Emergent frustrated magnetism in strain-patterned graphene

Abstract

Geometrically frustrated magnetism conventionally arises from pre-existing magnetic moments on lattices whose geometry prevents their interactions from being simultaneously satisfied, giving rise to highly degenerate states and rich collective behavior. Creating such frustration in an intrinsically non-magnetic material presents a fundamentally different challenge, requiring both the magnetism and the competing interactions to emerge from correlated electrons. Here we show that this can be realized in graphene through lithographically programmable strain engineering. Patterning strain and the associated pseudo-magnetic field (PMF) into superlattices creates a correlated electronic system with flat bands and strong interactions. Transport measurements reveal interaction-driven insulating behavior, anisotropic magnetic hysteresis, and slow relaxation dynamics reminiscent of spin freezing, qualitatively captured by Monte Carlo simulations of competing magnetic moments on the PMF-defined ruby superlattice. Cryogenic magnetic force microscopy further reveals magnetic textures associated with the PMF landscape. These observations demonstrate frustrated magnetism emerging from correlated electrons in otherwise non-magnetic graphene. Our results establish lithographic strain engineering as a general and scalable route to flat bands and correlated states in van der Waals materials, providing a versatile platform for programmable quantum matter.