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Intense sub-micrometre focusing of a soft X-ray free-electron laser (FEL) was achieved by using an ellipsoidal mirror with a high numerical aperture. A hybrid focusing system in combination with a Kirkpatrick-Baez mirror was applied for compensation of a small spatial acceptance of the ellipsoidal mirror. With this system, the soft X-ray FEL pulses were focused down to 480 nm × 680 nm with an extremely high intensity of 8.8×10 16  W cm -2 at a photon energy of 120 eV, which yielded saturable absorption at the L-edge of Si (99.8 eV) with a drastic increase of transmittance from 8% to 48%.

We report a method of femtosecond crystallography for solving radiation damage-free crystal structures of large proteins at sub-angstrom spatial resolution, using a large single crystal and the femtosecond pulses of an X-ray free-electron laser (XFEL). We demonstrated the performance of the method by determining a 1.9-Å radiation damage-free structure of bovine cytochrome c oxidase, a large (420-kDa), highly radiation-sensitive membrane protein.

We present femtosecond time-resolved X-ray absorption spectroscopy of aqueous solution using a hard x-ray free electron laser (SACLA) and a synchronized Ti:sapphire laser. The instrumental response time is 200 fs, and the repetition rate of measurement is 10 Hz. A cylindrical liquid beam 100 μm in diameter of aqueous ammonium iron(III) oxalate solution is photoexcited at 400 nm, and the transient X-ray absorption spectra are measured in the K-edge region of iron, 7.10 - 7.26 keV, using a dual X-ray beam dispersive detection method. Each of the dual beams has the pulse energy of 1.4 μJ, and pump-induced absorbance change on the order of 10(-3) is successfully detected. The photoexcited iron complex exhibits a red shifted iron K-edge with the appearance time constant of 260 fs. The X-ray absorption difference spectra, with and without the pump pulses, are independent of time delay after 1.5 ps up to 100 ps, indicating that the photoexcited species is long-lived.

X-ray free-electron lasers (FELs) enable crystallographic data collection using extremely bright femtosecond pulses from microscopic crystals beyond the limitations of conventional radiation damage. This diffraction-before-destruction approach requires a new crystal for each FEL shot and, since the crystals cannot be rotated during the X-ray pulse, data collection requires averaging over many different crystals and a Monte Carlo integration of the diffraction intensities, making the accurate determination of structure factors challenging. To investigate whether sufficient accuracy can be attained for the measurement of anomalous signal, a large data set was collected from lysozyme microcrystals at the newly established `multi-purpose spectroscopy/imaging instrument' of the SPring-8 Ångstrom Compact Free-Electron Laser (SACLA) at RIKEN Harima. Anomalous difference density maps calculated from these data demonstrate that serial femtosecond crystallography using a free-electron laser is sufficiently accurate to measure even the very weak anomalous signal of naturally occurring S atoms in a protein at a photon energy of 7.3 keV.

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.

Ultrabrilliant, femtosecond X-ray pulses from X-ray free-electron lasers (XFELs) have promoted the investigation of exotic interactions between intense X-rays and matters, and the observation of minute targets with high spatio-temporal resolution. Although a single X-ray beam has been utilized for these experiments, the use of multiple beams with flexible and optimum beam parameters should drastically enhance the capability and potentiality of XFELs. Here we show a new light source of a two-colour double-pulse (TCDP) XFEL in hard X-rays using variable-gap undulators, which realizes a large and flexible wavelength separation of more than 30% with an ultraprecisely controlled time interval in the attosecond regime. Together with sub-10-fs pulse duration and multi-gigawatt peak powers, the TCDP scheme enables us to elucidate X-ray-induced ultrafast transitions of electronic states and structures, which will significantly contribute to the advancement of ultrafast chemistry, plasma and astronomical physics, and quantum X-ray optics.

We determined the pulse duration of x-ray free electron laser light at 10 keV using highly resolved single-shot spectra, combined with an x-ray free electron laser simulation. Spectral profiles, which were measured with a spectrometer composed of an ultraprecisely figured elliptical mirror and an analyzer flat crystal of silicon (555), changed markedly when we varied the compression strength of the electron bunch. The analysis showed that the pulse durations were reduced from 31 to 4.5 fs for the strongest compression condition. The method, which is readily applicable to evaluate shorter pulse durations, provides a firm basis for the development of femtosecond to attosecond sciences in the x-ray region.