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The strong spin filtering effect can be produced by C-Ni atomic orbital hybridization in lattice-matched graphene/Ni (111) heterostructures, which provides an ideal platform to improve the tunnel magnetoresistance (TMR) of magnetic tunnel junctions (MTJs). However, large-area, high-quality graphene/ferromagnetic epitaxial interfaces are mainly limited by the single-crystal size of the Ni (111) substrate and well-oriented graphene domains. In this work, based on the preparation of a 2-inch single-crystal Ni (111) film on an Al 2 O 3  (0001) wafer, we successfully achieve the production of a full-coverage, high-quality graphene monolayer on a Ni (111) substrate with an atomically sharp interface via ambient pressure chemical vapor deposition (APCVD). The high crystallinity and strong coupling of the well-oriented epitaxial graphene/Ni (111) interface are systematically investigated and carefully demonstrated. Through the analysis of the growth model, it is shown that the oriented growth induced by the Ni (111) crystal, the optimized graphene nucleation and the subsurface carbon density jointly contribute to the resulting high-quality graphene/Ni (111) heterostructure. Our work provides a convenient approach for the controllable fabrication of a large-area homogeneous graphene/ferromagnetic interface, which would benefit interface engineering of graphene-based MTJs and future chip-level 2D spintronic applications.

Controlled Epitaxial Growth and Atomically Sharp Interface of Graphene/Ferromagnetic Heterostructure via Ambient Pressure Chemical Vapor Deposition