Symmetry-guided prediction of magnetic-ordered ground states

TL;DR

This paper introduces a symmetry-guided computational framework that efficiently predicts magnetic ground states in materials, reducing the need for experimental data and enabling large-scale exploration of magnetic configurations.

Contribution

It presents a novel hierarchical symmetry-breaking approach combining spin space group formalism with magnetic space groups for accurate magnetic state prediction.

Findings

Few dozen first-principles calculations suffice to identify ground states.

Successfully applied to various 2D and 3D magnets.

Reveals potential for discovering exotic magnetic properties.

Abstract

Given the scarcity of experimentally confirmed magnetic structures, the reliable prediction of magnetic ground states is crucial; however, it remains a long-sought challenge because of the complex magnetic potential energy landscape. Here, we propose a symmetry-guided framework that systematically generates realistic magnetic configurations without requiring any experimental input or prior assumptions such as propagation vectors. Within a hierarchical symmetry-breaking scenario, we integrate the recently developed spin space group formalism and conventional magnetic space group description, respectively capturing symmetry breaking induced by magnetic ordering and spin-orbit coupling. Furthermore, we perform both nonrelativistic and relativistic first-principles calculations to establish the energy ordering of selected magnetic configurations. Exemplified by three recently reported three-dimensional unconventional magnets MnTe, Mn3Sn, and CoNb3S6 and two two-dimensional magnets CrTe2 and NiI2, we demonstrate that only a few dozen first-principles calculations are sufficient to identify the ground-state magnetic configuration along with several low-energy metastable states, which may exhibit exotic physical properties such as p-wave magnetism. Our work provides a general and efficient strategy for large-scale prediction of three-dimensional and two-dimensional magnetic configurations and offers insight into the microscopic origins of magnetic interactions across diverse material systems.