Quantum Dot Photoluminescence Activation and Decay: Dark, Bright, and Reversible Populations in ZnS-Capped CdSe Nanocrystals

Semiconductor nanocrystals or quantum dots (QDs) exhibit a number of unique optical properties including fluorescence intermittency (FI), photoluminescence (PL) enhancement, and darkening. Here we report PL activation (PLA) and darkening over populations of single colloidal ZnS-capped CdSe QDs under continuous illumination, which is described well by a simple consecutive elementary reaction (CER) scheme in the 1 to 10 kW cm–2 excitation intensity regime. The scheme allows determination of rate constants for both fluorescence activation and decay processes as well as the measurement of initial bright, fluorescent and dark, nonfluorescent QD fractions. The latter parameters can function as a “quality control” on the total population of detectable QDs in an imaging experiment or a synthesis. We further show reversible PLA at low intensities