Abstract
In this work, we performed a systematic study on a hybrid plasmonic system to elucidate a new insight into the mechanisms governing the fluorescent enhancement process. Our lithographically defined plasmonic nanodisks with various diameters act as receiver and transmitter nano-antennas to outcouple efficiently the photoluminescence of the coupled dye molecules. We show that the enhancement of the spontaneous emission rate arises from the superposition of three principal phenomena: (i) metal enhanced fluorescence, (ii) metal enhanced excitation and (iii) plasmon-modulated photoluminescence of the photoexcited nanostructures. Overall, the observed enhanced emission is attributed to the bi-directional near-field coupling of the fluorescent dye molecules to the localized plasmonic field of nano-antennas. We identify the role of exciton–plasmon coupling in the recombination rate of the sp-band electrons with d-band holes, resulting in the generation of particle plasmons. According to our comprehensive experimental analyses, the mismatch between the enhanced emission and the emission spectrum of the uncoupled dye molecules is attributed to the plasmon-modulated photoluminescence of the photoexcited hybrid plasmonic system.
Highlights
The control over the spontaneous emission rate of a single quantum emitter (QE) has attracted particular interest, since it provides a powerful multifunctional tool for different promising applications [1,2,3,4,5]
This can be achieved by overlapping the localized surface plasmons (LSPs) mode of a plasmonic cavity with resonating mode of a QE, which is oscillating at the same polarization of the plasmonic cavity [19,20,21]
We explored different underlying mechanisms related to the observed emission enhancement in our designed plasmonic hybrid systems
Summary
The control over the spontaneous emission rate of a single quantum emitter (QE) has attracted particular interest, since it provides a powerful multifunctional tool for different promising applications [1,2,3,4,5]. In an engineered hybrid plasmonic system, the near-field coupling of an excitonic element to the enhanced local field of the plasmonic nano-antenna may speed up the radiative decay rate [15,16,17,18]. This can be achieved by overlapping the LSP mode of a plasmonic cavity with resonating mode of a QE, which is oscillating at the same polarization of the plasmonic cavity [19,20,21]. Such optimization can be done by changing the shape, size, composition and arrangement of the nano-resonators
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