Proximity-Induced Charge Transfer, Strain, and Possible Magnetic Exchange in Graphene/CrSBr Heterostructure

Abstract

Stacking van der Waals materials provides a powerful route to engineer emergent electronic and magnetic behaviors through proximity-driven interactions. The graphene/CrSBr heterostructure has emerged as a compelling platform in this frontier, exhibiting exotic macroscopic responses (including uniaxial surface-plasmon-polariton propagation and an unconventional quantum Hall effect) indicative of strong interfacial electronic and magnetic coupling. However, a microscopic electronic landscape governing these phenomena has remained elusive. Here, we provide a comprehensive spectroscopic characterization of the graphene/CrSBr interface using a combination of angle-resolved photoemission spectroscopy (ARPES), low-energy electron microscopy (LEEM), and density functional theory. We resolve a massive redistribution of interfacial charge that concurrently hole-dopes graphene and populates the quasi-one-dimensional spin-polarized conduction band of CrSBr, leading to interfacial metallization. Furthermore, electronic structure of CrSBr exhibits strong momentum-dependent renormalization distinct from conventional charge doping, and theoretical modeling supported by Raman spectroscopy points to additional interfacial compressive strain. In addition, ARPES reveals a splitting-like feature in the graphene Dirac cone consistent with spin degeneracy lifting, providing possible evidence of magnetic proximity coupling. These findings provide crucial microscopic insight into the system’s optical and transport responses and establish graphene/CrSBr as a versatile platform for charge-transfer control, strain-driven band engineering, magnetic-proximity coupling, and directionally confined excitations for next-generation spintronic and nanophotonic devices.