Large-area sputtered 2H-MoS2 thin films for spin and orbital charge conversion

Abstract Two-dimensional transition metal dichalcogenides (TMDs), such as molybdenum disulfide (MoS 2 ), are promising platforms for spin–orbitronic technologies, yet scalable growth of phase-pure films with controlled interfaces remains challenging. Here, we report the growth and characterization of large-area MoS 2 thin films synthesized by RF magnetron sputtering followed by in situ high-vacuum annealing. Post-deposition annealing stabilizes the semiconducting 2H phase, as confirmed by Raman spectroscopy, X-ray diffraction, and electron microscopy. Atomic force microscopy and X-ray reflectivity revealed smooth surfaces and sharp interfaces, with energy-dispersive spectroscopy confirming uniform stoichiometry and negligible interfacial diffusion. Scanning tunneling spectroscopy demonstrated semiconducting behavior with a tunable bandgap, consistent with interlayer coupling and quantum confinement. These results establish sputtering with optimized annealing as a reliable route to large-area, phase-pure MoS₂. Building on this platform, we investigated angular momentum transport using spin pumping via ferromagnetic resonance. MoS 2 /Py(Ni 81 Fe 19 ) bilayers showed pronounced signals, comparable to Pt/Py. MoS 2 /Pt/Py heterostructures, fabricated to enhance orbital current pumping, showed signal magnitudes differing strongly from Pt/Py, and remaining independent of MoS 2 thickness. This behavior highlights a dominant interfacial contribution to spin–orbital–charge conversion, positioning MoS₂ films as promising platforms for spin–orbitronics.