analyzing-melts-fluids-from-ab-initio-molecular-dynamics-simulations

Analyzing Melts and Fluids from Ab Initio Molecular Dynamics Simulations with the UMD Package

We have developed a Python-based open-source package to analyze the results stemming from ab initio molecular-dynamics simulations of fluids. The package ...

CEA, DAM, DIF

CNRS

We report the experimental study of the degassing dynamics through a thin layer of shear-thinning viscoelastic fluid when a constant air flow is imposed at its bottom. The fluid is an aqueous solution of cetyltrimethylammonium bromide (CTAB) and sodium salicylate (NaSal). Over a large range of parameters, the air is periodically released through a series of successive bubbles, hereafter named cascades. Each cascade is followed by a continuous degassing, lasting for several seconds, corresponding to an open channel crossing the fluid layer. The periodicity between two cascades does not depend on the injected flow rate. Inside one cascade, the properties of the overpressure signal associated with the successive bubbles vary continuously. The pressure threshold above which the fluid starts flowing, fluid deformation and pressure drop due to degassing through the thin fluid layer can be simply described by a Maxwell model.

Degassing cascades in a shear-thinning viscoelastic fluid.

Super-Earths are extremely common among the numerous exoplanets that have been discovered. The high pressures and temperatures in their interiors are likely to lead to long-lived magma oceans. If their electrical conductivity is sufficiently high, the mantles of Super-Earth would generate their own magnetic fields. With ab initio simulations, we show that upon melting, the behavior of typical mantle silicates changes from semi-conducting to semi-metallic. The electrical conductivity increases and the optical properties are substantially modified. Melting could thus be detected with high-precision reflectivity measurements during the short time scales of shock experiments. We estimate the electrical conductivity of mantle silicates to be of the order of 100 Ω cm, which implies that a magnetic dynamo process would develop in the magma oceans of Super-Earths if their convective velocities have typical values of 1 mm/s or higher. We predict exoplanets with rotation periods longer than 2 days to have multipolar magnetic fields.

Electrical conductivity and magnetic dynamos in magma oceans of Super-Earths.

With density functional molecular dynamics simulations, we computed the phase diagram of MgO from 50 to 2000 GPa up to 20 000 K. Via thermodynamic integration (TDI), we derive the Gibbs free energies of the B1, B2, and liquid phases and determine their phase boundaries. With TDI and a pseudo-quasi-harmonic approach, we show that anharmonic effects are important and stabilize the B1 phase in particular. As a result, the B1-B2 transition boundary in the pressure-temperature plane exhibits a steep slope. We predict the B1-B2-liquid triple point to occur at approximately T=10000  K and P=370  GPa, which is higher in pressure than was inferred with quasiharmonic methods alone. We predict the principal shock Hugoniot curve to enter the B2 phase stability domain but only over a very small range of parameters. This may render it difficult to observe this phase with shock experiments because of kinetic effects.

Anharmonicity and Phase Diagram of Magnesium Oxide in the Megabar Regime.

The ab initio (ai) Gibbs ensemble (GE) Monte Carlo (MC) method coupled with Kohn-Sham density functional theory is successful in predicting the liquid-vapour equilibrium of insulating systems. Here we show that the aiGEMC method can be used to study also metallic systems, where the excited electronic states play an important role and cannot be neglected. For this we include the electronic free energy in the formulation of the effective energy of the system to be used in the acceptance criteria for the MC moves. The application of this aiGEMC method to sodium yields a good agreement with available experimental data on the liquid-vapour equilibrium densities. We predict a critical point for sodium at 2338 ± 108 K and 0.24 ± 0.03 g cm-3. The liquid structure stemming from aiGEMC simulations is very similar to the one from ab initio molecular dynamics. Since this method can determine phase transition without computing the Gibbs free energy, it may offer a new possibility to study other materials with a reasonable computational cost.

Francois Soubiran

CEA, DAM, DIF

Analyzing Melts and Fluids from Ab Initio Molecular Dynamics Simulations with the UMD Package