Enhancement in the excitonic spontaneous emission rates for Si nanocrystal multi-layers covered with thin films of Au, Ag, and Al

Abstract

The enhancement in the spontaneous emission rate (SER) for Ag, Au, and Al films on multilayer Si nanocrystals (SiNCs) was probed with time-resolved cathodoluminescence (CL). The SiNCs were grown on Si(100) using plasma enhanced chemical vapor deposition. Electron-hole pairs were generated in the metal-covered SiNCs by injecting a pulsed high-energy electron beam through the thin metal films, which is found to be an ideal method of excitation for plasmonic quantum heterostructures and nanostructures that are opaque to laser or light excitation. Spatially, spectrally, and temporally resolved CL was used to measure the excitonic lifetime of the SiNCs in metal-covered and bare regions of the same samples. The observed enhancement in the SER for the metal-covered SiNCs, relative to the SER for the bare sample, is attributed to a coupling of the SiNC excitons with surface plasmon polaritons (SPPs) of the thin metal films. A maximum SER enhancement of ∼2.0, 1.4 and 1.2 was observed for the Ag, Au, and Al films, respectively, at a temperature of 55 K. The three chosen plasmonic metals of Ag, Au, and Al facilitate an interesting comparison of the exciton-SPP coupling for metal films that exhibit varying differences between the surface plasmon energy, ω(sp), and the SiNC excitonic emission energy. A modeling of the temperature dependence of the Purcell enhancement factor, Fp, was performed and included the temperature dependence of the dielectric properties of the metals.