Settling the matter of the role of vibrations in the stability of high-entropy carbides
Marco Esters, Corey Oses, David Hicks, Michael J. Mehl, Michal Jahnátek, Mohammad Delower Hossain, Jon‐Paul Maria, Donald W. Brenner, Cormac Toher, Stefano Curtarolo
Abstract
High-entropy ceramics are attracting significant interest due to their exceptional chemical stability and physical properties. While configurational entropy descriptors have been successfully implemented to predict their formation and even to discover new materials, the contribution of vibrations to their stability has been contentious. This work unravels the issue by computationally integrating disorder parameterization, phonon modeling, and thermodynamic characterization. Three recently synthesized carbides are used as a testbed: (HfNbTaTiV)C, (HfNbTaTiW)C, and (HfNbTaTiZr)C. It is found that vibrational contributions should not be neglected when precursors or decomposition products have different nearest-neighbor environments from the high-entropy carbide.