Enhanced Infrared Vision by Nonlinear Up-Conversion in Nonlocal Metasurfaces.

The ability to detect and image short-wave infrared light has important applications in surveillance, autonomous navigation, and biological imaging. However, the current infrared imaging technologies often pose challenges due to large footprint, large thermal noise and inability to augment infrared and visible imaging. Here, infrared imaging is demonstrated by nonlinear up-conversion to the visible in an ultra-compact, high-quality-factor lithium niobate resonant metasurface. Images with high conversion efficiency and resolution quality are obtained despite the strong nonlocality of the metasurface. The possibility of edge-detection image processing augmented with direct up-conversion imaging for advanced night vision applications is further shown.

Engineering Quantum Light Sources with Flat Optics.

Quantum light sources are essential building blocks for many quantum technologies, enabling secure communication, powerful computing, and precise sensing and imaging. Recent advancements have witnessed a significant shift toward the utilization of "flat" optics with thickness at subwavelength scales for the development of quantum light sources. This approach offers notable advantages over conventional bulky counterparts, including compactness, scalability, and improved efficiency, along with added functionalities. This review focuses on the recent advances in leveraging flat optics to generate quantum light sources. Specifically, the generation of entangled photon pairs through spontaneous parametric down-conversion in nonlinear metasurfaces, and single photon emission from quantum emitters including quantum dots and color centers in 3D and 2D materials are explored. The review covers theoretical principles, fabrication techniques, and properties of these sources, with particular emphasis on the enhanced generation and engineering of quantum light sources using optical resonances supported by nanostructures. The diverse application range of these sources is discussed and the current challenges and perspectives in the field are highlighted.

Multifunctional Metasurface Tuning by Liquid Crystals in Three Dimensions.

Optical metasurfaces present remarkable opportunities for manipulating wave propagation in unconventional ways, surpassing the capabilities of traditional optical devices. In this work, we introduce and demonstrate a multifunctional dynamic tuning of dielectric metasurfaces containing liquid crystals (LCs) through an effective three-dimensional (3D) control of the molecular orientation. We theoretically and experimentally study the spectral tuning of the electric and magnetic resonances of dielectric metasurfaces, which was enabled by rotating an external magnetic field in 3D. Our approach allows for the independent control of the electric and magnetic resonances of a metasurface, enabling multifunctional operation. The magnetic field tuning approach eliminates the need for the pre-alignment of LCs and is not limited by a finite set of directions in which the LC molecules can be oriented. Our results open new pathways for realizing dynamically reconfigurable metadevices and observing novel physical effects without the usual limitations imposed by the boundary conditions of LC cells and the external voltage.

Polarization Engineering of Entangled Photons from a Lithium Niobate Nonlinear Metasurface.

Complex polarization states of photon pairs are indispensable in various quantum technologies. Conventional methods for preparing desired two-photon polarization states are realized through bulky nonlinear crystals, which can restrict the versatility and tunability of the generated quantum states due to the fixed crystal nonlinear susceptibility. Here we present a solution using a nonlinear metasurface incorporating multiplexed silica metagratings on a lithium niobate film of 300 nm thickness. We fabricate two orthogonal metagratings on a single substrate with an identical resonant wavelength, thereby enabling the spectral indistinguishability of the emitted photons, and we demonstrate in experiments that the two-photon polarization states can be shaped by the metagrating orientation. Leveraging this essential property, we formulate a theoretical approach for generating arbitrary polarization-entangled qutrit states by combining three metagratings on a single metasurface, allowing the encoding of the desired quantum states or information. Our findings enable miniaturized optically controlled quantum devices by using ultrathin metasurfaces as polarization-entangled photon sources.

Spatially entangled photon pairs from lithium niobate nonlocal metasurfaces.

Metasurfaces consisting of nanoscale structures are underpinning new physical principles for the creation and shaping of quantum states of light. Multiphoton states that are entangled in spatial or angular domains are an essential resource for many quantum applications; however, their production traditionally relies on bulky nonlinear crystals. We predict and demonstrate experimentally the generation of spatially entangled photon pairs through spontaneous parametric down-conversion from a metasurface incorporating a nonlinear thin film of lithium niobate covered by a silica meta-grating. We measure the correlations of photon pairs and identify their spatial antibunching through violation of the classical Cauchy-Schwarz inequality, witnessing the presence of multimode entanglement. Simultaneously, the photon-pair rate is strongly enhanced by 450 times as compared to unpatterned films because of high-quality-factor resonances. These results pave the way to miniaturization of various quantum devices by incorporating ultrathin metasurfaces functioning as room temperature sources of quantum-entangled photons.

Nonlinear microscopy of lead iodide nanosheets.

Lead iodide (PbI2) is a van der Waals layered semiconductor with a direct bandgap in its bulk form and a hexagonal layered crystalline structure. The recently developed PbI2 nanosheets have shown great promise for high-performance optoelectronic devices, including nanolasers and photodetectors. However, despite being widely used as a precursor for perovskite materials, the optical properties of PbI2 nanomaterials remain largely unexplored. Here, we determine the nonlinear optical properties of PbI2 nanosheets by utilising nonlinear microscopy as a non-invasive optical technique. We demonstrate the nonlinearity enhancement dependent on excitonic resonances, crystalline orientation, thickness, and influence of the substrate. Our results allow for estimating the second- and third-order nonlinear susceptibilities of the nanosheets, opening new opportunities for the use of PbI2 nanosheets as nonlinear and quantum light sources.

Tunable unidirectional nonlinear emission from transition-metal-dichalcogenide metasurfaces.

Nonlinear light sources are central to a myriad of applications, driving a quest for their miniaturisation down to the nanoscale. In this quest, nonlinear metasurfaces hold a great promise, as they enhance nonlinear effects through their resonant photonic environment and high refractive index, such as in high-index dielectric metasurfaces. However, despite the sub-diffractive operation of dielectric metasurfaces at the fundamental wave, this condition is not fulfilled for the nonlinearly generated harmonic waves, thereby all nonlinear metasurfaces to date emit multiple diffractive beams. Here, we demonstrate the enhanced single-beam second- and third-harmonic generation in a metasurface of crystalline transition-metal-dichalcogenide material, offering the highest refractive index. We show that the interplay between the resonances of the metasurface allows for tuning of the unidirectional second-harmonic radiation in forward or backward direction, not possible in any bulk nonlinear crystal. Our results open new opportunities for metasurface-based nonlinear light-sources, including nonlinear mirrors and entangled-photon generation.

Steering and Encoding the Polarization of the Second Harmonic in the Visible with a Monolithic LiNbO3 Metasurface.

Nonlinear metasurfaces constitute a key asset in meta-optics, given their ability to scale down nonlinear optics to sub-micrometer thicknesses. To date, nonlinear metasurfaces have been mainly realized using narrow band gap semiconductors, with operation limited to the near-infrared range. Nonlinear meta-optics in the visible range can be realized using transparent materials with high refractive index, such as lithium niobate (LiNbO3). Yet, efficient operation in this strategic spectral window has been so far prevented by the nanofabrication challenges associated with LiNbO3, which considerably limit the aspect ratio and minimum size of the nanostructures (i.e., meta-atoms). Here we demonstrate the first monolithic nonlinear periodic metasurface based on LiNbO3 and operating in the visible range. Realized through ion beam milling, our metasurface features a second-harmonic (SH) conversion efficiency of 2.40 × 10-8 at a pump intensity as low as 0.5 GW/cm2. By tuning the pump polarization, we demonstrate efficient steering and polarization encoding into narrow SH diffraction orders, opening novel opportunities for polarization-encoded nonlinear meta-optics.

Highly Efficient Near-Infrared Detector Based on Optically Resonant Dielectric Nanodisks.

Fast detection of near-infrared (NIR) photons with high responsivity remains a challenge for photodetectors. Germanium (Ge) photodetectors are widely used for near-infrared wavelengths but suffer from a trade-off between the speed of photodetection and quantum efficiency (or responsivity). To realize a high-speed detector with high quantum efficiency, a small-sized photodetector efficiently absorbing light is required. In this paper, we suggest a realization of a dielectric metasurface made of an array of subwavelength germanium PIN photodetectors. Due to the subwavelength size of each pixel, a high-speed photodetector with a bandwidth of 65 GHz has been achieved. At the same time, high quantum efficiency for near-infrared illumination can be obtained by the engineering of optical resonant modes to localize optical energy inside the intrinsic Ge disks. Furthermore, small junction capacitance and the possibility of zero/low bias operation have been shown. Our results show that all-dielectric metasurfaces can improve the performance of photodetectors.

Multidimensional synthetic chiral-tube lattices via nonlinear frequency conversion.

Geometrical dimensionality plays a fundamentally important role in the topological effects arising in discrete lattices. Although direct experiments are limited by three spatial dimensions, the research topic of synthetic dimensions implemented by the frequency degree of freedom in photonics is rapidly advancing. The manipulation of light in these artificial lattices is typically realized through electro-optic modulation; yet, their operating bandwidth imposes practical constraints on the range of interactions between different frequency components. Here we propose and experimentally realize all-optical synthetic dimensions involving specially tailored simultaneous short- and long-range interactions between discrete spectral lines mediated by frequency conversion in a nonlinear waveguide. We realize triangular chiral-tube lattices in three-dimensional space and explore their four-dimensional generalization. We implement a synthetic gauge field with nonzero magnetic flux and observe the associated multidimensional dynamics of frequency combs, all within one physical spatial port. We anticipate that our method will provide a new means for the fundamental study of high-dimensional physics and act as an important step towards using topological effects in optical devices operating in the time and frequency domains.

Forward and Backward Switching of Nonlinear Unidirectional Emission from GaAs Nanoantennas.

High-index III-V semiconductor nanoantennas have gained great attention for enhanced nonlinear light-matter interactions, in the past few years. However, the complexity of nonlinear emission profiles imposes severe constraints on practical applications, such as in optical communications and integrated optoelectronic devices. These complexities include the lack of unidirectional nonlinear emission and the severe challenges in switching between forward and backward emissions, due to the structure of the susceptibility tensor of the III-V nanoantennas. Here, we propose a solution to both issues via engineering the nonlinear tensor of the nanoantennas. The special nonlinear tensorial properties of zinc-blende material can be used to engineer the nonlinear characteristics via growing the nanoantennas along different crystalline orientations. Based on the nonlinear multipolar effect, we have designed and fabricated (110)-grown GaAs nanoantennas, with engineered tensorial properties, embedded in a transparent low-index material. Our technique provides an approach not only for unidirectional second-harmonic generation (SHG) forward or backward emission but also for switching from one to another. Importantly, switching the SHG emission directionality is obtained only by rotating the polarization of the incident light, without the need for physical variation of the antennas or the environment. This characteristic is an advantage, as compared to other nonlinear nanoantennas, including (100)- and (111)-grown III-V counterparts or silicon and germanium nanoantennas. Indeed, (110)-GaAs nanoantennas allow for engineering the nonlinear nanophotonic systems including nonlinear "Huygens metasurfaces" and offer exciting opportunities for various nonlinear nanophotonics technologies, such as nanoscale light routing and light sources, as well as multifunctional flat optical elements.

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.

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.

Resonant harmonic generation in AlGaAs nanoantennas probed by cylindrical vector beams.

We investigate second- and third-harmonic generation from individual AlGaAs nanoantennas using far-field mapping with radially- and azimuthally-polarized cylindrical vector beams. Due to the unique polarization structure of these beams, we are able to determine the crystal orientation of the nanoantenna in a single scanning map. Our method thus provides a novel and versatile optical tool to study the crystal properties of semiconductor nanoantennas. We also demonstrate the influence of cylindrical vector beam excitation on the resonant enhancement of second- and third-harmonic generation driven by electric and magnetic anapole-like modes, despite falling in the strong absorption regime of AlGaAs. In particular, we observe a greater nonlinear conversion efficiency from a single nanoantenna excited with a radially-polarized beam as compared to an azimuthally polarized cylindrical vector beam. The fundamental field of the radially-polarized beam strongly couples to the multipoles increasing the near-field enhancement of the nanoantenna. Our work introduces new ways to study individual nanostructures and to tailor the efficiencies of nonlinear phenomena at the nanoscale using non-conventional optical techniques.

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.

Shaping the Nonlinear Emission Pattern of a Dielectric Nanoantenna by Integrated Holographic Gratings.

We demonstrate the shaping of the second-harmonic (SH) radiation pattern from a single AlGaAs nanodisk antenna using coplanar holographic gratings. The SH radiation emitted from the antenna toward the-otherwise forbidden-normal direction can be effectively redirected by suitably shifting the phase of the grating pattern in the azimuthal direction. The use of such gratings allows increasing the SH power collection efficiency by 2 orders of magnitude with respect to an isolated antenna and demonstrates the possibility of intensity-tailoring for an arbitrary collection angle. Such reconstruction of the nonlinear emission from nanoscale antennas represents the first step toward the application of all-dielectric nanostructures for nonlinear holography.

Quantum metasurface for multiphoton interference and state reconstruction.

Metasurfaces based on resonant nanophotonic structures have enabled innovative types of flat-optics devices that often outperform the capabilities of bulk components, yet these advances remain largely unexplored for quantum applications. We show that nonclassical multiphoton interferences can be achieved at the subwavelength scale in all-dielectric metasurfaces. We simultaneously image multiple projections of quantum states with a single metasurface, enabling a robust reconstruction of amplitude, phase, coherence, and entanglement of multiphoton polarization-encoded states. One- and two-photon states are reconstructed through nonlocal photon correlation measurements with polarization-insensitive click detectors positioned after the metasurface, and the scalability to higher photon numbers is established theoretically. Our work illustrates the feasibility of ultrathin quantum metadevices for the manipulation and measurement of multiphoton quantum states, with applications in free-space quantum imaging and communications.

Imaging-based molecular barcoding with pixelated dielectric metasurfaces.

Metasurfaces provide opportunities for wavefront control, flat optics, and subwavelength light focusing. We developed an imaging-based nanophotonic method for detecting mid-infrared molecular fingerprints and implemented it for the chemical identification and compositional analysis of surface-bound analytes. Our technique features a two-dimensional pixelated dielectric metasurface with a range of ultrasharp resonances, each tuned to a discrete frequency; this enables molecular absorption signatures to be read out at multiple spectral points, and the resulting information is then translated into a barcode-like spatial absorption map for imaging. The signatures of biological, polymer, and pesticide molecules can be detected with high sensitivity, covering applications such as biosensing and environmental monitoring. Our chemically specific technique can resolve absorption fingerprints without the need for spectrometry, frequency scanning, or moving mechanical parts, thereby paving the way toward sensitive and versatile miniaturized mid-infrared spectroscopy devices.

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.

Valley-selective directional emission from a transition-metal dichalcogenide monolayer mediated by a plasmonic nanoantenna.

Background: Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) with intrinsically crystal inversion-symmetry breaking have shown many advanced optical properties. In particular, the valley polarization in 2D TMDCs that can be addressed optically has inspired new physical phenomena and great potential applications in valleytronics. Results: Here, we propose a TMDC-nanoantenna system that could effectively enhance and direct emission from the two valleys in TMDCs into diametrically opposite directions. By mimicking the emission from each valley of the monolayer of WSe2 as a chiral point-dipole emitter, we demonstrate numerically that the emission from different valleys is directed into opposite directions when coupling to a double-bar plasmonic nanoantenna. The directionality derives from the interference between the dipole and quadrupole modes excited in the two bars, respectively. Thus, we could tune the emission direction from the proposed TMDC-nanoantenna system by tuning the pumping without changing the antenna structure. Furthermore, we discuss the general principles and the opportunities to improve the average performance of the nanoantenna structure. Conclusion: The scheme we propose here can potentially serve as an important component for valley-based applications, such as non-volatile information storage and processing.