Inverting asymmetric confinement potentials in core/thick-shell nanocrystals

We investigate CdSe/ZnSe core/thick-shell nanocrystals (a.k.a. giant-nanocrystal quantum dots [g-NQDs]) that have an asymmetric electron/hole confinement potential opposite to nonblinking CdSe/CdS g-NQDs. We deconstruct the photon streams into five different photoluminescence (PL) intensity levels and analyze second-order photon correlation (g⁽²⁾) traces of each PL intensity level. This analysis allows us to decouple the contribution of exciton charging from the g⁽²⁾ experiment and determine the quantum yield of neutral biexciton states to be in the range of ∼20-50%, a value comparable to that of CdSe/CdS g-NQDs. We also show that the Auger recombination rate of positive trion states is suppressed compared to that of negative trions. This suppression, however, is shown not to be strong enough to yield complete suppression of PL fluctuations due to the heavy effective mass of holes. Strong intensity fluctuations also result from the fact that hole charging occurs more readily in CdSe/ZnSe g-NQDs than electron charging in CdSe/CdS g-NQDs.