of structures with 100­200 nm periodic features directionally perpendicular to the chromosome axis in unlabeled isolated human chromosomes. We also visualized the 100­200 nm periodic features perpendicular to the chromosome axis in an isolated chromosome whose DNA molecules were specifically labeled with OsO4 using electron tomography in 300 keV and 1 MeV transmission electron microscopes.

Development of a Mach-Zehnder type electron interferometer on a 1.2-MV field-emission transmission electron microscope.

We have developed an amplitude-division type Mach-Zehnder electron interferometer (MZ-EI). The developed MZ-EI is composed of single crystals corresponding to amplitude-division beam splitters, lenses corresponding to mirrors and an objective aperture. The spacings and azimuth angles of interference fringes can be controlled by single crystal materials and their orientations and by diffraction spots selected by the objective aperture. We built the MZ-EI on a 1.2-MV field-emission transmission electron microscope and tested its performance. Results showed that interference fringes were created for various spacings and azimuth angles, which demonstrates the practicability of the MZ-EI as an amplitude-division type electron interferometer.

Automated acquisition of vast numbers of electron holograms with atomic-scale phase information.

An automated acquisition system for collecting a large number of electron holograms, to improve the statistical precision of phase analysis, was developed. A technique for shifting the electron beam in combination with stage movement allows data to be acquired over a wide area of a TEM-specimen grid. Undesired drift in the hologram position, which may occur during the hologram acquisition, can be corrected in real time by automated detection of the interference-fringe region in an image. To demonstrate the usefulness of the developed automated hologram acquisition system, gold nanoparticles dispersed on a carbon foil were observed with a 1.2-MV atomic resolution holography electron microscope. The system could obtain 1024 holograms, which provided phase maps for more than 500 nanoparticles with a lateral resolution of 0.14 nm, in just 1 h. The observation results revealed an anomalous increase in mean inner potential for a particle size smaller than 4 nm. The developed automated hologram acquisition system can be applied to improve the precision of phase measurement by averaging many phase images, as demonstrated by single particle analysis for biological entities. Moreover, the system makes it possible to study electrostatic potential of catalysts and other functional nanoparticles at atomic resolution.

Beam brightness and its reduction in a 1.2-MV cold field-emission transmission electron microscope.

In this paper we discuss probe properties in terms of probe currents, probe sizes, energy spread, virtual source sizes, and brightness in a 1.2-MV cold field-emission (cold FE) transmission electron microscope (TEM) equipped with a magnetic gun lens. The probe size increased gradually in proportion to the (3/8)th power of the probe current, very unusual behavior in cold FE guns but typical behavior in thermionic guns. This is due to the magnetic gun lens, which caused large emission angles for electron beams in the probe before being limited by aberrations at the gun and acceleration tube. The brightness reached the maximum at 1.62 × 1014 A/(m2sr) and then decreased with increasing the emission current. The energy spread of the beam, including the Boersch effect, was 0.32-0.50 eV, comparable to that of conventional cold FE guns without magnetic gun lens. Experimental analysis indicated that neither noises nor aberrations caused the probe size increase under the optimized illumination condition. The virtual source size increased from 11.1 to 24.7 nm with the increase in the emission current. To describe this behavior, we conjecture that this brightness reduction is due to increase in the virtual source size caused by trajectory displacement created by stochastic Coulomb interactions near the emitter.

Electron holography on Fraunhofer diffraction.

Electron holography in Fraunhofer region was realized by using an asymmetric double slit. A Fraunhofer diffraction wave from a wider slit worked as an objective wave interfered with a plane wave from a narrower slit as a reference wave under the pre-Fraunhofer condition and recorded as a hologram. Here, the pre-Fraunhofer condition means that the following conditions are simultaneously satisfied: single-slit observations are performed under the Fraunhofer condition and the double-slit observations are performed under the Fresnel condition. Amplitude and phase distributions of the Fraunhofer diffraction wave were reconstructed from the hologram by the Fourier transform reconstruction method. The reconstructed amplitude and phase images corresponded to Fraunhofer diffraction patterns; in particular, the phase steps of π at each band pattern in the phase image were confirmed. We hope that the developed Fraunhofer electron holography can be extended to a direct phase detection method in the reciprocal space.

A 0.5-T pure-in-plane-field magnetizing holder for in-situ Lorentz microscopy.

A side-entry specimen holder capable of applying a 0.5-tesla in-plane magnetic-induction field for in-situ transmission electron microscopy was developed. Three miniaturized electromagnets with 300 × 300-µm pole area and 180-µm pole gap are stacked along the electron-beam path in the holder. The middle magnet is used for magnetizing the specimen, which is inserted into the pole gap by using a 40-µm-width cantilever for atomic-force microscopy. The upper and lower magnets are used to keep the electron beam parallel to the optical axis. Magnetic-field magnitude was determined on the basis of experimentally measured electron-deflection angles and induction-field profiles along the electron-beam path calculated by finite element electromagnetic simulation. Magnetization reversal in 300-nm-thick Nd-Fe-B magnets from the saturated state was in-situ observed by using the holder and a 1-MeV cold-field-emission transmission electron microscope. The observation revealed that domain-wall pinning occurred in different manners at the c-plane and non-c-plane grain boundaries. The holder was thereby shown to be useful for analysis of magnetization-reversal behaviors of hard magnetic materials.

Illumination semiangle of 10-9 rad achieved in a 1.2-MV atomic resolution holography transmission electron microscope.

The coherency of a 1.2-MV transmission electron microscope was evaluated through illumination semiangles calculated from lengths over which Fresnel fringes can be observed. These lengths were determined from the diameters of circular holes fully filled with Fresnel fringes, i.e. this method allows lengths to be accurately measured even if micrographs are subjected to distortions. The smallest illumination semiangle of 4.0 × 10-9 rad was obtained for a circular hole with a diameter of 191 µm. In addition, electron beam brightness was estimated to be approximately 3 × 1014 A/m2·sr from the obtained illumination semiangle values and current densities. The results provide us with essential information that can be referred to in future electron holography studies aimed at detecting weak electromagnetic fields in materials.

Interference experiment with asymmetric double slit by using 1.2-MV field emission transmission electron microscope.

Advanced electron microscopy technologies have made it possible to perform precise double-slit interference experiments. We used a 1.2-MV field emission electron microscope providing coherent electron waves and a direct detection camera system enabling single-electron detections at a sub-second exposure time. We developed a method to perform the interference experiment by using an asymmetric double-slit fabricated by a focused ion beam instrument and by operating the microscope under a "pre-Fraunhofer" condition, different from the Fraunhofer condition of conventional double-slit experiments. Here, pre-Fraunhofer condition means that each single-slit observation was performed under the Fraunhofer condition, while the double-slit observations were performed under the Fresnel condition. The interference experiments with each single slit and with the asymmetric double slit were carried out under two different electron dose conditions: high-dose for calculation of electron probability distribution and low-dose for each single electron distribution. Finally, we exemplified the distribution of single electrons by color-coding according to the above three types of experiments as a composite image.

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.

Magnetic field observations in CoFeB/Ta layers with 0.67-nm resolution by electron holography.

Nanometre-scale magnetic field distributions in materials such as those at oxide interfaces, in thin layers of spintronics devices, and at boundaries in magnets have become important research targets in materials science and applied physics. Electron holography has advantages in nanometric magnetic field observations, and the realization of aberration correctors has improved its spatial resolution. Here we show the subnanometre magnetic field observations inside a sample at 0.67-nm resolution achieved by an aberration-corrected 1.2-MV holography electron microscope with a pulse magnetization system. A magnetization reduction due to intermixing in a CoFeB/Ta multilayer is analyzed by observing magnetic field and electrostatic potential distributions simultaneously. Our results demonstrate that high-voltage electron holography can be widely applied to pin-point magnetization analysis with structural and composition information in physics, chemistry, and materials science.

Information transfer of 25.5 nm-1 in a 1-MV field-emission transmission electron microscope.

Information transfer of a 1-MV field-emission transmission electron microscope (TEM) was improved by reducing mechanical vibrations and improving the stability of an acceleration voltage. The resulting mechanical stability was estimated from lattice fringes with an obtained spacing of 19.6 pm under achromatic conditions. This value corresponds to a vibration amplitude of <19.6 pm. The stability of the acceleration voltage was improved by reducing thermal noises in the power supply. As a result, 39.2-pm-spacing linear lattice fringes were obtained under chromatic conditions. This indicates that 25.5 nm(-1) information transfer was accomplished in the 1 MV field-emission TEM.

Three-dimensional observation of magnetic vortex cores in stacked ferromagnetic discs.

Electron holographic vector field electron tomography visualized three-dimensional (3D) magnetic vortices in stacked ferromagnetic discs in a nanoscale pillar. A special holder with two sample rotation axes, both without missing wedges, was used to reduce artifacts in the reconstructed 3D magnetic vectors. A 1 MV holography electron microscope was used to precisely measure the magnetic phase shifts. Comparison of the observed 3D magnetic field vector distributions in the magnetic vortex cores with the results of micromagnetic simulations based on the Landau-Lifshitz-Gilbert equation showed that the proposed technique is well suited for direct 3D visualization of the spin configurations in magnetic materials and spintronics devices.