Controlling the cooperative self-assembly of graphene oxide quantum dots in aqueous solutions

Abstract

Fascinating 3D cooperative self-assembly behavior was observed for 2D graphene oxide quantum dots (GOQDs) in dilute and semi dilute aqueous solutions. In addition the optical properties could be tuned by controlling the supramolecular structures. While the electrostatic interactions between the charged single sheets were assigned as the main secondary interactions that were responsible for the supramolecular fine structures, the concentration, temperature, salt concentration and pH could tune the repulsive/attractive forces and the molecular binding between the GOQD sheets. The morphological studies combined with UV-Vis and fluorescence evaluations proved that after a slow nucleation step, elongation preceded radially by H-aggregate self-association of the GOQD monomers, forming the final porous spheres by radial growth of rods. The quenching properties of the self-associated-assembled GOQDs together with the excitation wavelengths of the GOQD solutions enabled tuning of the fluorescence intensity and color of the final solutions, which could be utilized for e.g. bioimaging and smart spectroscopy.