Ultrafast all-optical second harmonic wavefront shaping.

Optical communication can be revolutionized by encoding data into the orbital angular momentum of light beams. However, state-of-the-art approaches for dynamic control of complex optical wavefronts are mainly based on liquid crystal spatial light modulators or miniaturized mirrors, which suffer from intrinsically slow (µs-ms) response times. Here, we experimentally realize a hybrid meta-optical system that enables complex control of the wavefront of light with pulse-duration limited dynamics. Specifically, by combining ultrafast polarization switching in a WSe2 monolayer with a dielectric metasurface, we demonstrate second harmonic beam deflection and structuring of orbital angular momentum on the femtosecond timescale. Our results pave the way to robust encoding of information for free space optical links, while reaching response times compatible with real-world telecom applications.

Roadmap for Optical Metasurfaces.

Metasurfaces have recently risen to prominence in optical research, providing unique functionalities that can be used for imaging, beam forming, holography, polarimetry, and many more, while keeping device dimensions small. Despite the fact that a vast range of basic metasurface designs has already been thoroughly studied in the literature, the number of metasurface-related papers is still growing at a rapid pace, as metasurface research is now spreading to adjacent fields, including computational imaging, augmented and virtual reality, automotive, display, biosensing, nonlinear, quantum and topological optics, optical computing, and more. At the same time, the ability of metasurfaces to perform optical functions in much more compact optical systems has triggered strong and constantly growing interest from various industries that greatly benefit from the availability of miniaturized, highly functional, and efficient optical components that can be integrated in optoelectronic systems at low cost. This creates a truly unique opportunity for the field of metasurfaces to make both a scientific and an industrial impact. The goal of this Roadmap is to mark this "golden age" of metasurface research and define future directions to encourage scientists and engineers to drive research and development in the field of metasurfaces toward both scientific excellence and broad industrial adoption.

Two-Color Spatially Resolved Tuning of Polymer-Coated Metasurfaces.

For the realization of truly reconfigurable metasurface technologies, dynamic spatial tuning of the metasurface resonance is required. Here we report the use of organic photoswitches as a means for the light-induced spatial tuning of metasurface resonances. Coating of a dielectric metasurface, hosting high-quality-factor resonances, with a spiropyran (SPA)-containing polymer enabled dynamic resonance tuning up to 4 times the resonance full-width at half-maximum with arbitrary spatial precision. A major benefit of employing photoswitches is the broad toolbox of chromophores available and the unique optical properties of each. In particular, SPA and azobenzene (AZO) photoswitches can both be switched with UV light but exhibit opposite refractive index changes. When applied to the metasurface, SPA induced a red shift in the metasurface resonance with a figure of merit of 97 RIU-1, while AZO caused a blue shift in the resonance with an even greater sensitivity of 100 RIU-1. Critically, SPA and AZO can be individually recovered with red and blue light, respectively. To exploit this advantage, we coated a dielectric metasurface with spatially offset SPA- and AZO-containing polymers to demonstrate wavelength-dependent, spatially resolved control over the metasurface resonance tuning.

Color Routing of the Emission from Magnetic and Electric Dipole Transitions of Eu3+ by Broken-Symmetry TiO2 Metasurfaces.

Manipulation of magnetic dipole emission with resonant photonic nanostructures is of great interest for both fundamental research and applications. However, obtaining selective control over the emission properties of magnetic dipole transitions is challenging, as they usually occur within a manifold of spectrally close emission lines associated with different spin states of the involved electronic levels. Here we demonstrate spectrally selective directional tailoring of magnetic dipole emission using designed photonic nanostructures featuring a high quality factor. Specifically, we employ a hybrid nanoscale optical system consisting of a Eu3+ compound coupled to a designed broken-symmetry TiO2 metasurface to demonstrate directional color routing of the compound's emission through its distinct electric and magnetic-dominated electronic transition channels. Using low numerical aperture collection optics, we achieve a fluorescence signal enhancement of up to 33.13 for the magnetic-dominated dipole transition at 590 nm when it spectrally overlaps with a spectrally narrow resonance of the metasurface. This makes the, usually weak, magnetic dipole transition the most intense spectral line in our recorded fluorescence spectra. By studying the directional emission properties for the coupled system using Fourier imaging and time-resolved fluorescence measurements, we demonstrate that the high-quality-factor modes in the metasurface enable free-space light routing, where forward-directed emission is established for the magnetic-dominated dipole transition, whereas the light emitted via the electric dipole transition is mainly directed sideways. Our results underpin the importance of magnetic light-matter interactions as an additional degree of freedom in photonic and optoelectronic systems. Moreover, they facilitate the development of spectrometer-free and highly integrated nanophotonic imaging, sensing, and probing devices.

Brightening and Directionality Control of Dark Excitons through Quasi-Bound States in the Continuum.

Thanks to their long lifetime, spin-forbidden dark excitons in transition metal dichalcogenides are promising candidates for storage applications in opto-electronics and valleytronics. To date, their study has been hindered by inefficient generation mechanisms and the necessity for elaborate detection schemes. In this work, we propose a new hybrid platform that simultaneously addresses both challenges. We study an all-dielectric metasurface with two symmetrically protected quasi-bound states in the continuum to enhance both the excitation and emission of dark excitons in a tungsten diselenide monolayer under normal light incidence. Our simulations show a giant photoluminescence signal enhancement (∼520) along with directional emission, thus offering distinct advantages for opto-electronic and valleytronic devices.

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.

Precision Tailoring Quasi-BIC Resonance of a-Si:H Metasurfaces.

The capability of tailoring the resonance wavelength of metasurfaces is important as it can alleviate the manufacturing precision required to produce the exact structure according to the design of the nanoresonators. Tuning of Fano resonances by applying heat has been theoretically predicted in the case of silicon metasurfaces. Here, we experimentally demonstrate the permanent tailoring of quasi-bound states in the continuum (quasi-BIC) resonance wavelength in an a-Si:H metasurface and quantitatively analyze the modification in the Q-factor with gradual heating. A gradual increment in temperature leads to a spectral shift in the resonance wavelength. With the support of ellipsometry measurements, the spectral shift resulting from the short-duration (ten minutes) heating is identified to be due to refractive index variations in the material rather than a geometric effect or amorphous/polycrystalline phase transition. In the case of quasi-BIC modes in the near-infrared, resonance wavelength could be adjusted from T = 350 °C to T = 550 °C without affecting the Q-factor considerably. Apart from the temperature-induced resonance trimming, large Q-factors can be attained at the highest analyzed temperature (T = 700 °C) in the near-infrared quasi-BIC modes. Resonance tailoring is just one of the possible applications of our results. We expect that our study is also insightful in the design of a-Si:H metasurfaces where large Q-factors are required at high temperatures.

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.

Acid-base responsive photoluminescence switching of CdSe/ZnS quantum dots coupled to plasmonic gold film using nanometer-thick poly[(2-diethylamino)ethyl methacrylate] layer.

The control of plasmon-nanoemitter interactions at the nanoscale enables the tailored modulation of optical properties, namely, the photoluminescence (PL) intensity of the nanoemitters. In this contribution, using a nanometer-thick poly[(2-diethylamino) ethyl methacrylate] (39 to 74 nm) as pH responsive spacer layer (pKa ∼ 6 to 6.5) between a plasmonic gold film and CdSe/ZnS Quantum Dots (QDs) nanoemitters, we could achieve reversible pH-responsive PL switching in QDs. In fact, the swelling (at pH 5) and shrinking (at pH 11) function of the pH-responsive spacer layer modulates the distance between the QDs and the gold surface, which dictates the plasmonic film-QDs nanoemitter interaction. Notably, we observed a high QDs' PL enhancement of up to a factor of 3.1 ± 0.4 through changing the pH value from 5 to 11. Furthermore, based on a systematic analysis of several samples with different spacer layer thicknesses and multiple pH cycles, our developed system revealed substantial stability, reversibility and PL enhancement reproducibility. Thus, the established acid-base responsive switchable systems may represent an appealing platform for applications such as sensors, biochemical assays, optoelectronics and logic gates and can be easily evolved to other multifunctional switchable systems using alternative stimuli-responsive polymers.

Toward Perfect Optical Diffusers: Dielectric Huygens' Metasurfaces with Critical Positional Disorder.

Conventional optical diffusers, such as thick volume scatterers (Rayleigh scattering) or microstructured surface scatterers (geometric scattering), lack the potential for on-chip integration and are thus incompatible with next-generation photonic devices. Dielectric Huygens' metasurfaces, on the other hand, consist of 2D arrangements of resonant dielectric nanoparticles and therefore constitute a promising material platform for ultrathin and highly efficient photonic devices. When the nanoparticles are arranged in a random but statistically specific fashion, diffusers with exceptional properties are expected to come within reach. This work explores how dielectric Huygens' metasurfaces can implement wavelength-selective diffusers with negligible absorption losses and nearly Lambertian scattering profiles that are largely independent of the angle and polarization of incident waves. The combination of tailored positional disorder with a carefully balanced electric and magnetic response of the nanoparticles is shown to be an integral requirement for the operation as a diffuser. The proposed metasurfaces' directional scattering performance is characterized both experimentally and numerically, and their usability in wavefront-shaping applications is highlighted. Since the metasurfaces operate on the principles of Mie scattering and are embedded in a glassy environment, they may easily be incorporated in integrated photonic devices, fiber optics, or mechanically robust augmented reality displays.

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.

Chiral Bilayer All-Dielectric Metasurfaces.

Three-dimensional chiral plasmonic metasurfaces were demonstrated to offer enormous potential for ultrathin circular polarizers and applications in chiral sensing. However, the large absorption losses in the metallic systems generally limit their applicability for high-efficiency devices. In this work, we experimentally and numerically demonstrate three-dimensional chiral dielectric metasurfaces exhibiting multipolar resonances and examine their chiro-optical properties. In particular, we demonstrate that record high circular dichroism of 0.7 and optical activity of 2.67 × 105 degree/mm can be achieved based on the excitation of electric and magnetic dipolar resonances inside the chiral structures. These large values are facilitated by a small amount of dissipative loss present in the dielectric nanoresonator material and the formation of a chiral supermode in a 4-fold symmetric metasurface unit cell. Our results highlight the mechanisms for maximizing the chiral response of photonic nanostructures and offer important opportunities for high-efficiency, ultrathin polarizing elements, which can be used in miniaturized devices, for example, integrated circuits.

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.

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.

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.