“…Graphene oxide (GO), whether a single layer or a few layers of exfoliated sheets from graphite oxide, has recently received a lot of attention in the literature due to a range of potential applications. − GO consists of graphene sheets with oxygenated groups, and a number of studies have revealed a wide range of oxygen functional groups, such as hydroxyls and epoxides, carboxylic acids, or sulfonates groups, , on these sheets as well as how these groups are arranged on the surface. − A key question that arises is how, depending on their number and partitioning, these oxygen functional groups can favor or prohibit reactions at the GO-liquid interface in aqueous media. To probe interfaces, several surface-specific techniques can be used such as environmental scanning electron microscopy (ESEM), secondary ion mass spectrometry (SIMS), Auger electron spectroscopy (AES), etc. − One method, vibrational sum-frequency generation (vSFG), , has received a lot of attention for characterizing interfaces experimentally − and in conjunction with simulations. ,,− The synergy between vSFG experiments and molecular simulations allows for an in-depth probing of the interface, permitting a finer molecular interpretation of the underlying interfacial region. In this paper, an analysis of the graphene-oxide-water interface by ab initio molecular dynamics (AIMD) at different levels of oxidation was performed to provide insight on the effect of the different structural domains of graphene-oxide (organic, aromatic rich regions vs oxygen-rich hydrophilic regions) on the...…”