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A synchrotron-based technique using Compton scattering imaging is presented. This technique has been applied to a coin battery (CR2023), and the cross-sectional image has been obtained in 34 ms without sample rotation. A three-dimensional image of the whole structure has been reconstructed from 74 cross-sectional images taken consecutively by scanning the incident, wide X-ray beam along one direction. This work demonstrates that quick cross-sectional imaging of regions of interest and three-dimensional image reconstruction without sample rotation are feasible using Compton scattering imaging.

The role of excess Ni in Ni2+xMn1−xSn (x = 0.05, 0.1) Heusler alloys has been reported using temperature dependent magnetic Compton spectroscopy. The experimental Compton profiles from magnetic electrons have been analyzed to quantify the contribution of Mn 3d electrons, Ni sites and sp-electrons in building-up the total spin moments. The experimentally deduced spin momentum densities, total and element-specific spin moments are examined using theoretical investigations within the spin polarized relativistic Korringa-Kohn-Rostoker method. The build-up of spin moments has been explored in terms of total and projected density of states. Site-dependent Ni magnetic moment is also discussed. Heisenberg exchange coupling parameters are also computed to study the change in Ruderman-Kittel-Kasuya-Yosida type exchange interaction on increasing Ni concentration in the Ni-Mn-Sn system.

High-resolution (0.12 a.u.) electron momentum density projections (Compton profiles) of a hexagonal Zn single crystal have been measured along five high-symmetry directions in reciprocal space. The experiment was performed with the use of 115.6 keV synchrotron radiation on the BL08W station at SPring-8. The quality of the measured Compton profiles is significantly better than that of previous medium- and high-resolution data. The experimental data were compared with the corresponding theoretical Korringa–Kohn–Rostoker (KKR) and density functional theory (DFT) calculations. Some minor and major differences between the two theoretical band-structure calculations have been observed. However, the good quality experimental results indicate their better agreement with DFT.

Spin momentum densities of ferromagnetic ZrFe2 and Zr0.8Sc0.2Fe2 have been measured using magnetic Compton scattering with 182.65 keV circularly polarized synchrotron radiations. Site specific spin moments, which are responsible for the formation of total spin moment, have been deduced from Compton line shapes. At room temperature, the computed spin moment of ZrFe2 is found to be slightly higher than that of Sc doped ZrFe2 which is in consensus with the magnetization data. To compare the experimental data, we have also computed magnetic Compton profiles (MCPs), total and partial spin projected density of states (DOS) and the site specific spin moments using spin-polarized relativistic Korringa-Kohn-Rostoker method. It is observed that the spin moment at Fe site is aligned antiparallel to that of Zr site in both ZrFe2 and Zr0.8Sc0.2Fe2. The MCP results when compared with vibrating sample magnetometer based magnetization data, show a very small contribution of orbital moment in the formation of total magnetic moments in both the compounds. The DOS of ferromagnetic ground state of ZrFe2 and Zr0.8Sc0.2Fe2 are interpreted on the basis of a covalent magnetic model beyond the Stoner rigid band model. It appears that on alloying between a magnetic and a non-magnetic partner (with low valence), a polarization develops on the non-magnetic atom which is anti-parallel to that of the magnetic atom.

Compton scattering is one of the most promising probes for quantitating Li under in operando conditions, since high-energy X-rays, which have high penetration power, are used as the incident beam and the Compton-scattered energy spectrum has specific line-shapes for each element. An in operando quantitation method to determine the Li composition in electrodes has been developed by using line-shape (S-parameter) analysis of the Compton-scattered energy spectrum. In this study, S-parameter analysis has been applied to a commercial coin cell Li-ion rechargeable battery and the variation of the S-parameters during the charge/discharge cycle at the positive and negative electrodes has been obtained. By using calibration curves for Li composition in the electrodes, the change in Li composition of the positive and negative electrodes has been determined using the S-parameters simultaneously.

We have studied the spin-dependent electron momentum density distribution in CoGa x Fe2−x O4 (x = 0.2, 0.3) at a low temperature (8 K) using magnetic Compton scattering technique. Further, the effect of Ga doping on the electronic structure is studied using X-ray photoemission spectroscopy (XPS). It is revealed that doping of Ga substitutes the Fe ions predominantly at tetrahedral (P) site, which promotes a gradual immigration of small amount of Co ions from tetrahedral to octahedral (Q) site. Total spin moment increases remarkably on increasing the doping concentration of nonmagnetic Ga (x = 0 → 0.3) in the base cobalt ferrite. It is seen that major contribution to total spin moment mainly arises from Co ions while itinerant electrons show negative polarization. On Ga doping, spin moment at Fe site increases dramatically with a minor increment at Co site. The increased spin moment is attributed to the increased Q/P occupancy ratio of Fe3+ as well as Co2+ ions as determined using XPS measurements. In contrast, orbital moment does not show such deviations, suggesting that a small amount of Ga doping can enhance the magnetization significantly, without inducing any significant distortion to modify the spin–orbit coupling.

X-ray Compton scattering measurements of the electron momentum distribution in water confined in both single-walled and double-walled carbon nanotubes (SWNT and DWNT), as a function of temperature and confinement size are presented here together with earlier measurements of the proton momentum distribution in the same systems using neutron Compton scattering. These studies provide a coherent picture of an anomalous state of water that exists because of nanoconfinement. This state cannot be described by the weakly interacting molecule picture. It has unique transport properties for both protons and water molecules. We suggest that knowledge of the excitation spectrum of this state is needed to understand the enhanced flow of water in cylinders with diameters on the order of 20 Å.

In this study the structural and magnetization properties of a CoFe2O4-based ferrofluid was investigated using x-ray diffraction (XRD), transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDS), Mossbauer spectroscopy, and magnetic Compton scattering (MCS) measurements. The XRD diagram indicates that the nanoparticles in the ferrofluid are inverse spinel and TEM graph shows that the ferrofluid consists of spherical nanoparticles with an average diameter of 18± 1 nm, in good agreement with the size, 19.4 nm, extracted from line broadening of the XRD peaks. According to EDS measurements the composition of the nanoparticles is CoFe2O4. Mossbauer spectroscopy shows that the cation distributions are (Co0.38Fe0.62)[Co0.62Fe1.38]O4. The MCS measurement, performed at 10 K, indicates that the magnetization of the nanoparticles is similar to magnetization of maghemite and magnetite. While the magnetization of the inverse spinels are in [111] direction, interestingly, the magnetization deduced from MCS is in [100] direction. The CoFe2O4-based ferrofluid is found to be stable at ambient conditions, which is important for applications.

Measurement of combustion gas by high-energy X-ray Compton scattering is reported., Measurement of combustion gas by high-energy X-ray Compton scattering is reported. The intensity of Compton-scattered X-rays has shown a position dependence across the flame of the combustion gas, allowing us to estimate the temperature distribution of the combustion flame. The energy spectra of Compton-scattered X-rays have revealed a significant difference across the combustion reaction zone, which enables us to detect the combustion reaction. These results demonstrate that high-energy X-ray Compton scattering can be employed as an in situ technique to probe inside a combustion reaction.

The new efficient Monte Carlo procedure for multiple scattering simulation in Compton experiments is presented. The simulation algorithm has proved its advantage in restricted geometry experiments., The first results of multiple scattering simulations of polarized high-energy X-rays for Compton experiments using a new Monte Carlo program, MUSCAT, are presented. The program is developed to follow the restrictions of real experimental geometries. The new simulation algorithm uses not only well known photon splitting and interaction forcing methods but it is also upgraded with the new propagation separation method and highly vectorized. In this paper, a detailed description of the new simulation algorithm is given. The code is verified by comparison with the previous experimental and simulation results by the ESRF group and new restricted geometry experiments carried out at SPring-8.

Spin-polarized Compton profiles of TbCo 2 have been measured to elucidate the interesting behavior of spin and orbital moments at different temperatures. The magnetic Compton profiles (MCPs) have been analyzed in terms of site specific spin moments due to Tb-4f electrons, Co and itinerant electrons. The temperature dependence of the orbital moment has been deduced using Compton and magnetometry data ranging between 6 and 300 K. The present data exhibit a decrease in the ratio of orbital to spin moments from 43.9% to 35.0% (while going from 6 to 300 K). First-principles calculations within DFT + U scheme have also been performed to confirm the spin-, orbital- and site specific-magnetic moments in TbCo 2 . An antiparallel exchange coupling between the Tb-4f and Co spin moments is found. The orbital moment is found to have a parallel coupling with the Tb spin moment, as evident from the experimental MCPs. From first-principles data it is seen that the orbital moments of Tb and Co sites are antiparallel to each other, as in the case of their spin magnetic moments. The present experimental study also shows an existence of an itinerant moment which is coupled ferromagnetically with the Tb-4f spin moment.

We have applied two kinds of experimental methods using elliptically polarized synchrotron X-rays, magnetic Compton and Bragg scattering experiments, to a single crystal of a disordered Pd0.80Co0.20 alloy, and have measured magnetic Compton profiles and magnetic form factors, respectively. The result of the Compton scattering experiment has shown that the electronic structure of Pd0.80Co0.20 is similar to that of Pd0.72Co0.28, and the spin moment has been evaluated. The result of the Bragg scattering experiment has reinforced that of the previous experiment [M. Ito et al.: Mater. Sci. Forum Vol. 459 (2011), p. 3.], and the spin moment estimated by the magnetic Bragg scattering has reproduced that by the magnetic Compton scattering. These results show that the joint study of the magnetic Compton and Bragg scattering provides a tool for investigating the magnetic property of alloys.

Synchrotron-based Compton scattering imaging has visualized the interior of a battery under in situ and operando conditions., Results of studies on Compton scattering imaging using synchrotron high-energy X-rays are reported. The technique is applied to a discharging coin cell, and the intensity of Compton scattered X-rays from the inside of the cell has been measured as a function of position and time. The position–time intensity map captures the migration of lithium ions in the positive electrode and reveals the structural change due to the volume expansion of the electrode. This experiment is a critical step in developing synchrotron-based Compton scattering imaging for electrochemical cells at a product level.

We present an X-ray Compton scattering study on aqueous trimethylamine N-oxide (TMAO) and guanidine hydrochloride solutions (GdnHCl) as a function of temperature. Independent from the concentration of the solvent, Compton profiles almost resemble results for liquid water as a function of temperature. However, the number of hydrogen bonds per water molecule extracted from the Compton profiles suggests a decrease of hydrogen bonds with rising temperature for all studied samples, and the differences between water and the solutions are weak. Nevertheless, the data indicate a reduced bond weakening with rising TMAO concentration up to 5 M of 7.2% compared to 8% for pure water. In contrast, the addition of GdnHCl appears to behave differently for concentrations up to 3.1 M with a weaker impact on the temperature response of the hydrogen bond structure.

Temperature dependent spin momentum densities of NiFe 2− x RE x O 4 ( x =0, 0.05; RE=Dy, Gd) ferrites have been measured using a magnetic Compton spectrometer available at SPring-8, Japan. The experimental profiles of NiFe 2 O 4 (NFO) with doping of Dy and Gd show almost similar spin moment as of undoped NFO. The contribution of different constituents in the formation of total spin moment is also deduced from the analysis of Compton line shape. It is seen that 5% doping of Dy 3+ or Gd 3+ ions at Fe 3+ sites leads to a redistribution of spin moment at Fe 3+ and RE 3+ sites. The magnetic Compton data when compared with the magnetization data (using a vibrating sample magnetometer) show almost a constant orbital moment (0.21±0.03 µ B /f.u.) in the doped and undoped NFO.

Magnetic Compton profiles (MCPs) of Co/Au multilayers have been measured and analyzed by DV-Xαcluster model calculations from a viewpoint of perpendicular magnetic anisotropy (PMA). The PMA and the MCPs are discussed for the presently obtained results for Co/Au, along with the previously obtained results for Co/Pd and Co/Pt. A Co/Au multilayer shows a weak PMA which is caused by |m|=1 states of Co 3d electrons at a smooth Co/Au interface. The increase of the interface-to-volume ratio plays the main role in determining the perpendicular anisotropy in Co/Au multilayers. The strain of a Co layer can have a secondary role in determining the magnetic anisotropy in Co/Au multilayers, although the strain dominates PMA in the case of Co/Pd and Co/Pt multilayers.

We have measured magnetic Compton scattering (MCS) for an Fe/MgO multilayer film at several magnetic field applying perpendicular to film plane. A spin specific magnetic hysteresis (SSMH) loop is obtained by the MCS for the Fe/MgO multilayer film. A knickpoint is observed in the SSMH loop around the magnetic field of 0.5 T. Orbital magnetization is enhanced within the magnetic field from-0.5 T to 0.5 T. A decomposition analysis for magnetic Compton profiles shows the suppressed |m|=0 states and enhanced |m|=1 and 2 states within the magnetic field from-0.5 T to 0.5 T. Heremdenotes magnetic quantum number. The knickpoint corresponds to a perpendicular magnetic anisotropy, which comes from the enhanced |m|=1 and 2 state and orbital magnetization in the Fe/MgO multilayer.

We have started to construct a nationwide forensic soil sediment database for Japan, based on the heavy mineral and trace heavy element compositions of stream sediments collected at 3024 points across Japan. The data were measured by high-resolution synchrotron radiation X-ray powder diffraction (SR-XRD) and high-energy SR X-ray fluorescence analysis (XRF) using the SR source of SPring-8, the SR radiation facility in Japan. The automated sampling systems allow the measurement of 130 powder diffraction patterns and 100 XRF spectra per day using sediment samples of just a few milligrams, which enabled us to construct a database of a large number of samples. The concentrations of heavy elements such as rare earth elements, Cs and W up to 500 ppm level in soil sediments can be determined by the calibration curve method by using high-energy SR-XRF utilizing monochromatic X-rays of 116 keV. A heavy element concentration map superimposed on a geographical map of Japan was successfully prepared from these analytical data. The heavy mineral compositions were quantitatively evaluated by using the peak intensity of characteristic XRD peaks of the component minerals measured by a Debye–Scherrer camera having a radius of 286.5 mm, recorded with an imaging plate and monochromatic X-rays (λ = 1.0 A). This study demonstrates that XRF and XRD data collected from the sediments of Shizuoka Prefecture closely reflect the geological and geographical signature of the sediment samples, which can be used for the provenance determination of soil evidence from a crime scene. Copyright © 2013 John Wiley & Sons, Ltd.

The crystallographic, magnetic and transport properties of Sr1−x Ca x Ru0.5Mn0.5O3 were studied to reveal the effects of crystal symmetry on the magnetism and the transport properties of antiferromagnetic SrRu1−y Mn y O3 (y > 0.2). The Ca-content dependences of the lattice constants and volume suggest that the mixed valence state of Mn3+, Mn4+, Ru4+, and Ru5+ ions in SrRu0.5Mn0.5O3 is held for Ca substitution. However, a structural transformation from tetragonal to orthorhombic symmetry occurs at a Ca content of x ∼ 0.2, and a ferromagnetic state appears simultaneously. The Weiss temperature of all samples has a positive value regardless of the magnetic state. The resistivity decreases as the Ca content increases, and the high temperature part of the resistivity could be fitted by using the variable range hopping (VRH) model. The localization length increases as soon as ferromagnetism appears. The Curie temperature seems to depend on the distance between transition metal ions. The antiferromagnetic state was explained by using the competition between a ferromagnetic interaction along the c-axis and an antiferromagnetic interaction in the ab-plane, and the orthorhombic ferromagnetic state was explained by using a three-dimensional ferromagnetic interaction between Mn ions.

Spin momentum density in Ni2Mn1.4Sn0.6 shape memory alloy has been measured using magnetic Compton scattering technique. The experiment has been performed using 182 keV circularly polarized synchrotron radiation at temperature 10 K at SPring-8, Japan. Experimental magnetic Compton profile has been decomposed to determine the site specific magnetic moments, where the magnetic moment at Mn site was found to be dominating. It is seen that the total spin moment in present non-stoichiometric alloy is smaller than that of stoichiometric Ni2MnSn.

The effects of strain and interface roughness at the Co/Pd interface are investigated from the viewpoint of perpendicular magnetic anisotropy (PMA) using the DV-Xα cluster model calculation method. It is found that spin projected occupation number ratio of magnetic quantum number |m| = 2 for the Co 3d electrons enhances by expanding the lattice within a close-packed plane of fcc stacking and, hence, enhances the PMA. Rough interface decreases the spin projected occupation number ratio of |m| = 2 and, hence, decreases the PMA. These results explain the PMA properties of Co/Pd multilayers fabricated using molecular beam epitaxy (MBE) technique and RF sputtering techniques.

Spin selective magnetic hysteresis (SSMH) curves, orbital selective magnetic hysteresis (OSMH) curves and magnetic quantum number selective SSMH curves are obtained for CoFeB/MgO multilayer films by combining magnetic Compton profile measurements and superconducting quantum interference device (SQUID) magnetometer measurements. Although the SQUID magnetometer measurements do not show perpendicular magnetic anisotropy (PMA) in the CoFeB/MgO multilayer film, PMA behavior is observed in the OSMH and SSMH curves for the |m| = 2 magnetic quantum number states. These facts indicate that magnetization switching behavior is dominated by the orbital magnetization of the |m| = 2 magnetic quantum number states.

We present a new planar Ni compound refractive lens for high energy X-rays (116 keV). The lens is composed of identical plano-concave elements with longitudinal parabolic grooves manufactured by a punch technique. In order to increase the lens transmission, the thickness of the single lens at the parabolic groove vertex was reduced to less than 5 μm and the radius of curvature was reduced to about 20 μm. The small radius of curvature allowed us to reduce the number of single elements needed to get the focal length of 3 m to 54 single lenses. The gain parameter has been significantly improved compared to the previous lenses due to higher transmission, but the focused beam size and its gain are not as good as expected, mostly due to the aberrations caused by the lens shape imperfections.

著者人数: 20名ほか, Accepted: 2016-09-28, 資料番号: SA1160249000

We have studied spin dependent electron momentum density in CoGa0.3Fe1.7O4 at 300 K using magnetic Compton spectroscopy. It is observed that major contribution to total spin moment mainly arises from Co ions while itinerant electrons show negative polarization. Orbital contribution has been deduced by comparing the magnetic Compton spectroscopy with the magnetization data. It is revealed that the anisotropy in magnetization in the system increases with the Ga doping.

We have started the construction of a nationwide forensic soil sediment database for Japan based on the heavy mineral and trace heavy element compositions of stream sediments collected at 3024 points all over Japan obtained by high-resolution synchrotron X-ray powder diffraction (SR-XRD) and high-energy synchrotron X-ray fluorescence analysis (HE-SR-XRF). In this study, the performance of both techniques was demonstrated by analyzing soil sediments from two different geological regions, the Kofu and Chiba regions in Kanto province, to construct database that can be applied in the future to provenance analysis of soil evidence from a crime scene. The sediments from the quaternary volcanic lithology of the Chiba region were found to be dominated by heavy minerals of volcanic origin - orthopyroxene, clinopyroxene, and amphibole, and the REEs (rare earth elements) within the region showed similar geochemical behavior. On the other hand, four distinct heavy mineral groups were identified in the sediments of the Kofu region, where there is a great variety of underlying bedrock, and the geochemical behavior of the REEs in the sediments also varied accordingly to their geological origins. As such, our study shows that high-resolution SR-XRD data can provide information on the spatial distribution patterns of heavy minerals in stream sediments, playing an important role in determining their likely geographical origin. Meanwhile, the highly sensitive HE-SR-XRF data allow us to study the geochemical behavior of trace heavy elements, especially the REEs in the sediments, providing additional support to further constrain the likely geographical origin of the sediments determined by heavy minerals.

Ge2Sb2Te5 (GST) has demonstrated its outstanding importance among rapid phase-change (PC) materials, being applied for optical and electrical data storage for over three decades. The mechanism of nanosecond phase change in GST, which is vital for its application, has long been disputed: various, quite diverse scenarios have been proposed on the basis of various experimental and theoretical approaches. Nevertheless, one central question still remains unanswered: why is amorphous GST stable at room temperature for long time while it can rapidly transform to the crystalline phase at high temperature? Here it is revealed for the first time, by modelling the amorphous structure based on synchrotron radiation anomalous X-ray scattering data, that germanium and tellurium atoms form a “core” Ge-Te network with ring formation. It is also suggested that the Ge-Te network can stabilize the amorphous phase at room temperature and can persist in the crystalline phase. On the other hand, antimony does not contribute to ring formation but constitutes a “pseudo” network with tellurium, in which the characteristic Sb–Te distance is somewhat longer than the covalent Sb–Te bond distance. This suggests that the Sb-Te pseudo network may act as a precursor to forming critical nuclei during the crystallization process. The findings conclude that the Ge-Te core network is responsible for the outstanding stability and rapid phase change of the amorphous phase while the Sb-Te pseudo network is responsible for triggering critical nucleation.

We compare two Co/Pd multilayers with correspondingly smooth and rough interfaces. The first is a Co (1.5 nm)/Pd (2.6 nm) multilayer with a smooth interface deposited by the MBE technique, and the second is a Co (1.6 nm)/Pd (4.0 nm) multilayer with a rough interface deposited by the sputter technique. Both multilayers have almost the same perpendicular magnetic anisotropy energy, 1.15 Merg/cc for the Co (1.5 nm)/Pd (2.6 nm) multilayer and 1.20 Merg/cc for the Co (1.6 nm)/Pd (4.0 nm) multilayer, respectively. The symmetry of the wave function, which is measured using the magnetic Compton profile, is almost the same for both multilayers. This suggests that the smooth interface controls the wave function and enhances the PMA energy even if the Co/Pd multilayer has a thinner Pd layer.

The deuteration-induced effect on the Fermi surface (FS) topology of V was investigated by the synchrotron-based Compton scattering technique with 115 keV X-rays. The three-dimensional occupation number density (OND) of α-VD 0.64 single crystal and V single crystal was reconstructed by the directional Compton profiles along 13–18 directions. The observed OND shows that the FS topology of α-VD 0.64 .differs from that of V at Γ, N, and H points in the crystal momentum space, which are hole position for V. This indicates that electrons that originate from deuterium modify the upper part of the host metal d bands (3rd and 4th bands) at the Fermi level E F , and forms the metal–hydrogen bonding states with the lower part of the host metal d band (1st band).

We have carried out x-ray diffraction and small-angle x-ray scattering measurements of expanded fluid alkali metal rubidium (Rb) and observed that the nearest neighbor distance decreases despite the fact that the average interatomic distance increases with volume expansion, indicating that the attractive force among ions is enhanced. Such structural change emerges in the density range where the fluid is still metallic. The density range also corresponds with the region where the instability of the electron gas has been theoretically predicted, suggesting the modulation in the charge fluctuations of the electron gas plays an essential role for such enhanced attraction among ions. Motivated by these unusual structural features, we have moved on investigating the electronic state in expanded fluid Rb through synchrotron-based high-resolution Compton scattering experiments. We have succeeded in measuring the Compton profile of fluid Rb using newly developed a high-pressure vessel for the Compton scattering experiments.

The combination of new experimental and theoretical techniques provides evidence of instantaneous electron correlation effects in directional Compton profiles of crystalline silicon, which cannot be reproduced when reference is made to a density matrix obtained from a single-determinantal wavefunction. These effects are instead accounted for by a recently implemented post-Hartree-Fock periodic scheme, which gives results in quite good agreement with the high-quality experimental data.

We have measured magnetic Compton profile of Co/Pd thin films sputtered on a substrate for studying the electronic structure. For the first time, a silicon nitride substrate of 100 nm thickness we used in the magnetic Compton scattering experiment. We have improved vacuum tubes of the Compton beam-line BL08W of SPring-8, and have reduced greatly the background scattering for the Compton profile. We have succeeded in measuring magnetic Compton profile of Co (0.8 nm)/Pd (1.6 nm) 400 nm multilayer.

The propagation of X-rays through a compound refractive lens (CRL) with imperfect CRL elements is investigated. The trajectories of random rays within the geometrical optics regime are calculated in one plane using Monte Carlo methods. Three different lenses were simulated: Be, Al and Ni lenses designed for photon energies of 20 keV, 60 keV and 175 keV, respectively. The results show that while transverse displacements of single elements in a CRL do not influence imaging resolution, rotational errors can be important. Systematic calculations of aberrations owing to the deviation of the element's surface from a perfect parabolic shape are also presented.

X-ray Compton scattering measurements have been carried out on germanium (Ge) and tin (Sn) in the solid and liquid states. While the shape of the Compton profiles (CPs) of Ge reflects the semiconductor-to-metal transition upon melting, it was found that even for Sn, which remains metallic during the solid–liquid phase transition, the shape of the CP in the liquid state exhibits more metallic characteristics than that in the solid state. The experimentally derived Fermi momenta of liquid Ge and Sn have systematically higher values than those of the electron gas at corresponding electron densities, which indicates a non-simple metallic nature of the group IV elements in the liquid state.

We present the first ever theoretical and experimental charge Compton profiles of Ni2MnGa Heusler alloy. The measurements have been made using magnetic Compton spectrometer at SPring8, Japan. The Compton profiles and energy bands have been computed using Hartree-Fock, density functional theory with local density and generalized gradient approximations. It is seen that the Hartree-Fock based Compton profile is relatively in better agreement with the experimental profiles. In addition, we also report the energy bands, density of states and valence charge densities using full potential linearized augmented plane-wave method.

We have carried out the magnetic Compton scattering of NpNiGa 5 . The signs of the magnetic effects in both ordered states are negative. These facts demonstrate that the contribution of the Np 5f electrons is dominant in the ordered states of NpNiGa 5 . The magnetic Compton profile shows significant change across the successive transitions. This suggests that the successive transitions are correlated with the 5f quadrupolar degrees of freedom and/or the change of the quantized axis.

Au–Si and Au–Ge alloys have a deep eutectic region around 19 at.% Si and 28 at.% Ge, respectively. The metallic glass was prepared by quenching around 25 at.% Si near the eutectic composition for the Au–Si alloys [2] which has stimulated many researchers to study on the structural properties of such liquid alloys. However their results were different from each other, which seems due to the experimental difficulties from heavy absorption of both X-ray and neutron beams by Au atom in diffraction experiments. X-ray diffraction measurements have been carried out for liquid Au–Si and Au–Ge alloys around the eutectic region by the transmission method using high-energy X-rays to investigate the atomic arrangements in the liquid state. From the temperature dependence of the observed structure factors, the partial pair correlation and the detailed atomic arrangements will be discussed by Reverse Monte Carlo analysis. The produced atomic arrangements around the eutectic region suggest a substitutional structure and also an increase in liquid density with decreasing temperature.

We report the change of electronic structure associated with the hidden-order (HO) transition in ${\mathrm{URu}}_{2}{\mathrm{Si}}_{2}$ through Compton scattering experiment on the (001) plane of the single crystal. The two-dimensional electron occupation number densities (EONDs) obtained at 14 and 20 K, which are the projection of Fermi volume onto the ${k}_{x}\ensuremath{-}{k}_{y}$ plane of the first Brillouin zone, clearly reflect a whole image of electronic structure in the HO and paramagnetic (PM) phases, respectively. The change in electronic structure is well described by theoretical EONDs derived from the result of a band calculation, where $\mathrm{U}\phantom{\rule{0.28em}{0ex}}5f$ electrons are treated as itinerant ones. We also evaluate the electron (hole) numbers in the HO and PM phases and, therefore, its change on the HO transition. The HO transition is deeply involved with a significant change in $5f$ electrons from partially localized to itinerant states through hybridization with conduction electrons, resulting in the reconstruction of Fermi-surface structure.

Anharmonic thermal effects on the electron momentum distribution of a lithium fluoride single crystal are experimentally measured through high-resolution Compton scattering and theoretically modeled with ab initio simulations, beyond the harmonic approximation to the lattice potential, explicitly accounting for thermal expansion. Directional Compton profiles are measured at two different temperatures, 10 and 300 K, with a high momentum space resolution (0.10 a.u. in full width at half maximum), using synchrotron radiation. The effect of temperature on measured directional Compton profiles is clearly revealed by oscillations extending almost up to |p|=4 a.u., which perfectly match those predicted from quantum-mechanical simulations. The wave-function-based Hartree-Fock method and three classes of the Kohn-Sham density functional theory (local-density, generalized-gradient, and hybrid approximations) are adopted. The lattice thermal expansion, as described with the quasiharmonic approach, is found to entirely account for the effect of temperature on the electron momentum density within the experimental accuracy.

In this study, the magnetic properties of FeAl alloys with different grain sizes produced by high-pressure torsion were probed by means of magnetic Compton scattering. The measurements were performed at 300 and 10 K. Magnetic Compton profiles of nanocrystalline (35 nm) and ultrafine-grained (160 nm) FeAl alloys were analyzed in terms of the integral area, the width, and the distinctive dip intensity at low momenta. The changes in total magnetic moment and the strength of spin-polarization of itinerant electrons are assumed to be caused by vacancies induced during the preparation of the samples. Despite local disordering due to interfacial regions and deviations in perfect stoichiometry for B2 structure, the effect of vacancies is considered as the major magnetic state contributor.

We present an incisive spectroscopic technique for directly probing redox orbitals based on bulk electron momentum density measurements via high-resolution x-ray Compton scattering. Application of our method to spinel Li{x}Mn{2}O{4}, a lithium ion battery cathode material, is discussed. The orbital involved in the lithium insertion and extraction process is shown to mainly be the oxygen 2p orbital. Moreover, the manganese 3d states are shown to experience spatial delocalization involving 0.16±0.05 electrons per Mn site during the battery operation. Our analysis provides a clear understanding of the fundamental redox process involved in the working of a lithium ion battery., リチウムイオン二次電池の電池電極反応に寄与する電子軌道の解明 -マンガン酸リチウム系正電極材料設計に新たな指針-.京都大学プレスリリース. 2015-02-05.

We have developed a high-pressure vessel and a cell for x-ray Compton scattering measurements of fluid alkali metals. Measurements have been successfully carried out for alkali metal rubidium at elevated temperatures and pressures using synchrotron radiation at SPring-8. The width of Compton profiles (CPs) of fluid rubidium becomes narrow with decreasing fluid density, which indicates that the CPs sensitively detect the effect of reduction in the valence electron density. At the request of all authors of the paper, and with the agreement of the Proceedings Editor, an updated version of this article was published on 10 September 2015. The original article supplied to AIP Publishing was not the final version and contained PDF conversion errors in Formulas (1) and (2). The errors have been corrected in the updated and re-published article.

The electron momentum distributions in icosahedral Al64Cu23Fe13, icosahedral Al63Cu23Ru13 and decagonal Al65Cu15Co20 quasicrystals have been studied using the high-resolution Compton scattering technique. The electron-per-atom ratios (e/a) of the quasicrystals were determined quantitatively for the first time from the Compton profiles. The radii of the Fermi spheres were evaluated from the values of e/a on the basis of the free-electron model. Comparisons between the radius of the Fermi spheres and the size of the quasi-Brillouin zones show that the icosahedral quasicrystals meet the empirical matching condition, while the decagonal quasicrystal does not do this so well. This implies that the Hume-Rothery mechanism works for the formation of the pseudogap near the Fermi level in the icosahedral quasicrystals, although it operates only slightly in the decagonal quasicrystal.

An X-eX spectrometer has been developed to obtain the two-dimensional and three-dimensional electron momentum density (2D- and 3D-EMD) directly from experiment. The spectrometer is equipped with a time-of-flight energy analyzer to record the flight direction and the kinetic energies of the recoiled electrons, and a position sensitive photon detector to record the directions of the Compton scattered photons. The signals from the electron branch and those from the photon branch are processed in coincidence mode. The obtained 2D-EMD on the (100) plane in Si and the 3D-EMD on the [100] and the [111] axes are compared with the FLAPW theoretical results.

The magnetic Compton profiles (MCPs) of Fe thin film with 1 μm thickness have been successfully measured, using polyethylene terephtalate (PET) substrates with 4 μm thickness to reduce scattering photons from substrate. We have succeeded for the first time to observe the anisotropy of MCPs in the Co/Pd multilayer. The magnetic out-of-plane anisotropy of the current Co (0.8 nm)/Pd (1.6 nm) multilayer sample can be explained by the model of a large number of the | m |=1 states of 3d-bands.