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Title: Benchmarking density functionals for hydrogen-helium mixtures with quantum Monte Carlo: Energetics, pressures, and forces

Journal Article · · Physical Review B
 [1];  [2];  [3];  [4]
  1. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Physics; Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Univ. of Grenoble (France)
  3. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Physics
  4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
+ Show Author Affiliations

Though density-functional-theory-based first-principles methods have the potential to provide the accuracy and computational efficiency required for this task, recent benchmarking in hydrogen has shown that achieving this accuracy requires a judicious choice of functional, and a quantification of the errors introduced. In this work, we present a quantum Monte Carlo (QMC) -based benchmarking study of a wide range of density functionals for use in hydrogen-helium mixtures at thermodynamic conditions relevant for Jovian planets. Not only do we continue our program of benchmarking energetics and pressures, but we deploy QMC-based force estimators and use them to gain insight into how well the local liquid structure is captured by different density functionals. We find that TPSS, BLYP, and vdW-DF are the most accurate functionals by most metrics, and that the enthalpy, energy, and pressure errors are very well behaved as a function of helium concentration. Beyond this, we highlight and analyze the major error trends and relative differences exhibited by the major classes of functionals, and we estimate the magnitudes of these effects when possible

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC05-00OR22725; AC52-07NA27344; NA0001789; NA0002911
OSTI ID:
1325453
Alternate ID(s):
OSTI ID: 1235751; OSTI ID: 1241957; OSTI ID: 1358610
Report Number(s):
LLNL-JRNL-676457; PRBMDO; KC0202030; ERKCK03
Journal Information:
Physical Review B, Vol. 93, Issue 3; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 33 works
Citation information provided by
Web of Science

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Cited By (9)

Nuclear quantum effects induce metallization of dense solid molecular hydrogen journal November 2017
Extent of Fock-exchange mixing for a hybrid van der Waals density functional? journal May 2018
Quantum Monte Carlo assessment of density functionals for π -electron molecules: ethylene and bifuran journal August 2018
Theory of finite size effects for electronic quantum Monte Carlo calculations of liquids and solids journal July 2016
First-principles prediction of the softening of the silicon shock Hugoniot curve journal September 2016
Quantum molecular dynamics study on the proton exchange, ionic structures, and transport properties of warm dense hydrogen-deuterium mixtures journal June 2018
Nuclear Quantum Effects Induce Metallization of Dense Solid Molecular Hydrogen preprint January 2017
QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids text January 2018
Extent of Fock-exchange mixing for a hybrid van der Waals density functional? text January 2018

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