Photoluminescence Enhancement of Monolayer WS2 by n-Doping with an Optically Excited Gold Disk.

In nanophotonics and quantum optics, we aim to control and manipulate light with tailored nanoscale structures. Hybrid systems of nanostructures and atomically thin materials are of interest here, as they offer rich physics and versatility due to the interaction between photons, plasmons, phonons, and excitons. In this study, we explore the optical and electronic properties of a hybrid system, a naturally n-doped monolayer WS2 covering a gold disk. We demonstrate that the nonresonant excitation of the gold disk in the high absorption regime efficiently generates hot carriers via localized surface plasmon excitation, which n-dope the monolayer WS2 and enhance the photoluminescence emission by regulating the multiexciton population and stabilizing the neutral exciton emission. The results are relevant to the further development of nanotransistors in photonic circuits and optoelectronic applications.

Nonlinear All-Optical Coherent Generation and Read-Out of Valleys in Atomically Thin Semiconductors.

With conventional electronics reaching performance and size boundaries, all-optical processes have emerged as ideal building blocks for high speed and low power consumption devices. A promising approach in this direction is provided by valleytronics in atomically thin semiconductors, where light-matter interaction allows to write, store, and read binary information into the two energetically degenerate but non-equivalent valleys. Here, nonlinear valleytronics in monolayer WSe2 is investigated and show that an individual ultrashort pulse with a photon energy tuned to half of the optical band-gap can be used to simultaneously excite (by coherent optical Stark shift) and detect (by a rotation in the polarization of the emitted second harmonic) the valley population.

Lasing modes in ZnO nanowires coupled to planar metals.

Semiconductor nanowire lasers can be subject to modifications of their lasing threshold resulting from a variation of their environment. A promising choice is to use metallic substrates to gain access to low-volume Surface-Plasmon-Polariton (SPP) modes. We introduce a simple, yet quantitatively precise model that can serve to describe mode competition in nanowire lasers on metallic substrates. We show that an aluminum substrate can decrease the lasing threshold for ZnO nanowire lasers while for a silver substrate, the threshold increases compared with a dielectric substrate. Generalizing from these findings, we make predictions describing the interaction between planar metals and semiconductor nanowires, which allow to guide future improvements of highly-integrated laser sources.

Photon Pairs from Resonant Metasurfaces.

All-dielectric optical metasurfaces are a workhorse in nano-optics, because of both their ability to manipulate light in different degrees of freedom and their excellent performance at light frequency conversion. Here, we demonstrate first-time generation of photon pairs via spontaneous parametric-down conversion in lithium niobate quantum optical metasurfaces with electric and magnetic Mie-like resonances at various wavelengths. By engineering the quantum optical metasurface, we tailor the photon-pair spectrum in a controlled way. Within a narrow bandwidth around the resonance, the rate of pair production is enhanced up to 2 orders of magnitude, compared to an unpatterned film of the same thickness and material. These results enable flat-optics sources of entangled photons-a new promising platform for quantum optics experiments.

Manipulation of quantum dot emission with semiconductor metasurfaces exhibiting magnetic quadrupole resonances.

Optical metasurfaces were suggested as a route for engineering advanced light sources with tailored emission properties. In particular, they provide a control over the emission directionality, which is essential for single-photon sources and LED applications. Here, we experimentally study light emission from a metasurface composed of III-V semiconductor Mie-resonant nanocylinders with integrated quantum dots (QDs). Specifically, we focus on the manipulation of the directionality of spontaneous emission from the QDs due to excitation of different magnetic quadrupole resonances in the nanocylinders. To this end, we perform both back focal plane imaging and momentum-resolved spectroscopy measurements of the emission. This allows for a comprehensive analysis of the effect of the different resonant nanocylinder modes on the emission characteristics of the metasurface. Our results show that the emission directionality can be manipulated by an interplay of the excited quadrupolar nanocylinder modes with the metasurface lattice modes and provide important insights for the design of novel smart light sources and new display concepts.

Second-Harmonic Generation in Resonant Nonlinear Metasurfaces Based on Lithium Niobate.

Lithium niobate is an excellent and widely used material for nonlinear frequency conversion due to its strong optical nonlinearity and broad transparency region. Here, we report the fabrication and experimental investigation of resonant nonlinear metasurfaces for second-harmonic generation based on thin-film lithium niobate. In the fabricated metasurfaces, we observe pronounced Mie-type resonances leading to enhanced second-harmonic generation in the direction normal to the metasurface. We find the largest second-harmonic generation efficiency for the resonance dominated by the electric contributions because its specific field distribution enables the most efficient usage of the largest element of the lithium niobate nonlinear susceptibility tensor. This is confirmed by polarization-resolved second-harmonic measurements, where we study contributions from different elements of the nonlinear susceptibility tensor to the total second-harmonic signal. Our work facilitates establishing lithium niobate as a material for resonant nanophotonics.

General design formalism for highly efficient flat optics for broadband applications.

The use of flat diffractive optical elements (DOEs) for broadband applications, e.g. conventional optical systems, requires DOEs that maintain high efficiencies across the required range of wavelengths, angles of incidence, and grating periods. Here we introduce a general framework for how dispersion engineering can be used to design DOEs that fulfill these requirements and use our approach to determine design rules for broadband DOEs. Our analysis shows that the key to making échelette-type gratings (EGs) suitable for broadband optical systems is the development of new optical materials with specific uncommon dispersion properties. Subsequently, we use our framework to design a representative range of prototype EGs, which allows us to link the specifications of an optical system to the requirements on the EGs' materials. Finally, we show that our design rules apply to all DOEs based on propagation delays including GRIN DOEs and metagratings. Our design rules therefore guide the way towards unlocking the full potential of DOEs for different kinds of broadband applications.

Manipulation of Magnetic Dipole Emission from Eu3+ with Mie-Resonant Dielectric Metasurfaces.

Mie-resonant high-index dielectric nanoparticles and metasurfaces have been suggested as a viable platform for enhancing both electric and magnetic dipole transitions of fluorescent emitters. While the enhancement of the electric dipole transitions by such dielectric nanoparticles has been demonstrated experimentally, the case of magnetic-dipole transitions remains largely unexplored. Here, we study the enhancement of spontaneous emission of Eu3+ ions, featuring both electric and magnetic-dominated dipole transitions, by dielectric metasurfaces composed of Mie-resonant silicon nanocylinders. By coating the metasurfaces with a layer of an Eu3+ doped polymer, we observe an enhancement of the Eu3+ emission associated with the electric (at 610 nm) and magnetic-dominated (at 590 nm) dipole transitions. The enhancement factor depends systematically on the spectral proximity of the atomic transitions to the Mie resonances as well as their multipolar order, both controlled by the nanocylinder size. Importantly, the branching ratio of emission via the electric or magnetic transition channel can be modified by carefully designing the metasurface, where the magnetic dipole transition is enhanced more than the electric transition for cylinders with radii of about 130 nm. We confirm our observations by numerical simulations based on the reciprocity principle. Our results open new opportunities for bright nanoscale light sources based on magnetic transitions.

Tailoring Second-Harmonic Emission from (111)-GaAs Nanoantennas.

Second-harmonic generation (SHG) in resonant dielectric Mie-scattering nanoparticles has been hailed as a powerful platform for nonlinear light sources. While bulk-SHG is suppressed in elemental semiconductors, for example, silicon and germanium due to their centrosymmetry, the group of zincblende III-V compound semiconductors, especially (100)-grown AlGaAs and GaAs, have recently been presented as promising alternatives. However, major obstacles to push the technology toward practical applications are the limited control over directionality of the SH emission and especially zero forward/backward radiation, resulting from the peculiar nature of the second-order nonlinear susceptibility of this otherwise highly promising group of semiconductors. Furthermore, the generated SH signal for (100)-GaAs nanoparticles depends strongly on the polarization of the pump. In this work, we provide both theoretically and experimentally a solution to these problems by presenting the first SHG nanoantennas made from (111)-GaAs embedded in a low index material. These nanoantennas show superior forward directionality compared to their (100)-counterparts. Most importantly, based on the special symmetry of the crystalline structure, it is possible to manipulate the SHG radiation pattern of the nanoantennas by changing the pump polarization without affecting the linear properties and the total nonlinear conversion efficiency, hence paving the way for efficient and flexible nonlinear beam-shaping devices.

Analyzing the polarization response of a chiral metasurface stack by semi-analytic modeling.

We investigate a class of stacked metasurfaces where the interaction between layers is dominated by their respective far-field response. Using a semi-analytic scattering matrix approach, we exploit the Fabry-Perot-type response for different layer distances to show the spectral tunability of the resonant effect. This method presents a faster and more intuitive route to modeling Fabry-Perot-type effects than rigorous numerical simulations. The results are illustrated for a chiral metasurface stack that exhibits asymmetric transmission. Here, the effect of asymmetric transmission is highly sensitive to the layer distance, which is used as a free parameter in our model. To prove our theoretical findings we fabricate two variants of the stack with different layer distances and show that far-field interaction between layers is sufficient to generate the effect while being accessible by semi-analytic modeling. The analyticity of the approach is promising for designing sophisticated layered media containing stacks of arbitrary metasurfaces.

Second harmonic generation in monolithic lithium niobate metasurfaces.

Second-order nonlinear metasurfaces have proven their ability to efficiently convert the frequency of incident signals over subwavelength thickness. However, the availability of second-order nonlinear materials for such metasurfaces has so far been limited to III-V semiconductors, which have low transparency in the visible and impose constraints on the excitation geometries due to the lack of diagonal second-order susceptibility components. Here we propose a new design concept for second-order nonlinear metasurfaces on a monolithic substrate, which is not limited by the availability of thin crystalline films and can be applied to any non-centrosymmetric material. We exemplify this concept in a monolithic Lithium Niobate metasurface with cylinder-shaped corrugations for enhanced field confinement. By optimizing the geometrical parameters, we show enhanced second harmonic generation from a near-infrared pump beam with conversion efficiency above 10-5 using 1 GW/cm2 pump intensity. Our approach enables new opportunities for practical designs of generic metasurfaces for nonlinear and quantum light sources.

Controlling second-harmonic diffraction by nano-patterning MoS2 monolayers.

Monolayers of transition metal dichalcogenides have a strong second-order nonlinear response enabling second-harmonic generation. Here, we control the spatial radiation properties of the generated second harmonic by patterning MoS2 monolayers using focused ion beam milling. We observe diffraction of the second harmonic into the zero and first diffraction orders via an inscribed one-dimensional grating. Additionally, we included a fork-like singularity into the grating to create a vortex beam in the first diffraction order.

Active Tuning of Spontaneous Emission by Mie-Resonant Dielectric Metasurfaces.

Mie-resonant dielectric metasurfaces offer comprehensive opportunities for the manipulation of light fields with high efficiency. Additionally, various strategies for the dynamic tuning of the optical response of such metasurfaces were demonstrated, making them important candidates for reconfigurable optical devices. However, dynamic control of the light-emission properties of active Mie-resonant dielectric metasurfaces by an external control parameter has not been demonstrated so far. Here, we experimentally demonstrate the dynamic tuning of spontaneous emission from a Mie-resonant dielectric metasurface that is situated on a fluorescent substrate and embedded into a liquid crystal cell. By switching the liquid crystal from the nematic state to the isotropic state via control of the cell temperature, we induce a shift of the spectral position of the metasurface resonances. This results in a change of the local photonic density of states, which, in turn, governs the enhancement of spontaneous emission from the substrate. Specifically, we observe spectral tuning of both the electric and magnetic dipole resonances, resulting in a 2-fold increase of the emission intensity at λ ≈ 900 nm. Our results demonstrate a viable strategy to realize flat tunable light sources based on dielectric metasurfaces.

Light-Emitting Metasurfaces: Simultaneous Control of Spontaneous Emission and Far-Field Radiation.

Light-emitting sources and devices permeate every aspect of our lives and are used in lighting, communications, transportation, computing, and medicine. Advances in multifunctional and "smart lighting" would require revolutionary concepts in the control of emission spectra and directionality. Such control might be possible with new schemes and regimes of light-matter interaction paired with developments in light-emitting materials. Here we show that all-dielectric metasurfaces made from III-V semiconductors with embedded emitters have the potential to provide revolutionary lighting concepts and devices, with new functionality that goes far beyond what is available in existing technologies. Specifically, we use Mie-resonant metasurfaces made from semiconductor heterostructures containing epitaxial quantum dots. By controlling the symmetry of the resonant modes, their overlap with the emission spectra, and other structural parameters, we can enhance the brightness by 2 orders of magnitude, as well as reduce its far-field divergence significantly.

The Role of Liquid Ink Transport in the Direct Placement of Quantum Dot Emitters onto Sub-Micrometer Antennas by Dip-Pen Nanolithography.

Dip-pen nanolithography (DPN) is used to precisely position core/thick-shell ("giant") quantum dots (gQDs; ≥10 nm in diameter) exclusively on top of silicon nanodisk antennas (≈500 nm diameter pillars with a height of ≈200 nm), resulting in periodic arrays of hybrid nanostructures and demonstrating a facile integration strategy toward next-generation quantum light sources. A three-step reading-inking-writing approach is employed, where atomic force microscopy (AFM) images of the pre-patterned substrate topography are used as maps to direct accurate placement of nanocrystals. The DPN "ink" comprises gQDs suspended in a non-aqueous carrier solvent, o-dichlorobenzene. Systematic analyses of factors influencing deposition rate for this non-conventional DPN ink are described for flat substrates and used to establish the conditions required to achieve small (sub-500 nm) feature sizes, namely: dwell time, ink-substrate contact angle and ink volume. Finally, it is shown that the rate of solvent transport controls the feature size in which gQDs are found on the substrate, but also that the number and consistency of nanocrystals deposited depends on the stability of the gQD suspension. Overall, the results lay the groundwork for expanded use of nanocrystal liquid inks and DPN for fabrication of multi-component nanostructures that are challenging to create using traditional lithographic techniques.

Huygens' Metasurfaces Enabled by Magnetic Dipole Resonance Tuning in Split Dielectric Nanoresonators.

Dielectric metasurfaces that exploit the different Mie resonances of nanoscale dielectric resonators are a powerful platform for manipulating electromagnetic fields and can provide novel optical behavior. In this work, we experimentally demonstrate independent tuning of the magnetic dipole resonances relative to the electric dipole resonances of split dielectric resonators (SDRs). By increasing the split dimension, we observe a blue shift of the magnetic dipole resonance toward the electric dipole resonance. Therefore, SDRs provide the ability to directly control the interaction between the two dipole resonances within the same resonator. For example, we achieve the first Kerker condition by spectrally overlapping the electric and magnetic dipole resonances and observe significantly suppressed backward scattering. Moreover, we show that a single SDR can be used as an optical nanoantenna that provides strong unidirectional emission from an electric dipole source.

Resonantly Enhanced Second-Harmonic Generation Using III-V Semiconductor All-Dielectric Metasurfaces.

Nonlinear optical phenomena in nanostructured materials have been challenging our perceptions of nonlinear optical processes that have been explored since the invention of lasers. For example, the ability to control optical field confinement, enhancement, and scattering almost independently allows nonlinear frequency conversion efficiencies to be enhanced by many orders of magnitude compared to bulk materials. Also, the subwavelength length scale renders phase matching issues irrelevant. Compared with plasmonic nanostructures, dielectric resonator metamaterials show great promise for enhanced nonlinear optical processes due to their larger mode volumes. Here, we present, for the first time, resonantly enhanced second-harmonic generation (SHG) using gallium arsenide (GaAs) based dielectric metasurfaces. Using arrays of cylindrical resonators we observe SHG enhancement factors as large as 10(4) relative to unpatterned GaAs. At the magnetic dipole resonance, we measure an absolute nonlinear conversion efficiency of ∼2 × 10(-5) with ∼3.4 GW/cm(2) pump intensity. The polarization properties of the SHG reveal that both bulk and surface nonlinearities play important roles in the observed nonlinear process.

Plasmonic fano nanoantennas for on-chip separation of wavelength-encoded optical signals.

Here we suggest and realize an ultracompact plasmonic spectral-band demultiplexer for telecommunication wavelengths integrated onto an optical waveguide that couples two wavelength-encoded optical signals in the O- and the C-band in opposite directions of a silicon waveguide. In this way, we demonstrate a plasmonic key element for on-chip optical data processing that can also be used as a functional link between on- and off-chip optical signals.

Ultrafast All-Optical Switching with Magnetic Resonances in Nonlinear Dielectric Nanostructures.

We demonstrate experimentally ultrafast all-optical switching in subwavelength nonlinear dielectric nanostructures exhibiting localized magnetic Mie resonances. We employ amorphous silicon nanodisks to achieve strong self-modulation of femtosecond pulses with a depth of 60% at picojoule-per-disk pump energies. In the pump-probe measurements, we reveal that switching in the nanodisks can be governed by pulse-limited 65 fs-long two-photon absorption being enhanced by a factor of 80 with respect to the unstructured silicon film. We also show that undesirable free-carrier effects can be suppressed by a proper spectral positioning of the magnetic resonance, making such a structure the fastest all-optical switch operating at the nanoscale.