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Nature Communications 12(1), 1638 (2021). doi:10.1038/s41467-021-21756-6, Key insights in materials at extreme temperatures and pressures can be gained by accurate measurements that determine the electrical conductivity. Free-electron laser pulses can ionize and excite matter out of equilibrium on femtosecond time scales, modifying the electronic and ionic structures and enhancing electronic scattering properties. The transient evolution of the conductivity manifests the energy coupling from high temperature electrons to low temperature ions. Here we combine accelerator-based, high-brightness multi-cycle terahertz radiation with a single-shot electro-optic sampling technique to probe the evolution of DC electrical conductivity using terahertz transmission measurements on sub-picosecond time scales with a multi-undulator free electron laser. Our results allow the direct determination of the electron-electron and electron-ion scattering frequencies that are the major contributors of the electrical resistivity., Published by Nature Publishing Group UK, [London]

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si$${_3}$$ 3 N$$_4$$ 4 , on sub-picosecond timescales. Si$${_3}$$ 3 N$$_4$$ 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si$${_3}$$ 3 N$$_4$$ 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si$${_3}$$ 3 N$$_4$$ 4 -based diagnostics tool.

Optics express 28(18), 25664-25681 (2020). doi:10.1364/OE.396755, Proper diagnostics of intense free-electron laser (FEL) X-ray pulses is indisputably important for experimental data analysis as well as for the protection of beamline optical elements. New challenges for beam diagnostic methods are introduced by modern FEL facilities capable of delivering powerful pulses at megahertz (MHz) repetition rates. In this paper, we report the first characterization of a defocused MHz 13.5-nm beam generated by the free-electron laser in Hamburg (FLASH) using the method of multi-pulse desorption imprints in poly(methyl methacrylate)(PMMA). The beam fluence profile is reconstructed in a novel and highly accurate way that takes into account the nonlinear response of material removal to total dose delivered by multiple pulses. The algorithm is applied to experimental data of single-shot ablation imprints and multi-shot desorption imprints at both low (10 Hz) and high (1 MHz) repetition rates. Reconstructed response functions show a great agreement with the theoretical desorption response function model., Published by Soc., Washington, DC

A split-and-delay unit for the XUV and soft X-ray spectral range has been installed at beamlines FL23 and FL24 at the FLASH2 Free-Electron Laser at DESY. It enables time-resolved pump-probe experiments covering the whole spectral range of FLASH2 from 30 eV up to 1500 eV. Using wavefront beam splitting and grazing incidence mirrors a sub-fs resolution with a relative pulse delay of -5 ps ≤ uτ ≤ +18 ps is achieved. Two different mirror coatings are required to cover the complete spectral range and thus, a design that is based on a three dimensional beam path was developed. This allows the choice between different sets of mirrors with either coating for the fixed branch. In the variable branch two coatings are available on the same set of mirrors. A Ni coating allows a total transmission above T > 0.50 for photon energies between hν ≈ 30 eV and 650 eV at a grazing angle of a ϑvariable = 1.8° in the beam path with variable delay. With a Pt coating a transmission of T > 13 % is possible for photon energies up to hν = 1500 eV. In the fixed beam path at a grazing angle of ϑfixed = 1.3° a transmission of T > 60 % with a Ni coating and T > 28 % with a Pt coating is possible.

Journal of synchrotron radiation 28(3), 688 - 706 (2021). doi:10.1107/S1600577521002551, The high-precision X-ray diffraction setup for work with diamond anvil cells (DACs) in interaction chamber 2 (IC2) of the High Energy Density instrument of the European X-ray Free-Electron Laser is described. This includes beamline optics, sample positioning and detector systems located in the multipurpose vacuum chamber. Concepts for pump–probe X-ray diffraction experiments in the DAC are described and their implementation demonstrated during the First User Community Assisted Commissioning experiment. X-ray heating and diffraction of Bi under pressure, obtained using 20 fs X-ray pulses at 17.8 keV and 2.2 MHz repetition, is illustrated through splitting of diffraction peaks, and interpreted employing finite element modeling of the sample chamber in the DAC., Published by Wiley-Blackwell, [S.l.]

Intense fs-XUV laser-induced transient optical properties following free electron generation are investigated experimentally and theoretically. Electron-dynamics and resulting transient changes of the reflectivity and transmissivity and recently also the change of phase of an additional fs-probe pulse is considered. This completes the information of optical properties during the interaction process, which is of importance for basic research and diagnostic purposes.

The free-free opacity in plasmas is fundamental to our understanding of energy transport in stellar interiors and for inertial confinement fusion research. However, theoretical predictions in the challenging dense plasma regime are conflicting and there is a dearth of accurate experimental data to allow for direct model validation. Here we present time-resolved transmission measurements in solid-density Al heated by an XUV free-electron laser. We use a novel functional optimization approach to extract the temperature-dependent absorption coefficient directly from an oversampled pool of single-shot measurements, and find a pronounced enhancement of the opacity as the plasma is heated to temperatures of order of the Fermi energy. Plasma heating and opacity enhancement are observed on ultrafast timescales, within the duration of the femtosecond XUV pulse. We attribute further rises in the opacity on ps timescales to melt and the formation of warm dense matter.

Journal of synchrotron radiation 25(1), 77 - 84 (2018). doi:10.1107/S1600577517017362, The durability of grazing- and normal-incidence optical coatings has been experimentally assessed under free-electron laser irradiation at various numbers of pulses up to 16 million shots and various fluence levels below 10% of the single-shot damage threshold. The experiment was performed at FLASH, the Free-electron LASer in Hamburg, using 13.5 nm extreme UV (EUV) radiation with 100 fs pulse duration. Polycrystalline ruthenium and amorphous carbon 50 nm thin films on silicon substrates were tested at total external reflection angles of 20° and 10° grazing incidence, respectively. Mo/Si periodical multilayer structures were tested in the Bragg reflection condition at 16° off-normal angle of incidence. The exposed areas were analysed post-mortem using differential contrast visible light microscopy, EUV reflectivity mapping and scanning X-ray photoelectron spectroscopy. The analysis revealed that Ru and Mo/Si coatings exposed to the highest dose and fluence level show a few per cent drop in their EUV reflectivity, which is explained by EUV-induced oxidation of the surface., Published by IUCr, Chester

The journal of chemical physics 154(20), 204706 (1-8) (2021). doi:10.1063/5.0041261, The response of a free-standing graphene monolayer exposed to a few tens of femtoseconds long extreme ultraviolet (XUV) pulse was studied theoretically in order to analyze and compare contributions of various mechanisms to the graphene damage, understood here as a global atomic disintegration. Our simulation results indicate that nonthermal disintegration of the atomic structure is the predominant damage mechanism for a free-standing graphene layer. Only at high absorbed doses, charge-induced disintegration of the graphene structure prevails. We also demonstrate that the progressing damage can be probed by femtosecond optical pulses in the soft UV regime (4 eV photon energy). The achieved quantitative understanding of the damage mechanisms may enable a better control of graphene-based devices when they are exposed to x-ray radiation, as well as an efficient processing of graphene layers with ultrashort intense XUV pulses., Published by American Institute of Physics, Melville, NY

An accurate transmission measurement of thin foils (usually made of elemental metals and/or semiconductors), which routinely are used as attenuators in soft x-ray beamlines, end-stations and instruments, represents a long standing problem over the wide experimentation field with photon beams, see for example [1-4]. Such foils are also frequently utilized for blocking long wavelength emission, i.e., UV-Vis-IR radiation, from plasma and high order harmonic sources, whilst soft x-rays emitted from the source pass through the foil with only a slight attenuation. Despite the enormous amount of data available in the literature, e.g., Henke’s tables [5], measurements made on real foils often provide surprising results. In this study, a procedure based on the ablation imprints method is utilized for determination of soft x-ray filter transmission, namely the f-scan technique [6,7]. This technique combines the GMD (Gas Monitor Detector) pulse energy measurement and attenuation of the beam by foils (made of different metallic/semiconducting elements of varying thickness) with areas of ablation imprints created on a suitable target, e.g. PMMA – Poly(methyl methacrylate). The results show only a partial overlap with transmission values found in Henke’s tables. Nevertheless, a good agreement with transmission values determined by conventional radiometry techniques at synchrotron radiation beamlines has been found. Such a difference between the experimentally obtained values and transmissions calculated for a pure element is usually explained by spontaneous formation of oxidized layers on the filter surface and in the near-surface layer and their possible alteration by intense FEL radiation. The first results obtained with Al, Nb, Zr and Si filters at FLASH/FLASH2 (Free-electron LASer in Hamburg tuned to 13.5 nm) facilities will be shown and discussed in this presentation. References 1. F. R. Powell, P. W. Vedder, J. F. Lindblom, S. F. Powell: Thin film filter performance for extreme ultraviolet and x-ray applications, Opt. Eng. 29, 614 (1990). 2. E. M. Gullikson, P. Denham, S. Mrowka, J. H. Underwood: Absolute photo absorption measurements of Mg, Al, and Si in the soft x-ray region below the L2,3 edges, Phys. Rev. B 49, 16 283 (1994). 3. R. Keenan, C. L. S. Lewis, J. S. Wark, E. Wolfrum: Measurements of the XUV transmission of aluminium with a soft x-ray laser, J. Phys. B 35, L449 (2002). 4. A. Joseph, M. H. Modi, A. Singh, R. K. Gupta, G. S. Lodha: Analysis of soft x-ray/VUV transmission characteristics of Si and Al filters, AIP Conf. Ser. 1512, 498 (2013). 5. B. L. Henke, E. Gullikson, J. C. Davis: X-ray interactions: photoabsorption, scattering, transmission, and reflection at E = 50-30000 eV, Z =1-92, At. Data Nucl. Data Tables 54, 181 (1993). 6. J. Chalupsky et al.: Spot size characterization of focused non-Gaussian X-ray laser beams, Opt. Express 18, 27836 (2010). 7. J. Chalupský, T. Burian, V. Hajkova, L. Juha, T. Polcar, J. Gaudin, M. Nagasono, R. Sobierajski, M. Yabashi, J. Krzywinski: Fluence scan: an unexplored property of a laser beam, Opt. Express 21, 26363 (2013).

The process of damage accumulation in thin ruthenium films exposed to multiple femtosecond extreme ultraviolet (XUV) free-electron laser (FEL) pulses below the critical angle of reflectance at the FEL facility in Hamburg (FLASH) was experimentally analyzed. The multi-shot damage threshold is found to be lower than the single-shot damage threshold. Detailed analysis of the damage morphology and its dependence on irradiation conditions justifies the assumption that cavitation induced by the FEL pulse is the prime mechanism responsible for multi-shot damage in optical coatings.

Measurement of transient optical properties (reflectivity and transmissivity) is performed widely in extreme-ultraviolet (XUV) pump–optical probe experiments to study the transient state of irradiated materials. In order to extend the material diagnostics, here we propose an additional measurement of the transient phase change of the optical probe pulse. It can be recorded in parallel to other transient optical properties, enabling access to full information on the complex refractive index and thickness of the radiation-modified material layer. The latter is essential for investigations of phase transitions progressing in XUV (and x-ray) irradiated materials. We perform a computational study that clearly shows that the measurement of the optical phase from a probe pulse at correctly tuned pulse parameters can provide a signal strong enough to extract information on transient material properties. The calculations suggest that in some cases, it is even more preferable to measure the transient phase change than other optical parameters. Such phase measurement, feasible with modern experimental setups, can then be a basis for an improved diagnostics tool for the temporal characteristics of an ultrashort XUV pulse.

We present an extreme ultraviolet (EUV) microscope using a Schwarzschild objective which is optimized for single-shot sub-micrometer imaging of laser-plasma targets. The microscope has been designed and constructed for imaging the scattering from an EUV-heated solid-density hydrogen jet. Imaging of a cryogenic hydrogen target was demonstrated using single pulses of the free-electron laser in Hamburg (FLASH) free-electron laser at a wavelength of 13.5 nm. In a single exposure, we observe a hydrogen jet with ice fragments with a spatial resolution in the sub-micrometer range. In situ EUV imaging is expected to enable novel experimental capabilities for warm dense matter studies of micrometer-sized samples in laser-plasma experiments.

Optics express 26(15), 19665 - 19685 (2018). doi:10.1364/OE.26.019665, Ruthenium is a perspective material to be used for XUV mirrors at free-electron laser facilities. Yet, it is still poorly studied in the context of ultrafast laser-matter interaction. In this work, we present single-shot damage studies of thin Ru films irradiated by femtosecond XUV free-electron laser pulses at FLASH. Ex-situ analysis of the damaged spots, performed by different types of microscopy, shows that the weakest detected damage is surface roughening. For higher fluences we observe ablation of Ru. Combined simulations using Monte-Carlo code XCASCADE(3D) and the two-temperature model reveal that the damage mechanism is photomechanical spallation, similar to the case of irradiating the target with optical lasers. The analogy with the optical damage studies enables us to explain the observed damage morphologies., Published by OSA, Washington, DC

Physical review / B 96(21), 214101 (2017). doi:10.1103/PhysRevB.96.214101, All carbon materials, e.g., amorphous carbon (a-C) coatings and $C_{60}$ fullerene thin films, play an important role in short-wavelength free-electron laser (FEL) research motivated by FEL optics development and prospective nanotechnology applications. Responses of a-C and $C_{60}$ layers to the extreme ultraviolet (SPring-8 Compact SASESource in Japan) and soft x-ray (free-electron laser in Hamburg) free-electron laser radiation are investigated by Raman spectroscopy, differential interference contrast, and atomic force microscopy. A remarkable difference in the behavior of covalent (a-C) and molecular ($C_{60}$) carbonaceous solids is demonstrated under these irradiation conditions. Low thresholds for ablation of a fullerene crystal (estimated to be around 0.15 eV/atom for $C_{60}$ vs 0.9 eV/atom for a-C in terms of the absorbed dose) are caused by a low cohesive energy of fullerene crystals. An efficient mechanism of the removal of intact $C_{60}$ molecules from the irradiated crystal due to Coulomb repulsion of fullerene-cage cation radicals formed by the ionizing radiation is revealed by a detailed modeling., Published by Inst., Woodbury, NY

Interaction of short-wavelength free-electron laser (FEL) beams with matter is undoubtedly a subject to extensive investigation in last decade. During the interaction various exotic states of matter, such as warm dense matter, may exist for a split second. Prior to irreversible damage or ablative removal of the target material, complicated electronic processes at the atomic level occur. As energetic photons impact the target, electrons from inner atomic shells are almost instantly photo-ionized, which may, in some special cases, cause bond weakening, even breaking of the covalent bonds, subsequently result to so-called non-thermal melting. The subject of our research is ablative damage to lead tungstate (PbWO4) induced by focused short-wavelength FEL pulses at different photon energies. Post-mortem analysis of complex damage patterns using the Raman spectroscopy, atomic-force (AFM) and Nomarski (DIC) microscopy confirms an existence of non-thermal melting induced by high-energy photons in the ionic monocrystalline target. Results obtained at Linac Coherent Light Source (LCLS), Free-electron in Hamburg (FLASH), and SPring-8 Compact SASE Source (SCSS) are presented in this Paper.

Silicon crystalline samples were exposed to intense single pulses of XUV radiation ( λ =13.5 nm) what lead to melting and ablation of the surface material. The deformation field around craters along the whole thickness of silicon wafers was observed by means of the synchrotron transmission section topography using the beam perpendicular to the surface of the sample. The geometrical shape and depth extension around craters was evaluated based on numerous, dense series of section topographs spaced by 10 µm. In the topographs we observed the direct image connected with the boundary of the crater associated with some deformation of the Kato fringes. The evaluated depth extension, different for individual craters, was in the range of 30–100 µm. The depth values were confirmed also by evaluations based on the Bragg case section topographs. It was possible to reproduce the contrast of the craters in transmission section topographs by numerical simulation based on integration of the Takagi–Taupin equations. The damage of the crystal defects connected with craters was approximated as droplet-like inclusions.

In this work, a laser-produced plasma extreme ultraviolet source and a free electron laser were used to create Ne photo-ionized plasmas. In both cases, a radiation beam was focused onto a gas stream injected into a vacuum chamber synchronously with the radiation pulse. Extreme ultraviolet radiation from the plasma spanned a wide spectral range with pronounced maximum centered at λ = 11 ± 1 nm while the free electron laser pulses were emitted at a wavelength of 32 nm. The power density of the focused plasma radiation was approximately 2 × 107 W/cm2 and was seven orders of magnitude lower compared with the focused free electron laser beam. Radiation fluences in both experimental conditions were comparable. Despite quite different spectral characteristics and extremely different power densities, emission spectra of both photo-ionized plasmas consist of the same spectral lines within a wavelength range of 20 to 50 nm, however, with different relative intensities of the corresponding lines. The dominating spectral lines originated from singly charged ions (Ne II); however, Ne III lines were also detected. Additionally, computer simulations of the emission spectra, obtained for photo-ionized plasmas, driven by the plasma extreme ultraviolet source, were performed. The corresponding measured and calculated spectra are presented. An electron temperature and ionic composition were estimated. Differences between the experimental spectra, obtained for both irradiation conditions, were analyzed. The differences were attributed mainly to different energies of driving photons.

We report on experiments aimed at the generation and characterization of solid density plasmas at the free-electron laser FLASH in Hamburg. Aluminum samples were irradiated with XUV pulses at 13.5 nm wavelength (92 eV photon energy). The pulses with duration of a few tens of femtoseconds and pulse energy up to 100 µJ are focused to intensities ranging between 1013 and 1017 W/cm2. We investigate the absorption and temporal evolution of the sample under irradiation by use of XUV and optical spectroscopy. We discuss the origin of saturable absorption, radiative decay, bremsstrahlung and atomic and ionic line emission. Our experimental results are in good agreement with simulations.

The article presents preliminary investigation results on the near-surface damage produced by single pulses of XUV free-electron laser in the amorphous α-SiO 2 , the monocrystalline silicon and the epitaxial films of gold. The irradiation was delivered with single pulses of only 25 fs at a wavelength of 32.5 nm and of energy up to 10 μJ. Structural modifications induced by irradiation were characterized by X-ray microdiffraction, as well as by the AFM and optical microscopy. Ablation craters of well-defined edges with smooth interiors and outer embankments surrounding the crater edges were found in the materials. Polycrystalline phases were revealed in Si and Au film samples, in the embankments and in central parts of some craters. In α-SiO 2 , a diffraction pattern typical of an amorphous material was observed without any traces of irradiation-initiated crystallization. A step-like, complete removal of gold film was evidenced inside craters, with only small gold residues in central part of craters exposed to higher fluences.

International audience; An irreversible response of inorganic scintillators to intense soft x-ray laser radiation was investigated at the FLASH (Free-electron LASer in Hamburg) facility. Three ionic crystals, namely, Ce:YAG (cerium-doped yttrium aluminum garnet), PbWO4 (lead tungstate), and ZnO (zinc oxide), were exposed to single 4.6 nm ultra-short laser pulses of variable pulse energy (up to 12 μJ) under normal incidence conditions with tight focus. Damaged areas produced with various levels of pulse fluences, were analyzed on the surface of irradiated samples using differential interference contrast (DIC) and atomic force microscopy (AFM). The effective beam area of 22.2 ± 2.2 μm2 was determined by means of the ablation imprints method with the use of poly(methyl methacrylate) - PMMA. Applied to the three inorganic materials, this procedure gave almost the same values of an effective area. The single-shot damage threshold fluence was determined for each of these inorganic materials. The Ce:YAG sample seems to be the most radiation resistant under the given irradiation conditions, its damage threshold was determined to be as high as 660.8 ± 71.2 mJ/cm2. Contrary to that, the PbWO4 sample exhibited the lowest radiation resistance with a threshold fluence of 62.6 ± 11.9 mJ/cm2. The threshold for ZnO was found to be 167.8 ± 30.8 mJ/cm2. Both interaction and material characteristics responsible for the damage threshold difference are discussed in the article.

International audience; Taking advantage of the new opportunities provided by x-ray free electron laser (FEL) sources when coupled to a long laser pulse as available at the Linear Coherent Light Source (LCLS), we have performed x-ray absorption near-edge spectroscopy (XANES) of laser shock compressed iron up to 420 GPa (±50) and 10 800 K (±1390). Visible diagnostics coupled with hydrodynamic simulations were used to infer the thermodynamical conditions along the Hugoniot and the release adiabat. A modification of the pre-edge feature at 7.12 keV in the XANES spectra is observed above pressures of 260 GPa along the Hugoniot. Comparing with ab initio calculations and with previous laser-heated diamond cell data, we propose that such changes in the XANES pre-edge could be a signature of molten iron. This interpretation then suggests that iron is molten at pressures and temperatures higher than 260 GPa (±29) and 5680 K (±700) along the principal Fe Hugoniot.

International audience; The time evolution of the electron structure is investigated in a molybdenum foil heated up to the warm dense matter regime by a femtosecond laser pulse, through time-resolved x-ray absorption near-edge spectroscopy. Spectra are measured with independent characterizations of temperature and density. They are successfully compared with ab initio quantum molecular dynamic calculations. We demonstrate that the observed white line in the L-3 edge reveals the time evolution of the electron density of state from the solid to the hot (a few eV) and expanding liquid. The data indicate a highly nonequilibrated state, 5 ps after heating.

We use a Mach-Zehnder type autocorrelator to split and delay XUV pulses from the FLASH soft X-ray laser for triggering and subsequently probing the explosion of aerosolised sugar balls. FLASH was running at 182 eV photon energy with pulses of 70 fs duration. The delay between the pump-probe pulses was varied between zero and 5 ps, and the pulses were focused to reach peak intensities above 1016 W/cm2 with an off-axis parabola. The direct pulse triggered the explosion of single aerosolised sucrose nano-particles, while the delayed pulse probed the exploding structure. The ejected ions were measured by ion time of flight spectrometry, and the particle sizes were measured by coherent diffractive imaging. The results show that sucrose particles of 560-1000 nm diameter retain their size for about 500 fs following the first exposure. Significant sample expansion happens between 500 fs and 1 ps. We present simulations to support these observations.

High-intensity x-ray pulses from an x-ray free-electron laser are used to heat and probe a solid-density aluminum sample. The photon-energy-dependent transmission of the heating beam is studied through the use of a photodiode. Saturable absorption is observed, with the resulting transmission differing significantly from the cold case, in good agreement with atomic-kinetics simulations.

We investigate subpicosecond dynamics of warm dense hydrogen at the XUV free-electron laser facility (FLASH) at DESY (Hamburg). Ultrafast impulsive electron heating is initiated by a â‰300-fs short x-ray burst of 92-eV photon energy. A second pulse probes the sample via x-ray scattering at jitter-free variable time delay. We show that the initial molecular structure dissociates within (0.9±0.2) ps, allowing us to infer the energy transfer rate between electrons and ions. We evaluate Saha and Thomas-Fermi ionization models in radiation hydrodynamics simulations, predicting plasma parameters that are subsequently used to calculate the static structure factor. A conductivity model for partially ionized plasma is validated by two-temperature density-functional theory coupled to molecular dynamic simulations and agrees with the experimental data. Our results provide important insights and the needed experimental data on transport properties of dense plasmas. © 2014 American Physical Society.

International audience; The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called "molecular movie'' within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level of the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes.

Highly charged ions are formed in the center of composite clusters by strong free-electron laser pulses and they emit fluorescence on a femtosecond time scale before competing recombination leads to neutralization of the nanoplasma core. In contrast to mass spectrometry that detects remnants of the interaction, fluorescence in the extreme ultraviolet spectral range provides fingerprints of transient states of high energy density matter. Spectra from clusters consisting of a xenon core and a surrounding argon shell show that a small fraction of the fluorescence signal comes from multiply charged xenon ions in the cluster core. Initially, these ions are as highly charged as the ions in the outer shells of pure xenon clusters with charge states up to at least $11+$.

A theoretical study of the ultrafast electron kinetics in solid SiO2, irradiated with a femtosecond X-ray laser pulse, is presented. A Monte Carlo code for event-by-event simulations of individual particles is applied to model the electron kinetics within the irradiated SiO2 bulk. The simulation includes photoionization, elastic and inelastic scatterings of electrons, Auger decays of core holes, and electron-hole recombination via exciton self-trapping mechanism. Transient electron density is followed, at different photon energies and pulse durations. The change of the optical properties (reflectance, transmittance) of the material is estimated with the help of the Drude model. The analysis of the results allows us to conclude that within the X-ray excited dielectric, the holes in the valence band give the predominant contribution to the transient changes of optical properties within the material. The increase rate of the free electron density is limited by the duration of secondary electron cascading. (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

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.

The role played by heat accumulation in multi-shot damage of silicon was studied. Bulk silicon samples were exposed to intense XUV monochromatic radiation of a 13.5 nm wavelength in a series of 400 femtosecond pulses, repeated with a 1 MHz rate (pulse trains) at the FLASH facility in Hamburg. The observed surface morphological and structural modifications are formed as a result of sample surface melting. Modifications are threshold dependent on the mean fluence of the incident pulse train, with all threshold values in the range of approximately 36-40 mJ/cm2. Experimental data is supported by a theoretical model described by the heat diffusion equation. The threshold for reaching the melting temperature (45 mJ/cm2) and liquid state (54 mJ/cm2), estimated from this model, is in accordance with experimental values within measurement error. The model indicates a significant role of heat accumulation in surface modification processes.

Pulse intensities greater than 10(17) Watt/cm(2) were reached at the FLASH soft X-ray laser in Hamburg, Germany, using an off-axis parabolic mirror to focus 15 fs pulses of 5-70 mu J energy at 13.5 nm wavelength to a micron-sized spot. We describe the interaction of such pulses with niobium and vanadium targets and their deuterides. The beam produced craters in the solid targets, and we measured the kinetic energy of ions ejected from these craters. Ions with several keV kinetic energy were observed from craters approaching 5 mu m in depth when the sample was at best focus. We also observed the onset of saturation in both ion acceleration and ablation with pulse intensities exceeding 10(16) W/cm(2), when the highest detected ion energies and the crater depths tend to saturate with increasing intensity. A general difficulty in working with micron and sub-micron focusing optics is finding the exact focus of the beam inside a vacuum chamber. Here we propose a direct method to measure the focal position to a resolution better than the Rayleigh length. The method is based on the correlation between the energies of ejected ions and the physical dimensions of the craters. We find that the focus position can be quickly determined from the ion time-of-flight (TOF) data as the target is scanned through the expected focal region. The method does not require external access to the sample or venting the vacuum chamber. Profile fitting employed to analyze the TOF data can extend resolution beyond the actual scanning step size. (C) 2011 Elsevier B.V. All rights reserved.

We investigated the damage mechanism of MoN/SiN multilayer XUV optics under two extreme conditions: thermal annealing and irradiation with single shot intense XUV pulses from the free-electron laser facility in Hamburg - FLASH. The damage was studied "post-mortem" by means of X-ray diffraction, interference-polarizing optical microscopy, atomic force microscopy, and scanning transmission electron microscopy. Although the timescale of the damage processes and the damage threshold temperatures were different (in the case of annealing it was the dissociation temperature of Mo2N and in the case of XUV irradiation it was the melting temperature of MoN) the main damage mechanism is very similar: molecular dissociation and the formation of N-2, leading to bubbles inside the multilayer structure. (C) 2010 Optical Society of America

As liver fibrosis is the result of persistent necroinflammation in the liver, pro-inflammatory cytokines secreted in response to cell injury have a central role in the pathogenesis of liver fibrosis. We aimed to investigate the association of cytokine gene polymorphism and liver fibrosis among Chinese patients with chronic hepatitis B.Polymorphisms at interleukin-10 (IL-10-627, -1117), interleukin-1-beta (IL-1beta-511, -31, -3964), interleukin-1 receptor antagonist (IL-1RN), and tumor necrosis factor-alpha (TNF-alpha-308, -238) among Chinese chronic hepatitis B patients were determined. Severe liver fibrosis was defined as Ishak fibrosis score = 4 (of 6).Fifty-nine of 273 (22%) patients had severe fibrosis. The distribution of genotypes for IL-10-627 was CC (11%), CA (41%), and AA (48%). The CC genotype at IL-10-627 was protective against severe fibrosis (odds ratio (OR) 0.11; 95% CI 0.014-0.82; P = 0.032). After adjusted for baseline variables, the adjusted OR of CC genotypes at IL-10-627 for severe fibrosis was 0.063 (95% CI 0.06-0.64; P = 0.063). Other gene polymorphisms at IL-1beta, IL-1RN, TNF-alpha, and IL-10 had no significant association with severe fibrosis. Weak linkage disequilibrium was observed between IL-10-627 and IL-10-1117 with linkage disequilibrium coefficient of 0.12 (P < 0.001). The distribution of haplotypes of IL-10-1117 and IL-10-627 was A-A (69%), A-C (26%), and G-C (5%). High and intermediate IL-10 production (A-C and G-C) haplotypes were protective against severe fibrosis (OR 0.62; 95% CI 0.39-0.99; P = 0.046).High production genotype and haplotypes of IL-10 were associated with less severe liver fibrosis in chronic hepatitis B in Chinese.

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. (C) 2010 Optical Society of America

We have focused a beam (BL3) of FLASH (Free-electron LASer in Hamburg: lambda = 13.5 nm, pulse length 15 fs, pulse energy 10-40 microJ, 5 Hz) using a fine polished off-axis parabola having a focal length of 270 mm and coated with a Mo/Si multilayer with an initial reflectivity of 67% at 13.5 nm. The OAP was mounted and aligned with a picomotor controlled six-axis gimbal. Beam imprints on poly(methyl methacrylate) - PMMA were used to measure focus and the focused beam was used to create isochoric heating of various slab targets. Results show the focal spot has a diameter of < or =1 microm. Observations were correlated with simulations of best focus to provide further relevant information.

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

Ultra-fast soft x-ray lasers have opened a new area of laser-matter interactions which in most cases differ from the well understood interaction of UV-vis radiation with solid targets. The photon energy >30eV essentially exceeds the width of band gap in any known material and excites the electrons from the deep atomic and valence levels directly to the conduction band. Both thermal and non-thermal phenomena can occur in such a material being caused by electron thermalization and bond breaking, respectively. We report the first observation of non-thermal single-shot soft x-ray laser induced desorption oc curring below the ablation th reshold 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 an 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 an d used to analyze single-shot imprints in PMMA. An intermediate regime of materials removal has been found, confir ming the model predictions. We also report below-threshold multiple-shot desorption of PMMA induced by high-order harmonics (HOH) at 32nm as a proof of an efficient material remova l in the desorption regime. Keywords: soft X-ray laser, laser beam profile, ablation, desorption, poly(meth yl methacrylate) - PMMA

Single shot radiation damage of bulk silicon induced by ultrashort XUV pulses was studied. The sample was chosen because it is broadly used in XUV optics and detectors where radiation damage is a key issue. It was irradiated at FLASH facility in Hamburg, which provides intense femtosecond pulses at 32.5 nm wavelength. The permanent structural modifications of the surfaces exposed to single shots were characterized by means of phase contrast optical microscopy and atomic force microscopy. Mechanisms of different, intensity dependent stages of the surface damage are described.

We have used the XUV FLASH laser at DESY to irradiate solid targets with intense XUV pulse at 13.5nm and ~1016 Wcm−2. XUV emission spectroscopy using a grating spectrometer has been used to observe both continuum radiation and line emission from Al IV. We present some preliminary results that indicate time integrated temperatures of below 20eV while simulation indicates higher initial temperatures.

We present the attempt to diagnose electron temperature and density of a plasma via Thomson Scattering in the Warm Dense Matter Regimew using soft x-ray Free Electron Laser radiation. A preliminary Self Thomson Scattering experiment has already been conducted. In a current pump-probe experiment, together with an optical heating laser, we will record the temporal evolution of the plasma achieving a resolution of approximately 250fs.

We present results of damage studies conducted at the Free Electron LASer in Hamburg (FLASH) facility with 13.5 nm (91.8 eV) and 7 nm (177.1 eV) radiations. The laser beam was focused on a sample of 890-nm-thick amorphous carbon coated on a silicon wafer mimicking a x-ray mirror. The fluence threshold for graphitization was determined for different grazing angles above and below the critical angle. The observed angular dependence of Fth is explained by the variation in absorption depth and reflectivity. Moreover, the absorbed local dose needed for the phase transition leading to graphitization is shown to vary with the radiation wavelength.

The first soft X-ray free-electron laser has recently been put into operation at DESY in Hamburg. Tunable soft X-ray coherent radiation can be generated at the FLASH (Free-electron LASer in Hamburg; formerly known as VUV FEL or TTF2 FEL). In the interaction experiments reported here, the laser system provided ~ 25-fs, ~ 10-μ J pulses of 32-nm radiation. We irradiated thin (500 nm) layers of poly (methyl methacrylate) – PMMA deposited on a silicon substrate by single, focused FLASH pulses. The pulse energy was adjusted using a gas attenuator.

The ablation of solids by high energy femtosecond pulses from an extreme ultraviolet (XUV) free electron laser has been investigated using picosecond optical imaging. The time-resolved measurements are supplemented by an analysis of the permanent structural surface modifications. Compared with femtosecond optical excitation, distinct differences in the material response are found which are attributed to the increased penetration depth of the XUV radiation and the absence of any absorption nonlinearities.

We exposed bulk SiC and films of SiC and B4C to single 25 fs long free-electron-laser pulses with wavelengths between 13.5 and 32 nm. The materials are candidates for x-ray free-electron laser optics. We found that the threshold for surface-damage of the bulk SiC samples exceeds the fluence required for thermal melting at all wavelengths. The damage threshold of the film sample shows a strong wavelength dependence. For wavelengths of 13.5 and 21.7 nm, the damage threshold is equal to or exceeds the melting threshold, whereas at 32 nm the damage threshold falls below the melting threshold.

International audience; 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 ardening making the beam profile measurement infeasible.