Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry.
We present all-dielectric gallium phosphide (GaP) nanoantennas as an e cient nanophotonic platform for surface-enhanced second harmonic generation (SHG) and uorescence (SEF), showing negligible losses in the visible range. Employing single GaP nanodisks, we observe an increase of more than three orders of magnitude in the SHG signal in comparison with the bulk. This constitutes an SHG e ciency as large as 0.0002%, which is, to the best of our knowledge, the highest yet achieved value produced by a single nano-object in the optical region. Furthermore, we show that GaP dimers with 35 nm gap can enhance up to 3600 times the uorescence emission of dyes located in the gap of the nanoantenna. This is accomplished by a uorescence lifetime reduction of, at least, 22 times, accompanied by a high intensity eld con nement in the gap region. These results open new avenues for low-loss nanophotonics in the optical regime.
Unique structural and optical properties of atomically thin two-dimensional semiconducting transition metal dichalcogenides enable in principle their efficient coupling to photonic cavities having the optical mode volume close to or below the diffraction limit. Recently, it has become possible to make all-dielectric nano-cavities with reduced mode volumes and negligible non-radiative losses. Here, we realise low-loss high-refractive-index dielectric gallium phosphide (GaP) nano-antennas with small mode volumes coupled to atomic mono- and bilayers of WSe. We observe a photoluminescence enhancement exceeding 10 compared with WSe placed on planar GaP, and trace its origin to a combination of enhancement of the spontaneous emission rate, favourable modification of the photoluminescence directionality and enhanced optical excitation efficiency. A further effect of the coupling is observed in the photoluminescence polarisation dependence and in the Raman scattering signal enhancement exceeding 10. Our findings reveal dielectric nano-antennas as a promising platform for engineering light-matter coupling in two-dimensional semiconductors.
A reduction in the number of loss decay channels present in optical nanoantennas could help enhance an emitter’s radiation efficiency. These losses get amplified for emitters in close proximity to metallic surfaces, such as for self-assembled monolayers, reducing the fluorescence rate. However, such a proximity strongly enhances Raman scattering. A dual-sensing scheme should bypass this shortcoming, and switching from metals to high refractive index dielectrics could aid in that direction. In order to show this, we fabricated silicon nanodimers and coated them with a β-carotenal monolayer for detecting surface-enhanced Raman scattering and fluorescence emission of the same probe. We obtained a surface-enhanced Raman scattering (SERS) factor of 1720 ± 300 for the C–C bond stretching of the polyene chain and a surface fluorescence enhancement (SEF) factor of 470 ± 90. Furthermore, our theoretical studies of different materials and emitters located on the surface of nanostructures demonstrate that low-loss dielectric materials provide a robust architecture for enhancing the response of efficient emitters. These results could have a direct impact on the development of deterministic high-rate single-photon sources.
Research on optically resonant dielectric nanostructures has accelerated the development of photonic applications, driven by their ability to strongly confine light on the nanoscale. However, as dielectric resonators are typically operated below their band gap to minimize optical losses, the usage of dielectric nanoantenna concepts for absorption enhancement has largely remained unexplored. In this work, we realize engineered nanoantennas composed of photocatalytic dielectrics and demonstrate increased light-harvesting capabilities in otherwise weakly absorptive spectral regions. In particular, we employ anapole excitations, which are known for their strong light confinement, in nanodisks of oxygen-vacancyrich TiO 2−x , a prominent photocatalyst that provides a powerful platform for exploring concepts in absorption enhancement in tunable nanostructures. The arising photocatalytic effect is monitored on the single particle level using the well-established photocatalytic silver reduction reaction on TiO 2 . With the freedom of changing the optical properties of TiO 2 through tuning the abundance of V O states, we discuss the interplay between cavity damping and the anapole-assisted field confinement for absorption enhancement. This concept is general and can be extended to other catalytic materials with higher refractive indices.
Atomically thin two-dimensional semiconducting transition metal dichalcogenides (TMDs) can withstand large levels of strain before their irreversible damage occurs. This unique property offers a promising route for control of the optical and electronic properties of TMDs, for instance, by depositing them on nanostructured surfaces, where position-dependent strain can be produced on the nanoscale. Here, we demonstrate strain-induced modifications of the optical properties of mono-and bilayer TMD WSe 2 placed on photonic nanoantennas made from gallium phosphide (GaP). Photoluminescence (PL) from the strained areas of the TMD layer is enhanced owing to the efficient coupling with the confined optical mode of the nanoantenna. Thus, by following the shift of the PL peak, we deduce the changes in the strain in WSe 2 deposited on the nanoantennas of different radii. In agreement with the presented theory, strain up to ≈1.4% is observed for WSe 2 monolayers. We also estimate that >3% strain is achieved in bilayers, accompanied by the emergence of a direct bandgap in this normally indirect-bandgap semiconductor. At cryogenic temperatures, we find evidence of the exciton confinement in the most strained nanoscale parts of the WSe 2 layers, as also predicted by our theoretical model. Our results of direct relevance for both dielectric and plasmonic nanoantennas, show that strain in atomically thin semiconductors can be used as an additional parameter for engineering light−matter interaction in nanophotonic devices.
We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order autocorrelation and cross-correlation functions show that the emitter is a single molecule and that the light emerging from the grating comes from that molecule. The coupling efficiency is found to be β W G = 11.6(1.5)%. This type of structure is promising for building new functionality into quantum-photonic circuits, where localised regions of strong emitter-guide coupling can be interconnected by low-loss dielectric guides.
Nanoscopic inspection of reactivity in single plasmonic photocatalysts.
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