Structural, mechanical and electronic properties and hardness of ionic vanadium dihydrides under pressure from first-principles computations

Abstract Based on a combination of the CALYPSO method for crystal structure prediction and first-principles calculations, we explore the crystal structures of VH 2 under the pressure range of 0−300 GPa. The cubic Fm- 3 m phase with regular VH 8 cubes is predicted to transform into orthorhombic Pnma structure with fascinating distorted VH 9 tetrakaidecahedrons at 47.36 GPa. Both the Fm- 3 m phase at 0 GPa and the Pnma phase at 100 GPa are mechanically and dynamically stable, as verified with the calculations of elastic constants and phonon dispersions, respectively. Moreover, the calculated electronic band structure and density of states indicate both stable phases are metallic. Remarkably, the analyses of the Poisson’s ratio, electron localization function (ELF) and Bader charge substantiate that both stable phases are ionic crystals on account of effective charges transferring from V atom to H. On the basis of the microscopic hardness model, the Fm -3 m and Pnma crystals of VH 2 are potentially incompressible and hard materials with the hardness values of 17.83 and 17.68 GPa, respectively.