Vacancy in graphene: insight on magnetic properties from theoretical modeling

TL;DR

This study uses advanced ab initio methods to clarify the magnetic properties of vacancies in graphene, demonstrating the importance of exchange-correlation effects and revealing potential for spin interactions.

Contribution

It provides a comprehensive theoretical analysis with multiple simulation protocols and DFT functionals, resolving previous discrepancies in magnetic moment predictions.

Findings

Inclusion of exchange-correlation is crucial for accurate magnetic moments.

Predicted magnetic moment for a single vacancy is 2 μB.

Periodic vacancies may lead to interesting spin interactions.

Abstract

Magnetic properties of a single vacancy in graphene is a relevant and still much discussed problem. The experimental results point to a clearly detectable magnetic defect state at the Fermi energy, while calculations based on density functional theory (DFT) yield widely varying results for the magnetic moment, in the range of $\mu=1.04-2.0$ $\mu_{B}$. We present a multi-tool \textit{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 Hartree-Fock exchange (XC). Our main conclusions are two-fold: First, we find that due to the $\pi$-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 $\mu=2\mu_{B}$. 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.