Deposition of DNA Nanostructures on Highly Oriented Pyrolytic Graphite

The integration of the addressability of DNA nanostructures and the electronic sensitivity of sp2 carbon‐based materials presents a promising avenue for the development of powerful sensitive biodevices for detecting biological signals and substances with high sensitivity. Essential to this prospect is the attainment of high‐shape fidelity immobilization of DNA nanostructures on these sp2 carbon substrates. However, it is challenging due to the stability of DNA nanostructures on these substrates. In this study, the adsorption behavior of DNA nanostructures is explored on a highly oriented pyrolytic graphite (HOPG) surface. The observations revealed a severe structural destabilization of DNA nanostructures upon interacting with bare HOPG. Immobilization of DNA nanostructures with high shape‐fidelity can be achieved by modifying the surface property of HOPG and enhancing the rigidity of DNA nanostructures. In addition, DNA tetrahedron origami is employed as a rigid, precise, and programmable three‐dimensional framework for controlled patterning of gold nanoparticles on HOPG surface, demonstrating the potential for constructing plasmonic devices and arranging other functional species on sp2 carbon‐based substrates for specific applications. This study shows the potential for customizable functionalization of sp2 carbon‐based substrates and tailored design of biodevices at the interface through integration with DNA nanostructures.