arXiv subjects

Naoya Shibata

Publications and source records attributed to Naoya Shibata.

12 recordsLinked to original sources

arXiv2026

Nano-scale visualization of magnetic vortices in metal nanoparticles

Magnetic vortices in individual nanoparticles are fundamental spin structures that govern the properties of next-generation magnetic devices and biomedical applications. However, directly imaging their complete structure, from the circulating in-plane magnetization to the nanometer scale out-of-plane core, remains challenging. Here, direct and quantitative visualization of magnetic vortex structures in individual cobalt nanoparticles is achieved by integrating a time-reversal methodology with tilt-scan-averaged differential phase contrast scanning transmission electron microscopy in a magnetic-field-free environment. This approach enables magnetic imaging in conjunction with atomic-scale analysis and reveals a correlation between particle geometry and internal demagnetizing fields. In addition, dynamic evolution of the vortex under in situ magnetic-field application is tracked, enabling unambiguous determination of the out-of-plane core polarity. This approach provides a powerful platform for correlating atomic-scale structure and magnetism within individual nanoparticles and for understanding the origins of nanoscale magnetic properties, thereby supporting the rational design of advanced nanomagnetic materials and devices.

cond-mat.mtrl-sci↗

arXiv2026

Three-Dimensional Atomic-Scale Structural Transformation in a SrTiO3 Grain Boundary

Grain boundaries (GBs) in complex oxides play critical roles in governing their functional properties, which are intrinsically linked to their three-dimensional (3D) atomic configurations and local chemical environments that can deviate markedly from those of the bulk. However, the 3D atomic structures of GBs remain poorly understood due to the projection limitations of conventional (S)TEM. Here, using multislice electron ptychography, we resolve the 3D atomic structure of a {\Sigma}13(510)/[001] tilt GB in SrTiO3 with simultaneous visualization of both cation and oxygen columns. Depth-resolved reconstruction reveals pronounced structural inhomogeneity along the GB, uncovering a transition from the canonical symmetric configuration (STR1) to an asymmetric configuration (STR2) that is hidden in conventional projection imaging. Quantitative analysis of atomic-column intensities demonstrates that these two GB configurations possess distinct local chemical and vacancy distributions. By further mapping the atomic displacement fields, we reveal that the transformation between STR1 and STR2 proceeds via local atomic shuffling at the GB core and collective shear displacement in the adjoining grains, mediated by the step and dislocation character of the junction, respectively. Moreover, analysis of oxygen octahedral rotations reveals a strong dependence on the local atomic structure with pronounced asymmetry around the STR2 region. These findings establish a direct link among the 3D atomic structure, local chemical composition, and lattice order parameters at the GB, underscoring the critical importance of depth-resolved characterization in understanding and engineering GB-mediated functionalities in complex oxides.

cond-mat.mtrl-sci↗

arXiv2025

Twisted oxide membrane interface by local atomic registry design

Interplay of lattice, orbital, and charge degrees of freedom in complex oxide materials has hosted a plethora of exotic quantum phases and physical properties. Recent advances in synthesis of freestanding complex oxide membranes and twisted heterostructures assembled from membranes provide new opportunities for discovery using moiré design with local lattice control. To this end, we designed moiré crystals at the coincidence site lattice condition, providing commensurate structure within the moiré supercell arising from the multi-atom complex oxide unit cell. We fabricated such twisted bilayers from freestanding SrTiO3 membranes and used depth sectioning-based TEM methods to discover ordered charge states at the moiré interface. By selectively imaging SrTiO3 atomic planes at different depths through the bilayer, we clearly resolved the moiré periodic structure at the twisted interface and found that it exhibits lattice-dependent charge disproportionation in the local atomic registry within the moiré supercell. Our density-functional modelling of the twisted oxide interface predicts that these moiré phenomena are accompanied by the emergence of a two-dimensional flat band that can drive new electronic phases. Our work provides a novel guideline for controlling moiré periodicity in twisted oxides and opens pathways to exploit the new functionalities via moiré lattice-driven charge-orbital correlation.

cond-mat.mtrl-sci↗

arXiv2024

ARIM-mdx Data System: Towards a Nationwide Data Platform for Materials Science

In modern materials science, effective and high-volume data management across leading-edge experimental facilities and world-class supercomputers is indispensable for cutting-edge research. However, existing integrated systems that handle data from these resources have primarily focused just on smaller-scale cross-institutional or single-domain operations. As a result, they often lack the scalability, efficiency, agility, and interdisciplinarity, needed for handling substantial volumes of data from various researchers. In this paper, we introduce ARIM-mdx data system, aiming at a nationwide data platform for materials science in Japan. Currently in its trial phase, the platform has been involving 11 universities and institutes all over Japan, and it is utilized by over 800 researchers from around 140 organizations in academia and industry, being intended to gradually expand its reach. The ARIM-mdx data system, as a pioneering nationwide data platform, has the potential to contribute to the creation of new research communities and accelerate innovations.

cs.DC↗

arXiv2024

Ultra-fast Digital DPC Yielding High Spatio-Temporal Resolution for Low-Dose Phase Characterisation

In the scanning transmission electron microscope, both phase imaging of beam-sensitive materials and characterisation of a material's functional properties using in-situ experiments are becoming more widely available. As the practicable scan speed of 4D-STEM detectors improves, so too does the temporal resolution achievable for both differential phase contrast (DPC) and ptychography. However, the read-out burden of pixelated detectors, and the size of the gigabyte to terabyte sized data sets, remain a challenge for both temporal resolution and their practical adoption. In this work, we show that a high-fidelity DPC phase reconstruction can be achieved from both annular segmented detectors or pixelated arrays with relatively few elements using signal digitisation. Unlike conventional analog data, even at the fastest scan speeds, phase reconstructions from digitised DPC-segment images yield reliable data. Finally, dose fractionation by fast scanning and multi-framing allows for post-process binning of frame streams to balance signal-to-noise ratio and temporal resolution for low-dose phase imaging for in-situ experiments.

cond-mat.mtrl-sci↗

arXiv2024

Real-space tilting method for atomic resolution STEM imaging of nanocrystalline materials

Atomic-resolution scanning transmission electron microscopy (STEM) characterization requires precise tilting of the specimen to high symmetric zone axis, which is usually processed in reciprocal space by following the diffraction patterns. However, for small-sized nanocrystalline materials, their diffraction patterns are too faint to guide the tilting process. Here, a simple and effective tilting method is developed based on the diffraction contrast change of the shadow image in the Ronchigram. We can calculate the misorientation angle of the specimen and tilt it to the zone axis based on the position of the shadow image with lowest intensity. This method requires no prior knowledge of the sample and the maximum misorientation angle we can correct is greater than +-6.9 degree with sub-mrad accuracy. It is processed in real space, without recording the diffraction patterns of the specimens, which can effectively apply to nanocrystalline materials. Combined with the scripting to control the microscope, we can automatically tilt the sample to the zone axis under low dose condition (<0.17 e-/A2/s), which could facilitate the imaging of beam sensitive materials such as zeolites or metal organic frameworks. This automated tilting method could contribute to the atomic-scale characterization of the nanocrystalline materials by STEM imaging.

cond-mat.mtrl-sci↗

arXiv2023

Surface step induced bending in two-dimensional oxide nanosheet

The surface steps play dramatic roles in surface dominated processes and the related properties, in which these roles would be significantly enhanced for the low-dimensional nano or quantum materials since the ratio of surface atoms is largely increased. However, the atomic structures of surface steps in the nano/quantum systems are poorly understood because it is extremely difficult to controllably introduce these defects experimentally. Here, by utilizing the focused sub-Angstrom high energy electron beam induced atomic precise etching in a scanning transmission electron microscope, we fabricate MgO two-dimensional (100) nanosheet as thin as 2 atomic layers, and controllably introduced the surface steps in the nanosheet. It is found that the surface steps could bend the MgO nanosheet and such step-induced bending becomes more pronounced for the nanosheet with less layer numbers. We reveal that the bending of the nanosheets is originated from the step induced step force and the reduced bending stiffness in the nanosheet system.

cond-mat.mtrl-sci↗

arXiv2023

Direct imaging of local atomic structures in zeolite using novel low-dose scanning transmission electron microscopy

Zeolites have been used in industrial applications such as catalysts, ion exchangers, and molecular sieves because of their unique porous atomic structures. However, the direct observation of zeolitic local atomic structures via electron microscopy is difficult owing to their low resistance to electron irradiation. Subsequently, the fundamental relationships between these structures and their properties remain unclear. A novel low-electron-dose imaging technique, optimum bright-field scanning transmission electron microscopy (OBF STEM) has recently been developed. It reconstructs images with a high signal-to-noise ratio and a dose efficiency approximately two orders of magnitude higher than that of conventional methods. Herein, we performed low-dose atomic-resolution OBF STEM observations of an FAU-type zeolite, effectively visualizing all the atomic sites in its framework. Additionally, the complex local atomic structure of the twin boundaries in the zeolite was directly characterized. The results of this study facilitate the characterization of the local atomic structures in many electron-beam-sensitive materials.

cond-mat.mtrl-sci↗

arXiv2020

Stabilization of a honeycomb lattice of IrO$_6$ octahedra in superlattices with ilmenite-type MnTiO$_3$

In the quest for quantum spin liquids, thin films are expected to open the way for the control of intricate magnetic interactions in actual materials by exploiting epitaxial strain and two-dimensionality. However, materials compatible with conventional thin-film growth methods have largely remained undeveloped. As a promising candidate towards the materialization of quantum spin liquids in thin films, we here present a robust ilmenite-type oxide with a honeycomb lattice of edge-sharing IrO$_6$ octahedra artificially stabilized by superlattice formation with an ilmenite-type antiferromagnetic oxide MnTiO$_3$. The stabilized sub-unit-cell-thick Mn-Ir-O layer is isostructural to MnTiO$_3$, having the atomic arrangement corresponding to ilmenite-type MnTiO$_3$ not discovered yet. By spin Hall magnetoresistance measurements, we found that antiferromagnetic ordering in the ilmenite Mn sublattice is suppressed by modified magnetic interactions in the MnO$_6$ planes via the IrO$_6$ planes. These findings lay the foundation for the creation of two-dimensional Kitaev candidate materials, accelerating the discovery of exotic physics and applications specific to quantum spin liquids.

cond-mat.mtrl-sci↗

arXiv2017

Atomic-Scale Structure Relaxation, Chemistry and Charge Distribution of Dislocation Cores in SrTiO3

By using the state-of-the-art microscopy and spectroscopy in aberration-corrected scanning transmission electron microscopes, we determine the atomic arrangements, occupancy, elemental distribution, and the electronic structures of dislocation cores in the 10°tilted SrTiO3 bicrystal. We identify that there are two different types of oxygen deficient dislocation cores, i.e., the SrO plane terminated Sr0.82Ti0.85O3-x (Ti3.67+, 0.48<x<0.91) and TiO2 plane terminated Sr0.63Ti0.90O3-y (Ti3.60+, 0.57<y<1). They have the same Burgers vector of a[100] but different atomic arrangements and chemical properties. Besides the oxygen vacancies, Sr vacancies and rocksalt-like titanium oxide reconstruction are also identified in the dislocation core with TiO2 plane termination. Our atomic-scale study reveals the true atomic structures and chemistry of individual dislocation cores, providing useful insights into understanding the properties of dislocations and grain boundaries.

cond-mat.mtrl-sci↗

arXiv2017

Picometer-scale atom position analysis in annular bright-field STEM imaging

We study the effects of specimen mistilt on the picometer-scale measurement of local structure by combing experiment and simulation in annular bright-field scanning transmission electron microscopy (ABF-STEM). A relative distance measurement method is proposed to separate the tilt effects from the scan noise and scan distortion. We find that under a typical experimental condition a small specimen tilt (~6 mrad) in 25 nm thick SrTiO3 along [001] causes 11.9 pm artificial displacement between O and Sr/TiO columns in ABF image, which is more than 3 times of scan noise and sample drift induced image distortion ~3.2 pm, suggesting the tilt effect could be dominant for the quantitative analysis of ABF images. The artifact depends the crystal mistilt angle, specimen thickness, defocus, convergence angle and uncorrected aberration. Our study provides useful insights into detecting and correcting tilt effects during both experiment operation and data analysis to extract the real structure information and avoid mis-interpretations of atomic structure as well as the properties such as oxygen octahedral distortion/shift.

cond-mat.mtrl-sci↗

arXiv2016

Mechanical force involved multiple fields switching of both local ferroelectric and magnetic domain in a Bi5Ti3FeO15 thin film

Multiferroics have received intense attention due to their great application potential in multi-state information storage devices and new types of sensors. Coupling among ferroic orders such as ferroelectricity, (anti-)ferromagnetism, ferroelasticity, etc. will enable dynamic interaction between these ordering parameters. Direct visualization of such coupling behaviour in single phase multiferroic materials is highly desirable for both applications and fundamental study. Manipulation of both ferroelectric and magnetic domains of Bi5Ti3FeO15 thin film using electric field and external mechanical force is reported, which confirms the magnetoelectric coupling in Bi5Ti3FeO15, indicates the electric and magnetic orders are coupled through ferroelasticity. Due to the anisotropic relaxation of ferroelastic strain, the back-switching of out-of-plane electric domains is not as obvious as in-plane. An inevitable destabilization of the coupling between elastic and magnetic ordering happens because of the elastic strain relaxation, which result in a subsequent decay of magnetic domain switching. Mechanical force applied on the surface of Bi5Ti3FeO15 film generates by an AFM tip will effectively drive a transition of the local ferroelastic strain state, reverse both the polarization and magnetization in a way similar to an electric field. Current work provides a framework for exploring cross-coupling among multiple orders and potential for developing novel nanoscale functional devices.

cond-mat.mtrl-sci↗