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A comparative study using state-of-the-art electronic structure theories on solid hydrogen phases under high pressures

Published version
Peer-reviewed

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Authors

Liao, K 
Li, XZ 
Grüneis, A 

Abstract

jats:titleAbstract</jats:title>jats:pIdentifying the atomic structure and properties of solid hydrogen under high pressures is a long-standing problem of high-pressure physics with far-reaching significance in planetary and materials science. Determining the pressure-temperature phase diagram of hydrogen is challenging for experiment and theory due to the extreme conditions and the required accuracy in the quantum mechanical treatment of the constituent electrons and nuclei, respectively. Here, we demonstrate explicitly that coupled cluster theory can serve as a computationally efficient theoretical tool to predict solid hydrogen phases with high accuracy. We present a first principles study of solid hydrogen phases at pressures ranging from 100 to 450 GPa. The computed static lattice enthalpies are compared to state-of-the-art diffusion Monte Carlo results and density functional theory calculations. Our coupled cluster theory results for the most stable phases including C2/c-24 and P2jats:inline-formulajats:alternativesjats:tex-math$${}_{1}$$</jats:tex-math><mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML">mml:msub<mml:mrow />mml:mrowmml:mn1</mml:mn></mml:mrow></mml:msub></mml:math></jats:alternatives></jats:inline-formula>/c-24 are in good agreement with those obtained using diffusion Monte Carlo, with the exception of Cmca-4, which is predicted to be significantly less stable. We discuss the scope of the employed methods and how they can contribute as efficient and complementary theoretical tools to solve the long-standing puzzle of understanding solid hydrogen phases at high pressures.</jats:p>

Description

Funder: Max-Planck-Gesellschaft (Max Planck Society); doi: https://doi.org/10.13039/501100004189


Funder: University of Cambridge; doi: https://doi.org/10.13039/501100000735

Keywords

51 Physical Sciences, 34 Chemical Sciences, 3406 Physical Chemistry

Journal Title

npj Computational Materials

Conference Name

Journal ISSN

2057-3960
2057-3960

Volume Title

5

Publisher

Springer Science and Business Media LLC