Quantum Chemical Molecular Dynamics Studies of Bilayer Graphene Growth on a Ni(111) Surface

The mechanism of bilayer graphene nucleation and growth has been investigated by using quantum chemical molecular dynamics simulations. The results indicate that the presence of embedded nickel atoms in the upper-layer (first-layer) graphene has little impact on the evolution mechanism of the second-layer graphene precursor. The nucleation process occurs after the rapid precipitation of internal carbon atoms along with the degradation of nickel catalyst and the formation of discrete carbon polyyne chains. The second-layer graphene exhibits an attachment-limited growth on the rugged Ni(111) surface. The quality of the second-layer graphene can be reduced, and large structural holes are induced when the metal atoms are involved in the upper-layer graphene. On the contrary, high-quality upper-layer graphene can act as an excellent template for the growth of the second-layer graphene. These simulations, therefore, suggest that through carefully controlling the growth conditions, different kinds of bilayer graphene can be fabricated in a layer-by-layer mode on the Ni(111) surface