Abstract

Quantum dot-based materials have been found to be excellent platforms for biosensing and bioimaging applications. Herein, self-propelled microrobots made of graphene quantum dots (GQD-MRs) have been synthesized and explored as unconventional dynamic biocarriers toward the optical "on-the-fly" monitoring of DNA. As a first demonstration of applicability, GQD-MRs have been first biofunctionalized with a DNA biomarker (i.e., fluorescein amidite-labeled, FAM-L) via hydrophobic π-stacking interactions and subsequently exposed toward different concentrations of a DNA target. The biomarker-target hybridization process leads to a biomarker release from the GQD-MR surface, resulting in a linear alteration in the fluorescence intensity of the dynamic biocarrier at the nM range (1-100 nM, R2 = 0.99), also demonstrating excellent selectivity and sensitivity, with a detection limit as low as 0.05 nM. Consequently, the developed dynamic biocarriers, which combine the appealing features of GQDs (e.g., water solubility, fluorescent activity, and supramolecular π-stacking interactions) with the autonomous mobility of MRs, present themselves as potential autonomous micromachines to be exploited as highly efficient and sensitive "on-the-fly" biosensing systems. This method is general and can be simply customized by tailoring the biomarker anchored to the GQD-MR's surface.

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