Martin Silies

Toward Plasmonics with Nanometer Precision: Nonlinear Optics of Helium-Ion Milled Gold Nanoantennas

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.

Ultrasmall bullets of light--focusing few-cycle light pulses to the diffraction limit.

We demonstrate an essentially dispersion-free and diffraction-limited focusing of few-cycle laser pulses through all-reflective microscope objectives. By transmitting 6-fs-pulses from a Ti:sapphire oscillator through an all-reflective 0.5 NA objective, we reach a focus with a beam diameter of 1.0 µm, preserving the time structure of the pulses. The temporal and spatial pulse profile is recorded simultaneously using a novel tip-enhanced electron emission autocorrelator, indicating a focal volume of these pulses of only 1.8 µm3. We anticipate that the demonstrated technique is of considerable interest for inducing and probing optical nonlinearities of individual nanostructures.

Distinguishing between ultrafast optical harmonic generation and multi-photon-induced luminescence from ZnO thin films by frequency-resolved interferometric autocorrelation microscopy.

The nonlinear optical properties of thin ZnO film are studied using interferometric autocorrelation (IFRAC) microscopy. Ultrafast, below-bandgap excitation with 6-fs laser pulses at 800 nm focused to a spot size of 1 µm results in two emission bands in the blue and blue-green spectral region with distinctly different coherence properties. We show that an analysis of the wavelength-dependence of the interference fringes in the IFRAC signal allows for an unambiguous assignment of these bands as coherent second harmonic emission and incoherent, multiphoton-induced photoluminescence, respectively. More generally our analysis shows that IFRAC allows for a complete characterization of the coherence properties of the nonlinear optical emission from nanostructures in a single-beam experiment. Since this technique combines a very high temporal and spatial resolution we anticipate broad applications in nonlinear nano-optics.

Suppression of Radiative Damping and Enhancement of Second Harmonic Generation in Bull’s Eye Nanoresonators

We report a drastic increase of the damping time of plasmonic eigenmodes in resonant bulls eye (BE) nanoresonators to more than 35 fs. This is achieved by tailoring the groove depth of the resonator and by coupling the confined plasmonic field in the aperture to an extended resonator mode such that spatial coherence is preserved over distances of more than 10 μm. Experimentally, this is demonstrated by probing the plasmon dynamics at the field level using broadband spectral interferometry. The nanoresonator allows us to efficiently concentrate the incident field inside the central aperture of the BE and to tailor its local optical nonlinearity by varying the aperture geometry. By replacing the central circular hole with an annular ring structure, we obtain 50-times higher second harmonic generation efficiency, allowing us to demonstrate the efficient concentration of long-lived plasmonic modes inside nanoapertures by interferometric frequency-resolved autocorrelation. Such a light concentration in a nanoresonator with high quality factor has high potential for sensing and coherent control of light-matter interactions on the nanoscale.

Fourier-transform spatial modulation spectroscopy of single gold nanorods

Abstract Sensing the scattered fields of single metallic nanostructures is a crucial step towards the applications of isolated plasmonic antennas, such as for the sensing of single molecules or nanoparticles. In the past, both near- and far-field spectroscopy methods have been applied to monitor single plasmonic resonances. So far, however, these spectral-domain techniques do not yet provide the femtosecond time resolution that is needed to probe the dynamics of plasmonic fields in the time domain. Here, we introduce a time-domain technique that combines broadband Fourier-transform spectroscopy and spatial modulation spectroscopy (FT-SMS) to quantitatively measure the extinction spectra of the isolated gold nanorods with a nominal footprint of 41×10 nm2. Using a phase-stable pulse pair for excitation, the technique is capable of rejecting off-resonant stray fields and providing absolute measurements of the extinction cross section. Our results indicate that the method is well suited for measuring the optical response of strongly coupled hybrid systems with high signal-to-noise ratio. It may form the basis for new approaches towards time-domain spectroscopy of single nanoantennas with few-cycle time resolution.

Ultrafast third-harmonic spectroscopy of single nanoantennas fabricated using helium-ion beam lithography

Metallic nanoantennas are able to spatially localize far-field electromagnetic waves on a few nanometer length scale in the form of surface plasmon excitations 1-3. Standard tools for fabricating bowtie and rod antennas with sub-20 nm feature sizes are Electron Beam Lithography or Ga-based Focused Ion Beam (FIB) Milling. These structures, however, often suffer from surface roughness and hence show only a limited optical polarization contrast and therefore a limited electric field localization. Here, we combine Ga- and He-ion based milling (HIM) for the fabrication of gold bowtie and rod antennas with gap sizes of less than 6 nm combined with a high aspect ratio. Using polarization-sensitive Third-Harmonic (TH) spectroscopy, we compare the nonlinear optical properties of single HIM-antennas with sub-6-nm gaps with those produced by standard Ga-based FIB. We find a pronounced enhancement of the total TH intensity of more than three in comparison to Ga-FIB antennas and a highly improved polarization contrast of the TH intensity of 250:1 for Heion produced antennas 4. These findings combined with Finite-Element Method calculations demonstrate a field enhancement of up to one hundred in the few-nanometer gap of the antenna. This makes He-ion beam milling a highly attractive and promising new tool for the fabrication of plasmonic nanoantennas with few-nanometer feature sizes.