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Yuichi Ikuhara

Publications and source records attributed to Yuichi Ikuhara.

At least 19 recordsLinked to original sources

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

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 Σ13(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

Switchable Polarization in an A-site Deficient Perovskite through Vacancy and Cation Engineering

While defects are unavoidable in crystals and often detrimental to material performance, they can be a key ingredient for inducing functionalities when tailored. Here, we demonstrate that an A-site-deficient perovskite Y$_{1/3}$TaO$_3$ exhibits room-temperature ferroelectricity in a $Pb2_1m$ phase, enabled by ordered vacancies coupled with TaO$_6$ octahedral rotations. Defect-ordered perovskites are frequently trapped in centrosymmetric incommensurate states due to competing structural instabilities; we circumvent this by favoring rotational over polar instability through compositional selection. Unlike canonical improper ferroelectrics that are \textit{ferrielectric}, the vanishing dipoles on vacancy layers in Y$_{1/3}$TaO$_3$ allow for a net ferroelectric alignment of local dipoles, resulting in enhanced polarization. Upon heating, Y$_{1/3}$TaO$_3$ transforms to a paraelectric incommensurate phase at $\simeq$750 K, whose atomic arrangement mirrors the domain topology observed in hybrid improper ferroelectrics. Superspace analysis of the modulated phase reveals a route to improve room-temperature polarization, achieved through epitaxial strain, as confirmed by our lattice-dynamics calculations. This defect-ordering strategy should be generalizable to other improper ferroelectrics, including magnetoelectric multiferroics, providing a pathway to amplify otherwise limited macroscopic polarization.

cond-mat.mtrl-sci

Metallic NbS2 one-dimensional van der Waals heterostructures

This study presents the experimental realization of metallic NbS2-based one-dimensional van der Waals heterostructures applying a modified NaCl-assisted chemical vapor deposition approach. By employing a "remote salt" strategy, precise control over NaCl supply was achieved, enabling the growth of high-quality coaxial NbS2 nanotubes on single-walled carbon nanotube-boron nitride nanotube (SWCNT-BNNT) templates. With the remote salt strategy, the morphologies of as synthesized NbS2 could be controlled from 1D nanotubes to suspended 2D flakes. Structural characterization via high-resolution transmission electron microscopy (HRTEM) and scanning transmission electron microscopy (STEM) confirms the formation of crystalline NbS2 nanotubes, revealing a distinct bi-layer preference compared to monolayer-dominated semiconducting transition metal dichalcogenide analogs. Optical analyses using UV-vis-NIR and FTIR spectroscopy highlight the metallic nature of NbS2. With Raman analysis, oxidation studies demonstrate relative higher degradation rate of 1D NbS2 under ambient conditions. Density functional theory (DFT) calculations further elucidate the stabilization mechanism of bi-layer NbS2 nanotubes, emphasizing interlayer charge transfer and Coulomb interactions. This work establishes a robust framework for synthesizing metallic 1D vdW heterostructures, advancing their potential applications in optoelectronics and nanodevices.

cond-mat.mtrl-sci

Establishment of global phase coherence in a highly disordered fractal MgO/MgB2 nanocomposite: Roles of interface, morphology and defect

Recently, we have reported that a highly disordered fractal MgO/MgB2 nanocomposite exhibits bulk-like superconducting properties with isotropic pinning, showing an excellent phase-coherent capability irrespective of the low volume fraction (~30 vol. %) of MgB2 [Uchino et al., Phys. Rev. B 101, 035146 (2020); Teramachi et al,, Phys. Rev. B 108, 155146 (2023)]. Hence, this nanocomposite provides a useful experimental system to investigate the relationship between the structural disorder and the establishment of the superconducting phase coherence. In this work, we show from 3D focused ion beam scanning electron microscopy (FIB-SEM) data that in the nanocomposite, a complex MgO/MgB2 microstructure spreads isotropically throughout the sample with a constant fractal dimension of ~1.67. Atomic-resolution scanning transmission electron microscopy (STEM) has revealed that the MgO/MgB2 interfaces are atomically clean and free from amorphous grain boundaries, even leading to atomically coherent interfaces. Detailed ac susceptibility measurements have demonstrated a smooth crossover from an intragranular to an intergranular superconducting regime, giving evidence of the establishment of the critical state due to strong intergranular coupling just below the superconducting transition temperature. Also, spatially-resolved cathodoluminescence measurements have demonstrated that oxygen vacancies in the MgO-rich phase tend to aggregate near the MgO/MgB2 boundary regions, forming long channels of oxygen vacancies through the nanocomposite. These channels of oxygen vacancies will contribute to the long-range carrier transfer and the related Andreev reflection via coherent tunneling of charge carriers among the oxygen vacancy sites.

cond-mat.supr-con

A Metal-Insulator Transition of the Buried MnO2 Monolayer in Complex Oxide Heterostructure

Functionalities in crystalline materials are determined by 3-dimensional collective interactions of atoms. The confinement of dimensionality in condensed matter provides an exotic research direction to understand the interaction of atoms, thus can be used to tailor or create new functionalities in material systems. In this study, a 2-dimensional transition metal oxide monolayer is constructed inside complex oxide heterostructures based on the theoretical predictions. The electrostatic boundary conditions of oxide monolayer in the heterostructure is carefully designed to tune the chemical, electronic, and magnetic states of oxide monolayer. The challenge of characterizing such an oxide monolayer is overcome by a combination of transmission electron microscopy, x-ray absorption spectroscopy, cross-sectional scanning tunneling microscopy, and electrical transport measurements. An intriguing metal-insulator transition associated with a magnetic transition is discovered in the MnO2 monolayer. This study paves a new route to understand the confinement of dimensionality and explore new intriguing phenomena in condensed matters.

cond-mat.mtrl-sci

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

High-performance solid-state electrochemical thermal switches with earth-abundant cerium oxide

Thermal switches, which electrically turn heat flow on and off, have attracted attention as thermal management devices. Electrochemical reduction/oxidation switches the thermal conductivity (\k{appa}\) of active metal oxide films. The performance of the previously proposed electrochemical thermal switches is low; on/off \k{appa}\-ratio is mostly less than 5 and \k{appa}\-switching width is less than 5 W/mK. We used CeO2 thin film as the active layer deposited on a solid electrolyte YSZ substrate. When the CeO2 thin film was reduced once (off-state) and then oxidized (on-state), \k{appa}\ was about 2.2 W/mK in the most reduced state, and \k{appa}\ increased with oxidation to 12.5 W/mK (on-state). This reduction (off-state)/oxidation (on-state) cycle was repeated 100 times and the average value of \k{appa}\ was 2.2 W/mK after reduction (off-state) and 12.5 W/mK after oxidation (on-state). The on/off \k{appa}\-ratio was 5.8 and \k{appa}\-switching width was 10.3 W/mK. The CeO2-based solid-state electrochemical thermal switches would be potential devices for thermal shutters and thermal displays.

cond-mat.mtrl-sci

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

Enhanced ferromagnetism in artificially stretched lattice in quasi two-dimensional Cr2Ge2Te6

In the fundamental understanding of magnetic interactions between atoms in solids, the crystal lattice is one of the key parameters. As the effective tool for controlling the lattice using tensile stress is limited, there are only few demonstrations of the control in magnetic properties with expanding the lattice structure. Here, we observe that the Curie temperature (Tc) of quasi two-dimensional Cr2Ge2Te6 with NiO overlayer doubles from ~60 K to ~120 K, describe a clear correlation of magnetic properties with lattice expansion, which is characterized by several probes and computational approaches, and address on the mechanisms leading to the increase in Tc via the change in exchange interactions.

cond-mat.mtrl-sci

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

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

Ultrahigh toughness polycrystalline ceramics without fading of strength

Zirconia ceramics have been known as a structural material with high fracture toughness and strength since Garvie et al. discovered phase transformation toughening in 1975 [1]. Although these mechanical properties are the most excellent among the advanced ceramics, the toughness has not yet reached the level of metallic materials. Here, we demonstrate for the first time that 2.9 mass% Y2O3-stabilized ZrO2s doped with Al2O3 greatly exceed the toughness of conventional zirconia ceramics which is comparable to those of metallic materials, even with slightly higher strength. The excellent mechanical properties in the proposed ceramic materials will be useful for further expanding the application of advanced ceramics to many engineering fields.

cond-mat.mtrl-sci

One-dimensional van der Waals Heterostructures: Growth Mechanism and Handedness Correlation Revealed by Non-destructive TEM

In this work, we perform a follow-up and comprehensive study on the structural details and formation mechanism of chemical vapor deposition (CVD) synthesized one-dimensional (1D) van der Waals heterostructures. Edge structures, nucleation sites, crystal epitaxial relationships are clearly revealed using transmission electron microscopy (TEM). This is achieved by the direct synthesis of heteronanotubes on a CVD-compatible Si/SiO2 TEM grid, which enabled a transfer-free and non-destructive access to many intrinsic structural details. In particular, we have distinguished different shaped boron nitride nanotube (BNNT) edges, which are confirmed, by electron diffraction at the same location, to be strictly associated with its own chiral angle and polarity. We also demonstrate the importance of surface cleanness and isolation for the formation of perfect 1D heterostructures. Furthermore, we elucidate the handedness correlation between SWCNT template and BNNT crystals. This work not only provides an in-depth understanding of this new 1D heterostructure material group, but also, in a more general perspective, serves as an interesting investigation on crystal growth on highly curved (radius of a couple of nm) atomic substrates.

cond-mat.mtrl-sci

High electrical conducting deep-ultraviolet-transparent oxide semiconductor La-doped SrSnO3 exceeding ~3000 S cm-1

La-doped SrSnO3 (LSSO) is known as one of deep-ultraviolet (DUV)-transparent conducting oxides with an energy bandgap of ~4.6 eV. Since LSSO can be grown heteroepitaxially on more wide bandgap substrates such as MgO (Eg ~7.8 eV), LSSO is considered to be a good candidate as a DUV-transparent electrode. However, the electrical conductivity of LSSO films are below 1000 S cm^-1, most likely due to the low solubility of La ion in the LSSO lattice. Here we report that high electrically conducting (>3000 S cm^-1) LSSO thin films with an energy bandgap of ~4.6 eV can be fabricated by pulsed laser deposition on MgO substrate followed by a simple annealing in vacuum. From the X-ray diffraction and the scanning transmission electron microscopy analyses, we found that lateral grain growth occurred during the annealing, which improved the activation rate of La ion, leading to a significant improvement of carrier concentration (3.26 x 10^20 cm^-3) and Hall mobility (55.8 cm^2 V^-1 s^-1). The present DUV-transparent oxide semiconductor would be useful as a transparent electrode for developing optoelectronic devices, which transmit and/or emit DUV-light.

cond-mat.mtrl-sci

One-dimensional van der Waals heterostructures

Property by design is one appealing idea in material synthesis but hard to achieve in practice. A recent successful example is the demonstration of van der Waals (vdW) heterostructures,1-3 in which atomic layers are stacked on each other and different ingredients can be combined beyond symmetry and lattice matching. This concept, usually described as a nanoscale Lego blocks, allows to build sophisticated structures layer by layer. However, this concept has been so far limited in two dimensional (2D) materials. Here we show a class of new material where different layers are coaxially (instead of planarly) stacked. As the structure is in one dimensional (1D) form, we name it "1D vdW heterostructures". We demonstrate a 5 nm diameter nanotube consisting of three different materials: an inner conductive carbon nanotube (CNT), a middle insulating hexagonal boron nitride nanotube (BNNT) and an outside semiconducting MoS2 nanotube. As the technique is highly applicable to other materials in the current 2D libraries,4-6 we anticipate our strategy to be a starting point for discovering a class of new semiconducting nanotube materials. A plethora of function-designable 1D heterostructures will appear after the combination of CNTs, BNNTs and semiconducting nanotubes.

cond-mat.mtrl-sci

Buffer layer-less fabrication of high-mobility transparent oxide semiconductor, La-doped BaSnO3

Transparent oxide semiconductors (TOSs) showing both high visible transparency and high electron mobility have attracted great attention towards the realization of advanced optoelectronic devices. La-doped BaSnO3 (LBSO) is one of the most promising TOSs because its single crystal exhibits a high electron mobility. However, in the LBSO films, it is very hard to obtain high mobility due to the threading dislocations, which are originated from the lattice mismatch between the film and the substrate. Therefore, many researchers have tried to improve the mobility by inserting a buffer layer. While the buffer layers increased the electron mobilities, this approach leaves much to be desired since it involves a two-step film fabrication process and the enhanced mobility values are still significantly lower than single crystal values. We show herein that the electron mobility of LBSO films can be improved without inserting any buffer layers if the films are grown under highly oxidative ozone (O3) atmospheres. The O3 environments relaxed the LBSO lattice and reduced the formation of Sn2+ states, which are known to suppress the electron mobility in LBSO. The resultant O3-LBSO films showed improved mobility values up to 115 cm2 V-1 s-1, which is among the highest in LBSO films on SrTiO3 substrates and comparable to LBSO films with buffer layers.

cond-mat.mtrl-sci

Large thickness dependence of the carrier mobility in a transparent oxide semiconductor, La-doped BaSnO3

We report herein that the carrier mobility of the 2%-La-doped BaSnO3 (LBSO) films on (001) SrTiO3 and (001) MgO substrates strongly depends on the thickness whereas it is unrelated to the lattice mismatch (+5.4% for SrTiO3, -2.3% for MgO). Although we observed large differences in the lattice parameters, the lateral grain size (~85 nm for SrTiO3, ~20 nm for MgO), the surface morphology and the density of misfit dislocations, the mobility increased almost simultaneously with the thickness in both cases and saturated at ~100 cm2 V-1 s-1, together with the approaching to the nominal carrier concentration (=[2% La3+]), clearly indicating that the behavior of mobility depends on the film thickness. The present results would be beneficial to understand the behavior of mobility and fruitful to further enhance the mobility of LBSO films.

cond-mat.mtrl-sci