Laser-driven ramp-compression experiments on the national ignition facility.

This report details the analyses and related uncertainties in measuring longitudinal-stress-density paths in indirect laser-driven ramp equation-of-state (EOS) experiments [Smith et al., Nat. Astron. 2(6), 452-458 (2018); Smith et al., Nature 511(7509), 330-333 (2014); Fratanduono et al., Science 372(6546), 1063-1068 (2021); and Fratanduono et al., Phys. Rev. Lett. 124(1), 015701 (2020)]. Experiments were conducted at the National Ignition Facility (NIF) located at the Lawrence Livermore National Laboratory. The NIF can deliver up to 2 MJ of laser energy over 30 ns and provide the necessary laser power and control to ramp compress materials to TPa pressures (1 TPa = 10 × 106 atmospheres). These data provide low-temperature solid-state EOS data relevant to the extreme conditions found in the deep interiors of giant planets. In these experiments, multi-stepped samples with thicknesses in the range of 40-120 µm experience an initial shock compression followed by a time-dependent ramp compression to peak pressure. Interface velocity measurements from each thickness combine to place a constraint on the Lagrangian sound speed as a function of particle velocity, which in turn allows for the determination of a continuous stress-density path to high levels of compressibility. In this report, we present a detailed description of the experimental techniques and measurement uncertainties and describe how these uncertainties combine to place a final uncertainty in both stress and density. We address the effects of time-dependent deformation and the sensitivity of ramp EOS techniques to the onset of phase transformations.

Evidence for Dissociation and Ionization in Shock Compressed Nitrogen to 800 GPa.

Triple bonding in the nitrogen molecule (N_{2}) is among the strongest chemical bonds with a dissociation enthalpy of 9.8 eV/molecule. Nitrogen is therefore an excellent test bed for theoretical and numerical methods aimed at understanding how bonding evolves under the influence of the extreme pressures and temperatures of the warm dense matter regime. Here, we report laser-driven shock experiments on fluid molecular nitrogen up to 800 GPa and 4.0 g/cm^{3}. Line-imaging velocimetry measurements and impedance matching method with a quartz reference yield shock equation of state data of initially precompressed nitrogen. Comparison with numerical simulations using path integral Monte Carlo and density functional theory molecular dynamics reveals clear signatures of chemical dissociation and the onset of L-shell ionization. Combining data along multiple shock Hugoniot curves starting from densities between 0.76 and 1.29 g/cm^{3}, our study documents how pressure and density affect these changes in chemical bonding and provides benchmarks for future theoretical developments in this regime, with applications for planetary interior modeling, high energy density science, and inertial confinement fusion research.

Measuring the melting curve of iron at super-Earth core conditions.

The discovery of more than 4500 extrasolar planets has created a need for modeling their interior structure and dynamics. Given the prominence of iron in planetary interiors, we require accurate and precise physical properties at extreme pressure and temperature. A first-order property of iron is its melting point, which is still debated for the conditions of Earth's interior. We used high-energy lasers at the National Ignition Facility and in situ x-ray diffraction to determine the melting point of iron up to 1000 gigapascals, three times the pressure of Earth's inner core. We used this melting curve to determine the length of dynamo action during core solidification to the hexagonal close-packed (hcp) structure. We find that terrestrial exoplanets with four to six times Earth's mass have the longest dynamos, which provide important shielding against cosmic radiation.

Simultaneous compression and opacity data from time-series radiography with a Lagrangian marker.

Time-resolved radiography can be used to obtain absolute shock Hugoniot states by simultaneously measuring at least two mechanical parameters of the shock, and this technique is particularly suitable for one-dimensional converging shocks where a single experiment probes a range of pressures as the converging shock strengthens. However, at sufficiently high pressures, the shocked material becomes hot enough that the x-ray opacity falls significantly. If the system includes a Lagrangian marker such that the mass within the marker is known, this additional information can be used to constrain the opacity as well as the Hugoniot state. In the limit that the opacity changes only on shock heating, and not significantly on subsequent isentropic compression, the opacity of the shocked material can be determined uniquely. More generally, it is necessary to assume the form of the variation of opacity with isentropic compression or to introduce multiple marker layers. Alternatively, assuming either the equation of state or the opacity, the presence of a marker layer in such experiments enables the non-assumed property to be deduced more accurately than from the radiographic density reconstruction alone. An example analysis is shown for measurements of a converging shock wave in polystyrene at the National Ignition Facility.

Nonideal mixing effects in warm dense matter studied with first-principles computer simulations.

We study nonideal mixing effects in the regime of warm dense matter (WDM) by computing the shock Hugoniot curves of BN, MgO, and MgSiO3. First, we derive these curves from the equations of state (EOS) of the fully interacting systems, which were obtained using a combination of path integral Monte Carlo calculations at high temperature and density functional molecular dynamics simulations at lower temperatures. We then use the ideal mixing approximation at constant pressure and temperature to rederive these Hugoniot curves from the EOS tables of the individual elements. We find that the linear mixing approximation works remarkably well at temperatures above ∼2 × 105 K, where the shock compression ratio exceeds ∼3.2. The shape of the Hugoniot curve of each compound is well reproduced. Regions of increased shock compression, which emerge because of the ionization of L and K shell electrons, are well represented, and the maximum compression ratio of the Hugoniot curves is reproduced with high precision. Some deviations are seen near the onset of the L shell ionization regime, where ionization equilibrium in the fully interacting system cannot be well reproduced by the ideal mixing approximation. This approximation also breaks down at lower temperatures, where chemical bonds play an increasingly important role. However, the results imply that the equilibrium properties of binary and ternary mixtures in the regime of WDM can be derived from the EOS tables of the individual elements. This significantly simplifies the characterization of binary and ternary mixtures in the WDM and plasma phases, which otherwise requires large numbers of more computationally expensive first-principles computer simulations.

A measurement of the equation of state of carbon envelopes of white dwarfs.

White dwarfs represent the final state of evolution for most stars1-3. Certain classes of white dwarfs pulsate4,5, leading to observable brightness variations, and analysis of these variations with theoretical stellar models probes their internal structure. Modelling of these pulsating stars provides stringent tests of white dwarf models and a detailed picture of the outcome of the late stages of stellar evolution6. However, the high-energy-density states that exist in white dwarfs are extremely difficult to reach and to measure in the laboratory, so theoretical predictions are largely untested at these conditions. Here we report measurements of the relationship between pressure and density along the principal shock Hugoniot (equations describing the state of the sample material before and after the passage of the shock derived from conservation laws) of hydrocarbon to within five per cent. The observed maximum compressibility is consistent with theoretical models that include detailed electronic structure. This is relevant for the equation of state of matter at pressures ranging from 100 million to 450 million atmospheres, where the understanding of white dwarf physics is sensitive to the equation of state and where models differ considerably. The measurements test these equation-of-state relations that are used in the modelling of white dwarfs and inertial confinement fusion experiments7,8, and we predict an increase in compressibility due to ionization of the inner-core orbitals of carbon. We also find that a detailed treatment of the electronic structure and the electron degeneracy pressure is required to capture the measured shape of the pressure-density evolution for hydrocarbon before peak compression. Our results illuminate the equation of state of the white dwarf envelope (the region surrounding the stellar core that contains partially ionized and partially degenerate non-ideal plasmas), which is a weak link in the constitutive physics informing the structure and evolution of white dwarf stars9.

High-temperature ion-thermal behavior from average-atom calculations.

Atom-in-jellium calculations of the Einstein frequency were used to calculate the mean displacement of an ion over a wide range of compression and temperature. Expressed as a fraction of the Wigner-Seitz radius, the displacement is a measure of the asymptotic freedom of the ion at high temperature, and thus of the change in heat capacity from six to three quadratic degrees of freedom per atom. A functional form for free energy was proposed based on the Maxwell-Boltzmann distribution as a correction to the Debye free energy, with a single free parameter representing the effective density of potential modes to be saturated. This parameter was investigated using molecular dynamics simulations, and found to be ∼0.2 per atom. In this way, the ion-thermal contribution can be calculated for a wide-range equation of state (EOS) without requiring a large number of molecular dynamics simulations. Example calculations were performed for carbon, including the sensitivity of key EOS loci to ionic freedom.

Non-iterative characteristics analysis for high-pressure ramp loading.

In the canonical ramp compression experiment, a smoothly increasing load is applied to the surface of the sample, and the particle velocity history is measured at two or more different distances into the sample, at interfaces where the surface of the sample can be probed. The velocity histories are used to deduce a stress-density relation, usually using iterative Lagrangian analysis to account for the perturbing effect of the impedance mismatch at the interface. In that technique, a stress-density relation is assumed in order to correct for the perturbation and is adjusted until it becomes consistent with the deduced stress-density relation. This process is subject to the usual difficulties of nonlinear optimization, such as the existence of local minima (sensitivity to the initial guess), possible failure to converge, and relatively large computational effort. We show that, by considering the interaction of successive characteristics reaching a free surface, the stress-density relation can be deduced directly by recursion rather than iteration. This calculation is orders of magnitude faster than iterative analysis and does not require an initial guess. Direct recursion may be less suitable for very noisy data, but it was robust when applied to trial data. The stress-density relation deduced was identical to the result from iterative Lagrangian analysis.

Atom-in-jellium equations of state in the high-energy-density regime.

Recent path-integral Monte Carlo and quantum molecular dynamics simulations have shown that computationally efficient average-atom models can predict thermodynamic states in warm dense matter to within a few percent. One such atom-in-jellium model has typically been used to predict the electron-thermal behavior only, although it was previously developed to predict the entire equation of state (EOS). We report completely atom-in-jellium EOS calculations for Be, Al, Si, Fe, and Mo, as elements representative of a range of atomic number and low-pressure electronic structure. Comparing the more recent method of pseudoatom molecular dynamics, atom-in-jellium results were similar: sometimes less accurate, sometimes more. All these techniques exhibited pronounced effects of electronic shell structure in the shock Hugoniot which are not captured by Thomas-Fermi based EOS. These results demonstrate the value of a hierarchical approach to EOS construction, using average-atom techniques with shell structure to populate a wide-range EOS surface efficiently, complemented by more rigorous three-dimensional multiatom calculations to validate and adjust the EOS.

Nanosecond X-ray diffraction of shock-compressed superionic water ice.

Since Bridgman's discovery of five solid water (H2O) ice phases1 in 1912, studies on the extraordinary polymorphism of H2O have documented more than seventeen crystalline and several amorphous ice structures2,3, as well as rich metastability and kinetic effects4,5. This unique behaviour is due in part to the geometrical frustration of the weak intermolecular hydrogen bonds and the sizeable quantum motion of the light hydrogen ions (protons). Particularly intriguing is the prediction that H2O becomes superionic6-12-with liquid-like protons diffusing through the solid lattice of oxygen-when subjected to extreme pressures exceeding 100 gigapascals and high temperatures above 2,000 kelvin. Numerical simulations suggest that the characteristic diffusion of the protons through the empty sites of the oxygen solid lattice (1) gives rise to a surprisingly high ionic conductivity above 100 Siemens per centimetre, that is, almost as high as typical metallic (electronic) conductivity, (2) greatly increases the ice melting temperature7-13 to several thousand kelvin, and (3) favours new ice structures with a close-packed oxygen lattice13-15. Because confining such hot and dense H2O in the laboratory is extremely challenging, experimental data are scarce. Recent optical measurements along the Hugoniot curve (locus of shock states) of water ice VII showed evidence of superionic conduction and thermodynamic signatures for melting16, but did not confirm the microscopic structure of superionic ice. Here we use laser-driven shockwaves to simultaneously compress and heat liquid water samples to 100-400 gigapascals and 2,000-3,000 kelvin. In situ X-ray diffraction measurements show that under these conditions, water solidifies within a few nanoseconds into nanometre-sized ice grains that exhibit unambiguous evidence for the crystalline oxygen lattice of superionic water ice. The X-ray diffraction data also allow us to document the compressibility of ice at these extreme conditions and a temperature- and pressure-induced phase transformation from a body-centred-cubic ice phase (probably ice X) to a novel face-centred-cubic, superionic ice phase, which we name ice XVIII2,17.

Absolute Hugoniot measurements from a spherically convergent shock using x-ray radiography.

The canonical high pressure equation of state measurement is to induce a shock wave in the sample material and measure two mechanical properties of the shocked material or shock wave. For accurate measurements, the experiment is normally designed to generate a planar shock which is as steady as possible in space and time, and a single state is measured. A converging shock strengthens as it propagates, so a range of shock pressures is induced in a single experiment. However, equation of state measurements must then account for spatial and temporal gradients. We have used x-ray radiography of spherically converging shocks to determine states along the shock Hugoniot. The radius-time history of the shock, and thus its speed, was measured by radiographing the position of the shock front as a function of time using an x-ray streak camera. The density profile of the shock was then inferred from the x-ray transmission at each instant of time. Simultaneous measurement of the density at the shock front and the shock speed determines an absolute mechanical Hugoniot state. The density profile was reconstructed using the known, unshocked density which strongly constrains the density jump at the shock front. The radiographic configuration and streak camera behavior were treated in detail to reduce systematic errors. Measurements were performed on the Omega and National Ignition Facility lasers, using a hohlraum to induce a spatially uniform drive over the outside of a solid, spherical sample and a laser-heated thermal plasma as an x-ray source for radiography. Absolute shock Hugoniot measurements were demonstrated for carbon-containing samples of different composition and initial density, up to temperatures at which K-shell ionization reduced the opacity behind the shock. Here we present the experimental method using measurements of polystyrene as an example.

Properties of plastic ablators in laser-driven material dynamics experiments.

Radiation hydrodynamics simulations were used to study the effect of plastic ablators in laser-driven shock experiments. The sensitivity to composition and equation of state was found to be 5%-10% in ablation pressure. As was found for metals, a laser pulse of constant irradiance gave a pressure history which decreased by several percent per nanosecond. The pressure history could be made more constant by adjusting the irradiance history. The impedance mismatch with the sample gave an increase o(100%) in the pressure transmitted into the sample, for a reduction of several tens of percent in the duration of the peak load applied to the sample, and structured the release history by adding a release step to a pressure close to the ablation pressure. Algebraic relations were found between the laser pulse duration, the ablator thickness, and the duration of the peak pressure applied to the sample, involving quantities calculated from the equations of state of the ablator and sample using shock dynamics.

X-ray diffraction from shock-loaded polycrystals.

X-ray diffraction was demonstrated from shock-compressed polycrystalline metals on nanosecond time scales. Laser ablation was used to induce shock waves in polycrystalline foils of Be, 25-125 microm thick. A second laser pulse was used to generate a plasma x-ray source by irradiation of a Ti foil. The x-ray source was collimated to produce a beam of controllable diameter, which was directed at the Be sample. X-rays were diffracted from the sample, and detected using films and x-ray streak cameras. The diffraction angle was observed to change with shock pressure. The diffraction angles were consistent with the uniaxial (elastic) and isotropic (plastic) compressions expected for the loading conditions used. Polycrystalline diffraction will be used to measure the response of the crystal lattice to high shock pressures and through phase changes.

Shock formation and the ideal shape of ramp compression waves.

We derive expressions for shock formation based on the local curvature of the flow characteristics during dynamic compression. Given a specific ramp adiabat, calculated for instance from the equation of state for a substance, the ideal nonlinear shape for an applied ramp loading history can be determined. We discuss the region affected by lateral release, which can be presented in compact form for the ideal loading history. Example calculations are given for representative metals and plastic ablators. Continuum dynamics (hydrocode) simulations were in good agreement with the algebraic forms. Example applications are presented for several classes of laser-loading experiment, identifying conditions where shocks are desired but not formed, and where long-duration ramps are desired.

On high explosive launching of projectiles for shock physics experiments.

The hydrodynamic operation of the "Forest Flyer" type of explosive launching system for shock physics projectiles was investigated in detail using one and two dimensional continuum dynamics simulations. The simulations were numerically converged and insensitive to uncertainties in the material properties; they reproduced the speed of the projectile and the shape of its rear surface. The most commonly used variant, with an Al alloy case, was predicted to produce a slightly curved projectile, subjected to some shock heating and likely exhibiting some porosity from tensile damage. The curvature is caused by a shock reflected from the case; tensile damage is caused by the interaction of the Taylor wave pressure profile from the detonation wave with the free surface of the projectile. The simulations gave only an indication of tensile damage in the projectile, as damage is not understood well enough for predictions in this loading regime. The flatness can be improved by using a case of lower shock impedance, such as polymethyl methacrylate. High-impedance cases, including Al alloys but with denser materials improving the launching efficiency, can be used if designed according to the physics of oblique shock reflection, which indicates an appropriate case taper for any combination of explosive and case material. The tensile stress induced in the projectile depends on the relative thickness of the explosive, expansion gap, and projectile. The thinner the projectile with respect to the explosive, the smaller the tensile stress. Thus if the explosive is initiated with a plane wave lens, the tensile stress is lower than that for initiation with multiple detonators over a plane. The previous plane wave lens designs did, however, induce a tensile stress close to the spall strength of the projectile. The tensile stress can be reduced by changes in the component thicknesses. Experiments verifying the operation of explosively launched projectiles should attempt to measure porosity induced in the projectile: arrival time measurements are likely to be insensitive to porous regions caused by damaged or recollected material.

Melting dynamics of superheated argon: nucleation and growth.

We investigate the microscopic melting process of a superheated argon solid using molecular dynamics simulations. We characterize the melting dynamics by following the temperature and time evolutions of liquid atoms and demonstrate the formation of a critical liquid nucleus via fluctuations and subsequent growth. The critical liquid nucleus size (about 120 atoms) obtained from our direct simulations is in accord with the prediction of the classical nucleation theory. The dynamic nucleation and growth of liquid also agree with the Johnson-Mehl-Avrami law, and the growth exponent n approximately 3 at the early stage followed by a substantial increase in n thereafter.

Vibrational density of states and Lindemann melting law.

We examine the Lindemann melting law at different pressures using the vibrational density of states (DOS), equilibrium melting curve, and Lindemann parameter delta(L) (fractional root-mean-squared displacement, rmsd, at equilibrium melting) calculated independently from molecular dynamics simulations of the Lennard-Jones system. The DOS is obtained using spectra analysis of atomic velocities and accounts for anharmonicity. The increase of delta(L) with pressure is non-negligible: delta(L) is about 0.116 and 0.145 at ambient and extreme pressures, respectively. If the component of rmsd normal to a reflecting plane as in the Debye-Waller-factor-type measurements using x rays is adopted for delta(L), these values are about 0.067 (+/-0.002) and 0.084 (+/-0.003), and are comparable with experimental and calculated values for face-centered-cubic elements. We find that the Lindemann relation holds accurately at ambient and high pressures. The non-negligible pressure dependence of delta(L) suggests that caution should be exerted in applying the Lindemann law to obtaining the high pressure melting curve anchored at ambient pressure.

Quasi-isentropic compression by ablative laser loading: response of materials to dynamic loading on nanosecond time scales.

The TRIDENT laser was used to induce quasi-isentropic compression waves to approximately 15 GPa in samples of Si, by ablative loading using a laser pulse whose intensity increased smoothly over 2.5 ns. The intensity history of the pulse and the velocity history at the opposite surface of the sample were recorded. Experiments were performed using samples of two different thicknesses simultaneously, in which the evolution of the compression wave was clearly visible. Isentropic stress states deduced were consistent with the previously investigated response of Si to uniaxial loading. The ablative loading was simulated using radiation hydrodynamics, with different equations of state in the plasma and condensed regions and including elasticity in the solid Si. These calculations reproduced the measured velocity histories quite well, demonstrating that quasi-isentropic compression was induced with no preheat from the laser drive. Normal continuum behavior was demonstrated to hold below nanosecond time scales for isentropic compression waves, with no evidence for nonequilibrium effects in the crystal lattice. Details of the velocity history over about 10 GPa were reproduced less well, suggesting a deficiency in the model used for compressed Si, which may be consistent with recent theoretical predictions of uniaxial compression at high strain rates.

Novel crystalline carbon-cage structure synthesized from laser-driven shock wave loading of graphite.

We report a novel crystalline carbon-cage structure synthesized from laser-driven shock wave loading of a graphite-copper mixture to about 14+/-2 GPa and 1000 +/- 200 K. Quite unexpectedly, it can be structurally related to an extremely compressed three-dimensional C60 polymer with random displacement of C atoms around average positions equivalent to those of distorted C60 cages. Thus, the present carbon-cage structure represents a structural crossing point between graphite interlayer bridging and C60 polymerization as the two ways of forming diamond from two-dimensional and molecular carbon.