Intrinsic i -Wave Altermagnetism in 2D Graphene Superlattices

Altermagnets feature unconventional magnetism due to their momentum-dependent spin splitting purely driven by magnetic order, for which a variety of transition-metal-based $d$ -wave altermagnets have been proposed. However, carbon-based altermagnets remain largely unexplored, even though magnetism of graphene nanostructures has been widely demonstrated. Here, through a comprehensive symmetry analysis, we establish a symmetry-guided design principle for realizing higher-order $i$ -wave altermagnetism in graphene antidot superlattices and demonstrate its emergence in both monolayer and bilayer graphene, particularly in the Bernal-stacked bilayer. By combining atomistic tight binding models and first principles methods, we show the appearance of an interaction-induced $i$ -wave altermagnetic splitting, originating from the intrinsic magnetic instability of 2D graphene antidot superlattices. Our work establishes a strategy to engineer $i$ -wave altermagnetism in a graphene platform, extending the materials landscape beyond conventional $d$ -wave altermagnets and putting forward a carbon-based platform for higher-order altermagnetic spintronics.