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Three-dimensional chiral plasmonic nanostructures have been shown to be able to dramatically boost photon-spin selective light-matter interactions, potentially leading to novel photonics, molecular spectroscopy, and light-harvesting applications based on circularly polarized light. Here, we show that chiral split-ring gold nanoresonators interfaced to a wide band gap semiconductor exhibit a contrast in hot-electron transfer rate between left-handed and right-handed visible light that essentially mimics the far-field circular dichroism of the structures. We trace down the origin of this effect to the differential excitation of the thinnest part of the split-ring structures using dichroic-sensitive cathodoluminescence imaging with nanometer spatial resolution. The results highlight the intricate interplay between the near-field and far-field chiral response of a nanostructure and establishes a clear link to the emerging field of hot carrier plasmonics with numerous potential applications in photocatalysis and solar light harvesting.

Emission of photoexcited hot electrons from plasmonic metal nanostructures to semiconductors is key to a number of proposed nanophotonics technologies for solar harvesting, water splitting, photocatalysis, and a variety of optical sensing and photodetector applications. Favorable materials and catalytic properties make systems based on gold and TiO2 particularly interesting, but the internal photoemission efficiency for visible light is low because of the wide bandgap of the semiconductor. We investigated the incident photon-to-electron conversion efficiency of thin TiO2 films decorated with Au nanodisk antennas in an electrochemical circuit and found that incorporation of a Au mirror beneath the semiconductor amplified the photoresponse for light with wavelength λ = 500–950 nm by a factor 2–10 compared to identical structures lacking the mirror component. Classical electrodynamics simulations showed that the enhancement effect is caused by a favorable interplay between localized surface plasmon excitatio...

Emission of photoexcited hot electrons from plasmonic metal nanostructures to semiconductors is key to a number of proposed nanophotonics technologies for solar harvesting, water splitting, photocatalysis, and a variety of optical sensing and photodetector applications. Favorable materials and catalytic properties make systems based on gold and TiO2 particularly interesting, but the internal photoemission efficiency for visible light is low because of the wide bandgap of the semiconductor. We investigated the incident photon-to-electron conversion efficiency of thin TiO2 films decorated with Au nanodisk antennas in an electrochemical circuit and found that incorporation of a Au mirror beneath the semiconductor amplified the photoresponse for light with wavelength λ = 500-950 nm by a factor 2-10 compared to identical structures lacking the mirror component. Classical electrodynamics simulations showed that the enhancement effect is caused by a favorable interplay between localized surface plasmon excitations and cavity modes that together amplify the light absorption in the Au/TiO2 interface. The experimentally determined internal quantum efficiency for hot electron transfer decreases monotonically with wavelength, similar to the probability for interband excitations with energy higher than the Schottky barrier obtained from a density functional theory band structure simulation of a thin Au/TiO2 slab.

Using polarization dependent scattering spectroscopy, we investigate plasmon propagation on branched silver nanowires. By controlling the polarization of the incident laser light, the wire plasmons can be routed into different wire branches and result in light emission from the corresponding wire ends. This routing behavior is found to be strongly dependent on the wavelength of light. Thus for certain incident polarizations, light of different wavelength will be routed into different branches. The branched nanowire can thus serve as a controllable router and multiplexer in integrated plasmonic circuits.

Nanowire plasmons can be launched by illumination at one terminus of the nanowire and emission can be detected at the other end of the wire. Using polarization dependent dark-field scattering spectroscopy, we measure how the polarization of the emitted light depends on the polarization of the incident light. We observe that the shape of the nanowire termination plays an important role in determining this polarization change. Depending on termination shape, a nanowire can serve as either a polarization-maintaining waveguide, or as a polarization-rotating, nanoscale half-wave plate. The understanding of how plasmonic waveguiding influence the polarization of the guided light is important for optimizing the structure of integrated plasmonic devices.

Using propagating plasmons on silver nanowires as an excitation source we perform surface-enhanced Raman scattering (SERS) at a nanoparticle/wire junction located remotely from the laser illumination spot with sensitivities in a few molecules range. Simultaneous multisite remote-excitation SERS sensing can also be achieved.