Long-range coupling of individual quantum dots with plasmonic nanoparticles in a thin-film hybrid material

Abstract

Semiconductor quantum dots (QDs) are widely used in photovoltaic and optoelectronic devices due to their unique optical properties. Photoluminescence (PL) properties of QDs can be significantly improved by their electromagnetic coupling with plasmonic nanoparticles (PNPs). The excitation of resonant localized plasmon modes leads to the enhancement of the density of photon states and increase of electromagnetic field near the surface of PNPs, what boosts the acceleration of the exciton radiative decay, known as the Purcell effect. To study the dependence of the degree of acceleration of radiative decay rate (Purcell factor) on the distance between QDs and PNPs, we fabricated thin-film hybrid structures based on CdSe(core)/ZnS/CdS/ZnS(multishell) QDs and silver or gold PNPs with a controllable distance between these components. The change in the radiative decay rate of excitons was calculated from the PL intensities and lifetimes before and after the deposition of PNPs on top of the QD thin film covered by a poly(methyl methacrylate) (PMMA) spacer. For both PNP types, the PL lifetime of underlying QDs decreased, whereas the PL intensity of the latter decreased only slightly for gold PNPs and even increased for silver PNPs. This indicates the acceleration of QDs radiative decay (Purcell effect) mediated by exciton-plasmon interaction. The Purcell factor was higher for silver PNPs than that for gold PNPs, what can be explained by the better spectral overlap between the QDs PL band and silver PNPs absorbance and the absence of interband absorption in silver at the wavelength of QDs PL. The results of this study provide better understanding of the Purcell effects in hybrid materials based on QDs and PNPs.