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The non-covalent functionalisation of graphene is an attractive strategy toalter the surface chemistry of graphene without damaging its superiorelectrical and mechanical properties. Using the facile method of aqueous-phasefunctionalisation on large-scale CVD-grown graphene, we investigated theformation of different packing densities in self-assembled monolayers (SAMs) ofperylene bisimide derivatives and related this to the amount of substratecontamination. We were able to directly observe wet-chemically deposited SAMsin scanning tunnelling microscopy (STM) on transferred CVD graphene andrevealed that the densely packed perylene ad-layers adsorb with the conjugated{\pi}-system of the core perpendicular to the graphene substrate. Thiselucidation of the non-covalent functionalisation of graphene has majorimplications on controlling its surface chemistry and opens new pathways foradaptable functionalisation in ambient conditions and on the large scale.

Understanding and optimising the packing density of perylene bisimide layers on CVD-grown graphene