Nucleation and growth of molybdenum disulfide grown by thermal atomic layer deposition on metal oxides

To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS2), here we report studies of the reactions of molybdenum hexafluoride (MoF6) and hydrogen sulfide (H2S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 degrees C revealed temperature-dependent nucleation behavior of the MoF6 precursor, which is attributed to variations in surface hydroxyl concentration with temperature. In situ Fourier transform infrared spectroscopy coupled with ex situ x-ray photoelectron spectroscopy (XPS) indicated the presence of molybdenum oxide and molybdenum oxyfluoride species during nucleation. Density functional theory calculations additionally support the formation of these species as well as predicted metal oxide to fluoride conversion. Residual gas analysis revealed reaction by-products, and the combined experimental and computational results provided insights into proposed nucleation surface reactions. With additional ALD cycles, Fourier transform infrared spectroscopy indicated steady film growth after similar to 13 cycles at 200 degrees C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 degrees C and below, while layered films with vertical platelets were observed at 250 degrees C. These results provide an improved understanding of MoS2 nucleation, which can guide surface preparation for the deposition of few-layer films and advance MoS2 toward integration into device manufacturing. Published under an exclusive license by the AVS.

Automated summary

This study investigates the reactions of molybdenum hexafluoride and hydrogen sulfide with metal oxide substrates during nucleation, providing insights into the nucleation mechanism of MoS2. The deposition temperature was found to play a crucial role in film morphology and MoS2 content. These findings contribute to the development of surface preparation techniques for MoS2 deposition and its integration into device manufacturing.