Ab initio Green-Kubo Approach for the Thermal Conductivity of Solids

Understand

We herein present a first-principles formulation of the Green-Kubo method that allows the accurate assessment of the non-radiative thermal conductivity of solid semiconductors and insulators in equilibrium ab initio molecular dynamics calculations.

• Using the virial for the nuclei, we propose a unique ab initio definition of the heat flux.
• Accurate size- and time convergence are achieved within moderate computational effort by a robust, asymptotically exact extrapolation scheme.
• We demonstrate the capabilities of the technique by investigating the thermal conductivity of extreme high and low heat conducting materials, namely diamond Si and tetragonal ZrO$_2$.