Prediction of single-atom-thick transition metal nitride CrN$_4$ with a square-planar network and high-temperature ferromagnetism (2203.05361v2)

Abstract: Single-atom-thick two-dimensional materials such as graphene usually have a hexagonal lattice while the square-planar lattice is uncommon in the family of two-dimensional materials. Here, we demonstrate that single-atom-thick transition metal nitride CrN$_4$ monolayer is a stable free-standing layer with a square-planar network. The stability of square-planar geometry is ascribed to the combination of N=N double bond, Cr-N coordination bond, and $\pi$-d conjugation, in which the double $\pi$-d conjugation is rarely reported in previous studies. This mechanism is entirely different from that of the reported two-dimensional materials, leading to lower formation energy and more robust stability compared to the synthesized g-C$_3$N$_4$ monolayer. On the other hand, CrN$_4$ layer has a ferromagnetic ground state, in which the ferromagnetic coupling between two Cr atoms is mediated by electrons of the half-filled large $\pi$ orbitals from $\pi$-d conjugation. The high-temperature ferromagnetism in CrN$_4$ monolayer is confirmed by solving the Heisenberg model with Monte Carlo method.