Dynamically patterning x-ray beam by a femtosecond optical laser.

Modern science and technology have greatly benefitted from our ability to precisely manipulate light waves, in both their spatial and temporal degrees of freedom. In the x-ray region, however, spatial control has been virtually static mainly due to stringent requirements for realizing high-performance optical elements. The lack of dynamic spatial control of x-ray beam has prevented researchers from realizing more sophisticated use of the wave field, which has rapidly advanced in the optical region in the past decades.

Hard X-ray Fourier transform holography at free electron lasers source.

We report on the feasibility of Fourier transform holography in the hard X-ray regime using a Free Electron Laser source. Our study shows successful single and multi-pulse holographic reconstructions of the nanostructures. We observe beam-induced heating of the sample exposed to the intense X-ray pulses leading to reduced visibility of the holographic reconstructions.

X-ray optics for the cavity-based X-ray free-electron laser.

A cavity-based X-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent X-ray sources. CBXFELs consist of a low-emittance electron source, a magnet system with several undulators and chicanes, and an X-ray cavity. The X-ray cavity stores and circulates X-ray pulses for repeated FEL interactions with electron pulses until the FEL reaches saturation.

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.

High-precision finishing method for narrow-groove channel-cut crystal x-ray monochromator using plasma chemical vaporization machining with wire electrode.

A channel-cut crystal monochromator (CCM) is a popular and powerful device for producing monochromatic x-ray beams with extreme angular stability at a nano-radian level. Narrowing the groove width of CCMs has various benefits; for example, it is made possible to design more compact CCMs with an equivalent working energy range and to reduce the optical delay and the amount of beam shift, enhancing compatibility with various experimental techniques. An obstacle to the use of narrow-groove CCMs is the lack of a high-precision finishing method for the inner-wall reflecting surfaces, which imposes the distortion of x-ray wavefronts and spectral purity.

A versatile pressure-cell design for studying ultrafast molecular-dynamics in supercritical fluids using coherent multi-pulse x-ray scattering.

Supercritical fluids (SCFs) can be found in a variety of environmental and industrial processes. They exhibit an anomalous thermodynamic behavior, which originates from their fluctuating heterogeneous micro-structure. Characterizing the dynamics of these fluids at high temperature and high pressure with nanometer spatial and picosecond temporal resolution has been very challenging.

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}.

Ultrafast X-Ray Scattering Reveals Composite Amplitude Collective Mode in the Weyl Charge Density Wave Material (TaSe_{4})_{2}I.

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe_{4})_{2}I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz amplitude mode derived primarily from a transverse acoustic mode of the high-symmetry structure.

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.

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.

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.

Split-pulse X-ray photon correlation spectroscopy with seeded X-rays from X-ray laser to study atomic-level dynamics.

With their brilliance and temporal structure, X-ray free-electron laser can unveil atomic-scale details of ultrafast phenomena. Recent progress in split-and-delay optics (SDO), which produces two X-ray pulses with time-delays, offers bright prospects for observing dynamics at the atomic-scale. However, their insufficient pulse energy has limited its application either to phenomena with longer correlation length or to measurement with a fixed delay-time.

Two-color X-ray free-electron laser consisting of broadband and narrowband beams.

A simple scheme is proposed and experimentally confirmed to generate X-ray free-electron lasers (XFELs) consisting of broadband and narrowband beams with a controllable intensity ratio and a large photon-energy separation. This unique two-color XFEL beam will open new opportunities for investigation of nonlinear interactions between intense X-rays and matter.

High-resolution micro channel-cut crystal monochromator processed by plasma chemical vaporization machining for a reflection self-seeded X-ray free-electron laser.

A high-resolution micro channel-cut crystal monochromator (µCCM) composed of an Si(220) crystal is developed for the purpose of narrowing the bandwidth of a reflection self-seeded X-ray free-electron laser. Subsurface damage on the monochromator, which distorts the wavefront and broadens the bandwidth of the monochromatic seed beam, was removed by using a plasma etching technique. High diffraction performance of the monochromator was confirmed through evaluation with coherent X-rays.

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.