Nuclear quantum effects induce metallization of dense solid molecular hydrogen
File(s)1710.09703v1.pdf (183.73 KB)
Accepted version
Author(s)
Azadi, S
Singh, R
Kühne, TD
Type
Journal Article
Abstract
We present an accurate computational study of the electronic structure and lattice dynamics of solid molecular hydrogen at high pressure. The band-gap energies of the C2/c, Pc, and P63/m structures at pressures of 250, 300, and 350 GPa are calculated using the diffusion quantum Monte Carlo (DMC) method. The atomic configurations are obtained from ab initio path-integral molecular dynamics (PIMD) simulations at 300 K and 300 GPa to investigate the impact of zero-point energy and temperature-induced motion of the protons including anharmonic effects. We find that finite temperature and nuclear quantum effects reduce the band-gaps substantially, leading to metallization of the C2/c and Pc phases via band overlap; the effect on the band-gap of the P63/m structure is less pronounced. Our combined DMC-PIMD simulations predict that there are no excitonic or quasiparticle energy gaps for the C2/c and Pc phases at 300 GPa and 300 K. Our results also indicate a strong correlation between the band-gap energy and vibron modes. This strong coupling induces a band-gap reduction of more than 2.46 eV in high-pressure solid molecular hydrogen. Comparing our DMC-PIMD with experimental results available, we conclude that none of the structures proposed is a good candidate for phases III and IV of solid hydrogen.
Date Issued
2018-02-15
Date Acceptance
2017-10-23
Citation
Journal of Computational Chemistry, 2018, 39 (5), pp.262-268
ISSN
0192-8651
Publisher
Wiley
Start Page
262
End Page
268
Journal / Book Title
Journal of Computational Chemistry
Volume
39
Issue
5
Copyright Statement
© 2018 Owner. This is the accepted version of the following article: Azadi, S., Singh, R., Kühne, T. D.. J. Comput. Chem. 2018, 39, 262– 268. DOI: 10.1002/jcc.25104, which has been published in final form at https://doi.org/10.1002/jcc.25104.
Subjects
cond-mat.mtrl-sci
cond-mat.mtrl-sci
physics.chem-ph
physics.comp-ph
0306 Physical Chemistry (incl. Structural)
0307 Theoretical and Computational Chemistry
Chemical Physics
Publication Status
Published
Date Publish Online
2017-11-08