Scale-Bridging Thermodynamic and Kinetic Simulation (STKS)
Anharmonicity, mechanical instability, and thermodynamic properties of the Cr-Re σ-phase
M. Palumbo, S. G. Fries, A. Pasturel, D. Alfe.
The Journal of Chemical Physics, 140, 144502, (2014)
Using density-functional theory in combination with the direct force method and molecular dynamics we investigate the vibrational properties of a binary Cr-Re σ-phase. In the harmonic approximation, we have computed phonon dispersion curves and density of states, evidencing structural and chemical effects. We found that the σ-phase is mechanically unstable in some configurations, for example, when all crystallographic sites are occupied by Re atoms. By using a molecular-dynamics-based method, we have analysed the anharmonicity in the system and found negligible effects (∼0.5 kJ/mol) on the Helmholtz energy of the binary Cr-Re σ-phase up to 2000 K (∼0.8 Tm). Finally, we show that the vibrational contribution has significant consequences on the disordering of the σ-phase at high temperature.