Luminescence blinking of a reacting quantum dot.

Abstract

Luminescence blinking is an inherent feature of optical emission from individual fluorescent molecules and quantum dots. There have been intense efforts, although not with complete resolution, toward the understanding of the mechanistic origin of blinking and also its mitigation in quantum dots. As an advance in our microscopic view of blinking, we show that the luminescence blinking of a quantum dot becomes unusually heavy in the temporal vicinity of a reactive transformation. This stage of heavy blinking is a result of defects/dopants formed within the quantum dot on its path to conversion. The evolution of blinking behavior along the reaction path allows us to measure the lifetime of the critical dopant-related intermediate in the reaction. This work establishes luminescence blinking as a single-nanocrystal level probe of catalytic, photocatalytic, and electrochemical events occurring in the solid-state or on semiconductor surfaces.