Abstract

Plasmonic excitation enhanced fluorescence of CdSe/ZnS core-shell quantum dots (QDs) in the presence of Au nanoparticles (NPs) has been studied for application in quantum dot solar concentrator (QDSC) devices. We observe that there is an optimal concentration of Au NPs that gives a maximum 53% fluorescence emission enhancement for the particular QD/Au NP composite studied. The optimal concentration depends on the coupling and spacing between neighboring QDs and Au NPs. We show the continuous transition from fluorescence enhancement to quenching, depending on Au NP concentration. The locally enhanced electromagnetic field induced by the surface plasmon resonance in the Au NPs leads to an increased excitation rate for the QDs. This is evidenced by excitation wavelength dependent fluorescence enhancement, where the locally enhanced field around the Au NPs is more pronounced close to the surface plasmon resonance (SPR) wavelength. However, at higher concentrations of Au NPs non-radiative energy transfer from the QDs to the Au NPs particles leads to a decrease of the emission, which is confirmed by detection of both a double exponential lifetime decay in, and a decrease in the lifetime of the QDs. The overall fluorescence emission enhancement depends on these competing effects; increased excitation rate and non-radiative energy transfer.

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