Azadi, S; Singh, R; Kühne, TD; (2018) Nuclear quantum effects induce metallization of dense solid molecular hydrogen. Journal of Computational Chemistry , 39 (5) pp. 262-268. 10.1002/jcc.25104.

Preview

Text 1710.09703v1.pdf - Accepted Version Download (188kB) | Preview

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/mstructures 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/mstructure 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. © 2017 Wiley Periodicals, Inc.

Download activity - last month

Export as XMLCSVJSON

Download activity - last 12 months

Export as XMLCSVJSON

Downloads by country - last 12 months

Export as JSONXMLCSV

Archive Staff Only

View Item