The fluorescence intermittency for quantum dots is not power-law distributed: a luminescence intensity resolved approach

ACS Nano. 2014 Apr 22;8(4):3506-21. doi: 10.1021/nn406562a. Epub 2014 Mar 7.

Abstract

The photoluminescence (PL) of single emitters like semiconductor quantum dots (QDs) shows PL intermittency, often called blinking. We explore the PL intensities of single CdSe/ZnS QDs in polystyrene (PS), on polyvenylalcohol (PVA), and on silicon oxide (SiOx) by the change-point analysis (CPA). By this, we relate results from the macrotime (sub-ms to 1000 s) and the microtime (0.1-100 ns) range to discrete PL intensities. We conclude that the intensity selected "on"-times in the ms range correspond to only a few (discrete) switching times, while the PL decays in the ns range are multiexponential even with respect to the same selected PL intensity. Both types of relaxation processes depend systematically on the PL intensity in course of a blinking time trace. The overall distribution of on-times does not follow a power law contrary to what has often been reported but can be compiled into 3-4 characteristic on-times. The results can be explained by the recently suggested multiple recombination centers model. Additionally, we can identify a well-defined QD state with a very low PL intensity above the noise level, which we assign to the strongly quenched exciton state. We describe our findings by a model of a hierarchical sequence of hole and electron trapping. Blinking events are the consequence of slow switching processes among these states and depend on the physicochemical properties of the heterogeneous nanointerface of the QDs.