Third Harmonic Generation Enhancement and Wavefront Control Using a Local High-Q Metasurface.

High quality factor optical nanostructures provide a great opportunity to enhance nonlinear optical processes such as third harmonic generation. However, the field enhancement in these high quality factor structures is typically accompanied by optical mode nonlocality. As a result, the enhancement of nonlinear processes comes at the cost of their local control as needed for nonlinear wavefront shaping, imaging, and holography. Here we show simultaneous strong enhancement and spatial control over third harmonic generation with a local high-Q metasurface relying on higher-order Mie resonant modes. Our results demonstrate third harmonic generation at an efficiency of up to 3.25 × 10-5, high quality wavefront shaping as illustrated by a third harmonic metalens, and a flatband, angle independent, third harmonic response up to ±11° incident angle. The demonstrated high level of local control and efficient frequency conversion offer promising prospects for realizing novel nonlinear optical devices.

A Quasi-Bound States in the Continuum Dielectric Metasurface-Based Antenna-Reactor Photocatalyst.

Metasurfaces are a class of two-dimensional artificial resonators, creating new opportunities for strong light-matter interactions. One type of nonradiative optical metasurface that enables substantial light concentration is based on quasi-Bound States in the Continuum (quasi-BIC). Here we report the design and fabrication of a quasi-BIC dielectric metasurface that serves as an optical frequency antenna for photocatalysis. By depositing Ni nanoparticle reactors onto the metasurface, we create an antenna-reactor photocatalyst, where the virtually lossless metasurface funnels light to drive a chemical reaction. This quasi-BIC-Ni antenna-reactor drives H2 dissociation under resonant illumination, showing strong polarization, wavelength, and optical power dependencies. Both E-field-induced electronic and photothermal heating effects drive the reaction, supported by load-dependent reactivity studies and our theoretical model. This study unlocks new opportunities for photocatalysis that employ dielectric metasurfaces for light harvesting in an antenna-reactor format.

Ultrahigh-Q Metasurface Transparency Band Induced by Collective-Collective Coupling.

The metasurface analogue of electromagnetically induced transparency (EIT) provides a chip-scale platform for achieving light delay and storage, high Q factors, and greatly enhanced optical fields. However, the literature relies on the coupling between localized and localized or localized and collective resonances, limiting the Q factor and related performance. Here, we report a novel approach for realizing collective EIT-like bands with a measured Q factor reaching 2750 in silicon metasurfaces in the near-infrared regime, exceeding the state of the art by more than 5 times. It employs the coupling between two collective resonances, the Mie electric dipole surface lattice resonance (SLR) and the out-of-plane/in-plane electric quadrupole SLR (EQ-SLR). Remarkably, the collective EIT-like resonance can have diverging Q factor and group delay due to the bound state in the continuum characteristics of the in-plane EQ-SLR. With these findings, our study opens a new route for tailoring light flow in metasurfaces.

High-Performance Refractive Index and Temperature Sensing Based on Toroidal Dipole in All-Dielectric Metasurface.

This article shows an all-dielectric metasurface consisting of "H"-shaped silicon disks with tilted splitting gaps, which can detect the temperature and refractive index (RI). By introducing asymmetry parameters that excite the quasi-BIC, there are three distinct Fano resonances with nearly 100% modulation depth, and the maximal quality factor (Q-factor) is over 104. The predominant roles of different electromagnetic excitations in three distinct modes are demonstrated through near-field analysis and multipole decomposition. A numerical analysis of resonance response based on different refractive indices reveals a RI sensitivity of 262 nm/RIU and figure of merit (FOM) of 2183 RIU-1. This sensor can detect temperature fluctuations with a temperature sensitivity of 59.5 pm/k. The proposed metasurface provides a novel method to induce powerful TD resonances and offers possibilities for the design of high-performance sensors.

High-Efficiency, 80 mm Aperture Metalens Telescope.

Metalenses promise potential for a paradigm shift of conventional optical devices. However, the aperture sizes of metalenses are usually bound within hundreds of micrometers by the commonly used fabrication methods, limiting their usage on practical optical devices like telescopes. Here, for the first time, we demonstrate a high-efficiency, single-lens, refractive metalens telescope. We developed a mass production-friendly workflow for fabricating wafer-scale (80 mm aperture) metalenses using deep-ultraviolet (DUV) photolithography. Our metalens works in the near-infrared region with nearly diffraction-limited focal spot sizes and a high peak focusing efficiency of 80.84% at 1450 nm experimentally. Based on the metalens, we built a single-lens telescope and acquired images of the lunar surface, revealing its geographical structures. We believe our demonstration of the metalens telescope proves the exciting potential lying in the metasurfaces and could bring new possibilities for areas involving large optical systems, including geosciences, planetary observation, and astrophysical science.

Color Printing and Encryption with Polarization-Switchable Structural Colors on All-Dielectric Metasurfaces.

Metasurface-based structural color with high resolution is promising for color printing and encryption. However, achieving tunable structural colors in practical applications is challenging owing to the immutability after the fabrication of metasurfaces. Herein, we proposed the polarization-switchable dielectric metasurfaces with full colors. The colorful images can be switched on/off by controlling the polarization of incident light. For the nanorods metasurfaces, all colors turned to black in the "off" mode because of the near-zero reflection, and the uniform black was advantageous for designing encryption applications. For the nanocrosses metasurfaces, colors reversed in two different "on" modes and images hidden in the "off" mode. With the polarization-sensitive metasurfaces, a fish-bird image, an overlapped dual-channel image, and a green-red heart image were obtained, respectively. The demonstrations can be applied to dynamic displays, optical cryptography, multichannel imaging, and optical data storage.

Metasurface Biosensors Enabling Single-Molecule Sensing of Cell-Free DNA.

In this study, we have revealed that highly fluorescence (FL)-enhancing all-dielectric metasurface biosensors are capable of detecting single-target DNA, which is cell-free DNA (cfDNA) specific to the human practice effect. The ultimately high-precision detection was achieved in a scheme combining the metasurface biosensors with a short-time nucleic acid amplification technique, that is, a reduced-cycle polymerase chain reaction (PCR). In this combined scheme, we obtained a series of FL signals at a single-molecule concentration, reflecting the Poisson distribution, and moreover elucidated that the FL signals exhibit the single-molecule cfDNA detection with more than 84% statistical confidence in an automated FL detection system and with 99.9% statistical confidence in confocal FL microscopy. As a result, we have found a simple and practical test to discriminate the target of 1 copy/test from zero using metasurface biosensors, which has not been realized by other elaborate techniques such as digital PCR.

Phase Interrogation Sensor Based on All-Dielectric BIC Metasurface.

The low performance of sensors based on an all-dielectric metasurface limits their application compared to metallic counterparts. Here, for the first time, an all-dielectric BIC (bound states in the continuum) metasurface is employed for highly sensitive phase interrogation refractive index sensing. The proposed sensor is well analyzed, fabricated, and characterized. Experimentally, a high-performance BIC-based microfluidic sensing chip with a Q factor of 1200 is achieved by introducing symmetry breaking. A refractive index sensor with high figure of merit of 418 RIU-1 is demonstrated, which is beneficial to the phase interrogation. Notably, we measure a record phase interrogation sensitivity of 2.7 × 104 deg/RIU to the refractive index, thus enabling the all-dielectric BIC to rival the refractive index detection capabilities of metal-based sensors such as surface plasmon resonance. This scheme establishes a pivotal role of the all-dielectric metasurface in the field of ultrahigh sensitivity sensors and opens possibilities for trace detection in biochemical analysis and environment monitoring.

Larger-Than-Unity External Optical Field Confinement Enabled by Metamaterial-Assisted Comb Waveguide for Ultrasensitive Long-Wave Infrared Gas Spectroscopy.

Nanophotonic waveguides that implement long optical pathlengths on chips are promising to enable chip-scale gas sensors. Nevertheless, current absorption-based waveguide sensors suffer from weak interactions with analytes, limiting their adoptions in most demanding applications such as exhaled breath analysis and trace-gas monitoring. Here, we propose an all-dielectric metamaterial-assisted comb (ADMAC) waveguide to greatly boost the sensing capability. By leveraging large longitudinal electric field discontinuity at periodic high-index-contrast interfaces in the subwavelength grating metamaterial and its unique features in refractive index engineering, the ADMAC waveguide features strong field delocalization into the air, pushing the external optical field confinement factor up to 113% with low propagation loss. Our sensor operates in the important but underdeveloped long-wave infrared spectral region, where absorption fingerprints of plentiful chemical bonds are located. Acetone absorption spectroscopy is demonstrated using our sensor around 7.33 µm, showing a detection limit of 2.5 ppm with a waveguide length of only 10 mm.

Engineering Electromagnetic Field Distribution and Resonance Quality Factor Using Slotted Quasi-BIC Metasurfaces.

Dielectric metasurfaces governed by bound states in the continuum (BIC) are actively investigated for achieving high-quality factors and strong electromagnetic field enhancements. Traditional approaches reported for tuning the performance of quasi-BIC metasurfaces include tuning the resonator size, period, and structure symmetry. Here we propose and experimentally demonstrate an alternative approach through engineering slots within a zigzag array of elliptical silicon resonators. Through analytical theory, three-dimensional electromagnetic modeling, and infrared spectroscopy, we systematically investigate the spectral responses and field distributions of the slotted metasurface in the mid-IR. Our results show that by introducing slots, the electric field intensity enhancement near the apex and the quality factor of the quasi-BIC resonance are increased by a factor of 2.1 and 3.3, respectively, in comparison to the metasurface without slots. Furthermore, the slotted metasurface also provides extra regions of electromagnetic enhancement and confinement, which holds enormous potential in particle trapping, sensing, and emission enhancement.

An All-Dielectric Polaritonic Metasurface with a Giant Nonlinear Optical Response.

Enhancing the efficiency of second-harmonic generation using all-dielectric metasurfaces to date has mostly focused on electromagnetic engineering of optical modes in the meta-atom. Further advances in nonlinear conversion efficiencies can be gained by engineering the material nonlinearities at the nanoscale, however this cannot be achieved using conventional materials. Semiconductor heterostructures that support resonant nonlinearities using quantum engineered intersubband transitions can provide this new degree of freedom. By simultaneously optimizing the heterostructures and meta-atoms, we experimentally realize an all-dielectric polaritonic metasurface with a maximum second-harmonic generation power conversion factor of 0.5 mW/W2 and power conversion efficiencies of 0.015% at nominal pump intensities of 11 kW/cm2. These conversion efficiencies are higher than the record values reported to date in all-dielectric nonlinear metasurfaces but with 3 orders of magnitude lower pump power. Our results therefore open a new direction for designing efficient nonlinear all-dielectric metasurfaces for new classical and quantum light sources.

Polarization-Dependent All-Dielectric Metasurface for Single-Shot Quantitative Phase Imaging.

Phase retrieval is a noninterferometric quantitative phase imaging technique that has become an essential tool in optical metrology and label-free microscopy. Phase retrieval techniques require multiple intensity measurements traditionally recorded by camera or sample translation, which limits their applicability mostly to static objects. In this work, we propose the use of a single polarization-dependent all-dielectric metasurface to facilitate the simultaneous recording of two images, which are utilized in phase calculation based on the transport-of-intensity equation. The metasurface acts as a multifunctional device that splits two orthogonal polarization components and adds a propagation phase shift onto one of them. As a proof-of-principle, we demonstrate the technique in the wavefront sensing of technical samples using a standard imaging setup. Our metasurface-based approach fosters a fast and compact configuration that can be integrated into commercial imaging systems.

Ultracompact Energy Transfer in Anapole-based Metachains.

Realization of electromagnetic energy confinement beyond the diffraction limit is crucial for high-performance on-chip devices. Herein we construct an array of nonradiative anapoles that originate from the destructive far-field interference of electric and toroidal dipole modes to achieve ultracompact and high-efficiency electromagnetic energy transfer without the coupler. We experimentally investigate the proposed metachain at mid-infrared frequencies and give the first near-field experimental evidence of anapole-based energy transfer, in which the spatial profile of the anapole mode is also unambiguously identified on the nanoscale. We further demonstrate that the metachain is intrinsically lossless and scalable at infrared wavelengths, realizing a 90° bending loss down to 0.32 dB at the optical communication wavelength. The present scheme bridges the gap between the energy confinement and the transfer of anapoles and opens a new gate for more compactly integrated photonic and energy devices, which can operate in a broad spectral range.

Tailoring Third-Harmonic Diffraction Efficiency by Hybrid Modes in High-Q Metasurfaces.

Metasurfaces are versatile tools for manipulating light; however, they have received little attention as devices for the efficient control of nonlinearly diffracted light. Here, we demonstrate nonlinear wavefront control through third-harmonic generation (THG) beaming into diffraction orders with efficiency tuned by excitation of hybrid Mie-quasi-bound states in the continuum (BIC) modes in a silicon metasurface. Simultaneous excitation of the high-Q collective Mie-type modes and quasi-BIC modes leads to their hybridization and results in a local electric field redistribution. We probe the hybrid mode by measuring far-field patterns of THG and observe the strong switching between (0,-1) and (-1,0) THG diffraction orders from 1:6 for off-resonant excitation to 129:1 for the hybrid mode excitation, showing tremendous contrast in controlling the nonlinear diffraction patterns. Our results pave the way to the realization of metasurfaces for novel light sources, telecommunications, and quantum photonics.

Simultaneous Measurements of Refractive Index and Methane Concentration through Electromagnetic Fano Resonance Coupling in All-Dielectric Metasurface.

Dual-parameter measurements of refractive index and methane concentration based on electromagnetic Fano resonance are proposed. Two independent Fano resonances can be produced through electric dipole and toroidal dipole resonance in an all-dielectric metasurface separately. The linear relationship between the spectral peak-shifts and the parameters to be measured will be obtained directly. The refractive index (RI) sensitivity and gas sensitivity are 1305.6 nm/refractive index unit (RIU), -0.295 nm/% for one resonance peak (dip1), and 456.6 nm/RIU, -0.61 nm/% for another resonance peak (dip2). Such a metasurface has simpler structure and higher sensitivity, which is beneficial for environmental gas monitoring or multi-parameter measurements.

All-Dielectric Silicon Nanoring Metasurface for Full-Color Printing.

Structural color has been particularly attractive as it provides a highly promising approach for next-generation color printing. Plasmonic nanostructures have been intensively investigated for color printing, while suffering from intrinsic loss that degrades the quality of the coloration. Dielectric materials have emerged as an alternative because of their high refractive index that enables highly confined optical modes within the nanostructure at the diffraction limit. Here, we demonstrate an all-dielectric nanoring metasurface for coloration. By harnessing the intrinsic nanoring structure design, vivid structural color has been achieved in the visible range. The color gamut is expected to occupy 115% of the standard color space (sRGB) on the chromaticity diagram of the International Commission on Illumination (CIE) 1931 in theory. Our structure can be applied to various complex devices and materials and find potential applications such as displays, information, and art works.

Quasi-BIC Resonant Enhancement of Second-Harmonic Generation in WS2 Monolayers.

Atomically thin monolayers of transition metal dichalcogenides (TMDs) have emerged as a promising class of novel materials for optoelectronics and nonlinear optics. However, the intrinsic nonlinearity of TMD monolayers is weak, limiting their functionalities for nonlinear optical processes such as frequency conversion. Here we boost the effective nonlinear susceptibility of a TMD monolayer by integrating it with a resonant dielectric metasurface that supports pronounced optical resonances with high quality factors: bound states in the continuum (BICs). We demonstrate that a WS2 monolayer combined with a silicon metasurface hosting BICs exhibits enhanced second-harmonic intensity by more than 3 orders of magnitude relative to a WS2 monolayer on top of a flat silicon film of the same thickness. Our work suggests a pathway to employ high-index dielectric metasurfaces as hybrid structures for enhancement of TMD nonlinearities with applications in nonlinear microscopy, optoelectronics, and signal processing.

Enhanced Nonlinear Light Generation in Oligomers of Silicon Nanoparticles under Vector Beam Illumination.

All-dielectric nanoparticle oligomers have recently emerged as promising candidates for nonlinear optical applications. Their highly resonant collective modes, however, are difficult to access by linearly polarized beams due to symmetry restraints. In this paper, we propose a new way to increase the efficiency of nonlinear processes in all-dielectric oligomers by tightly focused azimuthally polarized cylindrical vector beam illumination. We demonstrate two orders enhancement of the third-harmonic generation signal, governed by a collective optical mode represented by out-of-plane magnetic dipoles. Crucially, the collective mode is characterized by strong electromagnetic field localization in the bulk of the nonlinear material. For comparison, we measure third-harmonic generation in the same oligomer pumped with linearly and radially polarized fundamental beams, which both show significantly lower harmonic output. We also provide numerical analysis to describe and characterize the observed effect. Our findings open a new route to enhance and modulate the third-harmonic generation efficiency of Mie-resonant isolated nanostructures by tailoring the polarization of the pump beam.

All-Dielectric Nanostructures with a Thermoresponsible Dynamic Polymer Shell.

We suggest a new strategy for creating stimuli-responsive bio-integrated optical nanostructures based on Mie-resonant silicon nanoparticles covered by an ensemble of similarity negatively charged polyelectrolytes (heparin and sodium polystyrene sulfonate). The dynamic tuning of the nanostructures' optical response is due to light-induced heating of the nanoparticles and swelling of the polyelectrolyte shell. The resulting hydrophilic/hydrophobic transitions significantly change the shell thickness and reversible shift of the scattering spectra for individual nanoparticles up to 60 nm. Our findings bring novel opportunities for the application of smart nanomaterials in nanomedicine and bio-integrated nanophotonics.

Simultaneous Spectral and Spatial Modulation for Color Printing and Holography Using All-Dielectric Metasurfaces.

Metasurfaces possess the outstanding ability to tailor phase, amplitude, and even spectral responses of light with an unprecedented ultrahigh resolution and thus have attracted significant interest. Here, we propose and experimentally demonstrate a novel meta-device that integrates color printing and computer-generated holograms within a single-layer dielectric metasurface by modulating spectral and spatial responses at subwavelength scale, simultaneously. In our design, such metasurface appears as a microscopic color image under white light illumination, while encrypting two different holographic images that can be projected at the far-field when illuminated with red and green laser beams. We choose amorphous silicon dimers and nanofins as building components and use a modified parallel Gerchberg-Saxton algorithm to obtain multiple subholograms with arbitrary spatial shapes for image-indexed arrangements while avoiding the loss of phase information. Such a method can further extend the design freedom of metasurfaces. By exploiting spectral and spatial control at the level of individual pixels, multiple sets of independent information can be introduced into a single-layer device; the additional complexity and enlarged information capacity are promising for novel applications such as information security and anticounterfeiting.