Magnetic and chemical properties of ultrathin Fe films on molybdenum disulfide (MoS2) are investigated using magneto‐optic Kerr effect (MOKE) and X‐ray photoemission spectroscopy (XPS). A magnetization hysteresis loop is found after nominal 10 Å of Fe deposition on MoS2 at room temperature. The thickness‐dependent MOKE measurement evaluates that the magnetic dead layer (MDL) exists up to ≈2 Å of Fe on MoS2 due to the interaction between Fe and MoS2. XPS shows small peak shifting for Mo 3d and S 2p peaks toward lower binding energies with initial Fe deposition, indicating the modification of surface band bending. Fe 2p peaks for lower thickness of Fe are significantly broader than those for higher thickness, which is attributed to the coexistence of metallic and ionic Fe in the film. The presence of ionic Fe, localized at the interface, indicates strong interactions between Fe and MoS2, and the existence of chemical bonding at the interface is corroborated with the formation of MDL.
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