Plasmonic effect on photon antibunching and blinking behavior of single quantum dots near gold nanoparticles

In this work, we investigated how the blinking statistics and the photon antibunching behavior of single CdSe/CdS core/shell quantum dots(QDs) get modified in the presence of gold nanoparticles(Au NPs) overcoated with a silica shell of varying thickness.(Au@SiO2). The Au@SiO2 NPs have distinct plasmon resonance peaks which overlap with the absorption and emission of QDs, thereby effectively increasing the mutual plasmon-exciton interactions between them. From the second-order photoluminescence intensity cross-correlation measurements, we observed that in the regime of low excitation power, the relative ratio of the biexciton/exciton (BX/X) quantum yield (QY) and lifetimes of the single QDs in presence of the plasmonic substrates get significantly modified as compared to the QDs on glass. An electrodynamics model was developed to further quantify the effect of plasmons on the emission intensity, QY and lifetimes of X and BX of single QDs. The theoretical studies also indicated that the relative position of the QDs and orientation of the electric field are the critical factors regulating the emission properties of Xs and BXs.

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