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Phys Rev Lett. 2011 May 6;106(18):187401. Epub 2011 May 3.

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

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Chemistry Division, Los Alamos National Laboratory, New Mexico 87545, USA.


Biexciton photoluminescence (PL) quantum yields (Q(2X)) 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(2X) for some nanocrystals with an ultrathick 19-monolayer shell. High Q(2X)'s are, however, not universal and vary widely among nominally identical nanocrystals indicating a significant dependence of Q(2X) upon subtle structural differences. Interestingly, our measurements indicate that high Q(2X)'s are not required to achieve complete suppression of PL intensity fluctuations in individual nanocrystals.

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