Thickness-controlled
multilayer graphene has been attracting wide
interest in electronic and spintronic devices due to its tunable electronic
structure and spin transport properties. In particular, the strong
spin filtering effect in a lattice-matched Ni(111)/multilayer graphene
heterostructure provides an ideal platform for developing high-performance
spin valves and magnetic tunnel junctions. However, the thickness-controlled
synthesis of multilayer graphene on Ni(111) substrates is still a
large challenge, which seriously restricts the development of graphene
spintronic devices. Here, we report an approximate equilibrium segregation
method for large-area multilayer graphene films on Ni(111) substrates
by regulating the growth process of carbon dissolution and segregation.
The uniformity and coverage of multilayer graphene films are controlled
precisely in an atmospheric tube furnace system by modulating the
Ni film thickness, gas atmosphere, and cooling rate. Characterization
results systematically confirm the production of high-coverage, high-quality
multilayer graphene on Ni(111) substrates. This work provides a reliable
method for the controllable fabrication of multilayer graphene on
single-crystal ferromagnetic substrates, which would contribute to
the application of graphene spintronic devices.