Hydrogen Bond‐Mediated Self‐Assembly of Carbon Dots Enabling Precise Tuning of Particle and Cluster Luminescence for Advanced Optoelectronic Applications

Abstract The effective control over the self‐assembly process of carbon dots (CDs) and their cluster luminescence in the aggregated state is of paramount significance and challenge. This study, for the first time, systematically explores the photoluminescent behavior of CDs in their aggregated state, which is less understood compared to their discrete state. By investigating the effects of concentration and solvent environment, it's demonstrated that CDs could exhibit dual emission properties, shifting from blue particle emissions to red cluster emissions as they aggregate. The key to this tunable luminescence lies in hydrogen bonding, which drives the self‐assembly of CDs and modulates their photo physical properties. These findings reveal that through precise control of aggregation, CDs can be engineered for advanced optoelectronic applications, including tunable light‐emitting diodes (LEDs), secure information encryption, and fingerprint authentication. This report not only deepens the understanding of the underlying mechanisms governing CDs' cluster luminescence but also introduces a novel approach to exploiting their unique properties for technological innovation.