Design of metal/dielectric/nanocrystals core/shell/shell nano-structures for the fluorescence enhancement of cadmium-free semiconductor nanocrystals

Abstract

AgInS2-ZnS (ZAIS) quaternary semiconductors nanocrystals are versatile cadmium-free luminescent nanomaterials. Their broad emission spectrum and strong absorption make them ideal for the development of new white-LED devices taking advantage of nano-optical phenomena. We recently found strategies to increase the photoluminescence quantum yield of ZAIS nanocrystals up to 80%. In a second step toward high efficiency luminescent materials, we aim at increasing the net conversion efficiency of ZAIS nanocrystals by coupling them with metallic nano-antennae. Indeed, by grafting ZAIS nanocrystals onto carefully chosen metal/dielectric core/shell nanoparticles, both the absorption and emission processes can be tuned and enhanced. A finite-element simulation based on the discrete dipole approximation (DDA) was used to predict the nano-optical behavior of silver@oxide@ZAIS nanostructures. Desirable combinations of materials and geometry for the antennae were identified. A chemical method for the synthesis of the simulated nanostructures was developed. The coupling of ZAIS nanocrystals emission with the plasmonic structure is experimentally observed and is in accordance with our predictions.