Evidence of hydrogen-helium immiscibility at Jupiter-interior conditions.

The phase behaviour of warm dense hydrogen-helium (H-He) mixtures affects our understanding of the evolution of Jupiter and Saturn and their interior structures1,2. For example, precipitation of He from a H-He atmosphere at about 1-10 megabar and a few thousand kelvin has been invoked to explain both the excess luminosity of Saturn1,3, and the depletion of He and neon (Ne) in Jupiter's atmosphere as observed by the Galileo probe4,5. But despite its importance, H-He phase behaviour under relevant planetary conditions remains poorly constrained because it is challenging to determine computationally and because the extremes of temperature and pressure are difficult to reach experimentally. Here we report that appropriate temperatures and pressures can be reached through laser-driven shock compression of H2-He samples that have been pre-compressed in diamond-anvil cells. This allows us to probe the properties of H-He mixtures under Jovian interior conditions, revealing a region of immiscibility along the Hugoniot. A clear discontinuous change in sample reflectivity indicates that this region ends above 150 gigapascals at 10,200 kelvin and that a more subtle reflectivity change occurs above 93 gigapascals at 4,700 kelvin. Considering pressure-temperature profiles for Jupiter, these experimental immiscibility constraints for a near-protosolar mixture suggest that H-He phase separation affects a large fraction-we estimate about 15 per cent of the radius-of Jupiter's interior. This finding provides microphysical support for Jupiter models that invoke a layered interior to explain Juno and Galileo spacecraft observations1,4,6-8.

Metastability of diamond ramp-compressed to 2 terapascals.

Carbon is the fourth-most prevalent element in the Universe and essential for all known life. In the elemental form it is found in multiple allotropes, including graphite, diamond and fullerenes, and it has long been predicted that even more structures can exist at pressures greater than those at Earth's core1-3. Several phases have been predicted to exist in the multi-terapascal regime, which is important for accurate modelling of the interiors of carbon-rich exoplanets4,5. By compressing solid carbon to 2 terapascals (20 million atmospheres; more than five times the pressure at Earth's core) using ramp-shaped laser pulses and simultaneously measuring nanosecond-duration time-resolved X-ray diffraction, we found that solid carbon retains the diamond structure far beyond its regime of predicted stability. The results confirm predictions that the strength of the tetrahedral molecular orbital bonds in diamond persists under enormous pressure, resulting in large energy barriers that hinder conversion to more-stable high-pressure allotropes1,2, just as graphite formation from metastable diamond is kinetically hindered at atmospheric pressure. This work nearly doubles the highest pressure at which X-ray diffraction has been recorded on any material.

X-Ray Diffraction of Ramp-Compressed Silicon to 390 GPa.

Silicon (Si) exhibits a rich collection of phase transitions under ambient-temperature isothermal and shock compression. This report describes in situ diffraction measurements of ramp-compressed Si between 40 and 389 GPa. Angle-dispersive x-ray scattering reveals that Si assumes an hexagonal close-packed (hcp) structure between 40 and 93 GPa and, at higher pressure, a face-centered cubic structure that persists to at least 389 GPa, the highest pressure for which the crystal structure of Si has been investigated. The range of hcp stability extends to higher pressures and temperatures than predicted by theory.

Novel experimental setup for megahertz X-ray diffraction in a diamond anvil cell at the High Energy Density (HED) instrument of the European X-ray Free-Electron Laser (EuXFEL).

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.

Experimental Observations of Laser-Driven Tin Ejecta Microjet Interactions.

The study of high-velocity particle-laden flow interactions is of importance for the understanding of a wide range of natural phenomena, ranging from planetary formation to cloud interactions. Experimental observations of particle dynamics are sparse given the difficulty of generating high-velocity flows of many particles. Ejecta microjets are micron-scale jets formed by strong shocks interacting with imprinted surfaces to generate particle plumes traveling at several kilometers per second. As such, the interaction of two ejecta microjets provides a novel experimental methodology to study interacting particle streams. In this Letter, we report the first time sequences of x-ray radiography images of two interacting tin ejecta microjets taken on a platform designed for the OMEGA Extended Performance (OMEGA EP) laser. We observe that the microjets pass through each other unattenuated for the case of 11.7±3.2 GPa shock pressures and jet velocities of 2.2±0.5 km/s but show strong interaction dynamics for 116.0±6.1 GPa shock pressures and jet velocities of 6.5±0.5 km/s. We find that radiation-hydrodynamic simulations of the experiments are able to capture many aspects of the collisional behavior, such as the attenuation of jet velocity in the direction of propagation, but are unable to match the full spread of the strongly interacting cloud.

Melting of Tantalum at Multimegabar Pressures on the Nanosecond Timescale.

Tantalum was once thought to be the canonical bcc metal, but is now predicted to transition to the Pnma phase at the high pressures and temperatures expected along the principal Hugoniot. Furthermore, there remains a significant discrepancy between a number of static diamond anvil cell experiments and gas gun experiments in the measured melt temperatures at high pressures. Our in situ x-ray diffraction experiments on shock compressed tantalum show that it does not transition to the Pnma phase or other candidate phases at high pressure. We observe incipient melting at approximately 254±15 GPa and complete melting by 317±10 GPa. These transition pressures from the nanosecond experiments presented here are consistent with what can be inferred from microsecond gas gun sound velocity measurements. Furthermore, the observation of a coexistence region on the Hugoniot implies the lack of significant kinetically controlled deviation from equilibrium behavior. Consequently, we find that kinetics of phase transitions cannot be used to explain the discrepancy between static and dynamic measurements of the tantalum melt curve. Using available high pressure thermodynamic data for tantalum and our measurements of the incipient and complete melting transition pressures, we are able to infer a melting temperature 8070_{-750}^{+1250} K at 254±15 GPa, which is consistent with ambient and a recent static high pressure melt curve measurement.

Metastability of Liquid Water Freezing into Ice VII under Dynamic Compression.

The ubiquitous nature and unusual properties of water have motivated many studies on its metastability under temperature- or pressure-induced phase transformations. Here, nanosecond compression by a high-power laser is used to create the nonequilibrium conditions where liquid water persists well into the stable region of ice VII. Through our experiments, as well as a complementary theoretical-computational analysis based on classical nucleation theory, we report that the metastability limit of liquid water under nearly isentropic compression from ambient conditions is at least 8 GPa, higher than the 7 GPa previously reported for lower loading rates.

Equation of State of CO_{2} Shock Compressed to 1 TPa.

Equation-of-state (pressure, density, temperature, internal energy) and reflectivity measurements on shock-compressed CO_{2} at and above the insulating-to-conducting transition reveal new insight into the chemistry of simple molecular systems in the warm-dense-matter regime. CO_{2} samples were precompressed in diamond-anvil cells to tune the initial densities from 1.35 g/cm^{3} (liquid) to 1.74 g/cm^{3} (solid) at room temperature and were then shock compressed up to 1 TPa and 93 000 K. Variation in initial density was leveraged to infer thermodynamic derivatives including specific heat and Gruneisen coefficient, exposing a complex bonded and moderately ionized state at the most extreme conditions studied.

Probing the Solid Phase of Noble Metal Copper at Terapascal Conditions.

Ramp compression along a low-temperature adiabat offers a unique avenue to explore the physical properties of materials at the highest densities of their solid form, a region inaccessible by single shock compression. Using the National Ignition Facility and OMEGA laser facilities, copper samples were ramp compressed to peak pressures of 2.30 TPa and densities of nearly 30 g/cc, providing fundamental information regarding the compressibility and phase of copper at pressures more than 5 times greater than previously explored. Through x-ray diffraction measurements, we find that the ambient face-centered-cubic structure is preserved up to 1.15 TPa. The ramp compression equation-of-state measurements shows that there are no discontinuities in sound velocities up to 2.30 TPa, suggesting this phase is likely stable up to the peak pressures measured, as predicted by first-principal calculations. The high precision of these quasiabsolute measurements enables us to provide essential benchmarks for advanced computational studies on the behavior of dense monoatomic materials under extreme conditions that constitute a stringent test for solid-state quantum theory. We find that both density-functional theory and the stabilized jellium model, which assumes that the ionic structure can be replaced by an ionic charge distribution by constant positive-charge background, reproduces our data well. Further, our data could serve to establish new international secondary scales of pressure in the terapascal range that is becoming experimentally accessible with advanced static and dynamic compression techniques.

Ramp compression of diamond to five terapascals.

The recent discovery of more than a thousand planets outside our Solar System, together with the significant push to achieve inertially confined fusion in the laboratory, has prompted a renewed interest in how dense matter behaves at millions to billions of atmospheres of pressure. The theoretical description of such electron-degenerate matter has matured since the early quantum statistical model of Thomas and Fermi, and now suggests that new complexities can emerge at pressures where core electrons (not only valence electrons) influence the structure and bonding of matter. Recent developments in shock-free dynamic (ramp) compression now allow laboratory access to this dense matter regime. Here we describe ramp-compression measurements for diamond, achieving 3.7-fold compression at a peak pressure of 5 terapascals (equivalent to 50 million atmospheres). These equation-of-state data can now be compared to first-principles density functional calculations and theories long used to describe matter present in the interiors of giant planets, in stars, and in inertial-confinement fusion experiments. Our data also provide new constraints on mass-radius relationships for carbon-rich planets.

Measurement of Body-Centered Cubic Gold and Melting under Shock Compression.

We combined laser shock compression with in situ x-ray diffraction to probe the crystallographic state of gold (Au) on its principal shock Hugoniot. Au has long been recognized as an important calibration standard in diamond anvil cell experiments due to the stability of its face-centered cubic (fcc) structure to extremely high pressures (P >600 GPa at 300 K). This is in contrast to density functional theory and first principles calculations of the high-pressure phases of Au that predict a variety of fcc-like structures with different stacking arrangements at intermediate pressures. In this Letter, we probe high-pressure and high-temperature conditions on the shock Hugoniot and observe fcc Au at 169 GPa and the first evidence of body-centered cubic (bcc) Au at 223 GPa. Upon further compression, the bcc phase is observed in coexistence with liquid scattering as the Hugoniot crosses the Au melt curve before 322 GPa. The results suggest a triple point on the Au phase diagram that lies very close to the principal shock Hugoniot near ∼220 GPa.

Shock Compression of Liquid Deuterium up to 1 TPa.

We present laser-driven shock compression experiments on cryogenic liquid deuterium to 550 GPa along the principal Hugoniot and reflected-shock data up to 1 TPa. High-precision interferometric Doppler velocimetry and impedance-matching analysis were used to determine the compression accurately enough to reveal a significant difference as compared to state-of-the-art ab initio calculations and thus, no single equation of state model fully matches the principal Hugoniot of deuterium over the observed pressure range. In the molecular-to-atomic transition pressure range, models based on density functional theory calculations predict the maximum compression accurately. However, beyond 250 GPa along the principal Hugoniot, first-principles models exhibit a stiffer response than the experimental data. Similarly, above 500 GPa the reflected shock data show 5%-7% higher compression than predicted by all current models.

Identification of Phase Transitions and Metastability in Dynamically Compressed Antimony Using Ultrafast X-Ray Diffraction.

Ultrafast x-ray diffraction at the LCLS x-ray free electron laser has been used to resolve the structural behavior of antimony under shock compression to 59 GPa. Antimony is seen to transform to the incommensurate, host-guest phase Sb-II at ∼11 GPa, which forms on nanosecond timescales with ordered guest-atom chains. The high-pressure bcc phase Sb-III is observed above ∼15 GPa, some 8 GPa lower than in static compression studies, and mixed Sb-III/liquid diffraction are obtained between 38 and 59 GPa. An additional phase which does not exist under static compression, Sb-I^{'}, is also observed between 8 and 12 GPa, beyond the normal stability field of Sb-I, and resembles Sb-I with a resolved Peierls distortion. The incommensurate Sb-II high-pressure phase can be recovered metastably on release to ambient pressure, where it is stable for more than 10 ns.

Nonisentropic Release of a Shocked Solid.

We present molecular dynamics simulations of shock and release in micron-scale tantalum crystals that exhibit postbreakout temperatures far exceeding those expected under the standard assumption of isentropic release. We show via an energy-budget analysis that this is due to plastic-work heating from material strength that largely counters thermoelastic cooling. The simulations are corroborated by experiments where the release temperatures of laser-shocked tantalum foils are deduced from their thermal strains via in situ x-ray diffraction and are found to be close to those behind the shock.

Erratum: Measurement of Body-Centered-Cubic Aluminum at 475 GPa [Phys. Rev. Lett. 119, 175702 (2017)].

This corrects the article DOI: 10.1103/PhysRevLett.119.175702.

Erratum: Evidence for a Phase Transition in Silicate Melt at Extreme Pressure and Temperature Conditions [Phys. Rev. Lett. 108, 065701 (2012)].

This corrects the article DOI: 10.1103/PhysRevLett.108.065701.

Measurement of Body-Centered-Cubic Aluminum at 475 GPa.

Nanosecond in situ x-ray diffraction and simultaneous velocimetry measurements were used to determine the crystal structure and pressure, respectively, of ramp-compressed aluminum at stress states between 111 and 475 GPa. The solid-solid Al phase transformations, fcc-hcp and hcp-bcc, are observed at 216±9 and 321±12 GPa, respectively, with the bcc phase persisting to 475 GPa. The high-pressure crystallographic texture of the hcp and bcc phases suggests close-packed or nearly close-packed lattice planes remain parallel through both transformations.

Ultrafast X-Ray Diffraction Studies of the Phase Transitions and Equation of State of Scandium Shock Compressed to 82 GPa.

Using x-ray diffraction at the Linac Coherent Light Source x-ray free-electron laser, we have determined simultaneously and self-consistently the phase transitions and equation of state (EOS) of the lightest transition metal, scandium, under shock compression. On compression scandium undergoes a structural phase transition between 32 and 35 GPa to the same bcc structure seen at high temperatures at ambient pressures, and then a further transition at 46 GPa to the incommensurate host-guest polymorph found above 21 GPa in static compression at room temperature. Shock melting of the host-guest phase is observed between 53 and 72 GPa with the disappearance of Bragg scattering and the growth of a broad asymmetric diffraction peak from the high-density liquid.

Cost and mortality data of a regional limb salvage and hyperbaric medicine program for Wagner Grade 3 or 4 diabetic foot ulcers.

We obtained costs and mortality data in two retrospective cohorts totaling 159 patients who have diabetes mellitus and onset of a diabetic foot ulcer (DFU). Data were collected from 2005 to 2013, with a follow-up period through September 30, 2014. A total of 106 patients entered an evidence-based limb salvage protocol (LSP) for Wagner Grade 3 or 4 (WG3/4) DFU and intention-to-treat adjunctive hyperbaric oxygen (HBO2) therapy. A second cohort of 53 patients had a primary lower extremity amputation (LEA), either below the knee (BKA) or above the knee (AKA) and were not part of the LSP. Ninety-six of 106 patients completed the LSP/HBO2with an average cost of USD $33,100. Eighty-eight of 96 patients (91.7%) who completed the LSP/HBO2had intact lower extremities at one year. Thirty-four of the 96 patients (35.4%) died during the follow-up period. Costs for a historical cohort of 53 patients having a primary major LEA range from USD $66,300 to USD $73,000. Twenty-five of the 53 patients (47.2%) died. The difference in cost of care and mortality between an LSP with adjunctive HBO2therapy vs. primary LEA is staggering. We conclude that an aggressive limb salvage program that includes HBO2 therapy is cost-effective.