Experimental and theoretical evidence for the ferromagnetic edge in WSe2 nanosheets

Abstract

Bulk TMDCs are diamagnetic materials; however, two-dimensional TMDCs exhibit spin polarized edge states, which results in a coupling between the unsaturated transition metal and chalcogenide atoms at the edges. The magnetism in two-dimensional TMDCs broadens their applications in spintronic and multi-functional devices. Herein, by combining macro/micro-magnetic experimental measurements and density functional theory (DFT) calculations, we demonstrate that among five possible edge-terminated WSe₂ nanosheets only two types have a magnetic ground state, corresponding to the 100% Se edge terminated and 50% Se edge terminated nanosheets, respectively. The calculation results on WSe₂ clusters and WSe₂ zig-zag nanoribbons with different terminations and Se coverage rate confirmed that the unpaired electrons of the edge atoms play a crucial role in the appearance of ferromagnetism in WSe₂ nanosheets. Furthermore, due to the possible quantum confinement effect and surface effect, there exist thickness-dependent magnetic properties, and the magnitude of magnetism at the edge increases as the number of layers decreases.