Nonlocal free-energy density functional for warm dense matter

TL;DR

This paper introduces a new nonlocal free energy functional, XWMF, for finite-temperature orbital-free density functional theory, significantly improving accuracy, stability, and computational efficiency in simulating warm dense matter.

Contribution

A novel nonlocal free energy functional, XWMF, was derived using line integrals, enhancing FT-OFDFT's applicability to warm dense matter simulations.

Findings

XWMF achieves high accuracy in benchmark systems.

XWMF offers low computational cost for large-scale simulations.

FT-OFDFT with XWMF demonstrates excellent numerical stability.

Abstract

Finite-temperature orbital-free density functional theory (FT-OFDFT) holds significant promise for simulating warm dense matter due to its favorable scaling with both system size and temperature. However, the lack of the numerically accurate and transferable noninteracting free energy functionals results in a limit on the application of FT-OFDFT for warm dense matter simulations. Here, a nonlocal free energy functional, named XWMF, was derived by line integrals for FT-OFDFT simulations. Particularly, a designed integral path, wherein the electronic density varies from uniform to inhomogeneous, was employed to accurately describe deviations in response behavior from the uniform electron gas. The XWMF has been benchmarked by a range of warm dense matter systems including the Si, Al, H, He, and H-He mixture. The simulated results demonstrate that FT-OFDFT within XWMF achieves remarkable performance for accuracy and numerical stability. It is worth noting that XWMF exhibits a low computational cost for large-scale ab~initio simulations, offering exciting opportunities for the realistic simulations of warm dense matter systems covering a broad range of temperatures and pressures.