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, resulting insulator-to-metal transition in the interfacial CrSBr layer. 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.

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, resulting insulator-to-metal transition in the interfacial CrSBr layer. 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.

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, resulting insulator-to-metal transition in the interfacial CrSBr layer. 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.

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, resulting insulator-to-metal transition in the interfacial CrSBr layer. 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.