Ab initio Exchange-Correlation Free Energy of the Uniform Electron Gas at Warm Dense Matter Conditions

摘要

In a recent Letter [T. Dornheim et al., Phys. Rev. Lett. 117, 156403 (2016)], we presented the first quantum Monte Carlo (QMC) results for the warm dense electron gas in the thermodynamic limit. However, a complete parametrization of the exchange-correlation free energy with respect to density, temperature, and spin polarization remained out of reach due to the absence of (i) accurate QMC results below. theta = k(B)T/E-F = 0.5 and (ii) QMC results for spin polarizations different from the paramagnetic case. Here we overcome both remaining limitations. By closing the gap to the ground state and by performing extensive QMC simulations for different spin polarizations, we are able to obtain the first completely ab initio exchange-correlation free energy functional; the accuracy achieved is an unprecedented similar to 0.3%. This also allows us to quantify the accuracy and systematic errors of various previous approximate functionals.