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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}. The measurement reveals that the diffraction intensity is highly suppressed when the x-ray intensity reaches of the order of 10^{19}  W/cm^{2}. With a dedicated simulation, we confirm that the observed reduction of the diffraction intensity can be attributed to the femtosecond change in individual atomic scattering factors due to the ultrafast creation of highly ionized atoms through photoionization, Auger decay, and subsequent collisional ionization. We anticipate that this ultrafast reduction of atomic scattering factor will be a basis for new x-ray nonlinear techniques, such as pulse shortening and contrast variation x-ray scattering.

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. By comparing the experimental results and theoretical simulations, we interpret that electron excitation and relaxation triggered by the pump pulse modify the potential energy surface and drives the directional atomic displacements. Our results indicate that high-resolution x-ray structural analysis with the accuracy of 0.01 Å is feasible even with intense x-ray pulses by making the pulse duration shorter than the timescale needed to complete electron excitation and relaxation processes, which usually take up to a few tens of femtoseconds.

To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000 keV, duration: 6-7 fs, fluence: 2.0-3.5×10^{5}  J/cm^{2}) by ∼35%. This finding that core-hole atoms are applicable to nonlinear x-ray optics is an essential stepping stone for extending nonlinear technologies commonplace at optical wavelengths to the hard x-ray region.

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.

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.

X-ray fluorescence spectroscopy demonstrates that a single core-hole krypton with a 170-as lifetime can be photoionized again to a double core-hole state by an intense x-ray pulse. The observation indicates that unconventional interaction between intense x rays and atoms is no more negligible in applications with x-ray free-electron lasers. Quantitative analysis of the double core-hole creation including effects of a pulsed and spiky temporal structure enables estimation of the x-ray pulse duration in the sub-10-fs range.

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.

An atomic kinetics code is developed to gain insight into the generation of polarized Healpha by fast electron transport relevant to fast ignition. The calculation predicts a very small polarization in the dense region (>or=100 times the critical density) due to frequent elastic transitions between magnetic sublevels, while high polarization is observable in the low density region (