Dynamical stability of the lanthanum dihydride under high pressure: A density functional lattice dynamics approach

We report first-principles pseudopotential method and density functional linear response theory calculations of the structural, electronic, vibrational and thermodynamical properties of LaH2 in fluoride phase at zero and high pressures. The electronic band structure and first time calculated pressure dependent lattice dynamic properties show that the LaH2 is metallic in nature at zero pressure. The pressure dependent electronic band structure calculations show that the bands are closing and reopening with pressure. The phonon mode softens at 11 GPa indicating an instability in lattice structure and pressure induced transverse acoustic phonon mode driven displacive type structural phase transition. The LaH2 also shows weak superconductivity at zero pressure. The valence charge electron density at 46 GPa shows a cage type charge contour and a space where hydrogen can be absorbed and filled easily. There is a considerable charge accumulation in the bonding region of La and H atoms, which strengthens covalent character of LaH2, and henceforth this material can be one of the best materials for hydrogen storage application at high pressures.

► The electronic and vibrational properties of LaH2 at higher pressures are calculated. ► At ambient condition LaH2 shows weak superconducting and metallic nature. ► The PDC at 11 GPa shows an instability and results in structural phase transition. ► The valence charge electron density at 46 GPa shows a cage type charge contour.