First-Principles Study of Ferromagnetism in Two-Dimensional Silicene with Hydrogenation

Abstract

We performed first-principles simulation on the electronic structure and magnetic properties of two-dimensional hexagonal silicene, which was recently synthesized. The results show that the weak overlapping between 3pz orbitals of neighbor Si atoms leads to a very reactive surface, resulting in a more energetically stable semiconducting surface upon being fully hydrogenated. Half-hydrogenation breaks the extended π-bonding network of silicene, leaving the electrons in the unsaturated Si atoms localized and unpaired, and thus it exhibits ferromagnetic semiconducting behavior with a band gap of 0.95 eV. The long-range ferromagnetic coupling between Si atoms was also predicted, with a Curie temperature of about 300 K. These results demonstrated that hydrogenation is an efficient route to tune the electronic properties of silicene sheets.