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Title: Benchmarking exchange-correlation functionals for hydrogen at high pressures using quantum Monte Carlo

Journal Article · · Physical Review. B, Condensed Matter and Materials Physics
 [1];  [2];  [1];  [3];  [1];  [2]
  1. Univ. of Illinois, Urbana, IL (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Istituto Nazionale di Fisica Nucleare (INFN), L'aquila (Italy). Lab. Nazionali del Gran Sasso (INFN-LNGS)
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The ab initio phase diagram of dense hydrogen is very sensitive to errors in the treatment of electronic correlation. Recently, it has been shown that the choice of the density functional has a large effect on the predicted location of both the liquid-liquid phase transition and the solid insulator-to-metal transition in dense hydrogen. To identify the most accurate functional for dense hydrogen applications, we systematically benchmark some of the most commonly used functionals using quantum Monte Carlo. By considering several measures of functional accuracy, we conclude that the van der Waals and hybrid functionals significantly outperform local density approximation and Perdew-Burke-Ernzerhof. We support these conclusions by analyzing the impact of functional choice on structural optimization in the molecular solid, and on the location of the liquid-liquid phase transition.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
AC52-07NA27344; NA0001789
OSTI ID:
1136141
Journal Information:
Physical Review. B, Condensed Matter and Materials Physics, Vol. 89, Issue 18; ISSN 1098-0121: PRBMDO
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English

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