Microsecond Blinking Events in the Fluorescence of Colloidal Quantum Dots Revealed by Correlation Analysis on Preselected Photons

Abstract

Nearly all colloidal quantum dots, when measured at the single-emitter level, exhibit fluorescence "blinking". However, despite over 20 years of research on this phenomenon, its microscopic origins are still debated. One reason is a gap in available experimental information, specifically for dynamics at short (submillisecond) time scales. Here, we use photon-correlation analysis to investigate microsecond blinking events in individual quantum dots. While the strongly distributed kinetics of blinking normally makes such events difficult to study, we show that they can be analyzed by excluding photons emitted during long bright or dark periods. Moreover, we find that submillisecond blinking events are more common than one might expect from extrapolating the power-law blinking statistics observed on longer (millisecond) time scales. This result provides important experimental data for developing a microscopic understanding of blinking. More generally, our method offers a simple strategy for analyzing microsecond switching dynamics in the fluorescence of quantum emitters.