Understanding the Independent and Interdependent Role of Water and Oxidation on the Tribology of Ultrathin Molybdenum Disulfide (MoS2)

Abstract

In this work, the tribological behavior of ultrathin-MoS2 was investigated to understand the independent roles of water and oxidation. Water adsorption was identified as the primary interfacial mechanism for both SiO2/pristine-MoS2 and SiO2/graphene interfaces, however, tribological behavior of pristine-MoS2 was observed to be more sensitive to presence of water due to stronger MoS2-water interaction. Comparison of pristine-MoS2 and oxidized-MoS2 revealed that the oxidation of MoS2 significantly increased its friction and sensitivity to water by play a more detrimental role. The specific effect of oxygen on friction via chemical interactions was studied in isolation through density functional theory (DFT) simulations of a tip sliding on MoS2 basal planes and over edges before and after oxidation. The maximum change in energy, or energy barrier correlating with friction, as the tip moved across the surface, increased after oxidation by up to 66% for the basal plane and by 25% at the edge. Charge density analysis suggests that the more localized and non-uniform interfacial charge distribution on oxygen rich surfaces, as compared to pristine surfaces, leads to higher resistance to sliding. This confirms that oxygen presence alone increases friction and when coupled with the presence of water, both effects are additive in increasing friction.