“On”/“off” fluorescence intermittency of single semiconductor quantum dots

Abstract

Single molecule confocal microscopy is used to investigate the detailed kinetics of fluorescence intermittency in colloidal II–VI (CdSe) semiconductor quantum dots. Two distinct modes of behavior are observed corresponding to (i) sustained “on” episodes (τon) of rapid laser absorption/fluorescence cycling, followed by (ii) sustained “off” episodes (τoff) where essentially no light is emitted despite continuous laser excitation. Both on-time and off-time probability densities follow an inverse power law, P(τon/off)∝1/τon/offm, over more than seven decades in probability density and five decades in time. Such inverse power law behavior is an unambiguous signature of highly distributed kinetics with rates varying over 105-fold, in contrast with models for switching between “on” and “off” configurations of the system via single rate constant processes. The unprecedented dynamic range of the current data permits several kinetic models of fluorescence intermittency to be evaluated at the single molecule level and indicate the importance of fluctuations in the quantum dot environment.