Magnetism of MoS2 bilayers with intercalated and surface adsorbed Fe

Abstract

Magnetic thin films composed of two-dimensional van der Waals materials will play an important role in future spintronics devices. Recently, Tuli et al. performed in-situ MOKE measurements of Fe deposited on an MoS2 substrate and found that a magnetic dead layer (MDL) exists up to approximately 2 Å (Tuli et al. (2021)). To understand the origin of the MDL, we investigate MoS2 bilayers with intercalated and surface adsorbed Fe using first-principles calculations. The results show that the Fe-intercalated bilayer MoS2 is more stable than the bilayer MoS2 with surface adsorbed Fe. The Fe-intercalated bilayer MoS2 is non-magnetic and behaves as the MDL. The systematic investigation of variation in the inter-layer distance between the intercalated Fe layer and surface of MoS2 layer reveals that the strong hybridization between Fe and S is the origin of the MDL. We also show that further intercalation of Fe makes the film magnetic. The results provide a deep understanding of the MDL in two-dimensional van der Waals magnetic materials.