Magnetic order in the computational 2D materials database (C2DB) from high throughput spin spiral calculations

TL;DR

This study systematically investigates magnetic orders in 192 2D materials from the C2DB using spin spiral calculations, revealing diverse magnetic ground states and emphasizing the importance of non-collinear order in emergent properties.

Contribution

It introduces a comprehensive workflow combining spin spiral calculations and spin-orbit coupling to determine magnetic ground states in 2D materials, including chiral spin spirals.

Findings

58 ferromagnets identified

21 collinear antiferromagnets identified

85 non-collinear ground states found, including 15 chiral spin spirals

Abstract

We report a detailed investigation of the magnetic order in 192 stable magnetic two-dimensional materials from the Computational 2D Materials Database having one magnetic atom in the unit cell. The calculations are based on a systematic workflow that employs spin spiral calculations and yields the magnetic order in terms of a two-dimensional ordering vector $\mathbf{Q}$. We then include spin-orbit coupling to extract the easy and hard axes for collinear structures and the orientation of spiral planes in non-collinear structures. Finally, for all predicted ferromagnets we compute the Dzyaloshinskii-Moriya interactions and determine whether or not these are strong enough to overcome the magnetic anisotropy and stabilise a chiral spin spiral ground state. These steps completely determines the ground state order within the spiralling ansatz. We find 58 ferromagnets, 21 collinear anti-ferromagnets, and 85 non-collinear ground states of which 15 are chiral spin spirals driven by Dzyaloshinskii-Moriya interactions. The results show that non-collinear order is in fact as common as collinear order in these materials and emphasise the need for detailed investigation of the magnetic ground state when reporting magnetic properties of new materials. Furthermore, non-collinear order typically breaks symmetries inherent to the lattice and may give rise to emergent properties such as multiferroicity, magnetoelectricity or second order optical effects that would be predicted as absent based on a collinear assumption.