Stacking theory for bilayer two-dimensional magnets

TL;DR

This paper develops a comprehensive symmetry-based stacking theory for two-dimensional magnets, enabling the design of unconventional magnetic states and validated by first-principles calculations.

Contribution

It introduces spin layer groups and a general stacking theory applicable to various magnetic systems, expanding the understanding of 2D magnetism.

Findings

Designed 2D fully compensated ferrimagnetism using the theory

Validated the theory with first-principles calculations on CrF3

Provided a symmetry-guided platform for discovering new magnetic states

Abstract

Two-dimensional unconventional magnetism has recently attracted growing interest due to its intriguing physical properties and promising applications in spintronics. However, existing studies on stacking-induced unconventional magnetism mainly focus on specific materials and stacking configurations. Here, we develop a general symmetry-based stacking theory for two-dimensional magnets. We first introduce spin layer groups as the fundamental symmetry framework, providing the essential magnetic symmetry information for the stacking theory. Based on this framework, we construct the complete set of 448 collinear spin layer groups for describing two-dimensional collinear magnets. Subsequently, we develop a general magnetic stacking theory applicable to arbitrary magnetic systems and derive its general solutions. Using CrF$_3$ as an illustrative example, we show how this theory enables designs of two-dimensional unconventional magnetism, as validated by first-principles calculations. We realize two-dimensional fully compensated ferrimagnetism through our stacking theory. Our work provides a general symmetry-guided platform for discovering and designing stacking-induced unconventional magnetism.