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Non-covalent functionalization via physisorption of organic moleculesprovides a scalable approach for modifying the electronic structure of graphenewhile preserving its excellent carrier mobilities. Here we investigated thephysisorption of long-chain acenes, namely, hexacene and its fluorinatedderivative perfluorohexacene, on bilayer graphene for tunable graphene devicesusing first principles methods. We find that the adsorption of these moleculesleads to the formation of localized states in the electronic structure ofgraphene close to its Fermi level, which could be readily tuned by an externalelectric field. The electric field not only creates a variable band gap aslarge as 250 meV in bilayer graphene, but also strongly influences the chargeredistribution within the molecule-graphene system. This charge redistributionis found to be weak enough not to induce strong surface doping, but strongenough to help preserve the electronic states near the Dirac point of graphene.

Tunable Hybridization Between Electronic States of Graphene and Physisorbed Hexacene