Effect of shell thickness and composition on blinking suppression and the blinking mechanism in 'giant' CdSe/CdS nanocrystal quantum dots

We recently developed an inorganic shell approach for suppressing blinking in nanocrystal quantum dots (NQDs) that has the potential to dramatically improve the utility of these fluorophores for single-NOD tracking of individual molecules in cell biology. Here, we consider in detail the effect of shell thickness and composition on blinking suppression, focusing on the CdSe/CdS core/shell system. We also discuss the blinking mechanism as understood through profoundly altered blinking statistics. We clarify the dependence of blinking behavior and photostability on shell thickness, as well as on interrogation times. We show that, while the thickest-shell systems afford the greatest advantages in terms of enhanced optical properties, thinner-shell NQDs may be adequate for certain applications requiring relatively shorter interrogation times. Shell thickness also determines the sensitivity of the NOD optical properties to aqueous-phase transfer, a critical step in rendering NQDs compatible with bioimaging applications. Lastly, we provide a proof-of-concept demonstration of the utility of these unique NQDs for fluorescent particle tracking. [GRAPHICS] High-resolution image of an ultra-thick-shell 'giant' nanocrystal quantum dot (left). Suppressed blinking behavior afforded by this class of semiconductor nanocrystal yields new statistical relationships in the probability densities of fluorescence on- and off-time distributions (right).