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.

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.

Abstract:We report the first observation of single-shot soft x-ray laser induced desorption occurring below the ablation threshold in a thin layer of poly (methyl methacrylate) -PMMA. Irradiated by the focused beam from the Free-electron LASer in Hamburg (FLASH) at 21.7nm, the samples have been investigated by atomic-force microscope (AFM) enabling the visualization of mild surface modifications caused by the desorption. A model describing non-thermal desorption and ablation has been developed and used to analyze single-shot imprints in PMMA. An intermediate regime of materials removal has been found, confirming model predictions. We also report below-threshold multiple-shot desorption of PMMA induced by high-order harmonics (HOH) at 32nm. Short-time exposure imprints provide sufficient information about transverse beam profile in HOH's tight focus whereas long-time exposed PMMA exhibits radiation-initiated surface hardening making the beam profile measurement infeasible. B. Rus, A. Carillon, P. Dhez, P. Jaeglé, G. Jamelot, A. Klisnick, M. Nantel, and P. Zeitoun, "An efficient, high-brightness soft X-ray laser at 21.2 nm," Phys. Rev. A55, 3858-3873 (1997 S. Heinbuch, M. Grisham, D. Martz, and J. J. Rocca, "Demonstration of a desk-top size high repetition rate soft x-ray laser," Opt. Express 13, 4050-4055 (2005). 10. P. E. Dyer, "Excimer laser polymer ablation: twenty years on," Appl. Phys. A77, 167-173 (2003), and references cited therein. 11. L. V. Zhigilei, B. J. Garrison, "Molecular dynamics simulation study of the fluence dependence of particle yield and plume composition in laser desorption and ablation of organic solids," Appl. Phys. Lett. 74, 1341-1343 (1999)

Samples of B4C, amorphous C, chemical-vapor-deposition-diamond C, Si, and SiC were exposed to single 25fs long pulses of 32.5nm free-electron-laser radiation at fluences of up to 2.2J∕cm2. The samples were chosen as candidate materials for x-ray free-electron-laser optics. It was found that the threshold for surface damage is on the order of the fluence required for thermal melting. For larger fluences, the crater depths correspond to temperatures on the order of the critical temperature, suggesting that the craters are formed by two-phase vaporization.

Large-scale plasma was created in molecular gases (CO, CO2, N2, H2O) and their mixtures by high-power laser-induced dielectric breakdown (LIDB). Compositions of the mixtures used are those suggested for the early earth's atmosphere of neutral and/or mildly reducing character. Time-integrated optical spectra emitted from the laser spark have been measured and analyzed. The spectra of the plasma generated in the CO-containing mixtures are dominated by emission of both C2 and CN radicals. A vibrational temperature of approximately 10(4) K was determined according to an intensity distribution in a vibronic structure of the CN (B2Sigma(+)u-X2Sigma(+)g) violet band. For comparison, the NH3-CH4-H2-H2O mixture has been irradiated as a model of the strongly reducing version of the early earth's atmosphere. In this mixture, excited CN seems to be significantly less abundant than C2. The LIDB experiments were in the molecular gases carried out not only in the static cell but also using a large, double stream pulse jet (gas puff target) placed in the vacuum interaction chamber. The obtained soft X-ray emission spectra indicate the presence of highly charged atomic ions in the hot core of high-power laser sparks.