Search

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., Comment: IEEE BigData 2024, to appear. Project Page https://arim.mdx.jp/

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.

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., Comment: 19 pages, 7 figures with supporting information (12 pages, 11 figures, 1 table)

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.

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., Comment: 5 figures

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.

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.

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.

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., Comment: 19 pages, 7 figures

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., Comment: 16 pages including 5 figures

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.

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., Comment: 15 pages, including 4 figures

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{\deg}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

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., Comment: 25 pages, 10 figures

Thermoelectric energy conversion - the exploitation of the Seebeck effect to convert waste heat into electricity - has attracted an increasing amount of research attention for energy harvesting technology. Niobium-doped strontium titanate (SrTi1-xNbxO3) is one of the most promising thermoelectric material candidates, particularly as it poses a much lesser environmental risk in comparison to materials based on heavy metal elements. Two-dimensional electron confinement, e.g. through the formation of superlattices or two-dimensional electron gases, is recognized as an effective strategy to improve the thermoelectric performance of SrTi1-xNbxO3. Although electron confinement is closely related to the electronic structure, the fundamental electronic phase behavior of the SrTi1-xNbxO3 solid solution system has yet to be comprehensively investigated. Here, we present a thermoelectric phase diagram for the SrTi1-xNbxO3 (0.05 =< x =< 1) solid solution system, which we derived from the characterization of epitaxial films. We observed two thermoelectric phase boundaries in the system, which originate from the step-like decrease in carrier effective mass at x ~ 0.3, and from a local minimum in carrier relaxation time at x ~ 0.5. The origins of these phase boundaries are considered to be related to isovalent/heterovalent B-site substitution: parabolic Ti 3d orbitals dominate electron conduction for compositions with x < 0.3, whereas the Nb 4d orbital dominates when x > 0.3. At x ~ 0.5, a tetragonal distortion of the lattice, in which the B-site is composed of Ti4+ and Nb4+ ions, leads to the formation of tail-like impurity bands, which maximizes the electron scattering. These results provide a foundation for further research into improving the thermoelectric performance of SrTi1-xNbxO3., Comment: 20 pages, 6 figures

Although there are so many reports on the carrier effective mass (m*) of a transparent oxide semiconductor BaSnO3, it is almost impossible to know the intrinsic m* value because the reported m* values are scattered from 0.06 to 3.7 m0. Here we successfully clarified the intrinsic m* of BaSnO3, m*=0.40 0.01 m0, by the thermopower modulation clarification method. We also found the threshold of degenerate/non-degenerate semiconductor of BaSnO3; At the threshold, the thermopower value of both La-doped BaSnO3 and BaSnO3 TFT structure was 240 microvolt k-1, bulk carrier concentration was 1.4E19 cm-3, and two-dimensional sheet carrier concentration was 1.8E12 cm-2. When the EF locates above the parabolic shaped conduction band bottom, rather high mobility was observed. On the contrary, very low carrier mobility was observed when the EF lays below the threshold, most likely due to that the tail states suppress the carrier mobility. The present results are useful for further development of BaSnO3 based oxide electronics., Comment: 16 pages including 4 figures