Ab initio path integral Monte Carlo simulations of hydrogen snapshots at warm dense matter conditions

Abstract

We combine ab initio path integral Monte Carlo (PIMC) simulations with fixed ion configurations from density functional theory molecular dynamics (DFT-MD) simulations to solve the electronic problem for hydrogen under warm dense matter conditions [Böhme, Phys. Rev. Lett. 129, 066402 (2022)0031-900710.1103/PhysRevLett.129.066402]. The problem of path collapse due to the Coulomb attraction is avoided by utilizing the pair approximation, which is compared against the simpler Kelbg pair potential. We find very favorable convergence behavior towards the former. Since we do not impose any nodal restrictions, our PIMC simulations are afflicted with the notorious fermion sign problem, which we analyze in detail. While computationally demanding, our results constitute an exact benchmark for other methods and approximations within DFT. Our setup gives us the unique capability to study important properties of warm dense hydrogen such as the electronic static density response and exchange-correlation kernel without any model assumptions, which will be very valuable for a variety of applications such as the interpretation of experiments and the development of new XC functionals.