First-principles study of ground state properties of zirconium dihydride

TL;DR

This study uses density functional theory to analyze the structural, mechanical, electronic, and thermodynamic properties of zirconium dihydride's phases, revealing stability conditions and bonding characteristics.

Contribution

It provides a comprehensive first-principles analysis of ZrH₂ phases, identifying stable structures and elucidating bonding and stability features not previously detailed.

Findings

The stable fct phase has c/a=0.885, matching experiments.

The fcc phase and fct with c/a=1.111 are mechanically unstable.

The bonds exhibit weak covalent and ionic features, with about 1.5 electrons transferred.

Abstract

Structural, mechanical, electronic, and thermodynamic properties of fluorite and tetragonal phases of ZrH$_{2}$ are systematically studied by employing the density functional theory within generalized gradient approximation. The existence of the bistable structure for ZrH$_{2}$ is mainly due to the tetragonal distortions. And our calculated lattice constants for the stable face-centered tetragonal (fct) phase with \emph{c/a}=0.885 are consistent well with experiments. Through calculating elastic constants, the mechanically unstable characters of face-centered cubic (fcc) phase and fct structure with \emph{c/a}=1.111 are predicted. As for fct0.885 structure, our calculated elastic constants explicitly indicate that it is mechanically stable. Elastic moduli, Poisson's ratio, and Debye temperature are derived from elastic constants. After analyzing total and partial densities of states and valence electron charge distribution, we conclude that the Zr$-$H bonds in ZrH$_{2}$ exhibit weak covalent feature. But the ionic property is evident with about 1.5 electrons transferring from each Zr atom to H. Phonon spectrum results indicate that fct0.885 and fct1.111 structures are dynamically stable, while the fcc structure is unstable.