Martin Esmann

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.

Excitation of Mesoscopic Plasmonic Tapers by Relativistic Electrons: Phase Matching versus Eigenmode Resonances

We investigate the optical modes in three-dimensional single-crystalline gold tapers by means of electron energy-loss spectroscopy. At the very proximity to the apex, a broad-band excitation at all photon energies from 0.75 to 2 eV, which is the onset for interband transitions, is detected. At large distances from the apex, though, we observe distinct resonances with energy dispersions roughly proportional to the inverse local radius. The nature of these phenomena is unraveled by finite difference time-domain simulations of the taper and an analytical treatment of the energy loss in fibers. Our calculations and the perfect agreement with our experimental results demonstrate the importance of phase-matching between electron field and radiative taper modes in mesoscopic structures. The local taper radius at the electron impact location determines the selective excitation of radiative modes with discrete angular momenta.

k-space imaging of the eigenmodes of sharp gold tapers for scanning near-field optical microscopy

Summary We investigate the radiation patterns of sharp conical gold tapers, which were designed as adiabatic nanofocusing probes for scanning near-field optical microscopy (SNOM). Field calculations show that only the lowest order eigenmode of such a taper can reach the very apex and thus induce the generation of strongly enhanced near-field signals. Higher-order modes are coupled into the far field at finite distances from the apex. Here, we demonstrate experimentally how to distinguish and separate between the lowest and higher-order eigenmodes of such a metallic taper by filtering in the spatial frequency domain. Our approach has the potential to considerably improve the signal-to-background ratio in spectroscopic experiments at the nanoscale.

Wave front adaptation using a deformable mirror for adiabatic nanofocusing along an ultrasharp gold taper

We describe and demonstrate the use of an adaptive wave front optimization scheme for enhancing the efficiency of adiabatic nanofocusing of surface plasmon polariton (SPP) waves along an ultrasharp conical gold taper. Adiabatic nanofocusing is an emerging and promising scheme for controlled focusing of far field light into nanometric volumes. It comprises three essential steps: SPP excitation by coupling far field light to an SPP waveguide, SPP propagation along the waveguide and adiabatic SPP nanofocusing towards a geometric singularity. For commonly used complex waveguide geometries, such as, e.g., conical metal tapers, a realistic modeling and efficiency optimization is challenging. Here, we use a deformable mirror to adaptively control the wave front of the incident far field light. We demonstrate an eight-fold enhancement in nanofocusing efficiency and analyze the shape of the resulting optimized wave front. The introduced wave front optimization scheme is of general interest for guiding and controlling light on the nanoscale.

Plasmonic nanofocusing – grey holes for light

Abstract Improving the resolution and sensitivity in all-optical microscopy and spectroscopy is inevitably one of the most important challenges in contemporary optical and nanoscience. Here, we discuss a novel approach, plasmonic nanofocusing, towards broadband, coherent all-optical microscopy with ultrahigh temporal and spatial resolution. The conceptual idea is to launch radially symmetric surface plasmon polariton modes onto the shaft of a sharp, conical metal taper. While propagating towards the apex of the pointed taper, the spatial extent of the plasmonic mode gradually shrinks, from several microns in diameter to a spot size of less than 10 nm at the pointed apex of the conical taper. Concomitantly, the local field amplitude of the plasmon mode gradually increases, resulting in a pronounced field enhancement at the apex and – thus – a bright and spatially isolated coherent light source with dimensions far below the diffraction limit. In this review, we characterize the optical properties of such three-dimensional conical metal tapers and demonstrate nanofocusing of radially symmetric plasmon modes. We use this nanolight source for coherent light scattering spectroscopy and demonstrate the sensitivity enhancement resulting from the pronounced spatial field confinement. It is shown that such off-resonant plasmonic nanoantennas facilitate the creation of nanofocused light spots with few-cycle time resolution. As a first application of this ability to nanolocalize ultrashort plasmon wavepackets, we demonstrate remotely-triggered multiphoton-induced photoemission from the very apex of the taper and implement this novel ultrafast electron gun in a point-projection electron microscope. Our results not only indicate the favourable optical properties of this plasmonic nanolens but also suggest that it may find interesting applications in ultrafast scanning optical spectroscopy and might enable new types of ultrafast electron holography and scanning tunnelling microscopy.

Real-space Imaging of Plasmonic Modes of Gold Tapers by EFTEM and EELS

Plasmonic nanoparticles have been extensively studied in the literature due to their ability of supporting localized surface plasmon (LSP) modes. Such structures can localize optical energy on the nanometer scale which opens up the field of optical nanoantennas. Application of nanoantennas in ultrafast optics requires large bandwidth. Unfortunately, the bandwidths of presently realized nanoantennas are small, despite their large radiative and Ohmic losses. Moreover, the coupling efficiency of far-field optical radiation to single nanoantennas is quite low, which is because of the extremely small volume of interaction.

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.

Interaction between Relativistic Electrons and Mesoscopic Plasmonic Tapers

Plasmonic metallic tapers with conical shapes are one of the most common and simple structures, with concomitant capabilities of nanofocusing and strong field enhancement. Such tapers can serve either as waveguides or nanoantennas in near-field scanning optical microscopy and as a ultrafast photoemission point source in electron microscopy [1]. Electron energy-loss spectroscopy (EELS) is exploited to comprehensively study the plasmonic response of mesoscopic tapers in a wide energy range. However, the interpretation of EELS signatures is intricate by the fact that different resonance mechanisms are active when relativistic electrons interact with mesoscopic plasmonic tapers, namely phase matching [2] and reflection [3] (Fig.1a). It is of fundamental importance to clarify the reasons behind the EELS resonances explicitly.

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.

Plasmons in Mesoscopic Gold Tapers

The ability of metallic nanostructures to sustain localized surface plasmons (LSPs) makes them essential elements of future nanophotonic devices. The optical fields associated with these LSPs are concentrated in volumes much smaller than allowed by the diffraction limit and the field distribution and resonance energies depend critically on the size and shape of the nanostructure. Of particular interest are structures that allow optical fields to be steered (waveguides) or concentrated and focused to a certain position. An additional requirement for applications is a broad bandwidth and low radiative losses of such structures. Some of these requirements can be met by metallic tapers [1, 2].