Tunable Magnetism in Transition-Metal-Decorated Phosphorene

Abstract

We present a density functional theory study of 3d transition-metal (TM) atoms (Sc–Zn) adsorbed on a phosphorene sheet. We show that due to the existence of lone pair electrons on P atoms in phosphorene, all the TM atoms, except the closed-shell Zn atom, can bond strongly to the phosphorene with sizable binding energies. Moreover, the TM@phosphorene systems for TM from Sc to Co exhibit interesting magnetic properties, which arise from the exchange splitting of the TM 3d orbitals. We also find that strain is an effective way to control the magnetism of TM@phosphorene systems by tuning the interaction of the TM with phosphorene and, thus, the relative positions of in-gap TM 3d orbitals. In particular, a small biaxial strain could induce a magnetic transition from a low-spin to a high-spin state in phosphorene decorated by Sc, V, or Mn. These results clearly establish the potential for phosphorene utilization in innovative spintronic devices.