DNA-directed assembly of graphene homostructures

We present a DNA-directed strategy for the programmable assembly of graphene homostructures, enabled by covalent DNA functionalization of azidated graphene nanosheets. Azidated graphene was synthesized via established electrochemical exfoliation methods and further refined by cascade centrifugation to control flake size and thickness. Complementary single-stranded DNA linkers were covalently attached to the graphene surface using copper-free click chemistry. Upon hybridization, DNA strands bridged individual graphene flakes into vertical and lateral junctions. Fluorescence recovery based on Cy5 labeling and dynamic light scattering confirmed successful DNA-guided assembly. The assembled structure configurations were investigated by atomic force microscopy and conductive AFM, highlighting the linking and insulating role of DNA tethered between flakes. This approach offers a modular platform for the construction of graphene–graphene architectures via biomolecular assembly.