Miniaturized fractal optical nanoantennas defined by focused helium ion beam milling.

It has been shown in the past that fractal geometries are beneficial for radio and communication antenna designs in terms of bandwidth and gain. Recently, this concept was extended to plasmonic nanoantennas. Here, we present a fabrication method based on electron beam lithography and focused helium ion beam milling to further miniaturize dimer nanoantennas of 0th, 1st and 2nd order Sierpinski fractals. With this state-of-the-art approach, it becomes feasible to experimentally move their resonance conditions into the sub-micron wavelength regime, while maintaining excellent pattern definition and achieving sub-10 nm gap sizes for high near-field enhancement. These highly sophisticated nanostructures are numerically simulated and analyzed by dark-field scattering spectroscopy to monitor the effects of the fractal structuring on the scattering spectra and near-field enhancement.

Coupling single quantum dots to plasmonic nanocones: optical properties.

Coupling a single quantum emitter, such as a fluorescent molecule or a quantum dot (QD), to a plasmonic nanostructure is an important issue in nano-optics and nano-spectroscopy, relevant for a wide range of applications, including tip-enhanced near-field optical microscopy, plasmon enhanced molecular sensing and spectroscopy, and nanophotonic amplifiers or nanolasers, to mention only a few. While the field enhancement of a sharp nanoantenna increasing the excitation rate of a very closely positioned single molecule or QD has been well investigated, the detailed physical mechanisms involved in the emission of a photon from such a system are, by far, less investigated. In one of our ongoing research projects, we try to address these issues by constructing and spectroscopically analysing geometrically simple hybrid heterostructures consisting of sharp gold cones with single quantum dots attached to the very tip apex. An important goal of this work is to tune the longitudinal plasmon resonance by adjusting the cones' geometry to the emission maximum of the core-shell CdSe/ZnS QDs at nominally 650 nm. Luminescence spectra of the bare cones, pure QDs and hybrid systems were distinguished successfully. In the next steps we will further investigate, experimentally and theoretically, the optical properties of the coupled systems in more detail, such as the fluorescence spectra, blinking statistics, and the current results on the fluorescence lifetimes, and compare them with uncoupled QDs to obtain a clearer picture of the radiative and non-radiative processes.

Nonlinear optical point light sources through field enhancement at metallic nanocones.

A stable nonlinear optical point light source is investigated, based on field enhancement at individual, pointed gold nanocones with sub-wavelength dimensions. Exciting these cones with near-infrared, focused radially polarized femtosecond beams allows for tip-emission at the second harmonic wavelength (second harmonic generation, SHG) in the visible range. In fact, gold nanocones with ultra-sharp tips possess interesting nonlinear optical (NLO) properties for SHG and two-photon photoluminescence (TPPL) emission, due to the enhanced electric field confinement at the tip apex combined with centrosymmetry breaking. Using two complementary optical setups for bottom or top illumination a sharp tip SHG emission is discriminated from the broad TPPL background continuum. Moreover, comparing the experiments with theoretical calculations manifests that these NLO signatures originate either from the tip apex or the base edge of the nanocones, clearly depending on the cone size, the surrounding medium, and illumination conditions. Finally, it is demonstrated that the tip-emitted signal vanishes when switching from radial to azimuthal polarization.

Parallel fabrication of plasmonic nanocone sensing arrays.

A fully parallel approach for the fabrication of arrays of metallic nanocones and triangular nanopyramids is presented. Different processes utilizing nanosphere lithography for the creation of etch masks are developed. Monolayers of spheres are reduced in size and directly used as masks, or mono- and double layers are employed as templates for the deposition of aluminum oxide masks. The masks are transferred into an underlying gold or silver layer by argon ion milling, which leads to nanocones or nanopyramids with very sharp tips. Near the tips the enhancement of an external electromagnetic field is particularly strong. This fact is confirmed by numerical simulations and by luminescence imaging in a confocal microscope. Such localized strong fields can amongst others be utilized for high-resolution, high-sensitivity spectroscopy and sensing of molecules near the tip. Arrays of such plasmonic nanostructures thus constitute controllable platforms for surface-enhanced Raman spectroscopy. A thin film of pentacene molecules is evaporated onto both nanocone and nanopyramid substrates, and the observed Raman enhancement is evaluated.

Plasmonic mode conversion in individual tilted 3D nanostructures.

We investigate mode conversion in 3D asymmetric nanocones using angle-dependent linear optical spectroscopy and second-harmonic generation microscopy supported by corresponding simulations. The results prove the efficient excitation of the plasmonic out-of-plane mode that enhances the electric near-field at the sharp tip. Furthermore, we introduce two advanced fabrication processes including either etch mask transfer by tilted etching into a metallic layer or tilted electron-beam lithography followed by tilted evaporation and lift-off. These processes enable the fabrication of tilted nanostructures which can be optimized for a given purpose. The combination of the optical properties and the introduced fabrication processes enables a new design of plasmonic nanostructures for ultra-compact sensors or photon sources.

Continuous reversible tuning of the gap size and plasmonic coupling of bow tie nanoantennas on flexible substrates.

As a multifunctional device for sensing experiments and fundamental research, tailor-made plasmonic nanostructures with continuously tunable resonances are created by preparing bow tie-shaped nanostructures on a flexible substrate. The bow ties are fabricated by electron beam lithography on a chromium sacrificial layer and transferred to a polydimethylsiloxane (PDMS) substrate. The structures on PDMS are analyzed by reflection dark-field spectroscopy and scanning electron microscopy. Dark-field spectra of individual nano-antennas are obtained while the substrate is relaxed, and while strain is applied and the substrate is elastically stretched. Depending on the alignment of the bow ties relative to the direction of the strain, the deformation of the substrates leads to an increase or decrease of the nanostructure gaps, and therefore to a fully reversible decrease or increase of the antenna coupling, respectively. The continuous change in coupling is visible as a blue-shift in the resonance of the coupling mode for increasing gap widths, and a red-shift for decreasing gap widths. This configuration offers interesting perspectives for molecular transport and sensing investigations under variable coupling conditions as well as for tunable SERS substrates and optical strain sensor applications. In particular, very narrow gaps are within reach in the transversal configuration.

Self-aligned placement and detection of quantum dots on the tips of individual conical plasmonic nanostructures.

Hybrid structures of few or single quantum dots (QDs) coupled to single optical antennas are of prime interest for nano-optical research. The photoluminescence (PL) signal from single nanoemitters, such as QDs, can be enhanced, and their emission characteristics modified, by coupling them to plasmonic nanostructures. Here, a self-aligned technique for placing nanoscale QDs with about 10 nm lateral accuracy and well-defined molecular distances to the tips of individual nanocones is reported. This way the QDs are positioned exactly in the high near-field region that can be created near the cone apex. The cones are excited in the focus of a radially polarized laser beam and the PL signal of few or single QDs on the cone tips is spectrally detected.

A single particle plasmon resonance study of 3D conical nanoantennas.

Metallic nanocones are well-suited optical antennas for near-field microscopy and spectroscopy, exhibiting a number of different plasmonic modes. A major challenge in using nanocones for many applications is maximizing the signal at the tip while minimizing the background from the base. It is shown that nanocone plasmon resonance properties can be shifted over a wide range of wavelengths by variation of the substrate, material, size and shape, enabling potential control over specific modes and field distributions. The individual resonances are identified and studied by correlated single particle dark field scattering and scanning electron microscopy in combination with numerical simulations.