Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy

Biexciton photoluminescence (PL) quantum yields (Q2X) of individual CdSe/CdS core-shell nanocrystal quantum dots with various shell thicknesses are derived from independent PL saturation and two-photon correlation measurements. We observe a near-unity Q{sub 2X} for some nanocrystals with an ultrathick 19-monolayer shell. High Q2X’s are, however, not universal and vary widely among nominally identical nanocrystals indicating a significant dependence of Q2X upon subtle structural differences. Interestingly, our measurements indicate that high Q2X’s are not required to achieve complete suppression of PL intensity fluctuations in individual nanocrystals.