On the connection between structural distortion and magnetism in graphene with a single vacancy

TL;DR

This study explores how structural distortions around a vacancy in graphene influence its magnetic properties, revealing that planarity correlates with magnetism and that non-planar configurations can suppress magnetic moments.

Contribution

It provides a detailed first-principles analysis of the relationship between local structural distortions and magnetism in vacancy-containing graphene, highlighting metastable non-magnetic states.

Findings

Graphene with a vacancy is inherently magnetic and planar.

Out-of-plane distortions can lead to non-magnetic metastable states.

Magnetism is linked to the local structural configuration around the vacancy.

Abstract

The correlation between structural distortion and emergence of magnetism in graphene containing a single vacancy was investigated using first-principles calculations based on density functional theory (DFT). Our results have shown that a local distortion is formed around the vacancy, with reconstruction of two atomic bonds and with a dangling bond remaining at the third atom adjacent to the vacancy. A systematic investigation of the possible out-of-plane displacement of this third atom was then carried out, in order to ascertain its effects on the magnetic features of the system. The ground state was definitely found to be magnetic and planar, with spin-resolved $\sigma$ and $\pi$ bands contributing to the total magnetic moment. However, we have also found that metastable solutions can be achieved if an initial shift of the third atom above a minimum threshold from the graphene plane is provided, which leads to a non-planar geometry and a non-magnetic state.