Nanophase separation in monomolecularly thin water-ethanol films controlled by graphene

Control over nanoscale patterning of ultrathin molecular films plays an important role both in natural as well as artificial nanosystems. Here we report on nanophase separated patterns of water and ethanol within monomolecularly thin films confined between the cleavage plane of mica and single or a few layers of graphene. Employing scanning force microscopy of the graphene layers conforming to the molecular films we quantify the patterns using the ethanol-water cross correlation and the autocorrelation of domain wall directions. They reveal that lateral pattern dimensions grow and the domain walls stiffen upon increasing the thickness of the graphene multilayers. We attribute the control of the patterns through the graphene layers to the competition between the mechanical deformation energy of the graphene sheets and the electrostatic repulsion of dipoles normal to the interface. The latter results from charge transfer between graphene and the molecules confined between mica and graphene.