Carbon dots produced via space-confined vacuum heating: maintaining efficient luminescence in both dispersed and aggregated states

Abstract

Aggregation-induced quenching (AIQ) of emission is an obstacle for the development of carbon dots (CDots) for solid-state luminescent devices. In this work, we introduce a method to avoid AIQ and to produce highly luminescent CDots through a space-confined vacuum heating synthesis. In the presence of CaCl₂, a mixture of citric acid and urea forms an inflated foam under vacuum heating at 120 °C. Upon gradually increasing the heating temperature to 250 °C, blue emissive molecular species are first formed, and are then transformed into uniform-sized green emissive CDots through dehydration and carbonization processes taking place in the confined ultrathin spaces of the foam walls. The green luminescence of these CDots originates from conjugated sp² domains, and these CDots exhibit a high photoluminescence quantum yield (PLQY) of 72% in ethanol solution. Remarkably, due to the existence of only one type of recombination center in these nanoparticles, AIQ does not take place in CDot-based close-packed films, which show strong emission with a PLQY of 65%. Utilizing the differences in the emission properties of vacuum heating produced CDots, CDots synthesized through microwave-assisted heating, and commercial green fluorescent organic ink (namely, excitation-dependent vs. excitation-independent emission, and different stability against photobleaching), multilevel data encryption has been demonstrated.