Electronic and Vibrational Properties of Fe₂NiAl and Co₂NiAl Full Heusler Alloys: A First-Principles Comparison

We provide a comparative first-principles investigation of the structural, electronic, vibrational, and thermodynamic properties of the full Heusler compounds, cubic Fe ₂ NiAl, and tetragonally distorted Co ₂ NiAl. In both cases, we find the inverse Heusler structure to be in close competition with a layered arrangement of the elements, which breaks cubic symmetry and is accompanied by significant absolute values for the magnetocrystalline anisotropy energy. While for Fe ₂ NiAl the layered arrangement is predicted as a new ground state, we show evidence that it might become dynamically stable around room temperatures also for Co ₂ NiAl. We identify in both systems subtle differences in the electronic and vibrational density of states between the different structures, which might be related to their particular stability.