Aggregation-induced emission of matrix-free graphene quantum dots via selective edge functionalization of rotor molecules.

Abstract

Graphene quantum dots (GQDs) are nanosized graphene derivatives with unique photoluminescence (PL) properties that have advantages in optoelectronic applications due to their stable blue light emission. However, aggregation-caused quenching (ACQ) of GQDs limits the practical applications on light-emitting diodes. Here, we suppress the ACQ phenomena of GQDs by reducing the size and converting GQDs into aggregation-induced emission (AIE)-active materials. As the size of GQDs is reduced from 5 to 1 nm, their solid-state PL quantum yields (PLQYs) are improved from 0.5 to 2.5%, preventing ACQ. Two different rotor molecules, benzylamine (BA) and 4,4'-(1,2-diphenylethene-1,2-diyl)diphenol (TPE-DOH), are selectively functionalized by substituting carboxylic acid and carbonyl functional groups. All functionalized GQDs show AIE behaviors with significantly enhanced solid-state PLQYs, up to 16.8%. Afterglow measurements and theoretical calculations reveal that selective functionalization hinders inter- and intramolecular charge transfer, which enhances the fluorescence rate of GQDs and corresponding PLQY.