Anhydride-Terminated Solid-State Carbon Dots with Bright Orange Emission Induced by Weak Excitonic Electronic Coupling

In this work, fluorescent solid carbon dots (CDs) welcome a new member, namely anhydride-terminated CDs, which have a photoluminescence quantum yield (PLQY) of 28% for orange-emitted CDs at 580 nm in powder form. For the first time, we revealed that the electronic coupling of the functional groups should be a crucial factor affecting the optical properties of solid CDs. Due to the negligible hydrogen bonding interaction between the anhydride groups, the electronic coupling of excitons between neighboring anhydride groups is weak, leading to a high PLQY of 28% and an immobile emission peak at 580 nm in solid state. Anhydride-terminated CDs can be partly converted into carboxyl-terminated CDs after dispersion in ethanol. However, the strong electronic coupling of carboxyl groups at high concentration generates the stacking mode of J-aggregates, giving rise to a red-shifted emission from 450 to 515 nm as well as quenched fluorescence in solid state. In comparison, a useful blue emission for solid-state CDs occurs from low sp2 hybridized carbon atoms, which possess weak electronic coupling and a stationary emission band at 450 nm in both solution and solid state. By adjusting the feed ratio of the reactants, the relevant intensities between the emission from low sp2 hybridized carbon atoms at 450 nm and the emission from anhydride groups at 580 nm can be controlled. As a result, single-component anhydride-terminated CD powder with tunable emission color from orange to white light can be achieved. As-prepared anhydride-terminated CDs can be used for fabricating light-emitting diodes (LEDs), white LEDs, and luminescent solar concentrators (LSCs).