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One of the important challenges in condensed matter science is to understand ultrafast, atomic-scale fluctuations that dictate dynamic processes in equilibrium and non-equilibrium materials. Here, we report an important step towards reaching that goal by using a state-of-the-art perfect crystal based split-and-delay system, capable of splitting individual X-ray pulses and introducing femtosecond to nanosecond time delays. We show the results of an ultrafast hard X-ray photon correlation spectroscopy experiment at LCLS where split X-ray pulses were used to measure the dynamics of gold nanoparticles suspended in hexane. We show how reliable speckle contrast values can be extracted even from very low intensity free electron laser (FEL) speckle patterns by applying maximum likelihood fitting, thus demonstrating the potential of a split-and-delay approach for dynamics measurements at FEL sources. This will enable the characterization of equilibrium and, importantly also reversible non-equilibrium processes in atomically disordered materials.

X-ray two-photon absorption (TPA) spectrum of metallic copper is measured using a free-electron laser (XFEL). The spectrum differs from that measured by the conventional one-photon absorption (OPA), and characterized by a peak below the Fermi level, which is assigned to the transition to the 3d state. The impact of the XFEL pulse on the OPA spectrum is discussed by analyzing the pulse-energy dependence, which indicates that the intrinsic TPA spectrum is measured.

We report a Bragg beam splitter developed for utilization of hard x-ray free-electron lasers. The splitter is based on an ultrathin silicon crystal operating in the symmetric Bragg geometry to provide high reflectivity and transmissivity simultaneously. We fabricated frame-shaped Si(511) and (110) crystals with thicknesses below 10 μm by a reactive dry etching method using atmospheric-pressure plasma. The thickness variation over an illuminated area is less than 300 nm peak-to-valley. High crystalline perfection was verified by topographic and diffractometric measurements. The crystal thickness was evaluated from the period of the Pendellösung beats measured with a highly monochromatic and collimated x-ray probe. The crystals provide two replica pulses with uniform wavefront [(<1/50)λ] and low spatial intensity variation (<5%). These Bragg beam splitters will play an important role in innovating XFEL applications.

A method of fabricating multilayer focusing mirrors that can focus X-rays down to 10 nm or less was established in this study. The wavefront aberration induced by multilayer Kirkpatrick–Baez mirror optics was measured using a single grating interferometer at a photon energy of 9.1 keV at SPring-8 Angstrom Compact Free Electron Laser (SACLA), and the mirror shape was then directly corrected by employing a differential deposition method. The accuracies of these processes were carefully investigated, considering the accuracy required for diffraction-limited focusing. The wavefront produced by the corrected multilayer focusing mirrors was characterized again in the same manner, revealing that the root mean square of the wavefront aberration was improved from 2.7 (3.3) rad to 0.52 (0.82) rad in the vertical (horizontal) direction. A wave-optical simulator indicated that these wavefront-corrected multilayer focusing mirrors are capable of achieving sub-10-nm X-ray focusing.

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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. The 15 fs time delay observed between the bond breaking and atomic disordering indicates nonisothermality of electron and lattice subsystems on this timescale. From these observations and simulation results, we interpret that the x-ray-induced change of the interatomic potential drives the ultrafast atomic disordering underway to the following nonthermal melting.

The photoproduction process of neutral kaons on a liquid deuterium target is investigated near the threshold region, Eγ = 0.8-1.1 GeV. K 0 events are reconstructed from positive and negative pions, and differential cross sections are derived. Experimental momentum spectra are compared with those calculated in the spectator model using a realistic deuteron wave function. Elementary amplitudes as given by recent isobar models and a simple phenomenological model are used to study the effect of the new data on the angular behavior of the elementary cross section. The data favor a backward-peaked angular distribution of the elementary n(γ, K 0 )Λ process, which provides additional constraints on current models of kaon photoproduction. The present study demonstrates that the n(γ, K 0 )Λ reaction can provide key information on the mechanism of the photoproduction of strangeness.