Two-Dimensional Crystal Grain Size Tuning in WS2 Atomic Layer Deposition: An Insight in the Nucleation Mechanism

Abstract

When two-dimensional (2D) group-VI transition metal dichalcogenides such as tungsten disulfide (WS2) are grown by atomic layer deposition (ALD) for atomic growth control at low deposition temperatures (≤450 °C), they often suffer from a nanocrystalline grain structure limiting the carrier mobility. The crystallinity and monolayer thickness control during ALD of 2D materials is determined by the nucleation mechanism, which is currently not well understood. Here, we propose a qualitative model for the WS2 nucleation behavior on dielectric surfaces during plasma-enhanced (PE-) ALD using tungsten hexafluoride (WF6), dihydrogen (H2) plasma and dihydrogen sulfide (H2S) based on analyses of the morphology of the WS2 crystals. The WS2 crystal grain size increases from ∼20 to 200 nm by lowering the nucleation density. This is achieved by lowering the precursor adsorption rate on the starting surface using an inherently less reactive starting surface, by decreasing the H2 plasma reactivity, and by enhancing the mob...