Wetting of mono and few-layered WS2 and MoS2 films supported on Si/SiO2 substrates

The recent interest and excitement in graphene has also opened up a pandora's box of other two-dimensional (2D) materials and material combinations which are now beginning to come to the fore. One family of these emerging 2D materials is transition metal dichalcogenides (TMDs). So far there is very limited understanding on the wetting behavior of "monolayer" TMD materials. In this study, we synthesized large-area, continuous monolayer tungsten disulfide (WS2) and molybdenum disulfide (MoS2) films on SiO2/Si substrates by the thermal reduction and sulfurization of WO3 and MO3 thin films. The monolayer TMD films displayed an advancing water contact angle of ∼83° as compared to ∼90° for the bulk material. We also prepared bilayer and trilayer WS2 films and studied the transition of the water contact angle with increasing number of layers. The advancing water contact angle increased to ∼85° for the bilayer and then to ∼90° for the trilayer film. Beyond three layers, there was no significant change in the measured water contact angle. This type of wetting transition indicates that water interacts to some extent with the underlying silica substrate through the monolayer TMD sheet. The experimentally observed wetting transition with numbers of TMD layers lies in-between the predictions of one continuum model that considers only van der Waals attractions and another model that considers only dipole-dipole interactions. We also explored wetting as a function of aging. A clean single-layer WS2 film (without airborne contaminants) was shown to be strongly hydrophilic with an advancing water contact angle of ∼70°. However, over time, the sample ages as hydrocarbons and water present in air adsorb onto the clean WS2 sheet. After ∼7 days, the aging process is completed and the advancing water contact angle of the aged single-layer WS2 film stabilizes at ∼83°. These results suggest that clean (i.e., nonaged) monolayer TMDs are hydrophilic materials. We further show that substitution of sulfur atoms by oxygen in the lattice of aged monolayer WS2 and MoS2 films can be used to generate well-defined 'hydrophobic-hydrophilic' patterns that preferentially accumulate and create microdrop arrays on the surface during water condensation and evaporation experiments.