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.

Light-driven microdrones.

When photons interact with matter, forces and torques occur due to the transfer of linear and angular momentum, respectively. The resulting accelerations are small for macroscopic objects but become substantial for microscopic objects with small masses and moments of inertia, rendering photon recoil very attractive to propel micro- and nano-objects. However, until now, using light to control object motion in two or three dimensions in all three or six degrees of freedom has remained an unsolved challenge. Here we demonstrate light-driven microdrones (size roughly 2 µm and mass roughly 2 pg) in an aqueous environment that can be manoeuvred in two dimensions in all three independent degrees of freedom (two translational and one rotational) using two overlapping unfocused light fields of 830 and 980 nm wavelength. To actuate the microdrones independent of their orientation, we use up to four individually addressable chiral plasmonic nanoantennas acting as nanomotors that resonantly scatter the circular polarization components of the driving light into well-defined directions. The microdrones are manoeuvred by only adjusting the optical power for each motor (the power of each circular polarization component of each wavelength). The actuation concept is therefore similar to that of macroscopic multirotor drones. As a result, we demonstrate manual steering of the microdrones along complex paths. Since all degrees of freedom can be addressed independently and directly, feedback control loops may be used to counteract Brownian motion. We posit that the microdrones can find applications in transport and release of cargos, nanomanipulation, and local probing and sensing of nano and mesoscale objects.

Atomically Smooth Single-Crystalline Platform for Low-Loss Plasmonic Nanocavities.

Nanoparticle-on-mirror plasmonic nanocavities, capable of extreme optical confinement and enhancement, have triggered state-of-the-art progress in nanophotonics and development of applications in enhanced spectroscopies. However, the optical quality factor and thus performance of these nanoconstructs are undermined by the granular polycrystalline metal films (especially when they are optically thin) used as a mirror. Here, we report an atomically smooth single-crystalline platform for low-loss nanocavities using chemically synthesized gold microflakes as a mirror. Nanocavities constructed using gold nanorods on such microflakes exhibit a rich structure of plasmonic modes, which are highly sensitive to the thickness of optically thin (down to ∼15 nm) microflakes. The microflakes endow nanocavities with significantly improved quality factor (∼2 times) and scattering intensity (∼3 times) compared with their counterparts based on deposited films. The developed low-loss nanocavities further allow for the integration with a mature platform of fiber optics, opening opportunities for realizing nanocavity-based miniaturized photonic devices for practical applications.

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.

The patterning toolbox FIB-o-mat: Exploiting the full potential of focused helium ions for nanofabrication.

Focused beams of helium ions are a powerful tool for high-fidelity machining with spatial precision below 5 nm. Achieving such a high patterning precision over large areas and for different materials in a reproducible manner, however, is not trivial. Here, we introduce the Python toolbox FIB-o-mat for automated pattern creation and optimization, providing full flexibility to accomplish demanding patterning tasks. FIB-o-mat offers high-level pattern creation, enabling high-fidelity large-area patterning and systematic variations in geometry and raster settings. It also offers low-level beam path creation, providing full control over the beam movement and including sophisticated optimization tools. Three applications showcasing the potential of He ion beam nanofabrication for two-dimensional material systems and devices using FIB-o-mat are presented.

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.

Space- and time-resolved UV-to-NIR surface spectroscopy and 2D nanoscopy at 1 MHz repetition rate.

We describe a setup for time-resolved photoemission electron microscopy with aberration correction enabling 3 nm spatial resolution and sub-20 fs temporal resolution. The latter is realized by our development of a widely tunable (215-970 nm) noncollinear optical parametric amplifier (NOPA) at 1 MHz repetition rate. We discuss several exemplary applications. Efficient photoemission from plasmonic Au nanoresonators is investigated with phase-coherent pulse pairs from an actively stabilized interferometer. More complex excitation fields are created with a liquid-crystal-based pulse shaper enabling amplitude and phase shaping of NOPA pulses with spectral components from 600 to 800 nm. With this system we demonstrate spectroscopy within a single plasmonic nanoslit resonator by spectral amplitude shaping and investigate the local field dynamics with coherent two-dimensional (2D) spectroscopy at the nanometer length scale ("2D nanoscopy"). We show that the local response varies across a distance as small as 33 nm in our sample. Further, we report two-color pump-probe experiments using two independent NOPA beamlines. We extract local variations of the excited-state dynamics of a monolayered 2D material (WSe2) that we correlate with low-energy electron microscopy (LEEM) and reflectivity measurements. Finally, we demonstrate the in situ sample preparation capabilities for organic thin films and their characterization via spatially resolved electron diffraction and dark-field LEEM.

Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas.

The optimization of nonlinear optical processes on the nanoscale is a crucial step for the integration of complex functionalities into compact photonic devices and metasurfaces. In such systems, photon upconversion can be achieved with higher efficiencies via third-order processes, such as third-harmonic generation (THG), thanks to the resonantly enhanced volume currents. Conversely, second-order processes, such as second-harmonic generation (SHG), are often inhibited by the symmetry of metal lattices and of common nanoantenna geometries. SHG and THG processes in plasmonic nanostructures are generally treated independently because they typically represent small perturbations in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold for plasmon-enhanced nonlinear optics by providing evidence of a sum-frequency generation (SFG) process seeded by SHG, which sizably contributes to the overall THG yield. We address this mechanism by unveiling a characteristic fingerprint in the polarization state of the THG emission from gold noncentrosymmetric nanoantennas, which directly reflects the asymmetric distribution of second-harmonic fields within the structure and does not depend on the model one employs to describe photon upconversion. We suggest that such cascaded processes may also appear for structures that exhibit only moderate SHG yields. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows us to gain further insight into the physics of plasmon-enhanced nonlinear optical processes. This could be crucial in the realization of nanoscale elements for photon conversion and manipulation operating at room temperature.

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.

Spatial Variations in Femtosecond Field Dynamics within a Plasmonic Nanoresonator Mode.

Plasmonic resonators can be designed to support spectrally well-separated discrete modes. The associated characteristic spatial patterns of intense electromagnetic hot-spots can be exploited to enhance light-matter interaction. Here, we study the local field dynamics of individual hot-spots within a nanoslit resonator by detecting characteristic changes of the photoelectron emission signal on a scale of ∼12 nm using time-resolved photoemission electron microscopy (TR-PEEM) and by excitation with the output from a 20 fs, 1 MHz noncollinear optical parametric amplifier (NOPA). Surprisingly, we detect apparent spatial variations of the Q-factor and resonance frequency that are commonly considered to be global properties for a single mode. By using the concept of quasinormal modes we explain these local differences by crosstalk of adjacent resonator modes. Our findings are important in view of time-domain studies of plasmon-mediated strong light-matter coupling at ambient conditions.

Reversible Mapping and Sorting the Spin of Photons on the Nanoscale: A Spin-Optical Nanodevice.

The photon spin is an important resource for quantum information processing as is the electron spin in spintronics. However, for subwavelength confined optical excitations, polarization as a global property of a mode cannot be defined. Here, we show that any polarization state of a plane-wave photon can reversibly be mapped to a pseudospin embodied by the two fundamental modes of a subwavelength plasmonic two-wire transmission line. We design a device in which this pseudospin evolves in a well-defined fashion throughout the device reminiscent of the evolution of photon polarization in a birefringent medium and the behavior of electron spins in the channel of a spin field-effect transistor. The significance of this pseudospin is enriched by the fact that it is subject to spin-orbit locking. Combined with optically active materials to exert external control over the pseudospin precession, our findings could enable spin-optical transistors, that is, the routing and processing of quantum information with light on a subwavelength scale.

High-Q, low-mode-volume and multiresonant plasmonic nanoslit cavities fabricated by helium ion milling.

Helium ion milling of chemically-synthesized micron-sized gold flakes is performed to fabricate ultra-narrow nanoslit cavities with a varying length and width down to 5 nm. Their plasmon resonances are characterized by one-photon photoluminescence spectroscopy. The combination of fabrication based on single-crystalline gold and resonant modes with low radiative losses leads to remarkably high quality factors of up to 24. Multiple Fabry-Pérot-type resonances in the visible/near infrared spectral range are observed due to the achieved narrow slit widths and the resulting short effective wavelengths of nanoslit plasmons. These features make nanoslit cavities attractive for a range of applications such as surface-enhanced spectroscopy, ultrafast nano-optics and strong light-matter coupling.

Parallel mapping of optical near-field interactions by molecular motor-driven quantum dots.

In the vicinity of metallic nanostructures, absorption and emission rates of optical emitters can be modulated by several orders of magnitude1,2. Control of such near-field light-matter interaction is essential for applications in biosensing3, light harvesting4 and quantum communication5,6 and requires precise mapping of optical near-field interactions, for which single-emitter probes are promising candidates7-11. However, currently available techniques are limited in terms of throughput, resolution and/or non-invasiveness. Here, we present an approach for the parallel mapping of optical near-field interactions with a resolution of <5 nm using surface-bound motor proteins to transport microtubules carrying single emitters (quantum dots). The deterministic motion of the quantum dots allows for the interpolation of their tracked positions, resulting in an increased spatial resolution and a suppression of localization artefacts. We apply this method to map the near-field distribution of nanoslits engraved into gold layers and find an excellent agreement with finite-difference time-domain simulations. Our technique can be readily applied to a variety of surfaces for scalable, nanometre-resolved and artefact-free near-field mapping using conventional wide-field microscopes.

Near-field strong coupling of single quantum dots.

Strong coupling and the resultant mixing of light and matter states is an important asset for future quantum technologies. We demonstrate deterministic room temperature strong coupling of a mesoscopic colloidal quantum dot to a plasmonic nanoresonator at the apex of a scanning probe. Enormous Rabi splittings of up to 110 meV are accomplished by nanometer-precise positioning of the quantum dot with respect to the nanoresonator probe. We find that, in addition to a small mode volume of the nanoresonator, collective coherent coupling of quantum dot band-edge states and near-field proximity interaction are vital ingredients for the realization of near-field strong coupling of mesoscopic quantum dots. The broadband nature of the interaction paves the road toward ultrafast coherent manipulation of the coupled quantum dot-plasmon system under ambient conditions.

Limits of Kirchhoff's Laws in Plasmonics.

The validity of Kirchhoff's laws in plasmonic nanocircuitry is investigated by studying a junction of plasmonic two-wire transmission lines. We find that Kirchhoff's laws are valid for sufficiently small values of a phenomenological parameter κ relating the geometrical parameters of the transmission line with the effective wavelength of the guided mode. Beyond such regime, for large values of the phenomenological parameter, increasing deviations occur and the equivalent impedance description (Kirchhoff's laws) can only provide rough, but nevertheless useful, guidelines for the design of more complex plasmonic circuitry. As an example we investigate a system composed of a two-wire transmission line and a nanoantenna as the load. By addition of a parallel stub designed according to Kirchhoff's laws we achieve maximum signal transfer to the nanoantenna.

Mode Matching for Optical Antennas.

The emission rate of a point dipole can be strongly increased in the presence of a well-designed optical antenna. Yet, optical antenna design is largely based on radio-frequency rules, ignoring, e.g., Ohmic losses and non-negligible field penetration in metals at optical frequencies. Here, we combine reciprocity and Poynting's theorem to derive a set of optical-frequency antenna design rules for benchmarking and optimizing the performance of optical antennas driven by single quantum emitters. Based on these findings a novel plasmonic cavity antenna design is presented exhibiting a considerably improved performance compared to a reference two-wire antenna. Our work will be useful for the design of high-performance optical antennas and nanoresonators for diverse applications ranging from quantum optics to antenna-enhanced single-emitter spectroscopy and sensing.

Plasmonic nanoantenna design and fabrication based on evolutionary optimization.

Nanoantennas can tailor light-matter interaction for optical communication, sensing, and spectroscopy. Their design is inspired by radio-frequency rules which partly break down at optical frequencies. Here we find unexpected nanoantenna designs exhibiting strong light localization and enhancement by using a general and scalable evolutionary algorithm based on FDTD simulations that also accounts for geometrical fabrication constraints. The resulting nanoantennas are "printed" directly by focused-ion beam milling and their fitness ranking is validated experimentally by two-photon photoluminescence. We find the best antennas' operation principle deviating from that of classical radio wave-inspired designs. Our work sets the stage for a widespread application of evolutionary optimization in nano photonics.

On-Chip Single-Plasmon Nanocircuit Driven by a Self-Assembled Quantum Dot.

Quantum photonics holds great promise for future technologies such as secure communication, quantum computation, quantum simulation, and quantum metrology. An outstanding challenge for quantum photonics is to develop scalable miniature circuits that integrate single-photon sources, linear optical components, and detectors on a chip. Plasmonic nanocircuits will play essential roles in such developments. However, for quantum plasmonic circuits, integration of stable, bright, and narrow-band single photon sources in the structure has so far not been reported. Here we present a plasmonic nanocircuit driven by a self-assembled GaAs quantum dot. Through a planar dielectric-plasmonic hybrid waveguide, the quantum dot efficiently excites narrow-band single plasmons that are guided in a two-wire transmission line until they are converted into single photons by an optical antenna. Our work demonstrates the feasibility of fully on-chip plasmonic nanocircuits for quantum optical applications.