Nonequilibrium warm dense matter investigated with laser-plasma-based XANES down to the femtosecond.

The use of laser-plasma-based x-ray sources is discussed, with a view to carrying out time-resolved x-ray absorption spectroscopy measurements, down to the femtosecond timescale. A review of recent experiments performed by our team is presented. They concern the study of the nonequilibrium transition of metals from solid to the warm dense regime, which imposes specific constraints (the sample being destroyed after each shot). Particular attention is paid to the description of experimental devices and methodologies. Two main types of x-ray sources are compared, respectively, based on the emission of a hot plasma, and on the betatron radiation from relativistic electrons accelerated by laser.

Ultrafast Thermal Melting in Nonequilibrium Warm Dense Copper.

The ultrafast dynamics of the loss of crystalline periodicity is investigated in femtosecond laser heated warm dense copper, by the original use of x-ray absorption near-edge specific structures just above the L3 edge. The characteristic time is observed near 1 ps, for specific energy density ranging from 1 to 5 MJ/kg, using ps-resolution x-ray absorption spectroscopy. The overall experimental data are well reproduced with two-temperature hydrodynamic simulations, supporting a thermal phase transition.

Femtosecond Resolution of the Nonballistic Electron Energy Transport in Warm Dense Copper.

The ultrafast electron energy transport is investigated in laser-heated warm dense copper in a high flux regime (2.5±0.7×10^{13} W/cm^{2} absorbed). The dynamics of the electron temperature is retrieved from femtosecond time-resolved x-ray absorption near-edge spectroscopy near the Cu L3 edge. A characteristic time of ∼1 ps is observed for the increase in the average temperature in a 100 nm thick sample. Data are well reproduced by two-temperature hydrodynamic simulations, which support energy transport dominated by thermal conduction rather than ballistic electrons.

Proof-of-concept Talbot-Lau x-ray interferometry with a high-intensity, high-repetition-rate, laser-driven K-alpha source.

Talbot-Lau x-ray interferometry is a grating-based phase-contrast technique, which enables measurement of refractive index changes in matter with micrometric spatial resolution. The technique has been established using a variety of hard x-ray sources, including synchrotron, free-electron lasers, and x-ray tubes, and could be used in the optical range for low-density plasmas. The tremendous development of table-top high-power lasers makes the use of high-intensity, laser-driven K-alpha sources appealing for Talbot-Lau interferometer applications in both high-energy-density plasma experiments and biological imaging. To this end, we present the first, to the best of our knowledge, feasibility study of Talbot-Lau phase-contrast imaging using a high-repetition-rate laser of moderate energy (100 mJ at a repetition rate of 10 Hz) to irradiate a copper backlighter foil. The results from up to 900 laser pulses were integrated to form interferometric images. A constant fringe contrast of 20% is demonstrated over 100 accumulations, while the signal-to-noise ratio continued to increase with the number of shots. Phase retrieval is demonstrated without prior ex-situ phase stepping. Instead, correlation matrices are used to compensate for the displacement between reference acquisition and the probing of a PMMA target rod. The steps for improved measurements with more energetic laser systems are discussed. The final results are in good agreement with the theoretically predicted outcomes, demonstrating the applicability of this diagnostic to a range of laser facilities for use across several disciplines.

Generation of a large compressive strain wave in graphite by ultrashort-pulse laser irradiation.

We have studied strain wave generation in graphite induced by an intense ultrashort laser pulse. The study was performed in the intensity regime above the ablation threshold of graphite. The aim was to maximize the strain and, thus, also the internal pressure (stress). Laser pulses with a 1 ps temporal duration melt the surface of graphite resulting in a molten material which initially exists at the solid density. As the molten material expands, a compressive strain wave starts propagating into the crystal below the molten layer. The strain pulse was studied with time-resolved X-ray diffraction. At a temporal delay of 100 ps after laser excitation, we observed >10% compressive strain, which corresponds to a pressure of 7.2 GPa. This strain could be reproduced by hydrodynamic simulations, which also provided a temperature map as a function of time and depth.

Probing warm dense matter using femtosecond X-ray absorption spectroscopy with a laser-produced betatron source.

Exploring and understanding ultrafast processes at the atomic level is a scientific challenge. Femtosecond X-ray absorption spectroscopy (XAS) arises as an essential experimental probing method, as it can simultaneously reveal both electronic and atomic structures, and thus potentially unravel their nonequilibrium dynamic interplay which is at the origin of most of the ultrafast mechanisms. However, despite considerable efforts, there is still no femtosecond X-ray source suitable for routine experiments. Here we show that betatron radiation from relativistic laser-plasma interaction combines ideal features for femtosecond XAS. It has been used to investigate the nonequilibrium dynamics of a copper sample brought at extreme conditions of temperature and pressure by a femtosecond laser pulse. We measured a rise-time of the electron temperature below 100 fs. This experiment demonstrates the great potential of the table-top betatron source which makes possible the investigation of unexplored ultrafast processes in manifold fields of research.

Polycapillary lenses for soft x-ray transmission in ITER: Model, comparison with experiments, and potential application.

Measuring Soft X-Ray (SXR) radiation [0.1 keV; 15 keV] in tokamaks is a standard way of extracting valuable information on the particle transport and magnetohydrodynamic activity. Generally, the analysis is performed with detectors positioned close to the plasma for a direct line of sight. A burning plasma, like the ITER deuterium-tritium phase, is too harsh an environment to permit the use of such detectors in close vicinity of the machine. We have thus investigated in this article the possibility of using polycapillary lenses in ITER to transport the SXR information several meters away from the plasma in the complex port-plug geometry.

High-pressure structural changes in liquid silica.

The structural properties of liquid silica at high pressure and moderate temperature conditions, also referred to as the warm dense matter regime, were investigated using time-resolved K-edge x-ray absorption spectroscopy and ab initio calculations. We used a nanosecond laser beam to compress uniformly a solid SiO_{2} target and a picosecond laser beam to generate a broadband x-ray source. We obtained x-ray absorption spectra at the Si K edge over a large pressure-temperature domain to probe the liquid phase up to 3.6 times the normal solid density. Using ab initio simulations, we are able to interpret the changes in the x-ray absorption near-edge structure with increasing densities as an increase in the coordination number of silicon by oxygen atoms from 4 to 9. This indicates that, up to significant temperatures, the liquid structure becomes akin to what is found in the solid SiO_{2} phases.

Experimental station for laser-based picosecond time-resolved x-ray absorption near-edge spectroscopy.

We present an experimental station designed for time-resolved X-ray Absorption Near-Edge Spectroscopy (XANES). It is based on ultrashort laser-plasma x-ray pulses generated from a table-top 100 mJ-class laser at 10 Hz repetition rate. A high transmission (10%-20%) x-ray beam line transport using polycapillary optics allows us to set the sample in an independent vacuum chamber, providing high flexibility over a wide spectral range from 0.5 up to 4 keV. Some XANES spectra are presented, demonstrating 1% noise level in only ∼1 mn and ∼100 cumulated laser shots. Time-resolved measurements are reported, indicating that the time resolution of the entire experimental station is 3.3 ± 0.6 ps rms.

Metallization of warm dense SiO(2) studied by XANES spectroscopy.

We investigate the evolution of the electronic structure of fused silica in a dense plasma regime using time-resolved x-ray absorption spectroscopy. We use a nanosecond (ns) laser beam to generate a strong uniform shock wave in the sample and a picosecond (ps) pulse to produce a broadband x-ray source near the Si K edge. By varying the delay between the two laser beams and the intensity of the ns beam, we explore a large thermodynamical domain with densities varying from 1 to 5 g/cm^{3} and temperatures up to 5 eV. In contrast to normal conditions where silica is a well-known insulator with a wide band gap of 8.9 eV, we find that shocked silica exhibits a pseudogap as a semimetal throughout this thermodynamical domain. This is in quantitative agreement with density functional theory predictions performed using the generalized gradient approximation.

Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments.

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.

Ultrafast short-range disordering of femtosecond-laser-heated warm dense aluminum.

We have probed, with time-resolved x-ray absorption near-edge spectroscopy (XANES), a femtosecond-laser-heated aluminum foil with fluences up to 1 J/cm2. The spectra reveal a loss of the short-range order in a few picoseconds. This time scale is compared with the electron-ion equilibration time, calculated with a two-temperature model. Hydrodynamic simulations shed light on complex features that affect the foil dynamics, including progressive density change from solid to liquid (∼10 ps). In this density range, quantum molecular dynamics simulations indicate that XANES is a relevant probe of the ionic temperature.

X-ray diagnosis of the pressure induced Mott nonmetal-metal transition.

The evolution of the K-edge x-ray absorption near-edge spectroscopy (XANES) spectrum is investigated for an aluminum plasma expanding from the solid density down to 0.5 g/cm{3}, with temperatures lying from 5 down to 2 eV. The dense plasma is generated by nanosecond laser-induced shock compression. These conditions correspond to the density-temperature region where a metal-nonmetal transition occurs as the density decreases. This transition is directly observed in XANES spectra measurements through the progressive formation of a preedge structure for densities around 1.6 g/cm{3}. Ab initio calculations based on density functional theory and a jellium model have been efficiently tested through direct comparison with the experimental measurements and show that this preedge corresponds to the relocalization of the 3p atomic orbital as the system evolves from a dense plasma toward a partially ionized atomic fluid.

Relativistic high-current electron-beam stopping-power characterization in solids and plasmas: collisional versus resistive effects.

We present experimental and numerical results on intense-laser-pulse-produced fast electron beams transport through aluminum samples, either solid or compressed and heated by laser-induced planar shock propagation. Thanks to absolute K(α) yield measurements and its very good agreement with results from numerical simulations, we quantify the collisional and resistive fast electron stopping powers: for electron current densities of ≈ 8 × 10(10) A/cm(2) they reach 1.5 keV/µm and 0.8 keV/µm, respectively. For higher current densities up to 10(12)A/cm(2), numerical simulations show resistive and collisional energy losses at comparable levels. Analytical estimations predict the resistive stopping power will be kept on the level of 1 keV/µm for electron current densities of 10(14)A/cm(2), representative of the full-scale conditions in the fast ignition of inertially confined fusion targets.

Electronic structure investigation of highly compressed aluminum with K edge absorption spectroscopy.

The electronic structure evolution of highly compressed aluminum has been investigated using time resolved K edge x-ray absorption spectroscopy. A long laser pulse (500 ps, I(L)≈8×10(13) W/cm(2)) was used to create a uniform shock. A second ps pulse (I(L)≈10(17) W/cm(2)) generated an ultrashort broadband x-ray source near the Al K edge. The main target was designed to probe aluminum at reshocked conditions up to now unexplored (3 times the solid density and temperatures around 8 eV). The hydrodynamical conditions were obtained using rear side visible diagnostics. Data were compared to ab initio and dense plasma calculations, indicating potential improvements in either description. This comparison shows that x-ray-absorption near-edge structure measurements provide a unique capability to probe matter at these extreme conditions and severally constrains theoretical approaches currently used.

Magnetically guided fast electrons in cylindrically compressed matter.

Fast electrons produced by a 10 ps, 160 J laser pulse through laser-compressed plastic cylinders are studied experimentally and numerically in the context of fast ignition. K(α)-emission images reveal a collimated or scattered electron beam depending on the initial density and the compression timing. A numerical transport model shows that implosion-driven electrical resistivity gradients induce strong magnetic fields able to guide the electrons. The good agreement with measured beam sizes provides the first experimental evidence for fast-electron magnetic collimation in laser-compressed matter.

Unraveling the solid-liquid-vapor phase transition dynamics at the atomic level with ultrafast x-ray absorption near-edge spectroscopy.

X-ray absorption near-edge spectroscopy (XANES) is a powerful probe of electronic and atomic structures in various media, ranging from molecules to condensed matter. We show how ultrafast time resolution opens new possibilities to investigate highly nonequilibrium states of matter including phase transitions. Based on a tabletop laser-plasma ultrafast x-ray source, we have performed a time-resolved (∼3 ps) XANES experiment that reveals the evolution of an aluminum foil at the atomic level, when undergoing ultrafast laser heating and ablation. X-ray absorption spectra highlight an ultrafast transition from the crystalline solid to the disordered liquid followed by a progressive transition of the delocalized valence electronic structure (metal) down to localized atomic orbitals (nonmetal-vapor), as the average distance between atoms increases.

Double conical crystal x-ray spectrometer for high resolution ultrafast x-ray absorption near-edge spectroscopy of Al K edge.

An x-ray spectrometer devoted to dynamical studies of transient systems using the x-ray absorption fine spectroscopy technique is presented in this article. Using an ultrafast laser-induced x-ray source, this optical device based on a set of two potassium acid phthalate conical crystals allows the extraction of x-ray absorption near-edge spectroscopy structures following the Al absorption K edge. The proposed experimental protocol leads to a measurement of the absorption spectra free from any crystal reflectivity defaults and shot-to-shot x-ray spectral fluctuation. According to the detailed analysis of the experimental results, a spectral resolution of 0.7 eV rms and relative fluctuation lower than 1% rms are achieved, demonstrated to be limited by the statistics of photon counting on the x-ray detector.

Picosecond short-range disordering in isochorically heated aluminum at solid density.

Using ultrafast x-ray probing, we experimentally observed a progressive loss of ordering within solid-density aluminum as the temperature raises from 300 K to >10{4} K. The Al sample was isochorically heated by a short ( approximately ps), laser-accelerated proton beam and probed by a short broadband x-ray source around the Al K edge. The loss of short-range ordering is detected through the progressive smoothing of the time-resolved x-ray absorption near-edge spectroscopy (XANES) structure. The results are compared with two different theoretical models of warm dense matter and allow us to put an upper bound on the onset of ion lattice disorder within the heated solid-density medium of approximately 10 ps.

Broadband, high dynamics and high resolution charge coupled device-based spectrometer in dynamic mode for multi-keV repetitive x-ray sources.

We present a new operating mode, using a charged coupled device as dispersionless spectrometer dedicated to repetitive x-ray sources in the multi-keV domain. This enables to get spectra with high statistics in a short acquisition time and a way compatible with the operation of other diagnostics requiring accumulation. Several reconstruction algorithms for the spreading events are discussed, and a near Fano-limited resolution is demonstrated by using single pixel events. In this case, a method to take into account partial canceling of the events is presented. Experimental characterization and detailed modeling of the detector are performed, which allow to determine absolute number of photon with +/-35% accuracy. Characterization of the 5-25 keV x rays emitted by a short pulse laser-produced plasma is reported, as well as their dependency with the atomic number, the laser duration, and energy.