Towards accurate orbital-free simulations: A generalized gradient approximation for the noninteracting free energy density functional

Luo, K.; Karasiev, V. V.; Trickey, S. B.

doi:10.1103/PhysRevB.101.075116

Title: Towards accurate orbital-free simulations: A generalized gradient approximation for the noninteracting free energy density functional

Journal Article · 13 February 2020 · Physical Review B

DOI: https://doi.org/10.1103/PhysRevB.101.075116 · OSTI ID:1602230

^[1]; Karasiev, V. V. ^[2];

^[3]

Carnegie Inst. of Washington, Washington, DC (United States); Laboratory for Laser Energetics, University of Rochester
Univ. of Rochester, NY (United States)
Univ. of Florida, Gainesville, FL (United States)

For orbital-free ab initio molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free energy. This is achieved by systematic finite-temperature extension of our recent LKT ground state non-interacting kinetic energy GGA functional (Phys. Rev. B 98, 041111(R) (2018)). We test the performance of the new functional first via static lattice calculations on crystalline aluminum and silicon. Then we compare deuterium equation of state results against both path-integral Monte Carlo and conventional (orbital-dependent) Kohn-Sham results. The new functional, denoted LKTF, outperforms the previous best semi-local free energy functional, VT84F (Phys. Rev. B 88, 161108(R) (2013)), and provides modestly faster simulations. Finally, we discuss subtleties of identification of kinetic and entropic contributions to non-interacting free-energy functionals obtained by extension from ground state orbital-free kinetic energy functionals.

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Research Organization:: Univ. of Rochester, NY (United States); Univ. of Florida, Gainesville, FL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003856; SC0002139; NA0001944

OSTI ID:: 1602230

Report Number(s):: 2020-42; 1549; 2020-42, 2506, 1549

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 7 Vol. 101; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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