Intrinsic ferromagnetism and restrictive thermodynamic stability in MA${}_2$N${}_4$ and Janus VSiGeN${}_4$ monolayers

Abstract

The seminal experimental discovery of the remarkably stable MoSi${}_2$N${}_4$ monolayer has led to a handful of predicted magnetic two-dimensional (2D) materials in the MA${}_2$Z${}_4$ family (M = transition metals, A = Si, Ge, and Z = N, P, As). These magnetic monolayers were predicted to be dynamically stable, but none of them has been synthesized to date. In this Research Letter, from first-principles thermodynamic stability analysis, we demonstrate that only the nitrides are thermodynamically stable and this occurs under N-rich conditions. Based on this finding, we propose two ferromagnetic, semiconducting Janus monolayers in the family: VSiGeN${}_4$ and VSiSnN${}_4$. They are both dynamically and thermally stable, but only the former is thermodynamically stable. Intriguingly, Janus VSiGeN${}_4$ and VSiSnN${}_4$ monolayers show weak in-plane anisotropy compared with the VSi${}_2$N${}_4$ monolayer. These two emerging Janus magnetic semiconductors offer opportunities for studying 2D magnetism and spin control for spintronics applications.

Main article - 7 pages, 5 figures. Supplemental Material added