Ultrafast Laser Studies of Two-Photon Excited Fluorescence Intermittency in Single CdSe/ZnS Quantum Dots.

Two-photon fluorescence microscopy of single quantum dots conditions has been reported by several groups, with contrasting observations regarding the kinetics and dynamics of fluorescence intermittency or "blinking". Here, we investigate the power dependence, kinetics, and statistics of two photon-excited fluorescence intermittency from single CdSe/ZnS quantum dots in a solid PMMA film as a function of sub-bandgap laser intensity at 800 nm. Fluorescence intermittency is observed at all excitation powers and a quadratic (n = 1.

Size-dependent photoionization in single CdSe/ZnS nanocrystals.

Fluorescence intermittency in single semiconductor nanocrystals has been shown to follow power law statistics over many decades in time and in probability. Recently, several studies have shown that, while "off" dwell times are insensitive to almost all experimental parameters, "on" dwell times exhibit a pump-power dependent exponential truncation at long times, suggestive of enhanced biexciton photoionization probabilities at high excitation powers. Here we report the dependence of this on-time truncation on nanocrystal radius.

Coverage-mediated suppression of blinking in solid state quantum dot conjugated organic composite nanostructures.

Size-correlated single-molecule fluorescence measurements on CdSe quantum dots functionalized with oligo(phenylene vinylene) (OPV) ligands exhibit modified fluorescence intermittency (blinking) statistics that are highly sensitive to the degree of ligand coverage on the quantum dot surface. As evidenced by a distinct surface height signature, fully covered CdSe-OPV nanostructures (approximately 25 ligands) show complete suppression of blinking in the solid state on an integration time scale of 1 s. Some access to dark states is observed on finer time scales (100 ms) with average persistence times significantly shorter than those from ZnS-capped CdSe quantum dots.