Controlling self-assembly of reduced graphene oxide at the air-water interface: quantitative evidence for long-range attractive and many-body interactions.

Industrial-scale applications of two-dimensional materials are currently limited due to lack of a cost-effective and controlled synthesis method for large-area monolayer films. Self-assembly at fluid interfaces is one promising method. Here, we present a quantitative analysis of the forces governing reduced graphene oxide (rGO) assembly at the air-water interface using two unique approaches: area-based radial distribution functions and a theoretical Derjaguin-Landau-Verwey-Overbeek (DLVO) interaction potential for disks interacting edge-to-edge. rGO aggregates at the air-water interface when the subphase ionic strength results in a Debye screening length equal to the rGO thickness (∼1 mM NaCl), which is consistent with the DLVO interaction potential. At lower ionic strengths, area-based radial distribution functions indicate that rGO-rGO interactions at the air-water interface are dominated by long-range (tens of microns) attractive and many-body repulsive forces. The attractive forces are electrostatic in nature; that is, the force is weakened by minor increases in ionic strength. A quantitative understanding of rGO-rGO interactions at the air-water interface may allow for rational synthesis of large-area atomically thin films that have potential for planar electronics and membranes.