Tuning the Dirac Cone of Bilayer and Bulk Structure Graphene by Intercalating First Row Transition Metals Using First-Principles Calculations

Abstract

Modern nanoscience has focused on two-dimensional (2D) layer structure materials which have garnered tremendous attention due to their unique physical, chemical, and electronic properties since the discovery of graphene in 2004. A recent advancement in graphene nanotechnology opens a new avenue of creating 2D bilayer graphene (BLG) intercalates. Using first-principles dispersion-corrected DFT techniques, we have designed 20 new materials in silico by intercalating first-row transition metals (TMs) with BLG, i.e., 10-layered structure and 10 bulk crystal structures of TM intercalated in BLG. More specifically, we investigated the equilibrium structure and electronic properties of layered and bulk structure BLG intercalated with first-row TMs (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn). The present DFT-D calculations show that the 2pz subshells of C atoms in graphene and the 3dyz subshells of the TM atoms provide the electron density near the Fermi energy level, controlling the material properties of the BLG-intercalated materials. This article highlights how the Dirac point moves in both the BLG and bulk-BLG given different TM-intercalated materials. The implications of controllable electronic structure and properties of intercalated BLG-TM materials for future device applications are discussed. This work opens up new avenues for the efficient production of two-dimensional and three-dimensional carbon-based intercalated materials with promising future applications in nanomaterial science. © 2018 American Chemical Society.