Abstract

The emergence of all-d-metal Heusler alloys has opened up new pathways for the design of advanced functional materials. In this work, we employ first-principles electronic structure calculations to systematically investigate the electronic and magnetic properties of 27 all-d-metal Heusler compounds following the stoichiometry X2YZ, where X= Co, Rh, Ir, Y= V, Cr, Mn, and Z= Ti, Zr, Hf. Electronic band structure calculations show a consistent minority-spin pseudogap across the series, the width and characteristics of which are strongly dependent on the d-band broadening introduced by 4d (Rh, Zr) and 5d (Ir, Hf) transition metals. Magnetically, these materials largely follow the Mt=Zt−24 Slater–Pauling rule, driven by exactly 12 occupied minority-spin bands at the Γ point. Notably, substituting Co with Rh or Ir significantly redistributes the magnetization, drastically reducing the X-site spin magnetic moment while amplifying the spin magnetic moments on the Y-site atoms. This study provides a comprehensive understanding of the interplay between structural symmetry, orbital hybridization, and magnetism in all-d-metal Heuslers, highlighting their promise for future spintronic applications.

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