Thin film synthesis, structural analysis, and magnetic properties of novel ternary transition metal nitride MnCoN2

Recent high-throughput computational searches have predicted many novel ternary nitride compounds providing new opportunities for materials discovery in underexplored phase spaces. Nevertheless, there are hardly any predictions and/or syntheses that incorporate only transition metals into new ternary nitrides. Here, we report on the synthesis, structure, and properties of MnCoN2, a new ternary nitride material comprising only transition metals and N. We find that crystalline MnCoN2 can be stabilized over its competing binaries, and over a tendency of this system to become amorphous, by controlling growth temperature within a narrow window slightly above ambient condition. We find that single-phase MnCoN2 thin films form in a cation-disordered rocksalt crystal structure. X-ray photoelectron spectroscopy analysis suggests that MnCoN2 is sensitive to oxygen through various oxides and hydroxides binding to cobalt on the surface. X-ray absorption spectroscopy is used to verify that Mn3+ and Co3+ cations exist in an octahedrally coordinated environment, which is distinct from a combination of CoN and MnN binaries and in agreement with the rocksalt-based crystal structure prediction. Magnetic measurements suggest that MnCoN2 has a canted antiferromagnetic ground state below 10 K. We extract a Weiss temperature of theta = - 49 . 7 K, highlighting the antiferromagnetic correlations in MnCoN2.