Enhancement of the UV emission from gold/ZnO nanorods exhibiting no green luminescence

TL;DR

This study demonstrates a sixfold increase in UV emission from gold-coated ZnO nanorods through a defect-independent plasmonic mechanism, revealing a new excitonic relaxation pathway that enhances emission efficiency.

Contribution

It introduces a defect-free plasmonic enhancement method for ZnO UV emission using gold nanoparticles, bypassing the need for ZnO defect levels.

Findings

Sixfold UV emission enhancement achieved

New fast excitonic relaxation pathway identified

Charge transfer mechanism ruled out

Abstract

Large reflection losses at interfaces in light emitting semiconductor devices cause a significant reduction in their light emission and energy efficiencies. Metal nanoparticle (NP) surface coatings have been demonstrated to increase the light extraction efficiency from planar high refractive index semiconductor surfaces. This emission enhancement in Au NP-coated ZnO is widely attributed to involvement of a green (~ 2.5 eV) deep level ZnO defect exciting localized surface plasmons in the NPs that non-radiatively decay into hot electrons, which return to ZnO and radiatively recombine. In this work, we achieve a 6 times enhancement of the ultra-violet excitonic emission in ZnO nanorods that are coated with 5 nm Au NPs without the aid of ZnO defects. Cathodoluminescence (CL), photoluminescence (PL) and a novel concurrent CL-PL technique as well as time resolved PL spectroscopy revealed that the increase in UV emission is due to the formation of an additional fast excitonic relaxation pathway that increases the exciton spontaneous emission rate. Concurrent CL-PL measurements ruled out the presence of charge transfer mechanism in the emission enhancement process. While time resolved PL results confirmed the existence of a new excitonic recombination channel that is attributed to exciton relaxation via the plasmon-assisted excitation of rapid non-radiative Au interband transitions. Our results establish that ZnO defect levels ~ 2.5 eV are not required to facilitate Au NP induced enhancement of the ZnO UV emission.