Large-Area Deposition of MoS₂ by Pulsed Laser Deposition with In Situ Thickness Control

A scalable and catalyst-free method to deposit stoichiometric molybdenum disulfide (MoS2) films over large areas is reported, with the maximum area limited by the size of the substrate holder. The method allows deposition of MoS2 layers on a wide range of substrates without any additional surface preparation, including single-crystal (sapphire and quartz), polycrystalline (HfO2), and amorphous (SiO2) substrates. The films are deposited using carefully designed MoS2 targets fabricated with excess sulfur and variable MoS2 and sulfur particle size. Uniform and layered MoS2 films as thin as two monolayers, with an electrical resistivity of 1.54 × 10(4) Ω cm(-1), were achieved. The MoS2 stoichiometry was confirmed by high-resolution Rutherford backscattering spectrometry. With the method reported here, in situ graded MoS2 films ranging from ∼1 to 10 monolayers can be deposited.