Extended X-ray absorption fine structure of dynamically-compressed copper up to 1 terapascal.

Large laser facilities have recently enabled material characterization at the pressures of Earth and Super-Earth cores. However, the temperature of the compressed materials has been largely unknown, or solely relied on models and simulations, due to lack of diagnostics under these challenging conditions. Here, we report on temperature, density, pressure, and local structure of copper determined from extended x-ray absorption fine structure and velocimetry up to 1 Terapascal. These results nearly double the highest pressure at which extended x-ray absorption fine structure has been reported in any material. In this work, the copper temperature is unexpectedly found to be much higher than predicted when adjacent to diamond layer(s), demonstrating the important influence of the sample environment on the thermal state of materials; this effect may introduce additional temperature uncertainties in some previous experiments using diamond and provides new guidance for future experimental design.

Energetics of polymeric carbon monoxide.

The transformation of carbon monoxide (CO) from a molecular liquid to a polymeric solid under isothermal compression at room temperature is investigated using first principles theory. We report structural and thermodynamic properties from ambient density up to 2.45 g/cc obtained using density functional theory molecular dynamics simulations, including hybrid exchange corrections. The theoretical results are compared with newly obtained polymeric CO samples, synthesized in a large volume press. The explosive performance of polymeric CO is predicted and discussed. Under most favorable assumptions, it is found to be comparable to trinitrotoluene.

Lattice dynamics of dense lithium.

We report low-frequency high-resolution Raman spectroscopy and ab-initio calculations on dense lithium from 40 to 200 GPa at low temperatures. Our experimental results reveal rich first-order Raman activity in the metallic and semiconducting phases of lithium. The computed Raman frequencies are in excellent agreement with the measurements. Free energy calculations provide a quantitative description and physical explanation of the experimental phase diagram only when vibrational effect are correctly treated. The study underlines the importance of zero-point energy in determining the phase stability of compressed lithium.

Structural and optical properties of liquid CO2 for pressures up to 1 TPa.

We report on the use of first-principles molecular dynamics calculations to examine properties of liquid carbon dioxide in the pressure-temperature range of 0-1 TPa and 200-100 000 K. The computed equations of state points are used to predict a series of shock Hugoniots with initial starting conditions that are relevant to existing and ongoing shock-wave experiments. A comparison with published measurements up to 70 GPa shows excellent agreement. We find that the liquid undergoes a gradual phase transition along the Hugoniot and have characterized this transition based on changes in bonding and structural properties as well as the conductivity and reflectivity of the fluid.

High-pressure phases of calcium: density-functional theory and diffusion quantum Monte Carlo approach.

The phase diagram of Ca is examined using a combination of density-functional theory (DFT) and diffusion quantum Monte Carlo (DMC) calculations. Gibbs free energies of several competing structures are computed at pressures near 50 GPa. Existing disagreements for the stability of Ca both at low and room temperature are resolved with input from DMC. Furthermore, DMC calculations are performed on 0 K crystalline structures up to 150 GPa and it is demonstrated that the widely used generalized gradient approximation of DFT is insufficient to accurately account for the relative stability of the high-pressure phases of Ca. The results indicate that the theoretical phase diagram of Ca needs a revision.

High-pressure molecular phases of solid carbon dioxide.

We present a theoretical study of solid CO2 up to 50 GPa and 1500 K using first-principles calculations. In this pressure-temperature range, interpretations of recent experiments have suggested the existence of CO2 phases which are intermediate between molecular and covalent-bonded solids. We reexamine the concept of intermediate phases in the CO2 phase diagram and propose instead molecular structures, which provide an excellent agreement with measurements.

Enhanced Friedel structure and proton pairing in dense solid hydrogen.

The mechanism of proton pairing in dense solid hydrogen, and its progression with density, are both studied using effective potentials between protons which include electronic response up to quadratic terms. For high pressures nonlinear effects originating with different pairs are crucial in establishing the net attraction within a given pair, and in this picture Friedel oscillations are considerably enhanced by quadratic response, subsequently playing a very important role in the overall pairing. Calculated vibron frequencies also show substantial agreement with experiment, reflecting at the same time significant changes in the physical character of the pairing itself.