Excitation Wavelength-Dependent Photoluminescence Decay of Hybrid Gold/Quantum Dot Nanostructures

Hybrid nanostructures comprised of metal nanoparticles (MNPs) and quantum dots (QDs) have been found to exhibit unique, new optical properties due to the interaction that occurs between the MNPs and QDs. The aim of this work is to understand how the exciton-plasmon interaction in these systems is dependent on the excitation wavelength. The nanoassemblies consisted of gold (Au) NPs coated in a silica (SiO₂) shell of a controlled thickness and core/shell CdSe/CdS QDs adsorbed onto the SiO₂ shells. Our findings show that the photoluminescence lifetimes of the hybrid constructs are dependent on the excitation wavelength relative to the localized surface plasmon resonance (LSPR) of the Au NPs. When the excitation wavelength is closer to the LSPR, the photoluminescence decay of the hybrid structures is faster. We demonstrate that by tuning the excitation wavelength close to the resonance, there is an enhancement in the exciton-plasmon coupling between the Au NPs and QDs resulting in a shortening in the QD photoluminescence lifetime. We then propose a possible mechanism to explain this excitation wavelength-dependent phenomenon.