Nickel Intercalation in Epitaxial Graphene on SiC(0001): A Novel Platform for Engineering Two-Dimensional Heterostructures.

Two-dimensional (2D) magnetic materials integrated with graphene offer a compelling platform for next-generation spintronic devices. Yet nickel in its 2D form remains largely unexplored, due to fundamental synthesis limitations. Here, we report the controlled intercalation of Ni beneath epitaxial graphene on the Si-face of SiC(0001), achieved through a scalable colloidal nanoparticle deposition route. Chemically synthesized Ni nanoparticles ( ∼ 10 nm diameter) are uniformly deposited onto graphene via immersion in colloidal solution at room temperature; subsequent thermal annealing at 650 ∘ C drives intercalation, yielding well-ordered Ni islands at the graphene/buffer-layer interface with morphology dictated by annealing conditions. Scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES), supported by density functional theory (DFT) calculations, elucidate the atomic and electronic structure of the intercalated layers. DFT simulations further confirm the thermodynamic stability of the 2D nanostructures as a function of shape and lateral size, predicting a robust average magnetic moment of 0.9 μ B per atom. The resulting Ni-intercalated graphene on SiC constitutes a well-defined 2D heterostructure combining preserved graphene band structure with robust interfacial magnetism, stable under ambient conditions. These findings establish a reproducible, scalable pathway to engineer magnetic graphene-based heterostructures and open new avenues for their integration into spintronic architectures.