A self-healing multispectral transparent adhesive peptide glass.

Despite its disordered liquid-like structure, glass exhibits solid-like mechanical properties1. The formation of glassy material occurs by vitrification, preventing crystallization and promoting an amorphous structure2. Glass is fundamental in diverse fields of materials science, owing to its unique optical, chemical and mechanical properties as well as durability, versatility and environmental sustainability3. However, engineering a glassy material without compromising its properties is challenging4-6. Here we report the discovery of a supramolecular amorphous glass formed by the spontaneous self-organization of the short aromatic tripeptide YYY initiated by non-covalent cross-linking with structural water7,8. This system uniquely combines often contradictory sets of properties; it is highly rigid yet can undergo complete self-healing at room temperature. Moreover, the supramolecular glass is an extremely strong adhesive yet it is transparent in a wide spectral range from visible to mid-infrared. This exceptional set of characteristics is observed in a simple bioorganic peptide glass composed of natural amino acids, presenting a multi-functional material that could be highly advantageous for various applications in science and engineering.

External chirality enhancing downconversion in a waveguide-coupled nonlinear plasmonic metasurface.

Metasurfaces, typically constructed from spatial arrangements of localized building blocks, can enhance light-matter interactions through local field enhancement or by coherent coupling to extended photonic modes. Recent works have explored how guided mode resonances influence the performance of nonlinear metasurfaces. Here we investigate the modal impact on difference-frequency generation in a waveguide-coupled metasurface platform. The system is constructed from gold split-ring resonators on a high-index TiO2 waveguide. We find that a symmetric configuration of the metasurface's localized modes and the extended waveguide modes lead to a modest enhancement of the downconversion process. However, when the mirror symmetry of the localized modes with respect to the guided mode propagation breaks, it introduces external chirality. This enables coupling to a higher quality mode, resulting in a 70-fold enhancement of the difference-frequency generation. The capacity to manipulate the nonlocal modes through the design offers broader control over the interaction and new avenues to tailor the nonlinear processes.

Enhancing THz emission from nonlinear metasurfaces by a Bragg perfect absorber.

Nonlinear plasmonic metasurfaces were demonstrated recently as ultracompact tetrahertz (THz) sources, emitting relatively strong single-cycle THz pulses after femtosecond laser illumination. There has been great progress in their ability to generate controlled THz wavepackets; however, their overall emission strength has not yet been optimized. Here we numerically show that by designing a Bragg assisted perfect absorber we can improve the coupling of the pumping laser to the nonlinear metasurface. This results in over an order of magnitude enhancement of the THz signal. Moreover, we show that this method can be combined with other independent optimization schemes to further enhance the radiated THz, reaching over two orders of magnitude emission enhancement compared with previously studied plasmonic metasurfaces.

Second-Harmonic Enhancement from a Nonlinear Plasmonic Metasurface Coupled to an Optical Waveguide.

Metasurfaces are commonly constructed from two-dimensional arrangements of nanoresonators. Coherent coupling of the nanoresonators through extended photonic modes of the metasurface results in a modified collective optical response, and enhances light-matter interactions. Here we experimentally demonstrate that strong collective resonances can arise also from coupling the metasurface to an optical waveguide. We explore the effect this waveguide-assisted collective interaction has on second-harmonic generation from the hybrid system. Our measurements indicate an enhancement factor of 8 for the transmitted second harmonic in comparison to incoherent collective scattering. In addition, complementary simulations predict about a 100-fold enhancement for the second harmonic that remains confined inside the waveguide. The ability to control the hybrid modes by the waveguide's design provides broader control over the formation of the collective interaction and new tools to tailor the nonlinear interactions. Our findings pave a promising direction to realize nonlinear photonic circuits with metasurfaces.

Terahertz Metagrating Emitters with Beam Steering and Full Linear Polarization Control.

We report the realization of broadband THz plasmonic metagrating emitters for simultaneous beam steering and all-optical linear polarization control. Two types of metagratings are designed and experimentally demonstrated. First, the plasmonic meta-atoms are arranged in a metagrating with a binary phase modulation which results in the nonlinear generation of THz waves to the ±1 diffraction orders, with complete suppression of the zeroth order. Complete tunability of the diffracted THz linear polarization direction is demonstrated through simple rotation of the pump polarization. Then, the concept of lateral phase shift is introduced into the design of the metagratings using interlaced phase gradients. By controlling the spatial shift of the submetagrating, we are able to continuously control the linear polarization states of the generated THz waves. This method results in a higher nonlinear diffraction efficiency relative to binary phase modulation. These functional THz metagratings show exciting promise to meet the challenges associated with the current diverse array of applications utilizing THz technology.

The Role of Epsilon Near Zero and Hot Electrons in Enhanced Dynamic THz Emission from Nonlinear Metasurfaces.

We study theoretically and experimentally the nonlinear THz emission from plasmonic metasurfaces and show that a thin indium-tin oxide (ITO) film significantly affects the nonlinear dynamics of the system. Specifically, the presence of the ITO film leads to 2 orders of magnitude stronger THz emission compared to a metasurface on glass. It also shows a different power law, signifying different dominant emission mechanisms. In addition, we find that the hot-electron dynamics in the system strongly modify the coupling between the plasmonic metasurface and the free electrons in the ITO at the picosecond time scale. This results in striking dynamic THz emission phenomena that were not observed to date. Specifically, we show that the generated THz pulse can be shortened in time and thus broadened in frequency with twice the bandwidth compared to previous studies and to an uncoupled system. Our findings open the door to design efficient and dynamic metasurface THz emitters.

Tuning the phase and amplitude response of plasmonic metasurface etalons.

We study the optical response of plasmonic metasurface etalons in reflection. The etalons consist of a metallic mirror and a plasmonic metasurface separated by wavelength-scale dielectric spacer. We show that tuning the localized surface plasmon resonance and spacer thickness can be used to achieve both enhanced reflectivity and perfect absorption, in addition to full 2π range phase control, and tunable regions of normal and anomalous dispersion. We validate our claims by measuring the spectral reflection and phase response of metasurface etalons consisting aluminum nanodisks of different radii separated from an aluminum reflector by a SiO2 spacer. In addition, we use this approach to demonstrate a simple Hermite-Gaussian (HG) wavelength selective beam-shaping reflective mask. The concept can be further extended by using multilayers to obtain multi-functional elements.

Metasurface-based contact lenses for color vision deficiency: reply.

The filtering of overlapping spectral regions may be used to increase the observer's gamut in some cases. Therefore, metasurface-based contact lenses (M-CL) may improve the color coding for specific stimuli and deuteranomaly conditions. Here, we address the concerns made by Huertas et al. [Opt. Lett.45, 5117 (2020)OPLEDP0146-959210.1364/OL.394717], regarding the color perception improvement obtained by color filters, in general, and specifically by our M-CL, in case of deuteranomaly.

Metasurface-based contact lenses for color vision deficiency.

We embed large-scale, plasmonic metasurfaces into off-the-shelf rigid gas permeable contact lenses and study their ability to serve as visual aids for color vision deficiency. In this study, we specifically address deuteranomaly, which is the most common class of color vision deficiency. This condition is caused by a redshift of the medium-type cone photoreceptor and leads to ambiguity in the color perception of red and green and their combinations. The effect of the metasurface-based contact lenses on the color perception was simulated using Commission Internationale de l'Eclairage (CIE) color spaces and conventional models of the human color-sensitive photoreceptors. Comparison between normal color vision and uncorrected and corrected deuteranomaly by the proposed element demonstrates the ability offered by the nanostructured contact lens to shift back incorrectly perceived pigments closer to the original pigments. The maximal improvement in the color perception error before and after the proposed correction for deuteranomaly is up to a factor of $\sim{10}$∼10. In addition, an Ishihara-based color test was also simulated, showing the contrast restoration achieved by the element, for deuteranomaly conditions.

Nonlinear Metasurface Fresnel Zone Plates for Terahertz Generation and Manipulation.

We introduce a nanoengineered nonlinear metasurface based optical element that acts as an emitting Fresnel zone plate of terahertz (THz) waves. We show that the nonlinear zone plate generates broadband THz radiation and focuses each generated frequency on a different focal point along the optical axis. Therefore, a narrow beam waist and spectral selectivity of both the bandwidth and central frequency are achieved. Furthermore, we measure and analyze the temporal structure of the focused THz electric field and show that it comprises of few cycles with an axially varying carrier frequency in agreement with the calculated dispersion of the zone plate. This demonstration of controlled emission and focusing of THz waves opens the door for the development of a wide variety of additional holographic metasurface-based THz emitters and can lead to the development of efficient, active, integrated, and ultracompact optical devices for the THz spectral region.

Direct space to time terahertz pulse shaping with nonlinear metasurfaces.

We present a method for the generation of THz pulses with tailored temporal shape from nonlinear metasurfaces. The method is based on single-cycle THz emission by the metasurface inclusions. We show that the spatial amplitude and phase structure of the nonlinear response is mapped to the temporal shape of pulses emitted at certain angles. We specifically show a method for reconstruction of desired pulses, generation of few-cycles pulses with tailored carrier-envelope and all-optical control over the pulse shape by the pump pulse characteristics.

Terahertz generation in parallel plate waveguides activated by nonlinear metasurfaces.

We present an extended Maxwell-Hydrodynamic model of free electron dynamics on metal-dielectric interfaces that allows us to study numerically the THz emission from nonlinear metasurfaces. This model is applied on a metasurface consisting of split ring resonators, which has been previously studied and shown to produce broadband terahertz (THz) radiation. Investigations of the emitted THz radiation as function of the duration of the excitation laser reveal a tuning mechanism in terms of both spectral peak position and intensity. We also use the model to propose a new metasurface-activated waveguide platform that efficiently generates THz waveguide modes. Tunability mechanisms of the generated THz are shown. Due to its unique characteristics, we believe that this new platform might play a major role in forthcoming THz applications.

Strong light-matter interaction in tungsten disulfide nanotubes.

Transition metal dichalcogenide materials have recently been shown to exhibit a variety of intriguing optical and electronic phenomena. Focusing on the optical properties of semiconducting WS2 nanotubes, we show here that these nanostructures exhibit strong light-matter interaction and form exciton-polaritons. Namely, these nanotubes act as quasi 1-D polaritonic nano-systems and sustain both excitonic features and cavity modes in the visible-near infrared range. This ability to confine light to subwavelength dimensions under ambient conditions is induced by the high refractive index of tungsten disulfide. Using "finite-difference time-domain" (FDTD) simulations we investigate the interactions between the excitons and the cavity mode and their effect on the extinction spectrum of these nanostructures. The results of FDTD simulations agree well with the experimental findings as well as with a phenomenological coupled oscillator model which suggests a high Rabi splitting of ∼280 meV. These findings open up possibilities for developing new concepts in nanotube-based photonic devices.

Temporal Dynamics of Localized Exciton-Polaritons in Composite Organic-Plasmonic Metasurfaces.

We use femtosecond transient absorption spectroscopy to study the temporal dynamics of strongly coupled exciton-plasmon polaritons in metasurfaces of aluminum nanoantennas coated with J-aggregate molecules. Compared with the thermal nonlinearities of aluminum nanoantennas, the exciton-plasmon hybridization introduces strong ultrafast nonlinearities in the composite metasurfaces. Within femtoseconds after the pump excitation, the plasmonic resonance is broadened and shifted, showcasing its high sensitivity to excited-state modification of the molecular surroundings. In addition, we observe temporal oscillations due to the deep subangstrom acoustic breathing modes of the nanoantennas in both bare and hybrid metasurfaces. Finally, unlike the dynamics of hybrid states in optical microcavities, here, ground-state bleaching is observed with a significantly longer relaxation time at the upper polariton band.

Spectral shaping of lasing in vertically aligned coupled nanowire lasers.

We use numerical simulations to study the effects of nanowire geometry on the emission spectra of nanowire-based lasers. The studied nanowire lasers are made from gallium-nitride and the simulations are performed using finite difference time domain method. We show that changes in the diameter of the nanowire lasers also change the effective refractive index of their optical guided modes, which allows control over their Fabry-Perot spectrum. In addition, we show that evanescent coupling of two vertically standing nanowire lasers, having different cross section sizes, leads to a Vernier effect, which results in single mode emission from the small footprint coupled lasers system.

Nonlinear Surface Lattice Resonance in Plasmonic Nanoparticle Arrays.

We study experimentally second-harmonic generation from arrays of split-ring resonators at oblique incidence and find conditions of more than 30-fold enhancement of the emitted second harmonic with respect to normal incidence. We show that these conditions agree well with a nonlinear Rayleigh-Wood anomaly relation and the existence of a surface lattice resonance at the second harmonic. The existence of a nonlinear surface lattice resonance is theoretically confirmed by extending the coupled dipole approximation to the nonlinear case. We further show that the localized surface plasmon modes that collectively contribute to the surface lattice resonance are inherently dark modes that become highly bright due to the collective interaction.

Fully Tunable Silicon Nanowire Arrays Fabricated by Soft Nanoparticle Templating.

We demonstrate a fabrication breakthrough to produce large-area arrays of vertically aligned silicon nanowires (VA-SiNWs) with full tunability of the geometry of the single nanowires and of the whole array, paving the way toward advanced programmable designs of nanowire platforms. At the core of our fabrication route, termed "Soft Nanoparticle Templating", is the conversion of gradually compressed self-assembled monolayers of soft nanoparticles (microgels) at a water-oil interface into customized lithographical masks to create VA-SiNW arrays by means of metal-assisted chemical etching (MACE). This combination of bottom-up and top-down techniques affords excellent control of nanowire etching site locations, enabling independent control of nanowire spacing, diameter and height in a single fabrication route. We demonstrate the fabrication of centimeter-scale two-dimensional gradient photonic crystals exhibiting continuously varying structural colors across the entire visible spectrum on a single silicon substrate, and the formation of tunable optical cavities supported by the VA-SiNWs, as unambiguously demonstrated through numerical simulations. Finally, Soft Nanoparticle Templating is combined with optical lithography to create hierarchical and programmable VA-SiNW patterns.

Aluminum Nanoantenna Complexes for Strong Coupling between Excitons and Localized Surface Plasmons.

We study the optical dynamics in complexes of aluminum nanoantennas coated with molecular J-aggregates and find that they provide an excellent platform for the formation of hybrid exciton-localized surface plasmons. Giant Rabi splitting of 0.4 eV, which corresponds to ∼10 fs energy transfer cycle, is observed in spectral transmittance. We show that the nanoantennas can be used to manipulate the polarization of hybrid states and to confine their mode volumes. In addition, we observe enhancement of the photoluminescence due to enhanced absorption and increase in the local density of states at the exciton-localized surface plasmon energies. With recent emerging technological applications based on strongly coupled light-matter states, this study opens new possibilities to explore and utilize the unique properties of hybrid states over all of the visible region down to ultraviolet frequencies in nanoscale, technologically compatible, integrated platforms based on aluminum.

Metasurfaces based dual wavelength diffractive lenses.

We demonstrate experimentally and by simulations a method for using thin nanostructured plasmonic metasurfaces to design diffractive Fresnel zone plate lenses that focus pairs of wavelengths to a single focal point. The metasurfaces are made of tightly packed cross and rod shaped optical nanoantennas with strong polarization and wavelength selectivity. This selectivity allows multiplexing two different lenses with low spectral crosstalk on the same substrate and to address any superposition of the two colors at the focus of the lenses by controlling the polarization of light. This concept can open the door to use ultrathin diffractive lenses in fluorescence microscopy and in stimulated emission depletion microscopy.

Off-axis interferometer with adjustable fringe contrast based on polarization encoding.

We propose a compact, close-to-common-path, off-axis interferometric system for low polarizing samples based on a spatial polarization encoder that is placed at the Fourier plane after the output port of a conventional transmission microscope. The polarization encoder erases the sample information from one polarization state and maintains it on the orthogonal polarization state while retaining the low spatial frequencies of the sample, and thus enabling quantitative phase acquisition. In addition, the interference fringe visibility can be controlled by polarization manipulations. We demonstrate this concept experimentally by quantitative phase imaging of a USAF 1951 phase test target and human red blood cells, with optimal fringe visibility and a single-exposure phase reconstruction.