In megabar shock waves, materials compress and undergo a phase transition to a dense charged-particle system that is dominated by strong correlations and quantum effects. This complex state, known as warm dense matter, exists in planetary interiors and many laboratory experiments (for example, during high-power laser interactions with solids or the compression phase of inertial confinement fusion implosions). Here, we apply record peak brightness X-rays at the Linac Coherent Light Source to resolve ionic interactions at atomic (ångström) scale lengths and to determine their physical properties. Our in situ measurements characterize the compressed lattice and resolve the transition to warm dense matter, demonstrating that short-range repulsion between ions must be accounted for to obtain accurate structure factor and equation of state data. In addition, the unique properties of the X-ray laser provide plasmon spectra that yield the temperature and density with unprecedented precision at micrometre-scale resolution in dynamic compression experiments. M aterials exposed to high pressures of 1 Mbar and above have recently been the subject of increased attention due to their importance for the physics of planetary formation 1-3 , for material science 4 and for inertial confinement fusion research 5 . The behaviour of shock-compressed aluminium is of particular interest because it has been proposed as a standard for shock-wave experiments 6 and is widely used for equation-of-state 7,8 and warm dense matter (WDM) 9,10 studies. At room temperature, aluminium has three delocalized electrons, so it provides a prototype for an ideal electron fluid. As temperatures and pressures increase, compressing and breaking ionic lattice bonds, strong ionic forces remain, resulting in significant deviations from a simple fluid.Simulations using density functional theory coupled to manyparticle molecular dynamics (DFT-MD) have evolved into an ab initio tool to explore this regime of high-pressure physics 11,12 . To date, these simulations have been used to predict physical properties derived from optical observations of particle and shock velocities. Studies of structural properties that are sensitive to many-particle electron-ion and ion-ion interaction physics 13 have been challenging 14 , although recent progress has been made using X-ray absorption spectroscopy 15,16 . Early experiments on fourth-generation light sources 17 have made use of X-ray diffraction and measured the structural evolution from elastic to plastic states 18 . However, pressures in the Mbar regime, as required for melting many solids, have only recently become available at the Matter in Extreme Conditions (MEC) instrument at the Linac Coherent Light Source (LCLS).Here we visualize, for the first time, the evolution of compressed matter across the melting line and the coexistence regime into a WDM state. The combination of high-power optical lasers and the X-ray beam at MEC provides high-resolution X-ray scattering at multi-Mbar pressures. Our data provide the io...
We investigate ultrafast (fs) electron dynamics in a liquid hydrogen sample, isochorically and volumetrically heated to a moderately coupled plasma state. Thomson scattering measurements using 91.8 eV photons from the free-electron laser in Hamburg (FLASH at DESY) show that the hydrogen plasma has been driven to a nonthermal state with an electron temperature of 13 eV and an ion temperature below 0.1 eV, while the free-electron density is 2:8 Â 10 20 cm À3 . For dense plasmas, our experimental data strongly support a nonequilibrium kinetics model that uses impact ionization cross sections based on classical free-electron collisions. The investigation of warm dense matter (WDM) is one of the grand challenges of contemporary physics [1]. WDM is a plasma state characterized by moderate-tostrong interparticle coupling which takes place at freeelectron temperatures of several eV and free-electron densities around solid density [1]. It is present in many physical environments, such as planetary interiors [2,3], gravitationally collapsing protostellar disks, laser matter interaction and particularly during the implosion of an inertial confinement fusion capsule [4]. While in the astrophysical context WDM exists under stable conditions, in the laboratory it is achieved only as a transient state bridging condensed matter and hot plasma regimes. Here, we report on the first investigation of the nonequilibrium transition of hydrogen from a liquid to a moderately coupled plasma on the fs time scale, induced by highly intense soft-x-ray irradiation. This is an important step towards the investigation of strongly-coupled plasmas which are within reach of current light sources such as the Linac Coherent Light Source (LCLS). Our measurement enables unprecedented direct tests of nonequilibrium statistical models beyond mean field theories in a regime where collision and relaxation processes are dominant [5][6][7].The use of x-ray scattering for the investigation of dense, strongly-coupled plasmas was successfully demonstrated in the past decade [5,[7][8][9][10][11]. This technique is the x-ray analog of optical Thomson scattering (TS) [12] and enables the experimental determination of plasma parameters in dense systems where optical light cannot penetrate. While previous experiments were carried out using highenergy laser facilities, the advent of soft-and hard-x-ray free-electron lasers (FELs) makes ultrashort high brightness beams available for this type of research [13,14]. This Letter reports on ultrafast heating of liquid hydrogen and TS measurement of dense plasma parameters using softx-ray FEL radiation. For the first time, nonequilibrium distributions are observed and the underlying relaxation dynamics are compared with kinetic models showing electron relaxation times in the order of 20 fs, thus, shorter than the pulse duration.The scattering taking place is collective TS, which is characterized by a spectrally blue and red shifted response due to collective electron motion, plasmons, and nearly elastic scattering due t...
Saturable absorption is a phenomenon readily seen in the optical and infrared wavelengths. It has never been observed in core-electron transitions owing to the short lifetime of the excited states involved and the high intensities of the soft X-rays needed. We report saturable absorption of an L-shell transition in aluminium using record intensities over 10 16 W cm −2 at a photon energy of 92 eV. From a consideration of the relevant timescales, we infer that immediately after the X-rays have passed, the sample is in an exotic state where all of the aluminium atoms have an L-shell hole, and the valence band has approximately a 9 eV temperature, whereas the atoms are still on their crystallographic positions. Subsequently, Auger decay heats the material to the warm dense matter regime, at around 25 eV temperatures. The method is an ideal candidate to study homogeneous warm dense matter, highly relevant to planetary science, astrophysics and inertial confinement fusion. Saturable absorption, the decrease in the absorption of light with increasing intensity, is a well-known effect in the visible and near-visible region of the electromagnetic spectrum 1 , and is a widely exploited phenomenon in laser technology. Although there are many ways to induce this effect, in the simplest two-level system it will occur when the population of the lower, absorbing level is severely depleted, which requires light intensities sufficiently high to overcome relaxation from the upper level. Here, we report on the production of saturable absorption of a metal in the soft X-ray regime by the creation of highly uniform warm dense conditions, a regime that is of great interest in high-pressure science 2,3 , the geophysics of large planets 4,5 , astrophysics 6 , plasma production and inertial confinement fusion 7 . Furthermore, the process by which the saturation of the absorption occurs will lead, after the X-ray pulse, to the storage of about 100 eV per atom, which in turn evolves to a warm dense state. This manner of creation is unique as it requires intense, subpicosecond, soft X-rays. As such, it has not hitherto been observed in this region of the spectrum, owing both to the lack of high-intensity sources, and the rapid recombination times associated with such high photon energies. However, with the advent of new fourth-generation X-ray light sources, including the free-electron laser in Hamburg 8 (FLASH), soft X-ray intensities that have previously remained the province of high-power optical lasers can now be produced. Experiments at such high intensities using gas jets have already exhibited novel absorption phenomena 9 , and the possibility of irradiating solid samples with intense soft and hard X-rays has aroused interest as a possible means of producing warm dense matter (WDM) at known atomic densities 10,11 .We present the first measurements of the absorption coefficient of solid samples subject to subpicosecond soft X-ray pulses with intensities up to and in excess of 10 16 W cm −2 , two orders of magnitude higher than could ...
Detailed measurements of the electron densities, temperatures, and ionization states of compressed CH shells approaching pressures of 50 MBar have been achieved with spectrally resolved x-ray scattering. Laser-produced 9 keV x-rays probe the plasma during the transient state of threeshock-coalescence. High signal-to-noise x-ray scattering spectra show direct evidence of continuum depression in highly degenerate warm dense matter states with electron densities ne > 10 24 cm −3 . The measured densities and temperatures agree well with radiation-hydrodynamic modeling when accounting for continuum lowering in calculations that employ detailed configuration accounting.
Thomson scattering in non-ideal (collision-dominated) two-component plasmas is calculated accounting for electron-ion collisions as well as electron-electron correlations. This is achieved by using a novel interpolation scheme for the electron-electron response function generalizing the traditional Mermin approach. Also, ions are treated as randomly distributed inert scattering centers. The collision frequency is taken as a dynamic and complex quantity and is calculated from a microscopic quantum-statistical approach. Implications due to different approximations for the electron-electron correlation, i.e. different forms of the OCP local field correction, are discussed.
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