Controlling Terahertz Spintronic Photocurrents in 2D-Semiconductor|Ferromagnet Heterostructures through a Functional Hybrid Interface

A profound understanding of terahertz (THz) spin and charge currents in heterostructures involving ferromagnets (FMs) and two-dimensional (2D) materials promises emerging applications in high-speed sensing and data processing. Yet, ultrafast experimental insights remain very limited. Here, we study the efficient photo-generation of THz spin and charge currents in bilayers made from the transition-metal dichalcogenide (TMD) MoS2 and the FM Co. We find that the efficiency of current generation strongly depends on the pump photon energy, as previously reported. Surprisingly, however, we observe that the current dynamics remain identical for pump photon energies above and below the MoS2 band gap. Supported by ab-initio calculations, we conclude that an interfacial hybrid metallic layer forms at the MoS2/Co boundary that has a pronounced photon-energy-dependent absorptance. Thus, the hybrid interfacial layer effectively acts like a pump-energy transducer that increases the spin-current generated in the nearby Co. Our results uncover the vital role of interfacial hybridization as a yet unexplored mechanism for efficient generation of ultrafast photocurrents in 2D-TMD|FM structures.