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Warm dense matter (WDM) is a ubiquitous state of matter encountered in various high energy density environments, at the frontier between a plasma and a condensed phase. It is key to astrophysics, planetary science and inertial confinement fusion research, but its electronic and ionic structure and dynamics remain poorly understood. Here, an intense and ultrafast X-ray free electron laser (XFEL) pulse is used to simultaneously create and characterize warm dense copper via L-edge X-ray absorption spectroscopy. The rich electron dynamics occurring within the 15-femtosecond pulse duration are revealed over a large irradiation intensity range. Below 1015 W cm-2, an absorption peak below the L-edge appears, originating from the depletion of the 3d band, and shows a distinct energy redshift with increasing intensity. This shift is a possible signature of ionization potential depression and electronic bond hardening. At higher intensities, massive ionization and collisions lead to the transition from reverse saturable absorption (opening absorption channels) to saturable absorption (material bleaching) of the XFEL pulse, an effect that holds promise for X-ray pulse shaping. The presented method is applicable to a wide range of materials and constitutes a robust benchmark for non-equilibrium models of electron dynamics in WDM.

A real-time and accurate characterization of the X-ray beam size is essential to enable a large variety of different experiments at free-electron laser facilities. Typically, ablative imprints are employed to determine shape and size of µm-focused X-ray beams. The high accuracy of this state-of-the-art method comes at the expense of the time required to perform an ex-situ image analysis. In contrast, diffraction at a curved grating with suitably varying period and orientation forms a magnified image of the X-ray beam, which can be recorded by a 2D pixelated detector providing beam size and pointing jitter in real time. In this manuscript, we compare results obtained with both techniques, address their advantages and limitations, and demonstrate their excellent agreement. We present an extensive characterization of the FEL beam focused to ≈1 µm by two Kirkpatrick-Baez (KB) mirrors, along with optical metrology slope profiles demonstrating their exceptionally high quality. This work provides a systematic and comprehensive study of the accuracy provided by curved gratings in real-time imaging of X-ray beams at a free-electron laser facility. It is applied here to soft X-rays and can be extended to the hard X-ray range. Furthermore, curved gratings, in combination with a suitable detector, can provide spatial properties of µm-focused X-ray beams at MHz repetition rate.

Symmetry is a powerful concept in physics, but its applicability to far-from-equilibrium states is still being understood. Recent attention has focused on how far-from-equilibrium states lead to spontaneous symmetry breaking. Conversely, ultrafast optical pumping can be used to drastically change the energy landscape and quench the magnetic order parameter in magnetic systems. Here, we find a distinct symmetry-dependent ultrafast behaviour by use of ultrafast x-ray scattering from magnetic patterns with varying degrees of isotropic and anisotropic symmetry. After pumping with an optical laser, the scattered intensity reveals a radial shift exclusive to the isotropic component and exhibits a faster recovery time from quenching for the anisotropic component. These features arise even when both symmetry components are concurrently measured, suggesting a correspondence between the excitation and the magnetic order symmetry. Our results underline the importance of symmetry as a critical variable to manipulate the magnetic order in the ultrafast regime.

Nature materials 20, 30 - 37 (2021). doi:10.1038/s41563-020-00807-1, Topological states of matter exhibit fascinating physics combined with an intrinsic stability. A key challenge is the fast creation of topological phases, which requires massive reorientation of charge or spin degrees of freedom. Here we report the picosecond emergence of an extended topological phase that comprises many magnetic skyrmions. The nucleation of this phase, followed in real time via single-shot soft X-ray scattering after infrared laser excitation, is mediated by a transient topological fluctuation state. This state is enabled by the presence of a time-reversal symmetry-breaking perpendicular magnetic field and exists for less than 300 ps. Atomistic simulations indicate that the fluctuation state largely reduces the topological energy barrier and thereby enables the observed rapid and homogeneous nucleation of the skyrmion phase. These observations provide fundamental insights into the nature of topological phase transitions, and suggest a path towards ultrafast topological switching in a wide variety of materials through intermediate fluctuating states., Published by Nature Publishing Group, Basingstoke

One of the intriguing problems of modern magnetism is unravelling the non-equilibrium spin dynamics following laser excitation on the nanometer length scale. In this work the ultrafast magnetic behavior of thin Co/Pt multilayers is studied by resonant magnetic SAXS in transmission geometry. We have for the first time observed a very bright transient scattering from nanometer scale magnetic fluctuations.

The analysis of the radiation damage of imaging systems is based on all different types-of aiialoiue/digital cameras with uncooled as well as actively cooled image sensors in the VIS/NIR/MWIR spectral ranges. The Monte Carlo N-Particle (MCNP) code has been used to determine the neutron fluence at different camera locations in JET. An explicit link between the sensor damage and the neutron fluence has been observed. Sensors show an increased dark-current and increased numbers of hot-pixels. Uncooled cameras must be replaced once per year after exposure to a neutron fluence of similar to 1.9-3.2 x 10(12)neutrons/cm(2). Such levels of fluence will be reached after approximate to 14-22 ELMy H-mode pulses during the future D-T campaign. Furthermore, dynamical noise seen as a random pattern of bright pixels was observed in the presence of hard radiation (neutrons and gammas). Failure of the digital electronics inside the cameras as well as of industrial controllers is observed beyond a neutron fluence of about similar to 4 x 10(9) neutrons/cm(2). The impact of hard radiation on the different types of electronics and possible application of cameras during future D-T campaign is discussed. EURATOM 633053

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

Amplified spontaneous XUV emission from Xenon clusters irradiated by free-electron laser pulses was experimentally observed. Theoretical modeling describes experi-mental trends and shows that collision processes in expanding clusters yield transient pop-ulation inversion and cause decoherence.

The Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL is a soft X-ray beamline aiming to unravel electronic, spin and structural properties of materials in ultrafast processes at the nanoscale. Various experimental techniques offered at SCS have different requirements in terms of beam size at the sample. Kirkpatrick-Baez (KB) refocusing optics equipped with mechanical benders allows for independent change of the horizontal and vertical beam size. We report here on the first characterization of the SCS KB mirrors by means of a novel diffraction-based technique which images the beam profile on a 2D pixelated detector. This approach provides a quick characterization of micrometer beam sizes. Results are compared with metrology measurements obtained with a non-contact slope profiler.

We present a comprehensive experimental and theoretical study on superfluorescence in the extreme ultraviolet wavelength regime. Focusing a free-electron laser pulse in a cell filled with Xe gas, the medium is quasi-instantaneously population inverted by $4d$-shell ionization on the giant resonance followed by Auger decay. On the timescale of $\ensuremath{\sim}10\text{ }\text{ }\mathrm{ps}$ to $\ensuremath{\sim}100\text{ }\text{ }\mathrm{ps}$ (depending on parameters) a macroscopic polarization builds up in the medium, resulting in superfluorescent emission of several Xe lines in the forward direction. As the number of emitters in the system is increased by either raising the pressure or the pump-pulse energy, the emission yield grows exponentially over four orders of magnitude and reaches saturation. With increasing yield, we observe line broadening, a manifestation of superfluorescence in the spectral domain. Our novel theoretical approach, based on a full quantum treatment of the atomic system and the irradiated field, shows quantitative agreement with the experiment and supports our interpretation.

Physical review letters 120(13), 133203 (2018). doi:10.1103/PhysRevLett.120.133203, We report the observation and analysis of the gain curve of amplified $Kα$ x-ray emission from solutions of Mn(II) and Mn(VII) complexes using an x-ray free electron laser to create the $1s$ core-hole population inversion. We find spectra at amplification levels extending over 4 orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ∼1.7 eV FWHM is constant over 3 orders of magnitude, pointing to the buildup of transform limited pulses of ∼1 fs duration. Driving the amplification into saturation leads to broadening and a shift of the line. Importantly, the chemical sensitivity of the stimulated x-ray emission to the Mn oxidation state is preserved at power densities of $∼10^{20}$ $W/cm^2$ for the incoming x-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) x-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear x-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis, and materials science., Published by APS, College Park, Md.

Faraday discussions 194, 305 - 324(2016). doi:10.1039/C6FD00103C, With the invention of femtosecond X-ray free-electron lasers (XFELs), studies of light-induced chemical reaction dynamics and structural dynamics reach a new era, allowing for time-resolved X-ray diffraction and spectroscopy. To ultimately probe coherent electron and nuclear dynamics on their natural time and length scales, coherent nonlinear X-ray spectroscopy schemes have been proposed. In this contribution, we want to critically assess the experimental realisation of nonlinear X-ray spectroscopy at current-day XFEL sources, by presenting first experimental attempts to demonstrate stimulated resonant X-ray Raman scattering in molecular gas targets., Published by Soc., Cambridge [u.a.]

International audience; We demonstrate that elemental analysis of glass with a measurement precision of about 10% can be performed via calibration-free laser-induced breakdown spectroscopy. Therefore, plasma emission spectra recorded during ultraviolet laser ablation of different glasses are compared to the spectral radiance computed for a plasma in local thermodynamic equilibrium. Using an iterative calculation algorithm, we deduce the relative elemental fractions and the plasma properties from the best agreement between measured and computed spectra. The measurement method is validated in two ways. First, the LIBS measurements are performed on fused silica composed of more than 99.9% of SiO2. Second, the oxygen fractions measured for heavy flint and barite crown glasses are compared to the values expected from the glass composing oxides. The measured compositions are furthermore compared with those obtained by X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy. It is shown that accurate LIBS analyses require spectra recording with short enough delays between laser pulse and detector gate, when the electron density is larger than 10(17) cm(-3). The results show that laser-induced breakdown spectroscopy based on accurate plasma modeling is suitable for elemental analysis of complex materials such as glasses, with an analytical performance comparable of even better than that obtained with standard techniques. (C) 2014 Elsevier B.V. All rights reserved.

International audience; The use of amorphous and transparent oxides is a key for the development of new thin film transistors and displays. Recently, indium zinc oxide (IZO) was shown to exhibit high transparency in the visible range, low resistivity, and high mobility. Since the properties and the cost of these films depend on the In/(In + Zn) values, the measurement of this ratio is paramount for future developments and applications. We report on accurate analysis of the elemental composition of IZO thin films synthesized using a Combinatorial Pulsed Laser Deposition technique. The monitoring of the thin films elemental composition by Laser-Induced Breakdown Spectroscopy was chosen in view of further in situ and real-time technological developments and process control during IZO fabrication. Our analytical approach is based on plasma modeling, the recorded spectra being then compared to the spectral radiance computed for plasmas in local thermal equilibrium. The cation fractions measured were compared to values obtained by complementary measurements using energy dispersive X-ray spectroscopy and Rutherford backscattering spectrometry. Spectroscopic ellipsometry assisted the scientific discussion. A good agreement between methods was found, independently of the relative fraction of indium and zinc that varied from about 65 to 90 and 35 to 10 at%, respectively, and the measurement uncertainties associated to each analytical method.

International audience; We report on accurate analysis of indium-zinc oxide thin films via laser-induced breakdown spectroscopy (LIBS) based on the calculation of the spectral radiance of the nonuniform laser-produced plasma. A thin film sample with variable elemental composition was irradiated with ultraviolet nanosecond laser pulses and the plasma emission spectra were characterized using time-resolved optical emission spectroscopy. Thus, the spectrum recorded with an Echelle Spectrometer coupled to a gated detector was compared to the spectral radiance computed for a plasma in local thermodynamic equilibrium conditions. The time evolution of the plasma was studied to find optimized recording conditions for which the self-absorption of spectral lines is minimized. In addition, the time-resolved measurements allowed us to determine the Stark broadening parameters of spectral lines used for the LIBS analysis. The metal fractions measured via LIBS were found to be in good agreement with the values obtained by complementary measurements using energy dispersive X-ray spectroscopy. The relative decay between fractions measured with both methods was smaller than 5% over the entire measurement range that implied the variation by a factor of four in the case of zinc. The present results show that LIBS measurement procedures based on plasma modeling could be used for fast quality control in the industrial production of thin films.

We desorb polymer films from fused silica with a femtosecond laser and characterize the results by atomic force microscopy. Our study as a function of beam geometry and energy reveals two ways of achieving spatially controlled nanodesorption. © Owned by the authors, published by EDP Sciences, 2013., Workshop on Progress in Ultrafast Laser Modifications of Materials, 2013, 14 April 2013 through 19 April 2013, Cargese

We desorb polymer films from fused silica with a femtosecond laser and characterize the results by atomic force microscopy. Our study as a function of beam geometry and energy reveals two ways of achieving spatially controlled nanodesorption. © OSA 2013., CLEO: Science and Innovations, CLEO_SI 2013, 9 June 2013 through 14 June 2013, San Jose, CA

26th Summer School and International Symposium on the Physics of Ionized Gases (SPIG), Zrenjanin, SERBIA, AUG 27-31, 2012; International audience; We investigate the composition of plasmas produced by laser ablation of metals with two time-delayed short laser pulses using fast imaging and time- and space-resolved optical emission spectroscopy. The ablated material is deposited on mica substrates and analyzed by atomic force microscopy. The laser-produced craters are inspected by optical microscopy to evaluate the ablated material quantity. It is shown that the fraction of nanoparticles in the ablation plume is strongly altered when a second laser pulse of sufficiently large delay is applied. Comparing the results obtained for different metals, we observe a significant nanoparticle reduction for interpulse delays of the order of the characteristic time of electron-lattice thermalization. More detailed analyses show that the plume changes occur on two different characteristic times, indicating two different mechanisms at its origin. Here, we discuss the involved processes and we propose a simple and efficient technique for the measurement of electron-lattice thermalization times based on plume observations during double pulse laser ablation.

By focusing femtosecond pulses on the front and rear surface of a fused silica coverslip, we desorb 8-nm thick polymer films at submicron scale. To determine the role of the substrate in the desorption process, we measure the threshold for nonlinear absorption in fused silica and compare it to the threshold for desorption, taking into account the enhancement of the field at the dielectric-air interface. The results indicate that absorption of energy only occurs in the film. We then measure the beam radius in situ by the knife-edge technique and characterize the desorption by atomic force microscopy. The radius of the laser desorbed area is determined by the desorption threshold intensity and can be a factor of 5 smaller than the beam waist.

International audience; We investigate the plasma produced by the interaction of ultraviolet nanosecond laser pulses with a carbon fiber composite tile from the inner wall of a fusion reactor. The experiments are carried out in argon at a pressure of 5 x 10(4) Pa. Fast imaging is used to characterize the plume expansion dynamics and excited plasma species are followed by time-and space-resolved emission spectroscopy. The measurements show that ionized and highly excited plasma species are located in the front of the expanding plume, whereas neutral atoms and lower excited species dominate in the plasma core. By measuring the excitation temperature of metallic ions and neutral atoms, we evidence the existence of a temperature gradient that appears during the early expansion stage and remains up to delays typically used in material analysis via laser-induced breakdown spectroscopy. The knowledge of the spatial distribution of the plasma properties is then used to model the plasma emission spectrum. Assuming two plasma zones in local thermodynamic equilibrium of different temperatures and electron densities, we calculate the spectral radiance and compare it to the spatially integrated spectrum recorded with an Echelle spectrometer. From the best agreement between measured and computed spectra we deduce the elemental concentrations of carbon, hydrogen and metal impurities. The validity of the model is critically discussed and the measurement uncertainties are evaluated. The present approach is foreseen to improve the accuracy of analysis via laser-induced breakdown spectroscopy in many applications, in particular when materials of elements with significantly different ionization potentials are investigated.