Two-dimensional 4f magnetic EuSn2X2 (X = P, As) monolayers: A first-principles study

Abstract

Two-dimensional (2D) ferromagnetic semiconductors (FMSs) hold exciting and promising potential for application in spintronic devices at the nanoscale. Currently, most 2D FMSs are based on 3d electrons; 4f electrons can provide nontrivial magnetism but have been much less studied to date. This paper presents a theoretical study, via first-principles calculations, of EuSn2X2 (X = P, As) monolayers based on rare-earth cations with f-electrons. The results show that EuSn2X2 monolayers possess a large magnetization (7 μB/Eu), a controllable magnetic anisotropy energy, and a unique d-electron-mediated f–f exchange mechanism. Both types of EuSn2X2 (X = P, As) monolayers are FMSs with indirect bandgaps of 1.00 and 0.99 eV, respectively, based on the Heyd–Scuseria–Ernzerhof (HSE06) method, which can be transform to direct bandgap semiconductors under biaxial strain. Interestingly, under the latter, spin–orbit coupling interaction gradually replaces the dipole–dipole interaction in the dominant position of magnetic anisotropy, resulting in the magnetic easy axis changing from in-plane to the more desirable out-of-plane. Considering their excellent dynamic, thermal, and mechanical stabilities and small cleavage energy, these EuSn2X2 monolayers can be exfoliated from their synthesized bulk. Our study not only helps to understand the properties of 2D 4f rare-earth magnets but also signposts a route toward improving the performance of EuSn2X2 monolayers in nano-electronic devices.