Spatially Resolved Click Patterning of Dyes on Graphene for 2D Hybrids with Regiotunable Fluorescence

Abstract Creating well‐defined and spatially resolved fluorescent graphene‐dye hybrid structures has long been a challenge, particularly in maintaining the dye's emission properties and preventing fluorescence quenching. A successful strategy is presented for covalent patterning of fluorescent dye moieties onto a graphene surface, enabling unprecedented precision in fluorescence modulation. This strategy combines lithography‐assisted reductive patterning to introduce ethynylbenzene anchors with a subsequent alkyne‐azide cycloaddition (copper(I)‐catalyzed click) reaction. The unique connection helps prevent the potential quenching of the dye. Comprehensive spectroscopic and microscopic analyses confirmed the formation of highly ordered and hierarchically organized hybrid nanoarchitectures with covalently integrated fluorescent dye units. This breakthrough overcomes the limitations of disordered and poorly defined structures in conventional graphene‐dye hybrids. The simplicity and versatility of this method allow for patterning a wide range of fluorescent dyes, opening up new possibilities for nanoarchitectures with potential uses in areas such as data storage, OLEDs, and anti‐counterfeiting.