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Sakata, Osami

Publications and source records attributed to Sakata, Osami.

Transient energy dissipation at the Fermi velocity in a magnetocaloric metal

Realizing fast energy dissipation in crystalline materials over macroscopic length scales is critical for energy-efficient devices and applications toward a carbon-neutral society but is usually dominated by electron-lattice interactions that cap the energy dissipation at the phonon velocity. Going beyond this velocity has been the focus of many studies, and the physical limit is the Fermi velocity where the energy is predominantly carried away by electrons throughout the materials. However, whether and how the Fermi velocity can be reached over macroscopic distances experimentally remain largely elusive. Here we show ultrafast energy dissipation at the Fermi velocity in the magnetocaloric metal LaFe 10.6 Co 1.0 Si 1.4 . Using time-resolved powder x-ray diffraction, we observe negative thermal expansion of the lattice throughout the micron-sized crystals in less than 600 fs with an incident optical fluence higher than 8 J cm -2 . The ultrafast timescale is in sharp contrast to the normal energy dissipation and shows the existence of a macroscopic momentum-relaxing electron mean free path immediately after the optical excitation. In conclusion, our findings open a different regime in energy dissipation and demonstrate the possibility of manipulating macroscopic material properties by strong optical pulses.

Chen, Yanna↗

Structure and properties of densified silica glass: characterizing the order within disorder

The broken symmetry in the atomic-scale ordering of glassy versus crystalline solids leads to a daunting challenge to provide suitable metrics for describing the order within disorder, especially on length scales beyond the nearest neighbor that are characterized by rich structural complexity. Here, we address this challenge for silica, a canonical network-forming glass, by using hot versus cold compression to (i) systematically increase the structural ordering after densification and (ii) prepare two glasses with the same high-density but contrasting structures. The structure was measured by high-energy X-ray and neutron diffraction, and atomistic models were generated that reproduce the experimental results. The vibrational and thermodynamic properties of the glasses were probed by using inelastic neutron scattering and calorimetry, respectively. Traditional measures of amorphous structures show relatively subtle changes upon compacting the glass. The method of persistent homology identifies, however, distinct features in the network topology that change as the initially open structure of the glass is collapsed. The results for the same high-density glasses show that the nature of structural disorder does impact the heat capacity and boson peak in the low-frequency dynamical spectra. Densification is discussed in terms of the loss of locally favored tetrahedral structures comprising oxygen-decorated SiSi 4<:sub> tetrahedra.

36 MATERIALS SCIENCE↗

Dynamic fracture of tantalum under extreme tensile stress

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power optical laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of Embedded Image ~2 × 10 8 to 3.5 × 10 8 s -1 . A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.

36 MATERIALS SCIENCE↗

Formation of (111) orientation-controlled ferroelectric orthorhombic HfO{sub 2} thin films from solid phase via annealing

0.07YO{sub 1.5}-0.93HfO{sub 2} (YHO7) films were prepared on various substrates by pulse laser deposition at room temperature and subsequent heat treatment to enable a solid phase reaction. (111)-oriented 10 wt. % Sn-doped In{sub 2}O{sub 3}(ITO)//(111) yttria-stabilized zirconia, (111)Pt/TiO{sub x}/SiO{sub 2}/(001)Si substrates, and (111)ITO/(111)Pt/TiO{sub x}/SiO{sub 2}/(001)Si substrates were employed for film growth. In this study, X-ray diffraction measurements including θ–2θ measurements, reciprocal space mappings, and pole figure measurements were used to study the films. The film on (111)ITO//(111)yttria-stabilized zirconia was an (111)-orientated epitaxial film with ferroelectric orthorhombic phase; the film on (111)ITO/(111)Pt/TiO{sub x}/SiO{sub 2}/(001)Si was an (111)-oriented uniaxial textured film with ferroelectric orthorhombic phase; and no preferred orientation was observed for the film on the (111)Pt/TiO{sub x}/SiO{sub 2}/(001)Si substrate, which does not contain ITO. Polarization–hysteresis measurements confirmed that the films on ITO covered substrates had saturated ferroelectric hysteresis loops. A remanent polarization (P{sub r}) of 9.6 and 10.8 μC/cm{sup 2} and coercive fields (E{sub c}) of 1.9 and 2.0 MV/cm were obtained for the (111)-oriented epitaxial and uniaxial textured YHO7 films, respectively. These results demonstrate that the (111)-oriented ITO bottom electrodes play a key role in controlling the orientation and ferroelectricity of the phase formation of the solid films deposited at room temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structural studies of metal nanoparticles using high-energy x-ray diffraction

The XRD patterns of nanoparticles exhibit broad Bragg peaks because of small size, where the contribution of diffuse component provides us with inherent structural information. Therefore, pair distribution function obtained from a Fourier transformation of high-energy XRD data and structure modeling on the basis of diffraction data becomes an essential tool to understand the structure of nanoparticles. This promising tool was utilized to obtain structural information of Pd/Pt bimetallic core/shell and solid-solution nanoparticles, which show much attention due to their improved hydrogen storage capacity and catalytic activity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Rietveld analysis using powder diffraction data with anomalous scattering effect obtained by focused beam flat sample method

Focused-beam flat-sample method (FFM) is a new trial for synchrotron powder diffraction method, which is a combination of beam focusing optics, flat shape powder sample and area detectors. The method has advantages for X-ray diffraction experiments applying anomalous scattering effect (anomalous diffraction), because of 1. Absorption correction without approximation, 2. High intensity X-rays of focused incident beams and high signal noise ratio of diffracted X-rays 3. Rapid data collection with area detectors. We applied the FFM to anomalous diffraction experiments and collected synchrotron X-ray powder diffraction data of CoFe{sub 2}O{sub 4} (inverse spinel structure) using X-rays near Fe K absorption edge, which can distinguish Co and Fe by anomalous scattering effect. We conducted Rietveld analyses with the obtained powder diffraction data and successfully determined the distribution of Co and Fe ions in CoFe{sub 2}O{sub 4} crystal structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of mechanical stress on ferroelectricity in (Hf{sub 0.5}Zr{sub 0.5})O{sub 2} thin films

To investigate the impact of mechanical stress on their ferroelectric properties, polycrystalline (Hf{sub 0.5}Zr{sub 0.5})O{sub 2} thin films were deposited on (111)Pt-coated SiO{sub 2}, Si, and CaF{sub 2} substrates with thermal expansion coefficients of 0.47, 4.5, and 22 × 10{sup −6}/ °C, respectively. In-plane X-ray diffraction measurements revealed that the (Hf{sub 0.5}Zr{sub 0.5})O{sub 2} thin films deposited on SiO{sub 2} and Si substrates were under in-plane tensile strain and that their volume fraction of monoclinic phase decreased as this strain increased. In contrast, films deposited on CaF{sub 2} substrates were under in-plane compressive strain, and their volume fraction of monoclinic phase was the largest among the three kinds of substrates. The maximum remanent polarization of 9.3 μC/cm{sup 2} was observed for Pt/(Hf{sub 0.5}Zr{sub 0.5})O{sub 2}/Pt/TiO{sub 2}/SiO{sub 2}, while ferroelectricity was barely observable for Pt/(Hf{sub 0.5}Zr{sub 0.5})O{sub 2}/Pt/TiO{sub 2}/SiO{sub 2}/CaF{sub 2}. This result suggests that the in-plane tensile strain effectively enhanced the ferroelectricity of the (Hf{sub 0.5}Zr{sub 0.5})O{sub 2} thin films.

36 MATERIALS SCIENCE↗

Orientation control and domain structure analysis of {100}-oriented epitaxial ferroelectric orthorhombic HfO{sub 2}-based thin films

Orientation control of {100}-oriented epitaxial orthorhombic 0.07YO{sub 1.5}-0.93HfO{sub 2} films grown by pulsed laser deposition was investigated. To achieve in-plane lattice matching, indium tin oxide (ITO) and yttria-stabilized zirconia (YSZ) were selected as underlying layers. We obtained (100)- and (001)/(010)-oriented films on ITO and YSZ, respectively. Ferroelastic domain formation was confirmed for both films by X-ray diffraction using the superlattice diffraction that appeared only for the orthorhombic symmetry. The formation of ferroelastic domains is believed to be induced by the tetragonal–orthorhombic phase transition upon cooling the films after deposition. The present results demonstrate that the orientation of HfO{sub 2}-based ferroelectric films can be controlled in the same manner as that of ferroelectric films composed of conventional perovskite-type material such as Pb(Zr, Ti)O{sub 3} and BiFeO{sub 3}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Note: An X-ray powder diffractometer with a wide scattering-angle range of 72° using asymmetrically positioned one-dimensional detectors

An X-ray powder diffractometer has been developed for a time-resolved measurement without the requirement of a scattering angle (2θ) scan. Six one-dimensional detector modules are asymmetrically arranged in a vertical line at a designed distance of 286.5 mm. A detector module actually covers a diffraction angle of about 12° with an angular resolution of 0.01°. A diffracted intensity pattern is simultaneously recorded in a 2θ angular range from 1.63° to 74.37° in a “one shot” measurement. We tested the performance of the diffractometer with reference CeO{sub 2} powders and demonstrated diffraction measurements from an operating lithium-air battery.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Negligible substrate clamping effect on piezoelectric response in (111)-epitaxial tetragonal Pb(Zr, Ti)O{sub 3} films

The converse piezoelectric responses of (111)- and (001)-epitaxial tetragonal Pb(Zr{sub 0.35}Ti{sub 0.65})O{sub 3} [PZT] films were compared to investigate the orientation dependence of the substrate clamping effect. Synchrotron X-ray diffraction (XRD) and piezoelectric force microscopy revealed that the as-grown (111)-PZT film has a polydomain structure with normal twin boundaries that are changed by the poling process to inclined boundaries, as predicted by Romanov et al. [Phys. Status Solidi A 172, 225 (1999)]. Time-resolved synchrotron XRD under bias voltage showed the negligible impact of substrate clamping on the piezoelectric response in the (111)-PZT film, unlike the case for (001)-PZT film. The origin of the negligible clamping effect in the (111)-PZT film is discussed from the viewpoint of the elastic properties and the compensation of lattice distortion between neighboring domains.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structure of β-AgGaO{sub 2}; ternary I–III–VI{sub 2} oxide semiconductor with a wurtzite-derived structure

The structure of the wurtzite-derived β-AgGaO{sub 2} was refined by Rietveld analysis of high-resolution powder diffraction data obtained using synchrotron X-ray radiation. The space group of the crystal is Pna2{sub 1} with lattice parameters of a{sub 0}=5.56175 Å, b{sub 0}=7.14749 Å, and c{sub 0}=5.46875 Å. The deviation of O–Ag–O and M–O–M bond angles from the regular tetrahedral angle of 109.5° was very large at ∼8° and ∼11°, respectively. The electronic structure of β-AgGaO{sub 2} is discussed based on its structure, and the indirect band gap of β-AgGaO{sub 2} was related to significant tetrahedral distortion. Although β-AgGaO{sub 2} decomposes into metallic silver and Ga{sub 2}O{sub 3} at a high temperature in any atmosphere, β-AgGaO{sub 2} is stable up to 690 °C under an O{sub 2} atmosphere. No direct transformation from the wurtzite-derived phase to a delafossite phase occurs in β-AgGaO{sub 2}. - Graphical abstract: Crystal structure of β-AgGaO{sub 2} was refined by Rietveld analysis. AgO{sub 4} and O(Ag,Ga){sub 4} tetrahedra are significantly distorted from ideal tetrahedron. - Highlights: • Orthorhombic β-AgGaO{sub 2} with a wurtzite-derived β-NaFeO{sub 2} structure was synthesized. • Its structure was refined by Rietveld analysis of high-resolution XRD data. • Silver and oxygen tetrahedra are significantly distorted from an ideal tetrahedron. • The extent of this tetrahedral distortion is related to the band gap nature. • β-AgGaO{sub 2} is a metastable phase but is stable up to 690 °C in an O{sub 2} atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The valence band structure of Ag{sub x}Rh{sub 1–x} alloy nanoparticles

The valence band (VB) structures of face-centered-cubic Ag-Rh alloy nanoparticles (NPs), which are known to have excellent hydrogen-storage properties, were investigated using bulk-sensitive hard x-ray photoelectron spectroscopy. The observed VB spectra profiles of the Ag-Rh alloy NPs do not resemble simple linear combinations of the VB spectra of Ag and Rh NPs. The observed VB hybridization was qualitatively reproduced via a first-principles calculation. The electronic structure of the Ag{sub 0.5}Rh{sub 0.5} alloy NPs near the Fermi edge was strikingly similar to that of Pd NPs, whose superior hydrogen-storage properties are well known.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Hard X-ray photoelectron spectroscopy of Li{sub x}Ni{sub 1−x}O epitaxial thin films with a high lithium content

The core-level and valence-band electronic structures of Li{sub x}Ni{sub 1−x}O epitaxial thin films with x = 0, 0.27, and 0.48 were studied by hard X-ray photoelectron spectroscopy. A double peak structure, consisting of a main peak and a shoulder peak, and a satellite structure were observed in the Ni 2p{sub 3/2} core-level spectra. The intensity ratio of the shoulder to main peak in this double peak structure increased with increasing lithium content in Li{sub x}Ni{sub 1−x}O. This lithium doping dependence of the Ni 2p{sub 3/2} core-level spectra was investigated using an extended cluster model, which included the Zhang–Rice (ZR) doublet bound states arising from a competition between O 2p – Ni 3d hybridization and the Ni on-site Coulomb interaction. The results indicated that the change in the intensity ratio in the main peak is because of a reduction in the ZR doublet bound states from lithium substitutions. This strongly suggests that holes compensating Li doping in Li{sub x}Ni{sub 1−x}O are of primarily ZR character.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Direct observation of intrinsic piezoelectricity of Pb(Zr,Ti)O{sub 3} by time-resolved x-ray diffraction measurement using single-crystalline films

Lead zirconate titanate, Pb(Zr,Ti)O{sub 3} or PZT, is one of the most widely investigated ferroelectric and piezoelectric materials due to its superior properties. However, the intrinsic properties of PZT have not been directly measured due to the lack of fabrication of single crystals even though a basic understanding of intrinsic properties has been of interest developing lead-free piezoelectric materials. We demonstrated the direct observation of the intrinsic piezoelectric property by means of the detection of electric-field induced crystal lattice distortion of thick Pb(Zr{sub 0.35}Ti{sub 0.65})O{sub 3} single-crystalline films with single polar-axis orientation and negligible residual strain using the time-resolved X-ray diffraction (XRD) together with the polarization response. Consequently, the effective converse piezoelectric response was experimentally revealed; hence, the electrostrictive coefficient, which is the conversion coefficient between the electrical and mechanical response, was determined. The obtained effective electrostrictive coefficient was 5.2–6.3 × 10{sup −2} m{sup 4}/C{sup 2}, which agrees with theoretical prediction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis of submicron metastable phase of silicon using femtosecond laser-driven shock wave

We measured the grain size of metastable phase of Si synthesized by shock compression. We analyzed the crystalline structures of the femtosecond laser-driven shock compressed silicon with x-ray diffraction measurements. We found that submicron grains of metastable Si-VIII exist in the silicon. We suggest that the pressure loading time is too short for the nucleated high-pressure phases to grow in case of the femtosecond laser-driven shock compression, therefore Si-VIII grains of submicron size are obtained. We are expecting to discover other unique crystalline structures induced by the femtosecond laser-driven shock wave.

36 MATERIALS SCIENCE↗

High-Angular-Resolution Microbeam X-Ray Diffraction with CCD Detector

We have introduced a CCD-type two-dimensional X-ray detector for a microbeam X-ray diffraction system using synchrotron radiation, so that we can measure local reciprocal space maps (RSM) of samples rapidly. A local RSM of a strain-relaxed SiGe 004 grown on a Si (001) substrate was measured in higher-angular-resolution and faster than a conventional way. The measurement was achieved in 1 h 40 min. with the 2theta resolution of 80 murad and the spatial resolution of 1.4(h)x0.5(v) {mu}m{sup 2}. The introduction of the CCD enabled us to measure RSMs at many points in a sample, that is, the distribution of strain fields and lattice tilts can be revealed in high-angular- and high-spatial-resolution.

36 MATERIALS SCIENCE↗