Site-selective functionalization of in-plane nanoelectrode-antennas.

Stacked organic optoelectronic devices make use of electrode materials with different work functions, leading to efficient large area light emission. In contrast, lateral electrode arrangements offer the possibility to be shaped as resonant optical antennas, radiating light from subwavelength volumes. However, tailoring electronic interface properties of laterally arranged electrodes with nanoscale gaps - to e.g. optimize charge-carrier injection - is rather challenging, yet crucial for further development of highly efficient nanolight sources. Here, we demonstrate site-selective functionalization of laterally arranged micro- and nanoelectrodes by means of different self-assembled monolayers. Upon applying an electric potential across nanoscale gaps, surface-bound molecules are removed selectively from specific electrodes by oxidative desorption. Kelvin-probe force microscopy as well as photoluminescence measurements are employed to verify the success of our approach. Moreover, we obtain asymmetric current-voltage characteristics for metal-organic devices in which just one of the electrodes is coated with 1-octadecanethiol; further demonstrating the potential to tune interface properties of nanoscale objects. Our technique paves the way for laterally arranged optoelectronic devices based on selectively engineered nanoscale interfaces and in principle enables molecular assembly with defined orientation in metallic nano-gaps.

Tunable Nanoplasmonic Photodetectors.

Visible and infrared photons can be detected with a broadband response via the internal photoeffect. By use of plasmonic nanostructures, i.e., nanoantennas, wavelength selectivity can be introduced to such detectors through geometry-dependent resonances. Also, additional functionality, like electronic responsivity switching and polarization detection, has been realized. However, previous devices consisted of large arrays of nanostructures to achieve detectable photocurrents. Here we show that this concept can be scaled down to a single antenna level, resulting in detector dimensions well below the resonance wavelength of the device. Our design consists of a single electrically connected plasmonic nanoantenna covered with a wide-bandgap semiconductor allowing broadband photodetection in the visible/near-infrared via injection of hot carriers. We demonstrate electrical switching of the color sensitivity as well as polarization detection. Our results hold promise for the realization of ultrasmall photodetectors with advanced functionality.

Color-Switchable Subwavelength Organic Light-Emitting Antennas.

Future photonic devices require efficient, multifunctional, electrically driven light sources with directional emission properties and subwavelength dimensions. Electrically driven plasmonic nanoantennas have been demonstrated as enabling technology. Here, we present the concept of a nanoscale organic light-emitting antenna (OLEA) as a color- and directionality-switchable point source. The device consists of laterally arranged electrically contacted gold nanoantennas with their gap filled by the organic semiconductor zinc phthalocyanine (ZnPc). Since ZnPc shows preferred hole conduction in combination with gold, the recombination zone relocates depending on the polarity of the applied voltage and couples selectively to either of the two antennas. Thereby, the emission characteristics of the device also depend on polarity. Contrary to large-area OLEDs where recombination at metal contacts significantly contributes to losses, our ultracompact OLEA structures facilitate efficient radiation into the far-field rendering transparent electrodes obsolete. We envision OLEA structures to serve as wavelength-scale pixels with tunable color and directionality for advanced display applications.

Nanoscale Electrical Excitation of Distinct Modes in Plasmonic Waveguides.

The electrical excitation of guided plasmonic modes at the nanoscale enables integration of optical nanocircuitry into nanoelectronics. In this context, exciting plasmons with a distinct modal field profile constitutes a key advantage over conventional single-mode integrated photonics. Here, we demonstrate the selective electrical excitation of the lowest-order symmetric and antisymmetric plasmonic modes in a two-wire transmission line. We achieve mode selectivity by precisely positioning nanoscale excitation sources, i.e., junctions for inelastic electron tunneling, within the respective modal field distribution. By using advanced fabrication that combines focused He-ion beam milling and dielectrophoresis, we control the location of tunnel junctions with sub-10 nm accuracy. At the far end of the two-wire transmission line, the guided plasmonic modes are converted into far-field radiation at separate spatial positions showing two distinct orthogonal polarizations. Hence, the resulting device represents the smallest electrically driven light source with directly switchable polarization states with possible applications in display technology.

Electrically-driven Yagi-Uda antennas for light.

Yagi-Uda antennas are a key technology for efficiently transmitting information from point to point using radio waves. Since higher frequencies allow higher bandwidths and smaller footprints, a strong incentive exists to shrink Yagi-Uda antennas down to the optical regime. Here we demonstrate electrically-driven Yagi-Uda antennas for light with wavelength-scale footprints that exhibit large directionalities with forward-to-backward ratios of up to 9.1 dB. Light generation is achieved via antenna-enhanced inelastic tunneling of electrons over the antenna feed gap. We obtain reproducible tunnel gaps by means of feedback-controlled dielectrophoresis, which precisely places single surface-passivated gold nanoparticles in the antenna gap. The resulting antennas perform equivalent to radio-frequency antennas and combined with waveguiding layers even outperform RF designs. This work paves the way for optical on-chip data communication that is not restricted by Joule heating but also for advanced light management in nanoscale sensing and metrology as well as light emitting devices.

Nonclassical Optical Properties of Mesoscopic Gold.

Gold nanostructures have important applications in nanoelectronics, nano-optics, and in precision metrology due to their intriguing optoelectronic properties. These properties are governed by the bulk band structure but to some extent are tunable via geometrical resonances. Here we show that the band structure of gold itself exhibits significant size-dependent changes already for mesoscopic critical dimensions below 30 nm. To suppress the effects of geometrical resonances and grain boundaries, we prepared atomically flat ultrathin films of various thicknesses by utilizing large chemically grown single-crystalline gold platelets. We experimentally probe thickness-dependent changes of the band structure by means of two-photon photoluminescence and observe a surprising 100-fold increase of the nonlinear signal when the gold film thickness is reduced below 30 nm allowing us to optically resolve single-unit-cell steps. The effect is well explained by density functional calculations of the thickness-dependent 2D band structure of gold.

Grazing-incidence optical magnetic recording with super-resolution.

Heat-assisted magnetic recording (HAMR) is often considered the next major step in the storage industry: it is predicted to increase the storage capacity, the read/write speed and the data lifetime of future hard disk drives. However, despite more than a decade of development work, the reliability is still a prime concern. Featuring an inherently fragile surface-plasmon resonator as a highly localized heat source, as part of a near-field transducer (NFT), the current industry concepts still fail to deliver drives with sufficient lifetime. This study presents a method to aid conventional NFT-designs by additional grazing-incidence laser illumination, which may open an alternative route to high-durability HAMR. Magnetic switching is demonstrated on consumer-grade CoCrPt perpendicular magnetic recording media using a green and a near-infrared diode laser. Sub-500 nm magnetic features are written in the absence of a NFT in a moderate bias field of only µ0H = 0.3 T with individual laser pulses of 40 mW power and 50 ns duration with a laser spot size of 3 µm (short axis) at the sample surface - six times larger than the magnetic features. Herein, the presence of a nanoscopic object, i.e., the tip of an atomic force microscope in the focus of the laser at the sample surface, has no impact on the recorded magnetic features - thus suggesting full compatibility with NFT-HAMR.

Silica-gold bilayer-based transfer of focused ion beam-fabricated nanostructures.

The demand for using nanostructures fabricated by focused ion beam (FIB) on delicate substrates or as building blocks for complex devices motivates the development of protocols that allow FIB-fabricated nanostructures to be transferred from the original substrate to the desired target. However, transfer of FIB-fabricated nanostructures is severely hindered by FIB-induced welding of structure and substrate. Here we present two (ex and in situ) transfer methods for FIB-fabricated nanostructures based on a silica-gold bilayer evaporated onto a bulk substrate. Utilizing the poor adhesion between silica and gold, the nanostructures can be mechanically separated from the bulk substrate. For the ex situ transfer, a spin-coated poly(methyl methacrylate) film is used to carry the nanostructures so that the bilayer can be etched away after being peeled off. For the in situ transfer, using a micro-manipulator inside the FIB machine, a cut-out piece of silica on which a nanostructure has been fabricated is peeled off from the bulk substrate and thus carries the nanostructure to a target substrate. We demonstrate the performance of both methods by transferring plasmonic nano-antennas fabricated from single-crystalline gold flakes by FIB milling to a silicon wafer and to a scanning probe tip.

SHG simulations of plasmonic nanoparticles using curved elements.

We demonstrate that simulating plasmonic nanostructures by means of curved elements (CEs) significantly increases the accuracy and computation speed not only in the linear but also in the nonlinear regime. We implemented CEs within the discontinuous Galerkin (DG) method and, as an example of a nonlinear effect, investigated second-harmonic generation (SHG) at a silver nanoparticle. The second-harmonic response of the material is simulated by an extended Lorentz model (ELM). In the linear regime the CEs are ≈ 9 times faster than ordinary elements for the same accuracy, provide a much better convergence and show fewer unphysical field artifacts. For DG-SHG calculations CEs are almost indispensable to obtain physically reasonable results at all. Additionally, their boundary approximation has to be of the same order as their polynomial degree to achieve artifact-free field distributions. In return, the use of such CEs with the DG method pays off more than evidently, since the additional computation time is only 1%.

Three-dimensional, arbitrary orientation of focal polarization.

We demonstrate a simple setup for generating a three-dimensional arbitrary orientation of the polarization vector in a laser focus. The key component is the superposition of a linearly and a radially polarized laser beam, which both can be controlled individually in intensity and relative phase. We exemplify the usefulness of this setup by determining the spatial orientation of a single silver nanorod in three-dimensional space by recording the angle-variable backscattered light intensity.

Polarization conversion through collective surface plasmons in metallic nanorod arrays.

For two-dimensional (2D) arrays of metallic nanorods arranged perpendicular to a substrate several methods have been proposed to determine the electromagnetic near-field distribution and the surface plasmon resonances, but an analytical approach to explain all optical features on the nanometer length scale has been missing to date. To fill this gap, we demonstrate here that the field distribution in such arrays can be understood on the basis of surface plasmon polaritons (SPPs) that propagate along the nanorods and form standing waves. Notably, SPPs couple laterally through their optical near fields, giving rise to collective surface plasmon (CSP) effects. Using the dispersion relation of such CSPs, we deduce the condition of standing-wave formation, which enables us to successfully predict several features, such as eigenmodes and resonances. As one such property and potential application, we show both theoretically and in an experiment that CSP propagation allows for polarization conversion and optical filtering in 2D nanorod arrays. Hence, these arrays are promising candidates for manipulating the light polarization on the nanometer length scale.