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Title: Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures

Abstract

Establishing the phase diagram of hydrogen is a major challenge for experimental and theoretical physics. Experiment alone cannot establish the atomic structure of solid hydrogen at high pressure, because hydrogen scatters X-rays only weakly. Instead, our understanding of the atomic structure is largely based on density functional theory (DFT). By comparing Raman spectra for low-energy structures found in DFT searches with experimental spectra, candidate atomic structures have been identified for each experimentally observed phase. Unfortunately, DFT predicts a metallic structure to be energetically favoured at a broad range of pressures up to 400 GPa, where it is known experimentally that hydrogen is non-metallic. Here we show that more advanced theoretical methods (diffusion quantum Monte Carlo calculations) find the metallic structure to be uncompetitive, and predict a phase diagram in reasonable agreement with experiment. This greatly strengthens the claim that the candidate atomic structures accurately model the experimentally observed phases.

Authors:
 [1];  [2];  [2];  [2];  [3];  [2]
  1. Lancaster Univ. (United Kingdom)
  2. Univ. of Cambridge (United Kingdom). Cavendish Lab.
  3. Univ. College London, Bloomsbury (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1565326
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Drummond, N. D., Monserrat, Bartomeu, Lloyd-Williams, Jonathan H., Ríos, P. López, Pickard, Chris J., and Needs, R. J. Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures. United States: N. p., 2015. Web. doi:10.1038/ncomms8794.
Drummond, N. D., Monserrat, Bartomeu, Lloyd-Williams, Jonathan H., Ríos, P. López, Pickard, Chris J., & Needs, R. J. Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures. United States. doi:10.1038/ncomms8794.
Drummond, N. D., Monserrat, Bartomeu, Lloyd-Williams, Jonathan H., Ríos, P. López, Pickard, Chris J., and Needs, R. J. Tue . "Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures". United States. doi:10.1038/ncomms8794. https://www.osti.gov/servlets/purl/1565326.
@article{osti_1565326,
title = {Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures},
author = {Drummond, N. D. and Monserrat, Bartomeu and Lloyd-Williams, Jonathan H. and Ríos, P. López and Pickard, Chris J. and Needs, R. J.},
abstractNote = {Establishing the phase diagram of hydrogen is a major challenge for experimental and theoretical physics. Experiment alone cannot establish the atomic structure of solid hydrogen at high pressure, because hydrogen scatters X-rays only weakly. Instead, our understanding of the atomic structure is largely based on density functional theory (DFT). By comparing Raman spectra for low-energy structures found in DFT searches with experimental spectra, candidate atomic structures have been identified for each experimentally observed phase. Unfortunately, DFT predicts a metallic structure to be energetically favoured at a broad range of pressures up to 400 GPa, where it is known experimentally that hydrogen is non-metallic. Here we show that more advanced theoretical methods (diffusion quantum Monte Carlo calculations) find the metallic structure to be uncompetitive, and predict a phase diagram in reasonable agreement with experiment. This greatly strengthens the claim that the candidate atomic structures accurately model the experimentally observed phases.},
doi = {10.1038/ncomms8794},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {2015},
month = {7}
}

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