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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

Journal of synchrotron radiation 27(1), 11 - 16 (2020). doi:10.1107/S1600577519014164, A simple and robust tool for spatio-temporal overlap of THz and XUV pulses in in-vacuum pump–probe experiments is presented. The technique exploits ultrafast changes of the optical properties in semiconductors (i.e. silicon) driven by ultrashort XUV pulses that are probed by THz pulses. This work demonstrates that this tool can be used for a large range of XUV fluences that are significantly lower than when probing by visible and near-infrared pulses. This tool is mainly targeted at emerging X-ray free-electron laser facilities, but can be utilized also at table-top high-harmonics sources., Published by Wiley-Blackwell, [S.l.]

Laser and particle beams 37(2), 235 - 241 (2019). doi:10.1017/S0263034619000326, Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. An example is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. We also show that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs, Published by Cambridge Univ. Press, Cambridge

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.]

The European physical journal / D 75, 224 (2021). doi:10.1140/epjd/s10053-021-00235-z, In this paper, we report on the Boltzmann kinetic equation approach adapted for simulations of warm dense matter created by irradiation of bulk gold with intense ultrashort X-ray pulses. X-rays can excite inner-shell electrons, which triggers creation of deep-lying core holes. Their relaxation, especially in heavier elements such as gold (atomic number Z=79) takes complicated pathways, involving collisional processes, and leading through a large number of active configurations. This number can be so high that solving a set of evolution equations for each configuration becomes computationally inefficient, and another modeling approach should be used instead. Here, we use the earlier introduced ���predominant excitation and relaxation path��� approach. It still uses true atomic configurations but limits their number by restricting material relaxation to a selected set of predominant pathways for material excitation and relaxation. With that, we obtain time-resolved predictions for excitation and relaxation in X-ray irradiated bulk of gold, including the respective change of gold optical properties. We compare the predictions with the available data from high-energy-density experiments. Their good agreement indicates ability of the Boltzmann kinetic equation approach to describe warm dense matter created from high-Z materials after their irradiation with X rays, which can be validated in future experiments., Published by Springer, Heidelberg

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.

Physical review / A covering atomic, molecular, and optical physics and quantum information 101(6), 063412 (2020). doi:10.1103/PhysRevA.101.063412, Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe$^{2+}$ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs., Published by Inst., Woodbury, NY

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 electrical conductivity of water under extreme temperatures and densities plays a central role in modeling planetary magnetic fields. Experimental data are vital to test theories of high-energy-density water and assess the possible development and presence of extraterrestrial life. These states are also important in biology and chemistry studies when specimens in water are confined and excited using ultrafast optical or free-electron lasers (FELs). Here we utilize femtosecond optical lasers to measure the transient reflection and transmission of ultrathin water sheet samples uniformly heated by a 13.6 nm FEL approaching a highly conducting state at electron temperatures exceeding 20 000 K. The experiment probes the trajectory of water through the high-energy-density phase space and provides insights into changes in the index of refraction, charge carrier densities, and AC electrical conductivity at optical frequencies. At excitation energy densities exceeding 10 MJ/kg, the index of refraction falls to n = 0.7, and the thermally excited free-carrier density reaches n$_e$ = 5 × 10$^{27}$ m$^{−3}$, which is over an order of magnitude higher than that of the electron carriers produced by direct photoionization. Significant specular reflection is observed owing to critical electron density shielding of electromagnetic waves. The measured optical conductivity reaches 2 × 10$^4$ S/m, a value that is one to two orders of magnitude lower than those of simple metals in a liquid state. At electron temperatures below 15 000 K, the experimental results agree well with the theoretical calculations using density-functional theory/molecular-dynamics simulations. With increasing temperature, the electron density increases and the system approaches a Fermi distribution. In this regime, the conductivities agree better with predictions from the Ziman theory of liquid metals.

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

Soft x-rays were applied to induce graphitization of diamond through a non-thermal solid-to-solid phase transition. This process was observed within poly-crystalline diamond with a time-resolved experiment using ultrashort soft x-ray pulses of duration 52.5 fs and cross correlated by an optical pulse of duration 32.8 fs. This scheme enabled for the first time the measurement of a phase transition on a timescale of ~150 fs. Excellent agreement between experiment and theoretical predictions was found, using a dedicated code that followed the non-equilibrium evolution of the irradiated diamond including all transient electronic and structural changes. These observations confirm that soft x-rays can induce a non-thermal ultrafast solid-to-solid phase transition on a hundred femtosecond timescale., Comment: 27 pages, 17 figures (includes supplementary materials)

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 physics and chemistry of liquid solutions play a central role in science, and our understanding of life on Earth. Unfortunately, key tools for interrogating aqueous systems, such as infrared and soft X-ray spectroscopy, cannot readily be applied because of strong absorption in water. Here we use gas dynamic forces to generate free-flowing, sub-micron, liquid sheets which are 2 orders of magnitude thinner than anything previously reported. Optical, infrared and X-ray spectroscopies are used to characterize the sheets, which are found to be tunable in thickness from over 1 micron down to less than 20 nanometers, which corresponds to fewer than 100 water molecules thick. At this thickness, aqueous sheets can readily transmit photons across the spectrum, leading to potentially transformative applications in infrared, X-ray, electron spectroscopies and beyond. The ultrathin sheets are stable for days in vacuum, and we demonstrate their use at free-electron laser and synchrotron light sources.

FLASH is the only high-repetition-rate FEL in the XUV/soft X-ray regime worldwide. Based on superconducting accelerator technology developed at DESY, it can provide up to 8000 pulses/s for experiments in such diverse fields as atomic, molecular, and optical physics, chemistry, condensed matter and nanoscience, life science, warm dense matter research, and FEL physics and technology, including development of new methods and instrumentation. The outstanding opportunities for time-resolved studies at FLASH, which are based on unique pump-probe instrumentation including fully synchronized optical lasers, a large suite of X-ray split-and-delay units, a THz source that is phase stable with respect to the FEL pulses, and sophisticated diagnostics for pulse arrival and duration, attract a large number of eminent researchers in ultrafast science to FLASH. The recent addition of a second FEL line, FLASH2, with variable-gap undulators that enable easy wavelength tuning and novel lasing schemes for users in parallel to the operation of FLASH1, along with the progress in creating and measuring ultrashort single-spike SASE pulses, and the new suite of dedicated state-of-the-art end stations have made FLASH even more attractive to users. To keep FLASH at the forefront of FEL science and technology, an ambitious upgrade program is currently planned. FLASH2020+ foresees operation of two FEL lines, with one line providing externally seeded pulses up to the full repetition rate of FLASH and the second line allowing for flexible novel lasing schemes based on a set of variable undulators. This line will be designed to deliver coherent radiation from THz to soft X-rays. The new ideas are fully in sync with the requirements of the community for breakthrough science with a high-repetition rate XUV/soft X-ray FEL.

Silicon, being one of the most abundant elements in nature, attracts wide-ranging scientific and technological interest. Specifically, in its elemental form, crystals of remarkable purity can be produced. One may assume that this would lead to silicon being well understood, and indeed, this is the case for many ambient properties, as well as for higher-pressure behaviour under quasi-static loading. However, despite many decades of study, a detailed understanding of the response of silicon to rapid compression—such as that experienced under shock impact—remains elusive. Here, we combine a novel free-electron laser-based X-ray diffraction geometry with laser-driven compression to elucidate the importance of shear generated during shock compression on the occurrence of phase transitions. We observe lowering of the hydrostatic phase boundary in elemental silicon, an ideal model system for investigating high-strength materials, analogous to planetary constituents. Moreover, we unambiguously determine the onset of melting above 14 GPa, previously ascribed to a solid–solid phase transition, undetectable in the now conventional shocked diffraction geometry; transitions to the liquid state are expected to be ubiquitous in all systems at sufficiently high pressures and temperatures.

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.

Nature Communications 9(1), 1353 (2018). doi:10.1038/s41467-018-03696-w, The physics and chemistry of liquid solutions play a central role in science, and our understanding of life on Earth. Unfortunately, key tools for interrogating aqueous systems, such as infrared and soft X-ray spectroscopy, cannot readily be applied because of strong absorption in water. Here we use gas-dynamic forces to generate free-flowing, sub-micron, liquid sheets which are two orders of magnitude thinner than anything previously reported. Optical, infrared, and X-ray spectroscopies are used to characterize the sheets, which are found to be tunable in thickness from over 1 μm down to less than 20 nm, which corresponds to fewer than 100 water molecules thick. At this thickness, aqueous sheets can readily transmit photons across the spectrum, leading to potentially transformative applications in infrared, X-ray, electron spectroscopies and beyond. The ultrathin sheets are stable for days in vacuum, and we demonstrate their use at free-electron laser and synchrotron light sources., Published by Springer Nature, [London]

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

Applied physics letters 113(11), 114102 (2018). doi:10.1063/1.5046070, Recent studies confirmed that the materials used in the extreme UV and soft X-ray regime for precise characterization of intense free-electron laser pulses (e.g., Si$_3$N$_4$) do not work efficiently in the hard X-ray regime, which is due to the fact that the impact of a hard X-ray photon is followed by a series of electron cascading processes. Following theoretical indication, we show that this limitation can be circumvented and the cascading time can be significantly reduced if the X-ray photon energy is double the ionization energy. We investigate an alternative material for pulse diagnostics, SnO$_2$, using the Linac Coherent Light Source at photon energies of 5 keV and 9 keV. We prove the validity of the concept and show that it has a large potential for practical applications. By applying the proposed criteria, the temporal accuracy of the non-invasive pulse diagnostic tools can be improved in current and emerging hard X-ray facilities., Published by American Inst. of Physics, Melville, NY

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.

Nature Communications 9(1), 2860 (2018). doi:10.1038/s41467-018-05365-4, The physics and chemistry of liquid solutions play a central role in science, and our understanding of life on Earth. Unfortunately, key tools for interrogating aqueous systems, such as infrared and soft X-ray spectroscopy, cannot readily be applied because of strong absorption in water. Here we use gas-dynamic forces to generate free-flowing, sub-micron, liquid sheets which are two orders of magnitude thinner than anything previously reported. Optical, infrared, and X-ray spectroscopies are used to characterize the sheets, which are found to be tunable in thickness from over 1 μm down to less than 20 nm, which corresponds to fewer than 100 water molecules thick. At this thickness, aqueous sheets can readily transmit photons across the spectrum, leading to potentially transformative applications in infrared, X-ray, electron spectroscopies and beyond. The ultrathin sheets are stable for days in vacuum, and we demonstrate their use at free-electron laser and synchrotron light sources., Published by Nature Publishing Group UK, [London]

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 review we discuss four examples of environment-dependent processes triggered by free-electron laser radiation within systems of various complexity. Those are: (i) non-thermal structural changes within irradiated solids, (ii) inverse bremsstrahlung during VUV irradiation of atomic clusters, (iii) shifts of ionic potentials due to a charged ion environment within a plasma, and (iv) fast thermalization of the electrons created after FEL irradiation. We show that FEL excitation enables access to a unique class of environment-influenced processes, depending on the radiation wavelength, pulse fluence and the structure of sample.

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.

Physical review letters 109, 245003 (2012). doi:10.1103/PhysRevLett.109.245003, Published by APS, College Park, Md.

We report on soft X-ray scattering experiments on cryogenic hydrogen and simple metal samples. As a source of intense, ultrashort soft X-ray pulses we have used free-electron laser radiation at 92 eV photon energy from FLASH at DESY, Hamburg. X-ray pulses with energies up to 150 μJ and durations 15-50 fs provide interaction with the sample leading simultaneously to plasma formation and scattering. Experiments exploiting both of these interactions have been carried out, using the same experimental setup. Firstly, recording of soft X-ray inelastic scattering from near-solid density hydrogen plasmas at few electron volt temperatures confirms the feasibility of this diagnostics technique. Secondly, the soft X-ray excitation of few electron volt solid-density plasmas in bulk metal samples could be studied by recording soft X-ray line and continuum emission integrated over emission times from fs to ns. © 2009 Elsevier B.V.

We report on the x-ray absorption of Warm Dense Matter experiment at the FLASH Free Electron Laser (FEL) facility at DESY. The FEL beam is used to produce Warm Dense Matter with soft x-ray absorption as the probe of electronic structure. A multilayer-coated parabolic mirror focuses the FEL radiation, to spot sizes as small as 0.3μm in a ∼15fs pulse of containing >10 12 photons at 13.5 nm wavelength, onto a thin sample. Silicon photodiodes measure the transmitted and reflected beams, while spectroscopy provides detailed measurement of the temperature of the sample. The goal is to measure over a range of intensities approaching 10 18 W/cm 2. Experimental results will be presented along with theoretical calculations. A brief report on future FEL efforts will be given. © 2009 SPIE.