Bright nonblinking photoluminescence with blinking lifetime from a nanocavity-coupled quantum dot (2311.11560v1)

Abstract: Colloidal semiconductor quantum dots (QDs) are excellent luminescent nanomaterials for a broad range of optoelectronic applications. Their photoluminescence blinking, however, hinders their practical use in many aspects. It has been shown that coupling QDs to plasmonic nanostructures may provide a viable way to suppress blinking. Nevertheless, the underlying mechanism of blinking suppression remains unclear and debated. Here, by deterministically coupling a single QD to a plasmonic nanocavity, we clarify the mechanism of blinking suppression, and demonstrate unprecedentedly bright emission from a single colloidal QD. In particular, we report for the first time that the coupled system exhibits nonblinking photoluminescence with blinking lifetime, which shows that the elimination of photoluminescence blinking originates from enhanced quantum yield of the charged states. We identify that the radiative decay rate is boosted from (48 ns)-1 to (0.7 ns)-1, which outcompetes Auger processes and enables similar quantum yields for charged and neutral excitons. Moreover, we demonstrate ultrabright photoluminescence of up to 17 million detected photons per second from a single QD. This work sheds new light on the goal of achieving ultrabright nonblinking QDs and may benefit a variety of QD-based applications.