Two-temperature pair potentials and phonon spectra for simple metals in the warm dense matter regime

TL;DR

This paper develops two-temperature ion-ion pair potentials for simple metals in the warm dense matter regime, enabling the study of non-equilibrium states relevant to ultra-fast laser interactions.

Contribution

It introduces a method to construct two-temperature pair potentials using linear-response theory and finite-temperature DFT, applicable to non-equilibrium warm dense matter conditions.

Findings

Equilibrium phonon spectra match experimental data well.

The method provides credible non-equilibrium phonon dispersion relations.

Facilitates study of thermophysical properties in WDM regimes.

Abstract

We develop ion-ion pair potentials for Al, Na and K for densities and temperatures relevant to the warm-dense-matter (WDM) regime. Furthermore, we emphasize non-equilibrium states where the ion temperature $T_i$ differs from the electron temperature $T_e$. This work focuses mainly on ultra-fast laser-metal interactions where the energy of the laser is almost exclusively transferred to the electron sub-system over femtosecond time scales. This results in a two-temperature system with $T_e>T_i$ and with the ions still at the initial room temperature $T_i=T_r$. First-principles calculations, such as density functional theory (DFT) or quantum Monte Carlo, are as yet not fully feasible for WDM conditions due to lack of finite-$T$ features, e.g. pseudopotentials, and extensive CPU time requirements. Simpler methods are needed to study these highly complex systems. We propose to use two-temperature pair potentials $U_{ii}(r, T_i,T_e)$ constructed from linear-response theory using the non-linear electron density $n(\mathbf{r})$ obtained from finite-$T$ DFT with a single ion immersed in the appropriate electron fluid. We compute equilibrium phonon spectra at $T_r$ which are found to be in very good agreement with experiments. This gives credibility to our non-equilibrium phonon dispersion relations which are important in determining thermophysical properties, stability, energy-relaxation mechanisms and transport coefficients.