Nonlinear vectorial holography with quad-atom metasurfaces.

Vectorial optical holography represents a solution to control the polarization and amplitude distribution of light in the Fourier space. While vectorial optical holography has been experimentally demonstrated in the linear optical regime, its nonlinear counterpart, which can provide extra degrees of freedom of light-field manipulation through the frequency conversion processes, remains unexplored. Here, we experimentally demonstrate the nonlinear vectorial holography through the second harmonic generation process on a quad-atom plasmonic metasurface. The quad-atom metasurface consists of gold meta-atoms with threefold rotational symmetry. Based on the concept of nonlinear geometric phase, we can simultaneously manipulate the phase and amplitude of the left and right circularly polarized second harmonic waves generated from the quad-atom metasurface. By superposing the two orthogonal polarization components, the quad-atom metasurface can produce nonlinear holographic images with vectorial polarization distributions. The proposed metasurface platform may have important applications in vectorial polarization nonlinear optical source, high-capacity optical information storage, and optical encryption.

Dynamic circular birefringence response with fractured geometric phase metasurface systems.

Control over symmetry breaking in three-dimensional electromagnetic systems offers a pathway to tailoring their optical activity. We introduce fractured Pancharatnam­Berry-phase metasurface systems, in which a full-waveplate geometric phase metasurface is fractured into two half-waveplate-based metasurfaces and actively configured using shear displacement. Local relative rotations between stacked half-nanowaveplates within the metasurface system are transduced by shear displacement, leading to dynamic modulation of their collective geometric phase properties. We apply this concept to pairs of periodic Pancharatnam­Berry-phase metasurfaces and experimentally show that these systems support arbitrary and reconfigurable broadband circular birefringence response. High-speed circular birefringence modulation is demonstrated with modest shearing speeds, indicating the potential for these concepts to dynamically control polarization states with fast temporal responses. We anticipate that fractured geometric phase metasurface systems will serve as a nanophotonic platform that leverages systems-level symmetry breaking to enable active electromagnetic wave control.

Multiwavelength Achromatic Deflector in the Visible Using a Single-Layer Freeform Metasurface.

Deflectors are essential for modulating beam direction in optical systems but often face form factor issues or chromatic aberration with conventional optical elements, such as prisms, mirrors, and diffractive/holographic optical elements. Despite recent efforts to address such issues using metasurfaces, their practicality remains limited due to operation wavelengths in the near-infrared or the fabrication difficulties inherent in the multilayer scheme. Here, we propose a novel single-layer metasurface achieving multiwavelength chromatic aberration-free deflection across the visible spectrum by employing the robust freeform design strategy to simplify the fabrication process. By properly selecting diffraction orders for red, green, and blue wavelengths to achieve identical wavelength-diffraction-order products, the metasurface deflects light at a consistent angle of 41.3° with a high efficiency. The coupled Bloch mode analysis explains the physical properties, and experimental fabrication and characterization confirm its effectiveness. This approach holds potential for various applications such as AR/VR, digital cameras, and high-quality optical systems.

Nanoimprinting Solution-Derived Barium Titanate for Electro-Optic Metasurfaces.

Electro-optic metasurfaces have demonstrated significant potential in enhancing the modulation speed and efficiency for fast and large-scale free-space optical devices. Barium titanate has a strong electro-optic Pockels coefficient, but its availability in thin-film form is restricted due to costly growth processes or low thickness. Here, we fabricated active metasurfaces using an etch-free bottom-up process with sol-gel-based polycrystalline barium titanate with a large electro-optic coefficient similar to bulk lithium niobate. We achieve strong hybrid Mie/surface lattice resonances with a quality-factor of 200 at 633 nm wavelength, enhancing the light-matter interaction and therefore the Pockels effect. The metasurface transmission is electro-optically modulated with up to 5 MHz driving frequency at low voltages of less than 1 V thanks to resonant enhancement of the modulation amplitude by 2 orders of magnitude. This successful demonstration of electro-optic modulation in nanoimprinted barium titanate structures paves the way for low-cost and large-scale free-space modulators or tunable metalenses.

Dynamic Spatial-Selective Metasurface with Multiple-Beam Interference.

The emergence of the metasurface has provided a versatile platform for the manipulation of light at the nanoscale. Recent research in metasurfaces has explored a plethora of dynamic control and switching of multifunctionalities, paving the way for innovative applications in fields such as imaging, sensing, and communication. However, current dynamic multifunctional metasurfaces face challenges in terms of functional scalability and selective activation. In this work, we introduce and experimentally demonstrate a strategy that utilizes multiple plane waves to create arbitrary periodic patterns on the metasurface, thus enabling the dynamic and arbitrary spatial-selective activation of its embedded multiplexed functionalities. Furthermore, our strategy facilitates dynamic light control through mechanical translation, as demonstrated by a high-speed, dynamically switchable beam deflection scenario. Our method effectively overcomes the limitations associated with traditional spatially multiplexing techniques, offering greater flexibility and selectivity for dynamic control in multifunctional metasurfaces.

Cylindrical Vector Beam Holography without Preservation of OAM Modes.

Orbital angular momentum (OAM) multiplexed holograms have attracted a great deal of attention recently due to their physically unbounded set of orthogonal helical modes. However, preserving the OAM property in each pixel hinders fine sampling of the target image in principle and requires a fundamental filtering aperture array in the detector plane. Here, we demonstrate the concept of metasurface-based vectorial holography with cylindrical vector beams (CVBs), whose unlimited polarization orders and unique polarization distributions can be used to boost information storage capacity. Although CVBs are composed of OAM modes, the holographic images do not preserve the OAM modes in our design, enabling fine sampling of the target image in a quasi-continuous way like traditional computer-generated holograms. Moreover, the images can be directly observed by passing them through a polarizer without the need for a fundamental mode filter array. We anticipate that our method may pave the way for high-capacity holographic devices.

Twist-Angle-Controlled Nonlinear Circular Dichroism on Gold-Crystal Hybrid Metasurfaces.

Optical chirality, which plays important roles in liquid crystal display and biological and chemical detection, has been attracting scientists' attention due to its potential applications in optical information processing. Usually, the chiral optical response of natural molecules is very weak. However, the emergence of metasurfaces offers a promising solution to solve this issue. By judiciously designing the geometry of meta-atoms, we have realized strong optical circular dichroism (CD) in both linear and nonlinear optical regimes. However, tuning of the CD with a metasurface remains challenging. Here, we propose the twist-angle-controlled nonlinear CD effect by using the second-harmonic generation process on a gold-crystal hybrid metasurface. The CD effect of the second-harmonic waves can be tuned well by controlling the twist angle between the two constituent materials. The proposed hybrid metasurface may open new avenues for developing ultracompact and multifunctional nonlinear optical devices.

Functionality Expansion of Guided Mode Radiation via On-Chip Metasurfaces.

On-chip metasurfaces play a crucial role in bridging the guided mode and free-space light, enabling full control over the wavefront of scattered free-space light in an optimally compact manner. Recently, researchers have introduced various methods and on-chip metasurfaces to engineer the radiation of guided modes, but the total functions that a single metasurface can achieve are still relatively limited. In this work, we propose a novel on-chip metasurface design that can multiplex up to four distinct functions. We can efficiently control the polarization state, phase, angular momentum, and beam profile of the radiated waves by tailoring the geometry of V-shaped nanoantennas integrated on a slab waveguide. We demonstrate several innovative on-chip metasurfaces for switchable focusing/defocusing and for multifunctional generators of orbital angular momentum beams. Our on-chip metasurface design is expected to advance modern integrated photonics, offering applications in optical data storage, optical interconnection, augmented reality, and virtual reality.

Near-Unity All-Optical Modulation of Third-Harmonic Generation with a Fano-Resonant Dielectric Metasurface.

We demonstrate all-optical modulation with a near-unity contrast of nonlinear light generation in a dielectric metasurface. We study third-harmonic generation from silicon Fano-resonant metasurfaces excited by femtosecond pulses at 1480 nm wavelength. We modulate the metasurface resonance by free carrier excitation induced by absorption of an 800 nm pump pulse, leading to up to 93% suppression of third-harmonic generation. Modulation and recovery occur on (sub)picosecond time scales. According to the Drude model, the pump-induced refractive index change blue-shifts the metasurface resonance away from the generation pulse, causing a strong modulation of third-harmonic conversion efficiency. The principle holds great promise for spatiotemporal programmability of nonlinear light generation.

Infrared Spectroscopy of Live Cells Using High-Aspect-Ratio Metal-on-Dielectric Metasurfaces.

Fourier transform infrared (FTIR) spectroscopy is widely used for molecular analysis. However, for the materials situated in an aqueous environment, a precondition for live biological objects such as cells, transmission-based FTIR is prevented by strong water absorption of mid-infrared (MIR) light. Reflection-based cellular assays using internal reflection elements (IREs) such as high-index prisms or flat plasmonic metasurfaces mitigate these issues but suffer from a shallow probing volume localized near the plasma membrane. Inspired by the recent introduction of high-aspect-ratio nanostructures as a novel platform for manipulating cellular behavior, we demonstrate that the integration of plasmonic metasurfaces with tall dielectric nanostructures dramatically enhances the sensing capabilities of FTIR spectroscopy. We also demonstrate the ability of a metal-on-dielectric metasurface to transduce intracellular processes, such as protein translocation to high-curvature membrane regions during cell adhesion, into interpretable spectral signatures of the reflected light.

Far-Field Phase-Shifting Structured Light Illumination Enabled by Polarization Multiplexing Metasurface for Super-Resolution Imaging.

The phase-shifting structured light illumination technique is widely used in imaging but often relies on mechanical translation stages or spatial light modulators, leading to system instability, low displacement accuracy, and limited integration feasibility. In response to these challenges, we propose and demonstrate an approach for generating far-field phase-shifting structured light using a polarization multiplexing metasurface. By controlling the polarization states of incident and transmitted light, the metasurface creates a three-step displacement of structured light, eliminating the need to move samples or illumination sources. As a proof of concept, we experimentally demonstrate microscopic imaging using structured light illumination generated by metasurfaces, extracting high-frequency information from objects, and surpassing the diffraction limit. The proposed metasurface platform offers a promising approach for developing compact and robust phase-shifting imaging systems, with broad prospects in quantitative detection, machine vision, and beyond.

Large-Area Perovskite Nanocrystal Metasurfaces for Direction-Tunable Lasing.

Perovskite nanocrystals (PNCs) are attractive emissive materials for developing compact lasers. However, manipulation of PNC laser directionality has been difficult, which limits their usage in photonic devices that require on-demand tunability. Here we demonstrate PNC metasurface lasers with engineered emission angles. We fabricated millimeter-scale CsPbBr3 PNC metasurfaces using an all-solution-processing technique based on soft nanoimprinting lithography. By designing band-edge photonic modes at the high-symmetry X point of the reciprocal lattice, we achieved four linearly polarized lasing beams along a polar angle of ∼30° under optical pumping. The device architecture further allows tuning of the lasing emission angles to 0° and ∼50°, respectively, by adjusting the PNC thickness to shift other high-symmetry points (Γ and M) to the PNC emission wavelength range. Our laser design strategies offer prospects for applications in directional optical antennas and detectors, 3D laser projection displays, and multichannel visible light communication.

Achromatic Full Stokes Polarimetry Metasurface for Full-Color Polarization Imaging in the Visible Range.

Metasurfaces provide an ultrathin platform for compact, real-time polarimetry. However, their applications in polychromatic scenes are restricted by narrow operating bandwidths that causes spectral information loss. Here, we demonstrate full-color polarization imaging using an achromatic polarimeter consisting of four polarization-dependent metalenses. Leveraging an intelligent design scheme, we achieve effective arbitrary phase compensation and multiobjective matching with a limited database. This system provides broadband achromaticity across wavelengths from 450 to 650 nm, resulting in a relative bandwidth of approximately 0.364 for full Stokes imaging. Experimental reconstruction errors for wavelengths of 450, 550, and 650 nm are 7.5%, 5.9%, and 3.8%, respectively. Performance is evaluated based on both achromatic bandwidth and crosstalk, with our design achieving three times the performance of the current state-of-the-art. The full-color, full-polarization imaging capability of the device is further validated with a customized object. The proposed scheme advances polarization imaging for practical applications.

Intrinsic Superchirality in Planar Plasmonic Metasurfaces.

Plasmonic metasurfaces with spatial symmetry breaking are crucial materials with significant applications in fields such as polarization-controlled photonic devices and nanophotonic platforms for chiral sensing. In this paper, we introduce planar plasmonic metasurfaces, less than one-tenth of a wavelength thick, featuring nanocavities formed by three equilateral triangles. This configuration creates uniform, thin metasurfaces. Through a combination of experimental measurements and numerical modeling, we demonstrate the inherent superchirality of these plasmonic metasurfaces. We address the challenge of achieving a strong enhancement of optical chirality in the visible spectrum, reaching levels comparable to those of 3D chiral metasurfaces.

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.

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.

Printable Light-Emitting Metasurfaces with Enhanced Directional Photoluminescence.

Nanoimprint lithography is gaining popularity as a cost-efficient way to reproduce nanostructures in large quantities. Recent advances in nanoimprinting lithography using high-index nanoparticles have demonstrated replication of photonic devices, but it is difficult to confer special properties on nanostructures beyond general metasurfaces. Here, we introduce a novel method for fabricating light-emitting metasurfaces using nanoimprinting lithography. By utilizing quantum dots embedded in resin, we successfully imprint dielectric metasurfaces that function simultaneously as both emitters and resonators. This approach to incorporating quantum dots into metasurfaces demonstrates an improvement in photoluminescence characteristics compared to the situation where quantum dots and metasurfaces are independently incorporated. Design of the metasurface is specifically tailored to support photonic modes within the emission band of quantum dots with a large enhancement of photoluminescence. This study indicates that nanoimprinting lithography has the capability to construct nanostructures using functionalized nanoparticles and could be used in various fields of nanophotonic applications.

Achromatic and Coma-Corrected Hybrid Meta-Optics for High-Performance Thermal Imaging.

Long-wave infrared (LWIR) imaging, or thermal imaging, is widely applied in night vision and security monitoring. However, the widespread use of LWIR imagers is impeded by their bulky size, considerable weight, and high cost. While flat meta-optics present a potential solution to these limitations, existing pure LWIR meta-optics face constraints such as severe chromatic or coma aberrations. Here, we introduce an approach utilizing large-scale hybrid meta-optics to address these challenges and demonstrate the achromatic, coma-corrected, and polarization-insensitive thermal imaging. The hybrid metalens doublet is composed of a metasurface corrector and a refractive lens, featuring a full field-of-view angle surpassing 20° within the 8-12 µm wavelength range. Employing this hybrid metalens doublet, we showcase high-performance thermal imaging capabilities both indoors and outdoors, effectively capturing ambient thermal radiation. The proposed hybrid metalens doublet holds considerable promise for advancing miniaturized, lightweight, and cost-effective LWIR optical imaging systems.

Cryogenic Electron-Beam Writing for Perovskite Metasurface.

Halide perovskites (HPs) metasurfaces have recently attracted significant interest due to their potential to not only further enhance device performance but also reveal the unprecedented functionalities and novel photophysical properties of HPs. However, nanopatterning on HPs is critically challenging as they are readily destructed by the organic solvents in the standard lithographic processes. Here, we present a novel, subtle, and fully nondestructive HPs metasurface fabrication strategy based on cryogenic electron-beam writing. This technique allows for high-precision patterning and in situ imaging of HPs with excellent compatibility. As a proof-of-concept, broadband absorption enhanced metasurfaces were realized by patterning nanopillar arrays on CH3NH3PbI3 film, which results in photodetectors with approximately 14-times improvement on responsivity and excellent stability. Our findings highlight the great feasibility of cryogenic electron-beam writing for producing perovskite metasurface and unlocking the unprecedented photoelectronic properties of HPs.

Broadband, High-Reflectivity Dielectric Mirrors at Wafer Scale: Combining Photonic Crystal and Metasurface Architectures for Advanced Lightsails.

Highly ambitious initiatives aspire to propel a miniature spacecraft to a neighboring star within a human generation, leveraging the radiation pressure of lasers for propulsion. One major challenge for this enormous feat is to build a meter-scale, ultralow mass lightsail with broadband reflectivity. In this work, we present the design and fabrication of a lightsail composed of two distinct dielectric layers with photonic crystal/metasurface structure covering a 4" wafer. We achieved broadband reflection of >70% spanning over the full Doppler-shifted laser wavelength range during spacecraft acceleration with a low total mass in the range of a few grams when scaled up to meter size. Furthermore, we find new paths to reliably fabricate these subwavelength structures over macroscopic areas and then systematically characterize their optical performance, confirming their suitability for future lightsail applications. Our innovative device and precise nanofabrication approaches represent a significant leap toward interstellar exploration.