Large spin gaps in the half-metals M N4 (M =Mn, Fe, Co) with N2 dimers

We predict that cubic MN4 (M=Mn, Fe, Co) are all half-metals with the largest spin gap up to ∼5 eV. They possess robust ferromagnetic ground states with the highest Curie temperature up to ∼103 K. Our calculations indicate these compounds are energetically favored, dynamically and mechanically stable. It is proposed that self-doping of these 3d transition metals occurs in MN4 due to the reduction in electronegativity of N2 dimers. This model can well explain the calculated integer magnetic moments, large spin gaps of MN4, and semiconducting behavior for NiN4 as well. Our results highlight the difference in electronegativity between transition metal ions and nonmetal entities in forming half-metals and the role of N2 dimer in enlarging the spin gaps for nitride half-metals.