Origin of Ubiquitous Stripes at the Graphite-Water Interface.

The investigation of solid-liquid interfaces is pivotal for understanding processes like wetting, corrosion, and mineral dissolution and growth. The graphite-water interface constitutes a prime example for studying the water structure at a seemingly hydrophobic surface. Surprisingly, in a large number of atomic force microscopy (AFM) experiments, well-ordered stripes have been observed at the graphite-water interface. Although many groups have reported on the observation of stripes at this interface, fundamental properties and, in particular, the origin of the stripes are still under debate. Proposed origins include contamination, interplanar stacking of graphene layers, formation of methanol-water nanostructures, and adsorption of nitrogen molecules. Especially, the latter interpretation has received considerable attention because of its potential impact on explaining the long-range nature of the hydrophobic interaction. In this study, we demonstrate that these stripes readily form when using standard plastic syringes to insert the water into the AFM instrument. In contrast, when clean glass syringes are used instead, no such stripes form even though nitrogen was present. We, therefore, conclude that contaminations from the plastic syringe rather than nitrogen constitute the origin of the stripes we observe. We provide high-resolution AFM data that reveal detailed structural insights into the arrangement of the stripes. The rich variability of our data suggests that the stripes might be composed of several different chemical species. Still, we cannot rule out that the stripes observed in the literature might originate from other sources; our study offers a rather straightforward explanation for the origin of the stripes. In the view of these results, we propose to carefully reconsider former assignments.