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For continual scaling in microelectronics, new processes for precise high volume fabrication are required. Area-selective atomic layer deposition (ASALD) can provide an avenue for self-aligned material patterning and offers an approach to correct edge placement errors commonly found in top-down patterning processes. Two-dimensional transition metal dichalcogenides also offer great potential in scaled microelectronic devices due to their high mobilities and few-atom thickness. In this work, we report ASALD of MoS2 thin films by deposition with MoF6 and H2S precursor reactants. The inherent selectivity of the MoS2 atomic layer deposition (ALD) process is demonstrated by growth on common dielectric materials in contrast to thermal oxide/ nitride substrates. The selective deposition produced few layer MoS2 films on patterned growth regions as measured by Raman spectroscopy and time-of-flight secondary ion mass spectrometry. We additionally demonstrate that the selectivity can be enhanced by implementing atomic layer etching (ALE) steps at regular intervals during MoS2 growth. This area-selective ALD process provides an approach for integrating 2D films into next-generation devices by leveraging the inherent differences in surface chemistries and providing insight into the effectiveness of a supercycle ALD and ALE process. 

To enable greater control over thermal atomic layer deposition (ALD) of molybdenum disulfide (MoS 2 ), here we report studies of the reactions of molybdenum hexafluoride (MoF 6 ) and hydrogen sulfide (H 2 S) with metal oxide substrates from nucleation to few-layer films. In situ quartz crystal microbalance experiments performed at 150, 200, and 250 °C revealed temperature-dependent nucleation behavior of the MoF 6 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 ∼13 cycles at 200 °C. XPS revealed that higher deposition temperatures resulted in a higher fraction of MoS 2 within the films. Deposition temperature was found to play an important role in film morphology with amorphous films obtained at 200 °C and below, while layered films with vertical platelets were observed at 250 °C. These results provide an improved understanding of MoS 2 nucleation, which can guide surface preparation for the deposition of few-layer films and advance MoS 2 toward integration into device manufacturing.