(Sub-)Picosecond Surface Correlations of Femtosecond Laser Excited Al-Coated Multilayers Observed by Grazing-Incidence X-ray Scattering.

Femtosecond high-intensity laser pulses at intensities surpassing 10 W/cm can generate a diverse range of functional surface nanostructures. Achieving precise control over the production of these functional structures necessitates a thorough understanding of the surface morphology dynamics with nanometer-scale spatial resolution and picosecond-scale temporal resolution. In this study, we show that single XFEL pulses can elucidate structural changes on surfaces induced by laser-generated plasmas using grazing-incidence small-angle X-ray scattering (GISAXS).

Seeded stimulated X-ray emission at 5.9 keV.

X-ray free-electron lasers (XFELs) provide intense pulses that can generate stimulated X-ray emission, a phenomenon that has been observed and studied in materials ranging from neon to copper. Two schemes have been employed: amplified spontaneous emission (ASE) and seeded stimulated emission (SSE), where a second color XFEL pulse provides the seed. Both phenomena are currently explored for coherent X-ray laser sources and spectroscopy.

Femtosecond Reduction of Atomic Scattering Factors Triggered by Intense X-Ray Pulse.

X-ray diffraction of silicon irradiated with tightly focused femtosecond x-ray pulses (photon energy, 11.5 keV; pulse duration, 6 fs) was measured at various x-ray intensities up to 4.6×10^{19}  W/cm^{2}.

Non-thermal structural transformation of diamond driven by x-rays.

Intense x-ray pulses can cause the non-thermal structural transformation of diamond. At the SACLA XFEL facility, pump x-ray pulses triggered this phase transition, and probe x-ray pulses produced diffraction patterns. Time delays were observed from 0 to 250 fs, and the x-ray dose varied from 0.

Transonic dislocation propagation in diamond.

The motion of line defects (dislocations) has been studied for more than 60 years, but the maximum speed at which they can move is unresolved. Recent models and atomistic simulations predict the existence of a limiting velocity of dislocation motion between the transonic and subsonic ranges at which the self-energy of dislocation diverges, though they do not deny the possibility of the transonic dislocations. We used femtosecond x-ray radiography to track ultrafast dislocation motion in shock-compressed single-crystal diamond.

Sub-nanometer scale depth patterning on sapphire crystal by femtosecond soft x-ray laser pulse irradiation.

Damage thresholds and structures on a metal aluminum and an aluminum oxide crystal induced by the soft x-ray free electron laser irradiations were evaluated. Distinctive differences in damage thresholds and structures were observed for these materials. On the aluminum oxide crystal surface, in particular, a novel, to the best of our knowledge, surface processing, which we suggest defining as "peeling," was recognized.

X-ray free electron laser observation of ultrafast lattice behaviour under femtosecond laser-driven shock compression in iron.

Over the past century, understanding the nature of shock compression of condensed matter has been a major topic. About 20 years ago, a femtosecond laser emerged as a new shock-driver. Unlike conventional shock waves, a femtosecond laser-driven shock wave creates unique microstructures in materials.

Two-dimensional Kβ-Kα fluorescence spectrum by nonlinear resonant inelastic X-ray scattering.

High sensitivity of the Kβ fluorescence spectrum to electronic state is widely used to investigate spin and oxidation state of first-row transition-metal compounds. However, the complex electronic structure results in overlapping spectral features, and the interpretation may be hampered by ambiguity in resolving the spectrum into components representing different electronic states. Here, we tackle this difficulty with a nonlinear resonant inelastic X-ray scattering (RIXS) scheme, where we leverage sequential two-photon absorption to realize an inverse process of the Kβ emission, and measure the successive Kα emission.

Diamond formation kinetics in shock-compressed C─H─O samples recorded by small-angle x-ray scattering and x-ray diffraction.

Extreme conditions inside ice giants such as Uranus and Neptune can result in peculiar chemistry and structural transitions, e.g., the precipitation of diamonds or superionic water, as so far experimentally observed only for pure C─H and HO systems, respectively.

Delayed Onset and Directionality of X-Ray-Induced Atomic Displacements Observed on Subatomic Length Scales.

Transient structural changes of Al_{2}O_{3} on subatomic length scales following irradiation with an intense x-ray laser pulse (photon energy: 8.70 keV; pulse duration: 6 fs; fluence: 8×10^{2}  J/cm^{2}) have been investigated by using an x-ray pump x-ray probe technique. The measurement reveals that aluminum and oxygen atoms remain in their original positions by ∼20  fs after the intensity maximum of the pump pulse, followed by directional atomic displacements at the fixed unit cell parameters.

Single-shot spectrometer using diamond microcrystals for X-ray free-electron laser pulses.

A simple spectrometer using diffraction from diamond microcrystals has been developed to diagnose single-shot spectra of X-ray free-electron laser (XFEL) pulses. The large grain size and uniform lattice constant of the adopted crystals enable characterizing the XFEL spectrum at a resolution of a few eV from the peak shape of the powder diffraction profile. This single-shot spectrometer has been installed at beamline 3 of SACLA and is used for daily machine tuning.

Generation of intense phase-stable femtosecond hard X-ray pulse pairs.

Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length scale and timescale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more than 3 × 107 photons at 5.

Fine microstructure formation in steel under ultrafast heating and cooling.

This study evaluates phase transformation kinetics under ultrafast cooling using femtosecond X-ray diffraction for the operand measurements of the dislocation densities in Fe-0.1 mass% C-2.0 mass% Mn martensitic steel.

Independent contribution of optical attenuation length in ultrafast laser-induced structural change.

Although laser irradiation with femtosecond pulses is known to generate crystallization and morphological changes, the contribution of optical parameters to material changes is still in discussion. Here, we compare two structures irradiated near Si-L2,3 edges by an extreme ultraviolet femtosecond pulse. Our result implies that, despite the femtosecond irradiation regime, these values of the optical attenuation length between the wavelengths of 10.

Spatially resolved single-shot absorption spectroscopy with x-ray free electron laser pulse.

A new method of spatially resolved single-shot absorption spectroscopy for an x-ray free electron laser (XFEL) pulse has been developed by using a dispersive spectrometer and an elliptical mirror to enhance the spatial resolution. As a demonstration, we performed x-ray absorption near-edge structure measurement of Cu with a pump-probe scheme combining an XFEL pulse and a high-power femtosecond laser pulse. In the experiment, changes of an absorption spectrum in a plasma generated with a laser shot were successfully observed.

Atomic-Scale Visualization of Ultrafast Bond Breaking in X-Ray-Excited Diamond.

Ultrafast changes of charge density distribution in diamond after irradiation with an intense x-ray pulse (photon energy, 7.8 keV; pulse duration, 6 fs; intensity, 3×10^{19}  W/cm^{2}) have been visualized with the x-ray pump-x-ray probe technique. The measurement reveals that covalent bonds in diamond are broken and the electron distribution around each atom becomes almost isotropic within ∼5  fs after the intensity maximum of the x-ray pump pulse.

Determination of X-ray pulse duration via intensity correlation measurement of X-ray fluorescence. Erratum.

Corrections to equations and experimental results in the paper by Inoue et al. [(2019). J.

Evidence of shock-compressed stishovite above 300 GPa.

SiO is one of the most fundamental constituents in planetary bodies, being an essential building block of major mineral phases in the crust and mantle of terrestrial planets (1-10 M). Silica at depths greater than 300 km may be present in the form of the rutile-type, high pressure polymorph stishovite (P4/mnm) and its thermodynamic stability is of great interest for understanding the seismic and dynamic structure of planetary interiors. Previous studies on stishovite via static and dynamic (shock) compression techniques are contradictory and the observed differences in the lattice-level response is still not clearly understood.

Laser-induced damage thresholds and mechanism of silica glass induced by ultra-short soft x-ray laser pulse irradiation.

Laser-induced damage thresholds (LIDTs) of silica glasses obtained by the femtosecond soft x-ray free-electron laser (SXFEL, 13.5 nm, 70 fs) and the picosecond soft x-ray laser (SXRL, 13.9 nm, 7 ps) are evaluated.

Determination of X-ray pulse duration via intensity correlation measurements of X-ray fluorescence.

A simple method using X-ray fluorescence is proposed to diagnose the duration of an X-ray free-electron laser (XFEL) pulse. This work shows that the degree of intensity correlation of the X-ray fluorescence generated by irradiating an XFEL pulse on metal foil reflects the magnitude relation between the XFEL duration and the coherence time of the fluorescence. Through intensity correlation measurements of copper Kα fluorescence, the duration of 12 keV XFEL pulses from SACLA was evaluated to be ∼10 fs.