田中 義人

Objective lenses are frequently employed in state-of-the-art ultrafast time-resolved microscopy techniques. While it enables tight spatial focusing, its dispersion causes a longer optical pulse duration. Since an objective lens is a combination of different lens materials, finding its correct dispersion can be challenging. In this paper, we propose a dispersion measurement method for an objective lens using white light interferometry. Our proposed method enables the experimental determination of the lens dispersion and improves the temporal resolution of ultrafast time-resolved microscopy techniques.

Abstract We have investigated the dependence of terahertz wave emissions on the internal electric field in undoped GaAs/n-type GaAs epitaxial structures irradiated by ultrashort laser pulses. The undoped layer has an electric field, the strength of which was controlled by the temperature in addition to the undoped layer thickness. We observed the electric field dependence of the terahertz waveform, and the results were explained by the calculation of the transient dynamics of electrons and phonons under electric fields. Furthermore, we indicated that the terahertz amplitude can be linearly controlled by the electric field strength in a wide electric field range.

The dissociation and ionization dynamics of CF3I and CH3I molecules were investigated using a pump-and-probe technique that employs a soft x-ray free-electron laser (SACLA) in Japan. First, time-resolved inner-shell photoelectron spectroscopy was employed to observe the ultrafast reaction of CF3I by monitoring iodine 4d electrons. The change in the I 4d state observed in the photoelectron spectra is found to occur with a rise time τ of approximately 40 fs after a pump laser pulse, which is faster than that observed when an ultrafast gas-phase electron diffraction technique is employed. This implies that the inner-shell photoelectron spectroscopy is more sensitive to the potential surface near the Franck–Condon region. Second, a strong laser intensity at 266 nm, corresponding to a power density of 1.9 × 1014 W cm−2, can easily ionize CH3I molecules via multiphoton ionization processes, and the time dependence of the valence photoelectron spectra clearly shows that at the picosecond timescale, this pump laser pulse causes spectral peaks to shift owing to space-charge effects in response to the large amount of ions generated. Thus, the SACLA can be a useful tool to investigate not only the dynamical process of molecular dissociation but also the ionization process through the shift in the peaks of photoelectron spectra.

An experimental and computational investigation of the space-charge effects occurring in ultrafast photoelectron spectroscopy from the gas phase is presented. The target sample CF3I is excited by ultrashort (100 fs) far-ultraviolet radiation pulses produced by a free-electron laser. The modification of the energy distribution of the photoelectrons, i.e. the shift and broadening of the spectral structures, is monitored as a function of the pulse intensity. The experimental results are compared with computational simulations which employ a Barnes-Hut algorithm to calculate the effect of individual Coulomb forces acting among the particles. In the presented model, a survey spectrum acquired at low radiation fluence is used to determine the initial energy distribution of the electrons after the photoemission event. The spectrum modified by the space-charge effects is then reproduced by N-body calculations that simulate the dynamics of the photoelectrons subject to the individual mutual Coulomb repulsion and to the attractive force of the positive ions. The employed numerical method accounts for the space-charge effects on the energy distribution and allows to reproduce the complete photoelectron spectrum and not just a specific photoemission structure. The simulations also provide information on the time evolution of the space-charge effects on the picosecond scale. Differences with the case of photoemission from solid samples are highlighted and discussed. The presented simulation procedure, although it omits the analysis of angular distribution, constitutes an effective simplified model that allows to predict and account for space-charge effects on the photoelectron energy spectrum in time-resolved photoemission experiments with high-intensity pulsed sources.

We investigate the structural dynamics of the incommensurately modulated phase of Sn 2 P 2 Se 6 by means of time-resolved X-ray diffraction following excitation by an optical pump. Tracking the incommensurable distortion in the time domain enables us to identify the transport effects leading to a complete disappearance of the incommensurate phase over the course of 100 ns. These observations suggest that a thin surface layer of the high-temperature phase forms quickly after photo-excitation and then propagates into the material with a constant velocity of 3.7 m/s. Complementary static structural measurements reveal previously unreported higher-order satellite reflection in the incommensurate phase. These higher-order reflections are attributed to cubic vibrational terms in the Hamiltonian.

Unraveling the origin of ultrafast demagnetization in multisublattice ferromagnetic materials requires femtosecond x-ray techniques to trace the magnetic moment dynamics on individual elements, but this could not yet be achieved in the hard x-ray regime. We demonstrate here the first ultrafast demagnetization dynamics in the ferromagnetic heavy 5d-transition metal Pt using circularly-polarized hard x-rays at an x-ray free electron laser (XFEL). The decay time of laser-induced demagnetization of L1(0)-FePt is determined to be tau(Pt) = 0.61 +/- 0.04 ps using time-resolved x-ray magnetic circular dichroism at the Pt L-3 edge, whereas magneto-optical Kerr measurements indicate the decay time for the total magnetization as tau(total) < 0.1 ps. A transient magnetic state with a photomodulated ratio of the 3d and 5d magnetic moments is demonstrated for pump-probe delays larger than 1 ps. We explain this distinct photo-modulated transient magnetic state by the induced-moment behavior of the Pt atom and the x-ray probing depth. Our findings pave the way for the future use of XFELs to disentangle atomic spin dynamics contributions.

We report on new results of a search for a two-photon interaction with axionlike particles (ALPs). The experiment is carried out at a synchrotron radiation facility using a "light shining through a wall (LSW)" technique. For this purpose, we develop a novel pulsed-magnet system, composed of multiple racetrack magnets and a transportable power supply. It produces fields of about 10 Tover 0.8 m with a high repetition rate of 0.2 Hz and yields a new method of probing a vacuum with high intensity fields. The data obtained with a total of 27 676 pulses provide a limit on the ALP-two-photon coupling constant that is more stringent by a factor of 5.2 compared to a previous x-ray LSW limit for the ALP mass less than or similar to 0.1 eV.

We report a search for photon-photon elastic scattering in vacuum in the X-ray region at an energy in the center of mass system of omega(cms) = 6.5 keV for which the QED cross section is sigma(QED)=2.5 x10(-47) m(2). An X-ray beam provided by the SACLA X-ray Free Electron Laser is split and the two beamlets are made to collide at right angle, with a total integrated luminosity of (1.24 +/- 0.08) x 10(28) m(-2). No signal X rays from the elastic scattering that satisfy the correlation between energy and scattering angle were detected. We obtain a 95% C.L. upper limit for the scattering cross section of 1.9 x 10(-27) m(2) at omega(cms) = 6.5 keV. The upper limit is the lowest upper limit obtained so far by keV experiments. (C) 2016 The Author(s). Published by Elsevier B.V.

Time-resolved hard X-ray photoelectron spectroscopy (trHAXPES) using microfocused X-ray free-electron laser (XFEL, h nu = 8 keV) pulses as a probe and infrared laser pulses (h nu = 1.55 eV) as a pump is employed to determine intrinsic charge-carrier recombination dynamics in La:SrTiO3. By means of a combination of experiments and numerical N-body simulations, we first develop a simple approach to characterize and decrease XFEL-induced vacuum space-charge effects, which otherwise pose a serious limitation to spectroscopy experiments. We then show that, using an analytical mean-field model, vacuum space-charge effects can be counteracted by pump laser-induced photoholes at high excitation densities. This provides us a method to separate vacuum space-charge effects from the intrinsic charge-carrier recombination dynamics in the time domain. Our trHAXPES results thus open a route to studies of intrinsic charge-carrier dynamics on picosecond time scales with lateral spatial resolution on the micrometer scale.

We report a comparative study of the electronic structure of the compounds LaTe and CeTe, both of which crystallize in the rock salt structure. LaTe is a paramagnetic metal while CeTe is known to exhibit anomalous Kondo-like transport behaviour and undergoes a transition to a complex magnetically ordered state at low temperature (T-N = 2.2 K). We carry out hard X-ray photoelectron spectroscopy (HAXPES) of the core-levels and valence band of LaTe and CeTe at T = 20 K, in order to characterize their intrinsic electronic structure, and to address the role of Kondo effect on the electronic structure of CeTe. The bulk sensitive core level HAXPES spectra show evidence of screened features in the La 3d and Ce 3d states mixed with plasmon features. From a careful analysis of the Te, La and Ce derived core levels, we separate out the respective origins of the satellites and show that CeTe indeed exhibits definitive but weak f(0) and f(2) satellites due to Kondo screening, in addition to the main f(1) peak. The comparison of the valence band spectra of CeTe obtained using HAXPES and soft X-ray PES clearly identifies the Ce 4f(1) derived features. Resonant photoelectron spectrosocopy across the Ce 3d - 4f threshold confirms the Ce 4f(1) final state at the Fermi level, corresponding to the tail of the Kondo resonance feature which occurs above the Fermi level, while the Ce 4f(0) final state feature is observed at a binding energy of 2.4 eV. The 4f(0) and 4f(1) final states show giant resonances compared to the off-resonant spectra. However, in contrast to typical Kondo systems, the tail of the Ce 4f(1) Kondo resonance at the Fermi level is relatively suppressed compared to the Ce 4f(0) feature, which exhibits an unusually strong resonance enhancement. The results are indicative of a weakened Kondo effect which favours the magnetically ordered ground state in CeTe. (C) 2015 Elsevier B.V. All rights reserved.

Fiber optics for controlling the x-ray beam trajectory has been examined at the synchrotron facility of SPring-8. Up to now, we have achieved beam deflection by several tens of milli-radian and axis shift of around 75 mm with a 1.5 m-long flexible hollow glass capillary. The achievable beam deflecting angle, axis shift, and timing delay are, in principle, proportional to the length, the square of length and the cube of length, respectively. Thus, for further applications, requiring larger beam shift and pulse delay, longer fibers are indispensable. In order to achieve long-distance transport using the fiber, we thus examined the connection transferring x-rays between fibers in an experimental hutch. The acceptance angle at the input end and the throughput efficiency of the second fiber is consistent with the consideration of the output beam divergence of the first fiber. The enhancement of the transfer efficiency is also discussed for the cases of a closer joint and the use of a refractive lens as a coupler.

Direct spectroscopic evidence for a hydride bridge in the Ni-R form of [NiFe] hydrogenase has been obtained using iron-specific nuclear resonance vibrational spectroscopy (NRVS). The Ni-H-Fe wag mode at 675 cm(-1) is the first spectroscopic evidence for a bridging hydride in Ni-R as well as the first iron-hydride-related NRVS feature observed for a biological system. Although density function theory (DFT) calculation assisted the determination of the Ni-R structure, it did not predict the Ni-H-Fe wag mode at similar to 675 cm(-1) before NRVS. Instead, the observed Ni-H-Fe mode provided a critical reference for the DFT calculations. While the overall science about Ni-R is presented and discussed elsewhere, this article focuses on the long and strenuous experimental journey to search for and experimentally identify the Ni-H-Fe wag mode in a Ni-R sample. As a methodology, the results presented here will go beyond Ni-R and hydrogenase research and will also be of interest to other scientists who use synchrotron radiation for measuring dilute samples or weak spectroscopic features.

The metabolism of many anaerobes relies on [NiFe]-hydrogenases, whose characterization when bound to substrates has proven non-trivial. Presented here is direct evidence for a hydride bridge in the active site of the Fe-57-labelled fully reduced Ni-R form of Desulfovibrio vulgaris Miyazaki F [NiFe]-hydrogenase. A unique 'wagging' mode involving H- motion perpendicular to the Ni(mu-H)Fe-57 plane was studied using Fe-57-specific nuclear resonance vibrational spectroscopy and density functional theory (DFT) calculations. On Ni(mu-D)Fe-57 deuteride substitution, this wagging causes a characteristic perturbation of Fe-CO/CN bands. Spectra have been interpreted by comparison with Ni(mu-H/D)Fe-57 enzyme mimics [(dppe)Ni(mu-pdt)(mu-H/D)Fe-57(CO) 3](+) and DFT calculations, which collectively indicate a low-spin Ni(II)(mu-H)Fe(II) core for Ni-R, with H- binding Ni more tightly than Fe. The present methodology is also relevant to characterizing Fe-H moieties in other important natural and synthetic catalysts.

Hydrogenases are complex metalloenzymes that catalyze the reversible splitting of molecular hydrogen into protons and electrons essentially without overpotential. The NAD(+)-reducing soluble hydrogenase (SH) from Ralstonia eutropha is capable of H-2 conversion even in the presence of usually toxic dioxygen. The molecular details of the underlying reactions are largely unknown, mainly because of limited knowledge of the structure and function of the various metal cofactors present in the enzyme. Here, all iron-containing cofactors of the SH were investigated by Fe-57 specific nuclear resonance vibrational spectroscopy (NRVS). Our data provide experimental evidence for one [2Fe2S] center and four [4Fe4S] clusters, which is consistent with the amino acid sequence composition. Only the [2Fe2S] cluster and one of the four [4Fe4S] clusters were reduced upon incubation of the SH with NADH. This finding explains the discrepancy between the large number of FeS clusters and the small amount of FeS cluster-related signals as detected by electron paramagnetic resonance spectroscopic analysis of several NAD(+)-reducing hydrogenases. For the first time, Fe-CO and Fe-CN modes derived from the [NiFe] active site could be distinguished by NRVS through selective C-13 labeling of the CO ligand. This strategy also revealed the molecular coordinates that dominate the individual Fe-CO modes. The present approach explores the complex vibrational signature of the Fe-S clusters and the hydrogenase active site, thereby showing that NRVS represents a powerful tool for the elucidation of complex biocatalysts containing multiple cofactors.

The properties of CO-inhibited Azotobacter vinelandii (Av) Mo-nitrogenase (N(2)ase) have been examined by the combined application of nuclear resonance vibrational spectroscopy (NRVS), extended X-ray absorption fine structure (EXAFS), and density functional theory (DFT). Dramatic changes in the NRVS are seen under high-CO conditions, especially in a 188 cm(1) mode associated with symmetric breathing of the central cage of the FeMo-cofactor. Similar changes are reproduced with the alpha-H195Q N(2)ase variant. In the frequency region above 450 cm(1), additional features are seen that are assigned to Fe-CO bending and stretching modes (confirmed by (CO)-C-13 isotope shifts). The EXAFS for wild-type N(2)ase shows evidence for a significant cluster distortion under high-CO conditions, most dramatically in the splitting of the interaction between Mo and the shell of Fe atoms originally at 5.08 angstrom in the resting enzyme. A DFT model with both a terminal -CO and a partially reduced -CHO ligand bound to adjacent Fe sites is consistent with both earlier FT-IR experiments, and the present EXAFS and NRVS observations for the wild-type enzyme. Another DFT model with two terminal CO ligands on the adjacent Fe atoms yields Fe-CO bands consistent with the alpha-H195Q variant NRVS. The calculations also shed light on the vibrational shake modes of the interstitial atom inside the central cage, and their interaction with the Fe-CO modes. Implications for the CO and N-2 reactivity of N(2)ase are discussed.

We report the first results of a search for real photon-photon scattering using X rays. A novel system is developed to split and collide X-ray pulses by applying interferometric techniques. A total of 6.5 x 10(5) pulses (each containing about 10(11) photons) from an X-ray Free-Electron Laser are injected into the system. No scattered events are observed, and an upper limit of 1.7 x 10(-2)4 m(2) (95% C.L.) is obtained on the photon-photon elastic scattering cross section at 6.5 keV. (C) 2014 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.orgilicensesiby/3.0/). Funded by SCOAP(3).

The continuing effort to utilize the unique properties present in a number of strongly correlated transition metal oxides for novel device applications has led to intense study of their transitional phase state behavior. Here we report on time-resolved coherent X-ray diffraction measurements on a single vanadium dioxide nanocrystal undergoing a solid-solid phase transition, using the SACLA X-ray Free Electron Laser (XFEL) facility. We observe an ultrafast transition from monoclinic to tetragonal crystal structure in a single vanadium dioxide nanocrystal. Our findings demonstrate that the structural change occurs in a number of distinct stages attributed to differing expansion modes of vanadium atom pairs.

In order to utilize high-brilliance photon sources, such as X-ray free-electron lasers (XFELs), for advanced time-resolved photoelectron spectroscopy (TR-PES), a single-shot CCD-based data acquisition system combined with a high-resolution hemispherical electron energy analyzer has been developed. The system's design enables it to be controlled by an external trigger signal for single-shot pump-probe-type TR-PES. The basic performance of the system is demonstrated with an offline test, followed by online core-level photoelectron and Auger electron spectroscopy in 'single-shot image', 'shot-to-shot image (image-to-image storage or block storage)' and 'shot-to-shot sweep' modes at soft X-ray undulator beamline BL17SU of SPring-8. In the offline test the typical repetition rate for image-to-image storage mode has been confirmed to be about 15 Hz using a conventional pulse-generator. The function for correcting the shot-to-shot intensity fluctuations of the exciting photon beam, an important requirement for the TR-PES experiments at FEL sources, has been successfully tested at BL17SU by measuring Au 4f photoelectrons with intentionally controlled photon flux. The system has also been applied to hard X-ray PES (HAXPES) in 'ordinary sweep' mode as well as shot-to-shot image mode at the 27 m-long undulator beamline BL19LXU of SPring-8 and also at the SACLA XFEL facility. The XFEL-induced Ti 1s core-level spectrum of La-doped SrTiO3 is reported as a function of incident power density. The Ti 1s core-level spectrum obtained at low power density is consistent with the spectrum obtained using the synchrotron source. At high power densities the Ti 1s core-level spectra show space-charge effects which are analysed using a known mean-field model for ultrafast electron packet propagation. The results successfully confirm the capability of the present data acquisition system for carrying out the core-level HAXPES studies of condensed matter induced by the XFEL.

We have realized element-specific pump-probe time-resolved hard X-ray photoelectron spectroscopy (TR-HAXPES) for the study of ultrafast electron dynamics in condensed matter. TR-HAXPES has been applied for the first time to determine the temporal evolution of space-charge effects on Ti 1s core-level photoelectron spectra of SrTiO₃ at the SACLA X-ray free electron laser facility. We found that the temporal evolution of Ti 1s kinetic energy shifts can be well explained by a mean-field model for the electron propagation in the vacuum. We also report preliminary results of a real-time laser-assisted valence-transition in YbInCu₄, observed by measuring Yb 3d_5/2 core-level HAXPES spectra at BL19LXU of SPring-8, under ON/OFF conditions of an optical pump-laser. We observed drastic changes in intensities of the Yb²⁺ and Yb³⁺ spectral components induced by pump-laser irradiation.

A metre-length flexible hollow glass fibre with 20 mm-bore and 1.5 mm-cladding diameters for transporting a synchrotron X-ray beam and controlling the trajectory has been examined. The large cladding diameter maintains a moderate curvature to satisfy the shallow glancing angle of total reflection. The observed transmission efficiency was more than 20% at 12.4 keV. As a demonstration, a wide-area scan of a synchrotron radiation beam was performed to identify the elements for a fixed metal film through its absorption spectra.

A sputtered phase-change material, Ge-10 Sb-90, processed into dots with a height and diameter of 50 nm, shows rapid crystallization triggered by 300 ps laser excitation. Crystallization takes place with a short time delay of approximately 70 ns for a sample with Sb seed layers. The delay becomes just 15-20 ns when a NiCr layer is provided to control the heating-cooling profile. The nanodot sample requires less energy for crystallization, with a large optical change equivalent to that of the blanket film. These results demonstrate that the nanodot phase-change material could be a possible candidate for next-generation "green" optical storage.

We have investigated the Ce 4f electronic states in the Ce-doped manganites Nd0.45-xCexSr0.55MnO3 (NCSMO) by means of x-ray absorption spectroscopy (XAS) and hard x-ray photoelectron spectroscopy (HAXPES). The Ce 3d XAS shows that the Ce ions exist in the form of the Ce3+ and Ce4+ mixed-valent states, and we have found that the XAS spectral features change with temperature. The Ce 3d XAS and HAXPES spectra for NCSMO agree reasonably well with calculated results based on the single-impurity Anderson model, which takes into account the atomic multiplets and two valence bands. The estimated Ce bulk valence of Nd0.15Ce0.3Sr0.55MnO3 decreases from 3.44 to 3.30 with cooling.

The dynamical behavior of polystyrene-grafted silica nanoparticles dispersed in an atactic polystyrene matrix was studied using x-ray photon correlation spectroscopy. The time-autocorrelation functions were subjected to fitting analyses based on continuous-time random walk models. The nanoparticles exhibited non-Brownian behavior, and as the temperature increased, the crossover from hyperdiffusion to subdiffusion occurred at 1.25T(g), where T-g is the glass transition temperature of the matrix polystyrene. Hyperdiffusive behavior is caused by the dynamical heterogeneity of the polymer matrix associated with the glass transition. When the temperature was higher than 1.25T(g), the interaction of the grafted polymers with the polymer matrix became relatively significant, and caused a dramatic change in the dynamical behavior of the nanoparticles.

We have developed a system of laser-pump and synchrotron radiation probe microdiffraction to investigate the phase-change process on a nanosecond time scale of Ge2Sb2Te5 film embedded in multi-layer structures, which corresponds to real optical recording media. The measurements were achieved by combining (i) the pump-laser system with a pulse width of 300 ps, (ii) a highly brilliant focused microbeam with wide peak-energy width (Delta E/E similar to 2%) made by focusing helical undulator radiation without monochromatization, and (iii) a precise sample rotation stage to make repetitive measurements. We successfully detected a very weak time-resolved diffraction signal by using this system from 100-nm-thick Ge2Sb2Te5 phase-change layers. This enabled us to find the dependence of the crystal-amorphous phase change process of the Ge2Sb2Te5 layers on laser power. (C) 2013 AIP Publishing LLC.

A search for paraphotons, or hidden U(1) gauge bosons, is performed using an intense X-ray beamline at SPring-8. "Light Shining through a Wall" technique is used in this search. No excess of events above background is observed. A stringent constraint is obtained on the photon-paraphoton mixing angle, χ&lt 8.06×10-5 (95% C.L.) for 0.04eV&lt mγ'&lt 26keV. © 2013 Elsevier B.V.

A Si(111) winged crystal has been designed to minimize anticlastic bending and improve sagittal focusing efficiency. The crystal was thin with wide stiffening wings. The length-to-width ratio of the crystal was optimized by finite element analysis, and the optimal value was larger than the 'golden value'. The analysis showed that the slope error owing to anticlastic bending is less than the Darwin width. The X-rays were focused two-dimensionally using the crystal and a tangentially bent mirror. The observed profiles of the focal spot agreed well with the results of a ray-tracing calculation in the energy range from 8 to 17.5 keV. X-ray diffraction measurements with a high signal-to-noise ratio using this focusing system were demonstrated for a small protein crystal. © 2013 International Union of Crystallography.

In the present review, we focus on the characterization of polymer brushes by quantum beam, which is regarded as a promising probe of surface and interface analysis. The polymer brushes were prepared on various shapes of surface, and proved to be benefit to various applications. Among them, the polymer brushes grafted on sphere nanoparticles and flat substrates are investigated as representative cases. The static structure of polymer brushes, especially the chain dimension of polymer brushes grafted on nanoparticles and a flat substrate, have been studied by small angle X-ray scattering (SAXS) and neutron reflectivity (NR), respectively. The microscopic dynamical properties of polymer brushes are also expected to be revealed by quantum beam. X-ray photon correlation spectroscopy (XPCS), a technique using a coherent X-ray, is one of the promising methods for microscopically understanding of dynamical properties of polymer brushes. Some of our recent studies about dynamical behavior of polymer brush immobilized nanoparticle by XPCS are also presented.

The effects of a thermal gradient on the dynamical behavior of nanoparticles dispersed in a polymer matrix were studied using X-ray photon correlation spectroscopy. Polystyrene (PS)-grafted silica nanoparticles (SiNPs-PS), which are nanoparticles dispersed in a PS matrix controlled at temperatures above the glass transition temperature, were used in this study. Anisotropic motions of the SiNPs-PS were observed when the sample was kept in a conventional capillary tube, whereas isotropic motion was observed when the sample was kept in a newly designed cell with a low thermal flow, demonstrating the importance of the thermal gradient on the dynamical behavior of the SiNPs-PS. Polymer Journal (2013) 45, 94-99; doi: 10.1038/pj.2012.193; published online 21 November 2012

We have developed an ultrafast pump and probe experimental system of SACLA combining XFEL and IR-UV lasers. Preliminary tests of pump and probe experiments have been conducted in the autumn of 2011.

Ultrafast time-resolved Bragg coherent X-ray diffraction (CXD) has been performed to investigate lattice dynamics in a thin crystal layer with a nanoscale thickness by using a SASE (Self-Amplified Spontaneous Emission)-XFEL (X-ray Free Electron Laser) facility, SACLA. Single-shot Bragg coherent diffraction patterns of a 100nm-thick silicon crystal were measured in the asymmetric configuration with a grazing exit using an area detector. The measured coherent diffraction patterns showed fringes extending in the surface normal direction. By using an optical femtosecond laser-pump and the XFEL-probe, a transient broadening of coherent diffraction pattern profile was observed at a delay time of around a few tens of picosecond, indicating transient crystal lattice fluctuation induced by the optical laser. A perspective application of the time-resolved Bragg CXD method to investigate small sized grains composing ceramic materials is discussed. © 2013 The Ceramic Society of Japan. All rights reserved.

X-ray beam deflection control method using a single flexible glass capillary is proposed to illuminate a fixed sample at a target position with different incidence angle. A 700 mm-long capillary with a bore diameter of 50 micron and an outer diameter of 2 mm, which gives suitable flexibility for the critical curvature, was employed for the test experiment in SPring-8. The X-ray beam with a wavelength of 0.1 nm was introduced into the capillary, whose axis at the input side was finely adjusted to be parallel to the X-ray beam axis with swivel-, rotation- and translation stages. The divergence angle of output beam was measured and is 1-2 mrad. By moving the output-side capillary-support transversely to the beam axis, the beam deflection angle was changed over the range of about 80 mrad. The maximum throughput was larger than 60 % in efficiency, and 8 × 1010 photons/s in flux. Mapping with the beam deflection system has also been demonstrated for X-ray absorption measurement of a test sample composed of copper and nickel films. The materials were identified by changing the X-ray photon energy around their absorption edges. © 2013 IOP Publishing Ltd.

A scanning tunneling microscope ( STM) dedicated to in- situ experiments under the irradiation of highly brilliant hard X-rays of synchrotron radiation (SR) can serve a variety of original scientific works. The primary thermal effect by irradiation on the SR- STM system was verified. To separate the thermal effect from the effect by electronic emission or surface photo- voltage (SPV), a geometry was attempted to irradiate deep areas of the sample that lie far from the surface. The results revealed quantitatively that the stripe appearing in the STM image that corresponds to the oneoff switching of the X-ray beam is attributed neither to the emission nor SPV, but rather to a thermal effect. Thermal disturbance could be effectively removed from the STM signal by reducing beam size from phi 200 mm to phi 10 mm in diameter. This process provides general clues for increasing the sensitivity of SR- STM for nanoscale chemical analyses. (C) 2012 Elsevier B. V. All rights reserved.

The performance of a fast pixel array detector with a grid mask resolution enhancer has been demonstrated for X-ray photon correlation spectroscopy (XPCS) measurements to investigate fast dynamics on a microscopic scale. A detecting system, in which each pixel of a single-photon-counting pixel array detector, PILATUS, is covered by grid mask apertures, was constructed for XPCS measurements of silica nanoparticles in polymer melts. The experimental results are confirmed to be consistent by comparison with other independent experiments. By applying this method, XPCS measurements can be carried out by customizing the hole size of the grid mask to suit the experimental conditions, such as beam size, detector size and sample-to-detector distance.

We have developed a soft x-ray time-resolved photoemission spectroscopy system using synchrotron radiation (SR) at SPring-8 BL07LSU and an ultrashort pulse laser system. Two-dimensional angle-resolved measurements were performed with a time-of-flight-type analyzer. The photoemission spectroscopy system is synchronized to light pulses of SR and laser using a time control unit. The performance of the instrument is demonstrated by mapping the band structure of a Si(111) crystal over the surface Brillouin zones and observing relaxation of the surface photo-voltage effect using the pump (laser) and probe (SR) method. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.3687428]

Seeding a Free-Electron Laser (FEL) drastically improves the temporal coherence of the self-amplified spontaneous emission and reduces the saturation length, even with very low-intensity seed. We report here on the achievement of single-shot nonlinear harmonics from the 2nd to the 7th order at 23 nm, on the FEL of the SCSS Test Accelerator operated at 150MeV and seeded at 160nm with harmonics generated in gas. In particular, a clear intensity enhancement leading to saturation effect observations and temporal coherence improvement for both odd and even harmonics are highlighted due to the seeding. Single-shot measurements both in spatial (vertical) and spectral domains are compared to analytical theory and numerical simulations. Copyright (C) EPLA, 2011

X-ray induced atomic motion on a Ge(111)-c(2 X 8) clean surface at room temperature was directly observed with atomic resolution using a synchrotron radiation (SR)-based scanning tunneling microscope (STM) system under ultra high vacuum condition. The atomic motion was visualized as a tracking image by developing a method to merge the STM images before and after X-ray irradiation. Using the tracking image, the atomic mobility was found to be strongly affected by defects on the surface, but was not dependent on the incident X-ray energy, although it was clearly dependent on the photon density. The atomic motion can be attributed to surface diffusion, which might not be due to core-excitation accompanied with electronic transition, but a thermal effect by X-ray irradiation. The crystal surface structure was possible to break even at a lower photon density than the conventionally known barrier. These results can alert X-ray studies in the near future about sample damage during measurements, while suggesting the possibility of new applications. Also the obtained results show a new availability of the in-situ SR-STM system.

FEL have been recently evolving very fast from vacuum-ultraviolet to soft X-ray region. Once seeded with high harmonics generated in gas, these light sources deliver amplified emissions with properties which are, for most of them, directly linked to the injected harmonic beam, e.g. the ultrashort pulse duration for FEL and the high temporal and spatial degree of coherence. Since the last two years the developments of techniques for improving the harmonic properties for seeding FEL lead to major results on tunability, intensity, repetition rate and polarization. Actually harmonics are nowadays used for numbers of applications, before limited to FEL facility. Also, FEL based on harmonic seeding can benefit from the natural synchronization between the FEL, the harmonic and the laser used for generation, which makes it a perfect candidate for pump-probe experiment with fs resolution.

X-ray photon correlation spectroscopy system was setup at SPring-8, BL19LXU, and the partial coherence scattering data from the silica particles grafted with polymer brush in polystyrene matrix were measured. Firstly, the static speckle patterns were checked. Below the glass transition temperature of polystyrene (T-g), speckles were clearly observed, on the other hand, above T-g, the scattering patterns became smooth and speckles were hardly observed. These variances of the speckle patterns result from the particle motion. Secondly, from the time variance of the speckle data, time autocorrelation functions g(2)(q,t) are calculated. While the flat behaviour of g(2)(q,t) without relaxation were observed below T-g, the relaxation behavior with relaxation time similar to 10(0)-10(1) were observed above T-g

We designed and installed two types of long-working-distance Kirkpatrick-Baez (KB) mirrors and mirror manipulators, which were customized into each experiment for hard x-ray undulator beamlines at SPring-8. For the BL32XU RIKEN Targeted Proteins beamline, 400-mm-long KB focusing mirrors for a beam size of 1 mu m with a 730-mm-long working distance were designed for carrying out the structural analysis of protein microcrystals. We realized a focusing beam size of 0.9 x 0.9 mu m(2) (FWHM) and a focusing intensity of 6 x 10(10) (photons/s) at an x-ray energy of 12.4 keV. For the BL19LXU RIKEN SR Physics beamline, we developed KB mirrors for 100-nm focusing with a 100-mm-working distance for the purpose of nano-focus x-ray diffraction. A focusing beam size of 100 x 100 nm(2) (FWHM) and a high focusing intensity of 3.7 x 10(10) (photons/s) at an x-ray energy of 12.4 keV were realized.