Saturable absorption is a phenomenon readily seen in the optical and infrared wavelengths. It has never been observed in core-electron transitions owing to the short lifetime of the excited states involved and the high intensities of the soft X-rays needed. We report saturable absorption of an L-shell transition in aluminium using record intensities over 10 16 W cm −2 at a photon energy of 92 eV. From a consideration of the relevant timescales, we infer that immediately after the X-rays have passed, the sample is in an exotic state where all of the aluminium atoms have an L-shell hole, and the valence band has approximately a 9 eV temperature, whereas the atoms are still on their crystallographic positions. Subsequently, Auger decay heats the material to the warm dense matter regime, at around 25 eV temperatures. The method is an ideal candidate to study homogeneous warm dense matter, highly relevant to planetary science, astrophysics and inertial confinement fusion. Saturable absorption, the decrease in the absorption of light with increasing intensity, is a well-known effect in the visible and near-visible region of the electromagnetic spectrum 1 , and is a widely exploited phenomenon in laser technology. Although there are many ways to induce this effect, in the simplest two-level system it will occur when the population of the lower, absorbing level is severely depleted, which requires light intensities sufficiently high to overcome relaxation from the upper level. Here, we report on the production of saturable absorption of a metal in the soft X-ray regime by the creation of highly uniform warm dense conditions, a regime that is of great interest in high-pressure science 2,3 , the geophysics of large planets 4,5 , astrophysics 6 , plasma production and inertial confinement fusion 7 . Furthermore, the process by which the saturation of the absorption occurs will lead, after the X-ray pulse, to the storage of about 100 eV per atom, which in turn evolves to a warm dense state. This manner of creation is unique as it requires intense, subpicosecond, soft X-rays. As such, it has not hitherto been observed in this region of the spectrum, owing both to the lack of high-intensity sources, and the rapid recombination times associated with such high photon energies. However, with the advent of new fourth-generation X-ray light sources, including the free-electron laser in Hamburg 8 (FLASH), soft X-ray intensities that have previously remained the province of high-power optical lasers can now be produced. Experiments at such high intensities using gas jets have already exhibited novel absorption phenomena 9 , and the possibility of irradiating solid samples with intense soft and hard X-rays has aroused interest as a possible means of producing warm dense matter (WDM) at known atomic densities 10,11 .We present the first measurements of the absorption coefficient of solid samples subject to subpicosecond soft X-ray pulses with intensities up to and in excess of 10 16 W cm −2 , two orders of magnitude higher than could ...

We present a new technique for the characterization of non-Gaussian laser beams which cannot be described by an analytical formula. As a generalization of the beam spot area we apply and refine the definition of so called effective area (A(eff)) [1] in order to avoid using the full-width at half maximum (FWHM) parameter which is inappropriate for non-Gaussian beams. Furthermore, we demonstrate a practical utilization of our technique for a femtosecond soft X-ray free-electron laser. The ablative imprints in poly(methyl methacrylate) - PMMA and amorphous carbon (a-C) are used to characterize the spatial beam profile and to determine the effective area. Two procedures of the effective area determination are presented in this work. An F-scan method, newly developed in this paper, appears to be a good candidate for the spatial beam diagnostics applicable to lasers of various kinds.

A linear accelerator based source of coherent radiation, FLASH (Free-electron LASer in Hamburg) provides ultra-intense femtosecond radiation pulses at wavelengths from the extreme ultraviolet (XUV; lambda<100nm) to the soft X-ray (SXR; lambda<30nm) spectral regions. 25-fs pulses of 32-nm FLASH radiation were used to determine the ablation parameters of PMMA - poly (methyl methacrylate). Under these irradiation conditions the attenuation length and ablation threshold were found to be (56.9+/-7.5) nm and approximately 2 mJ*cm(-2), respectively. For a second wavelength of 21.7 nm, the PMMA ablation was utilized to image the transverse intensity distribution within the focused beam at mum resolution by a method developed here.

Experimental results are presented from vacuum-ultraviolet free-electron laser (FEL) operating in the self-amplified spontaneous emission (SASE) mode. The generation of ultrashort radiation pulses became possible due to specific tailoring of the bunch charge distribution. A complete characterization of the linear and nonlinear modes of the SASE FEL operation was performed. At saturation the FEL produces ultrashort pulses (30-100 fs FWHM) with a peak radiation power in the GW level and with full transverse coherence. The wavelength was tuned in the range of 95-105 nm.

By use of high intensity XUV radiation from the FLASH free-electron laser at DESY, we have created highly excited exotic states of matter in solid-density aluminum samples. The XUV intensity is sufficiently high to excite an inner-shell electron from a large fraction of the atoms in the focal region. We show that soft-x-ray emission spectroscopy measurements reveal the electronic temperature and density of this highly excited system immediately after the excitation pulse, with detailed calculations of the electronic structure, based on finite-temperature density functional theory, in good agreement with the experimental results.

We investigated single shot damage of Mo/Si multilayer coatings exposed to the intense fs XUV radiation at the Free-electron LASer facility in Hamburg - FLASH. The interaction process was studied in situ by XUV reflectometry, time resolved optical microscopy, and "post-mortem" by interference-polarizing optical microscopy (with Nomarski contrast), atomic force microscopy, and scanning transmission electron microcopy. An ultrafast molybdenum silicide formation due to enhanced atomic diffusion in melted silicon has been determined to be the key process in the damage mechanism. The influence of the energy diffusion on the damage process was estimated. The results are of significance for the design of multilayer optics for a new generation of pulsed (from atto- to nanosecond) XUV sources.

Correspondence should be addressed to SPHR.Femtosecond pulses from soft-x-ray free-electron lasers (FELs) [1] are ideal for directly probing matter at atomic length scales and timescales of atomic motion. An important component of understanding ultrafast phenomena of light-matter interactions is concerned with the onset of atomic motion which is impeded by the atoms' inertia. This delay of structural changes will enable atomic-resolution flash-imaging [2][3] to be performed at upcoming x-ray FELs [4][5] with pulses intense enough to record the x-ray scattering from single molecules [6]. We explored this ultrafast high-intensity regime with the FLASH soft-x-ray FEL [7][8] by measuring the reflectance of nanostructured multilayer mirrors using pulses with fluences far in excess of the mirrors' damage threshold. Even though the nanostructures were ultimately completely destroyed, we found that they maintained their integrity and reflectance characteristics during the 25-fs-long pulse, with no evidence for any structural changes during that time over lengths greater than 3 Å.In the recently built FLASH FEL [7], x-rays are produced from short electron pulses oscillating in a periodic magnet array, called an undulator, by the principle of self-amplification of spontaneous emission [9][10]. The laser quality of the x-ray pulses can be quantified by the peak spectral brilliance of the source, which is 10 28 photons/(s mm 2 mrad 2 0.1% bandwidth) [8]; this is up to seven orders of magnitude higher than modern thirdgeneration synchrotron sources. For our studies, the machine operated with pulses of 25 fs duration at a wavelength of 32.5 nm and energies up to 21 μJ. We focused these pulses to 3x10 14 W/cm 2 onto our nanostructured samples, resulting in an the unprecedented heating rate of 5x10 18 K/s, while probing the irradiated structures at the nanometer length scale.The x-ray reflectivity of periodic nanometer-scale multilayers [11] is very sensitive to changes in the atomic positions and the refractive indices of the constituent materials, making them an ideal choice to study structural changes induced by ultrashort FEL pulses. The large multilayer reflectivity results from the cooperative interaction of the x-ray field with many layers of precisely fabricated thicknesses, each less than the x-ray wavelength. This Bragg or resonant reflection from the periodic structure is easily disrupted by any imperfection of the layers. The characteristics of the structure, such as periodicity or layer intermixing, can be precisely determined from the measurement of the Bragg reflectivity as a function of incidence angle. These parameters can be easily measured to a small fraction of the probe wavelength, as is well known in x-ray crystallography where average atomic positions of minerals or proteins are found to less than 0.01Å. Thus, we can explore ultrafast phenomena at length scales less than the wavelength, and investigate the conditions to overcome the effects of radiation damage by using ultrafast pulses.For our measurement...

We studied experimentally and theoretically the structural transition of diamond under an irradiation with an intense femtosecond extreme ultraviolet laser (XUV) pulse of 24-275 eV photon energy provided by free-electron lasers. Experimental results obtained show that the irradiated diamond undergoes a solid-to-solid phase transition to graphite, and not to an amorphous state. Our theoretical findings suggest that the nature of this transition is nonthermal, stimulated by a change of the interatomic potential triggered by the excitation of valence electrons. Ultrashort laser pulse duration enables to identify the subsequent steps of this process: electron excitation, band gap collapse, and the following atomic motion. A good agreement between the experimentally measured and theoretically calculated damage thresholds for the XUV range supports our conclusions. It is often observed that a femtosecond irradiation of a material induces an atomic disorder therein: amorphization, or defect creation. Graphitization of diamond is a counterexample as it is an order-to-order (solid-to-solid) phase transition. It illustrates the fundamental interplay between the bonding, respectively sp 3 and sp 2 bonds for diamond and graphite, and the structure, respectively cubic and hexagonal. The advent of extreme ultraviolet (XUV) and x-ray free-electron lasers (XFELs), delivering femtosecond intense pulses in the soft to hard x-ray domain allows investigating the structural transition of diamond within this unexplored regime and clarifying whether it leads to an ordered or disordered state. In our study we show the experimental results of the XUV irradiation of diamond followed by a dedicated theoretical analysis.Irradiation by an optical femtosecond laser pulse triggers a specific process known as a nonthermal phase transition, which has been demonstrated for a class of materials.1 However, there are still active debates over the nature of the observed nonthermal transitions, e.g., see Ref. 2. For this type of transition, models predict that the excitation of a few percent of the valence band electrons leads to a drastic modification of the potential energy surface, triggering the displacement of the atoms. This process occurs on a much faster time scale (subpicosecond) than the transfer of the absorbed laser energy to the lattice via electron-phonon coupling. Such a nonthermal phase transition still needs to be observed in the x-ray regime.In the XUV and x-ray domain the excitation of electrons is only due to single photon absorption, and the absorption by free electrons does not occur. As a result, the first stage of the interaction, electron excitation and heating, which are driving nonthermal processes, is quite different compared to the optical regime.1 It is then questionable if a nonthermal phase transition can be triggered by an XFEL pulse. In the present Rapid Communication we identify the phase transition, which diamond undergoes under femtosecond XUV irradiation, as the graphitization. We show that the final state of the...