Suppressed blinking behavior of CdSe/CdS QDs by polymer coating

Abstract

Semiconductor quantum dots (QDs) are very important fluorescent nanocrystals with excellent optical properties. However, QDs, at the single-particle level, show severe fluorescence intermittency (or blinking) on a wide time scale from milliseconds to minutes, which limits certain optical and biological applications. Generally, blinking behavior of QDs strongly depends on their surface state and surrounding environment. Therefore, current blinking suppression approaches are mostly focused on the introduction of an inorganic shell and organic small molecule compounds. In this study, we described a “bottom up” approach for the synthesis of CdSe/CdS/polymer core/shell/shell QDs via the in situ one-pot polymerization approach in order to control the blinking behavior of QDs. Three monomers (dithiothreitol (DTT), phenylenediamine (PDA), and hexamethylenediamine (HDA)) were respectively used to polymerize with hexachlorocyclotriphosphazene (HCCP), and then the polyphosphazene polymers were obtained with cyclotriphosphazene as the basic macromolecular backbone. By regulating the molar ratios of the activated comonomers, we can control the blinking behavior of CdSe/CdS/polymer QDs. Under the optimal conditions, the percentage of “non-blinking” CdSe/CdS/polymer QDs (the “on time” fraction > 99% of the overall observation time) was up to 78%. The suppression mechanism was attributed to the efficient passivation of QD surface traps by the sulfhydryl or phenyl groups in the polyphosphazene polymers.