Fundamental High-Pressure Calibration from All-Electron Quantum Monte Carlo Calculations

K. P. Esler, R. E. Cohen, B. Militzer, Jeongnim Kim, R. J. Needs, and M. D. Towler
Phys. Rev. Lett. 104, 185702 – Published 5 May 2010
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Abstract

We develop an all-electron quantum Monte Carlo (QMC) method for solids that does not rely on pseudopotentials, and use it to construct a primary ultra-high-pressure calibration based on the equation of state of cubic boron nitride. We compute the static contribution to the free energy with the QMC method and obtain the phonon contribution from density functional theory, yielding a high-accuracy calibration up to 900 GPa usable directly in experiment. We compute the anharmonic Raman frequency shift with QMC simulations as a function of pressure and temperature, allowing optical pressure calibration. In contrast to present experimental approaches, small systematic errors in the theoretical EOS do not increase with pressure, and no extrapolation is needed. This all-electron method is applicable to first-row solids, providing a new reference for ab initio calculations of solids and benchmarks for pseudopotential accuracy.

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  • Received 22 September 2009

DOI:https://doi.org/10.1103/PhysRevLett.104.185702

©2010 American Physical Society

Authors & Affiliations

K. P. Esler1,2,*, R. E. Cohen1, B. Militzer3, Jeongnim Kim2, R. J. Needs4, and M. D. Towler4

  • 1Geophysical Laboratory, Carnegie Institution of Washington, Washington, D.C. 20015, USA
  • 2NCSA, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA
  • 3Department of Earth and Planetary Science and of Astronomy, University of California Berkeley, Berkeley, California 94720, USA
  • 4TCM Group, Cavendish Laboratory, Cambridge CB3 0HE, United Kingdom

  • *esler@uiuc.edu

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Issue

Vol. 104, Iss. 18 — 7 May 2010

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