Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.

ZnO nanowire arrays were functionalized with colloidal CdSe quantum dots stabilized by 3-mercaptopropionic acid to form hybrid devices. The photoconductivity of the nanowire/quantum-dot devices was studied under selective photoexcitation of the quantum dots, and it was found that the dynamics strongly depend on the gas environment. Desorption of surface oxygen from both the ZnO nanowires and the CdSe quantum dots, activated by electron tunnelling between the nanowires and the quantum dots, is found to be the dominating process that determines the dynamics of the photoconductivity in the hybrid nanowire/quantum-dot devices.

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Surface plasmon polaritons (SPPs) are shortlived evanescent waves that can confine light at the surface of metallic nanostructures and transport energy over mesoscopic distances. They may be used to generate and process information encoded as optical signals to realize nanometerscale and ultrafast all-optical circuitry. The propagation properties of these SPPs are defined by the geometry and composition of the nanostructure. Due to their short, femtosecond lifetimes, it has so far proven difficult to track this propagation in the time domain and to directly study the effect of the propagation on the shape of a coherent SPP wavepacket. Here, we introduce an ultrabroadband far-field spectral interferometry method, allowing for the reconstruction of the plasmonic field in the time domain, to characterize coherent SPP propagation in metallic nanostructures. Group velocity and dispersion of SPPs are determined with high precision in a broad frequency range in the visible and near-infrared region, and the propagating SPP field is tracked with high time resolution over distances of tens of micrometers. Our results shed new light on the interplay between nanostructure geometry and coherent SPP propagation and hence are important for probing plasmon−matter interactions as well as for implementations of ultrafast plasmonic circuitry.

The excitation-intensity dependence of the excitonic near-band-edge emission (NBE) and deep-level related emission (DLE) bands in ZnO nanowires and bulk crystals is studied, which show distinctly different power laws. The behavior can be well explained with a rate-equation model taking into account deep donor and acceptor levels with certain capture cross sections for electrons from the conduction band and different radiative lifetimes. In addition, a further crucial ingredient of this model is the background n-type doping concentration inherent in almost all ZnO single crystals. The interplay of the deep defects and the background free-electron concentration in the conduction band at room temperature reproduces the experimental results well over a wide range of excitation intensities (almost five orders of magnitude). The results demonstrate that for many ZnO bulk samples and nanostructures, the relative intensity R = INBE/IDLE can be adjusted over a wide range by varying the excitation intensity, thus, showing that R should not be taken as an indicator for the crystalline quality of ZnO samples unless absolute photoluminescence intensities under calibrated excitation conditions are compared. On the other hand, the results establish an all-optical technique to determine the relative doping levels in different ZnO samples by measuring the excitation-intensity dependence of the UV and visible luminescence bands.