Atomic Layer Deposition of Large-Area Polycrystalline Transition Metal Dichalcogenides from 100 °C through Control of Plasma Chemistry

Two-dimensional transition metal dichalcogenides, such as MoS2, are intensely studied for applications in electronics. However, the difficulty of depositing large-area films of sufficient quality under application-relevant conditions remains a major challenge. Herein, we demonstrate deposition of polycrystalline, wafer-scale MoS2, TiS2, and WS2 films of controlled thickness at record-low temperatures down to 100 °C using plasma-enhanced atomic layer deposition. We show that preventing excess sulfur incorporation from H2S-based plasma is the key to deposition of crystalline films, which can be achieved by adding H2 to the plasma feed gas. Film composition, crystallinity, growth, morphology, and electrical properties of MoSx films prepared within a broad range of deposition conditions have been systematically characterized. Film characteristics are correlated with results of field-effect transistors based on MoS2 films deposited at 100 °C. The capability to deposit MoS2 on poly(ethylene terephthalate) substrates showcases the potential of our process for flexible devices. Furthermore, the composition control achieved by tailoring plasma chemistry is relevant for all low-temperature plasma-enhanced deposition processes of metal chalcogenides