Numerical convergence of the self-diffusion coefficient and viscosity obtained with Thomas-Fermi-Dirac molecular dynamics.

Computations of the self-diffusion coefficient and viscosity in warm dense matter are presented with an emphasis on obtaining numerical convergence and a careful evaluation of the standard deviation. The transport coefficients are computed with the Green-Kubo relation and orbital-free molecular dynamics at the Thomas-Fermi-Dirac level. The numerical parameters are varied until the Green-Kubo integral is equal to a constant in the t→+∞ limit; the transport coefficients are deduced from this constant and not by extrapolation of the Green-Kubo integral. The latter method, which gives rise to an unknown error, is tested for the computation of viscosity; it appears that it should be used with caution. In the large domain of coupling constant considered, both the self-diffusion coefficient and viscosity turn out to be well approximated by simple analytical laws using a single effective atomic number calculated in the average-atom model.

Orbital-free molecular dynamics simulations of a warm dense mixture: examination of the excess-pressure matching rule.

A form of the linear mixing rule involving the equality of excess pressures is tested with various mole fractions and various types of orbital-free molecular dynamics simulations. For all the cases considered, this mixing rule yields, within statistical error, the pressure of a mixture of helium and iron obtained by a direct simulation. In an attempt to interpret the robustness of the mixing rule, we show that it can be derived from thermodynamic stability if the system is regarded as a mixture of independent effective average atoms. The success of the mixing rule applied with equations of state including various degrees of approximation leads us to suggest its use in the thermodynamic domain where quantum molecular dynamics can be implemented.

Ab initio simulations of the K-edge shift along the aluminum Hugoniot.

We develop a first-principles approach to calculate the near-edge absorption spectrum of dense plasmas based on density functional electronic structure calculations and molecular dynamics simulations. We apply the method to the calculation of the K-edge shift along the aluminum shock compressed Hugoniot. We obtain a good agreement with measurements performed at moderate compression and find that the variation of the XANES spectra could be used as a signature for melting along the Hugoniot. We also show that the calculation of the K-edge shift along the Hugoniot formally requires a fully self-consistent calculation beyond the frozen-core approximation and provides an opportunity to test the accuracy of first principle simulation methods in the high-pressure high-temperature regime.

Direct verification of mixing rules in the hot and dense regime.

We perform orbital-free molecular dynamics simulations in the hot and dense regime for two mixtures: equimolar helium-iron and asymmetric deuterium-copper plasmas. For thermodynamic properties, we test two isobaric-isothermal mixing rules whose definitions involve either the equality of total pressures or the equality of the so-defined excess pressures of the components; the pressure and internal energy obtained by direct simulations are in very good agreement with those given by the mixing rule involving the equality of excess pressures. The viscosity of the deuterium-copper mixture is also extracted from a direct simulation and compared to the result given by a mixing rule applied to the viscosities of the pure elements. Finally, for structural properties, the effective charges given by the isobaric-isothermal mixing rule for the average atom model, used in the binary ionic mixture model, yield partial pair distribution functions in good agreement with those obtained by a direct simulation.

Ab initio molecular dynamics simulations of dense boron plasmas up to the semiclassical Thomas-Fermi regime.

We build an "all-electron" norm-conserving pseudopotential for boron which extends the use of ab initio molecular dynamics simulations up to 50 times the normal density rho0. This allows us to perform ab initio simulations of dense plasmas from the regime where quantum mechanical effects are important to the regime where semiclassical simulations based on the Thomas-Fermi approach are, by default, the only simulation method currently available. This study first allows one to establish, for the case of boron, the density regime from which the semiclassical Thomas-Fermi approach is legitimate and sufficient. It further brings forward various issues pertaining to the construction of pseudopotentials aimed at high-pressure studies.

Effect of intense laser irradiation on the lattice stability of semiconductors and metals.

The effect of intense ultrashort irradiation on interatomic forces, crystal stability, and possible melting transition of the underlying lattice is not completely elucidated. By using ab initio linear response to compute the phonon spectrum of gold, silicon, and aluminum, we found that silicon and gold behave in opposite ways when increasing radiation intensity: whereas a weakening of the silicon bond induces a lattice instability, gold undergoes a sharp increase of its melting temperature, while a significantly smaller effect is observed for aluminum for electronic temperatures up to 6 eV.

Ab-initio simulations of the optical properties of warm dense gold.

Using a combination of classical and ab-initio molecular dynamics simulations, we calculate the structure and the electrical conductivity of warm dense gold during the first picoseconds after a short-pulse laser illumination. We find that the ions remain in their initial fcc structure for several picoseconds, despite electron temperatures ranging from a few to several eV after the laser illumination. The electrical conductivities calculated under these nonequilibrium conditions and using the latter assumption are in remarkable agreement with recent measurements using a short-pulse laser interacting with gold thin films.

Parallel-in-time molecular-dynamics simulations.

While there have been many progress in the field of multiscale simulations in the space domain, in particular, due to efficient parallelization techniques, much less is known in the way to perform similar approaches in the time domain. In this paper we show on two examples that, provided we can describe in a rough but still accurate way the system under consideration, it is indeed possible to parallelize molecular dynamics simulations in time by using the recently introduced pararealalgorithm. The technique is most useful for ab initio simulations.

Multiscale recursion in dense hydrogen plasmas.

We present and assess a multiscale recursion method to calculate electronic density via the Green's function. The method lies within the framework of finite temperature density functional theory and uses a real space approach. It provides a satisfactory description of the first Brillouin zone without invoking k points. Unlike methods that explicitly calculate eigenstates, the computational workload decreases with temperature. Tests are performed on a system representing a hydrogen plasma with a local pseudopotential. Calculations are distributed on real space grids with different spacings using scaling properties of the recursion. The computational workload increases linearly with the size of the system and can be productively dispatched on an arbitrarily large number of processors.