Electronic structure evolution of the transition metals substituted tetragonal graphene: a first-principles...

Motivated by the possibilities of tuning the Fermi level of the metallic band structure of the planar tetragonal graphene (T-graphene), by using the transition metals (TMs) substitution (3d, 4dand 5dseries), the electronic structure investigation has been carried out at low concentration level (≈2.7%) throughab initiodensity functional theory method. We have investigated the influence of the valence electrons of the TM on the evolution of the electronic structure and magnetization and the induced magnetic moments at the carbon atoms in the T-graphene network. The investigations also explored the possibilities of inducing long-range magnetic ordering. In the case of multi TMs substitutions we found the dominance signature of the antiferromagnetic correlations for most of the TM substituted cases. The critical analysis of the magnetization densities indicated the important role of the hybridization between the carbonπandσorbitals with the TM-dstates. We explored that the observed non-monotonic nature of the magnetization and evolution of electronic structure was due to the competing energy scales of electronic correlation, hybridization and crystal field splitting. This study opens up the route for further investigations towards the possibilities of using T-graphene as a potential polymorph of graphene for device applications.