Vacancy in graphene: insight on magnetic properties from theoretical modeling

Magnetic properties of a single vacancy in graphene is a relevant and still unsolved problem. The experimental results point to a clearly detectable magnetic defect state at the Fermi energy, while several calculations based on density functional theory (DFT) yield widely varying results for the magnetic moment, in the range of μ = 1.04 − 2.0 μB . We present a multi-tool ab initio theoretical study of the same defect, using two simulation protocols for a defect in a crystal (cluster and periodic boundary conditions) and different DFT functionals bare and hybrid DFT, mixing a fraction of exact Hartree-Fock exchange (XC). Our main conclusions are two-fold: First, we find that due to the π-character of the Fermi-energy states of graphene, inclusion of XC is crucial and for a single isolated vacancy we can predict an integer magnetic moment μ = 2μB . Second, we find that due to the specific symmetry of the graphene lattice, periodic arrays of single vacancies may provide interesting diffuse spin-spin interactions.