All-Glass 100 mm Diameter Visible Metalens for Imaging the Cosmos.

Metasurfaces, optics made from subwavelength-scale nanostructures, have been limited to millimeter-sizes by the scaling challenge of producing vast numbers of precisely engineered elements over a large area. In this study, we demonstrate an all-glass 100 mm diameter metasurface lens (metalens) comprising 18.7 billion nanostructures that operates in the visible spectrum with a fast f-number (f/1.5, NA = 0.32) using deep-ultraviolet (DUV) projection lithography. Our work overcomes the exposure area constraints of lithography tools and demonstrates that large metasurfaces are commercially feasible. Additionally, we investigate the impact of various fabrication errors on the imaging quality of the metalens, several of which are specific to such large area metasurfaces. We demonstrate direct astronomical imaging of the Sun, the Moon, and emission nebulae at visible wavelengths and validate the robustness of such metasurfaces under extreme environmental thermal swings for space applications.

Simulational investigation of self-aligned bilayer linear grating enabling highly enhanced responsivity of MWIR InAs/GaSb type-II superlattice (T2SL) photodetector.

Linear gratings polarizers provide remarkable potential to customize the polarization properties and tailor device functionality via dimensional tuning of configurations. Here, we extensively investigate the polarization properties of single- and double-layer linear grating, mainly focusing on self-aligned bilayer linear grating (SABLG), serving as a wire grid polarizer in the mid-wavelength infrared (MWIR) region. Computational analyses revealed the polarization properties of SABLG, highlighting enhancement in TM transmission and reduction in TE transmission compared to single-layer linear gratings (SLG) due to optical cavity effects. As a result, the extinction ratio is enhanced by approximately 2724-fold in wavelength 3-6 µm. Furthermore, integrating the specially designed SABLG with an MWIR InAs/GaSb Type-II Superlattice (T2SL) photodetector yields a significantly enhanced spectral responsivity. The TM-spectral responsivity of SABLG is enhanced by around twofold than the bare device. The simulation methodology and analytical analysis presented herein provide a versatile route for designing optimized polarimetric structures integrated into infrared imaging devices, offering superior capabilities to resolve linear polarization signatures.

Highly Sensitive and Cost-Effective Polymeric-Sulfur-Based Mid-Wavelength Infrared Linear Polarizers with Tailored Fabry-Pérot Resonance.

Inverse-vulcanized polymeric sulfur has received considerable attention for application in waste-based infrared (IR) polarizers with high polarization sensitivities, owing to its high transmittance in the IR region and thermal processability. However, there have been few reports on highly sensitive polymeric sulfur-based polarizers by replication of pre-simulated dimensions to achieve a high transmission of the transverse magnetic field (TTM ) and extinction ratio (ER). Herein, a 400-nanometer-pitch mid-wavelength infrared bilayer linear polarizer with self-aligned metal gratings is introduced on polymeric sulfur gratings integrated with a spacer layer (SM-polarizer). The dimensions of the SM-polarizer can be closely replicated using pre-simulated dimensions via a systematic investigation of thermal nanoimprinting conditions. Spacer thickness is tailored from 40 to 5100 nm by adjusting the concentration of polymeric sulfur solution during spin-coating. A tailored spacer thickness can maximize TTM in the broadband MWIR region by satisfying Fabry-Pérot resonance. The SM-polarizer yields TTM of 0.65, 0.59, and 0.43 and ER of 3.12 × 103 , 5.19 × 103 , and 5.81 × 103 at 4 µm for spacer thicknesses of 90, 338, and 572 nm, respectively. This demonstration of a highly sensitive and cost-effective SM-polarizer opens up exciting avenues for infrared polarimetric imaging and for applications in polarization manipulation.

Maximized Frequency Doubling through the Inverse Design of Nonlinear Metamaterials.

The conventional process for developing an optimal design for nonlinear optical responses is based on a trial-and-error approach that is largely inefficient and does not necessarily lead to an ideal result. Deep learning can automate this process and widen the realm of nonlinear geometries and devices. This research illustrates a deep learning framework used to create an optimal plasmonic design for a nonlinear metamaterial. The algorithm produces a plasmonic pattern that can maximize the second-order nonlinear effect of a nonlinear metamaterial. A nanolaminate metamaterial is used as a nonlinear material, and plasmonic patterns are fabricated on the prepared nanolaminate to demonstrate the validity and efficacy of the deep learning algorithm. The optimal pattern produced yielded second-harmonic generation from the nanolaminate with normal incident fundamental light. The deep learning architecture applied in this research can be expanded to other optical responses and light-matter interaction processes.

Programmable Stepwise Collective Magnetic Self-Assembly of Micropillar Arrays.

Chain-like magnetic self-organizations have been documented for micron/submicron-scale magnetic particles. However, the positions of the particles are not stationary in a sustaining fluid owing to Brownian translational motion, resulting in irregular magnetic self-assembly. Toward the development of a programmable and reversible magnetic self-assembly, we report a stepwise collective magnetic self-assembly with periodic polymeric micropillar arrays containing magnetic particles. Under an external magnetic field, the individual micropillar acts as a micromagnet; magnetic polarities of embedded ferromagnetic particles are arranged in the same direction. The nearest pillar tops undergo a pairwise assembly owing to the anisotropic quadrupolar interaction, whereas the pillar bases remain stationary because of the presence of a magnetically inert substrate. By increasing the magnetic flux density, a collective quad-body assembly of vicinal paired micropillars is accomplished, finally leading to long-range connectivity of the pillar tops. Simple evaporation of the polymeric solution yields shape-fixation of the connected micropillar architectures even after magnetic fields are removed. We investigate geometric effects on this stepwise collective magnetic self-assembly using rectangular, square, and circular micropillars. Also, we demonstrate spatially selective magnetic self-assembly (e.g., arbitrary letters) using a masking technique. Finally, we demonstrate on-demand programming of bidirectional liquid spreading through long-range ordered magnetic self-assembly.

High-Efficiency Solar Vapor Generation Boosted by a Solar-Induced Updraft with Biomimetic 3D Structures.

Sunlight-based desalination is one of the most environment-friendly, low-cost methods for obtaining freshwater on the planet. We implemented a biomimetic three-dimensional (3D) solar evaporator, improved by a solar-induced air-flow updraft. A carbon-coated polyvinyl alcohol (PVA) foam allowed us to achieve perfect absorption of ultrabroadband sunlight and continuously provide water to tall 3D structures. Integrating the convection flower (Amorphophallus titanum) and solar chimney structure, we proposed a bio-inspired 3D solar evaporator system that generates an updraft airflow. This updraft replaces saturated vapor between neighboring PVA foams with dry air, resulting in a significant increase in the effectiveness of dry air-water contact interfaces. Under the 1 sun condition (1 kW m-2), we achieve a high solar-vapor conversion efficiency of 95.9%.

Replicable Quasi-Three-Dimensional Plasmonic Nanoantennas for Infrared Bandpass Filtering.

Quasi-three-dimensionally designed metal-dielectric hybrid nanoantennas have provided a unique capability to control light at the nanoscale beyond the diffraction limit, which has enabled powerful optical manipulation techniques. However, the fabrication of these nanoantennas has largely relied on the use of nanolithography techniques that are time- and cost-consuming, impeding their application in wide-ranging use. Herein, we report a versatile methodology enabling the repetitive replication of these nanoantennas from their silicon molds with tailored optical features for infrared bandpass filtering. Comprehensive experimental and computational analyses revealed the underlying mechanism of this methodology and also provided a technical guideline for pragmatic translation into infrared filters in multispectral imaging.

A Pearl Spectrometer.

Information recovery from incomplete measurements, typically performed by a numerical means, is beneficial in a variety of classical and quantum signal processing. Random and sparse sampling with nanophotonic and light scattering approaches has received attention to overcome the hardware limitations of conventional spectrometers and hyperspectral imagers but requires high-precision nanofabrications and bulky media. We report a simple spectral information processing scheme in which light transport through an Anderson-localized medium serves as an entropy source for compressive sampling directly in the frequency domain. As implied by the "lustrous" reflection originating from the exquisite multilayered nanostructures, a pearl (or mother-of-pearl) allows us to exploit the spatial and spectral intensity fluctuations originating from strong light localization for extracting salient spectral information with a compact and thin form factor. Pearl-inspired light localization in low-dimensional structures can offer an alternative of spectral information processing by hybridizing digital and physical properties at a material level.

Fractal Web Design of a Hemispherical Photodetector Array with Organic-Dye-Sensitized Graphene Hybrid Composites.

The vision system of arthropods consists of a dense array of individual photodetecting elements across a curvilinear surface. This compound-eye architecture could be a useful model for optoelectronic sensing devices that require a large field of view and high sensitivity to motion. Strategies that aim to mimic the compound-eye architecture involve integrating photodetector pixels with a curved microlens, but their fabrication on a curvilinear surface is challenged by the use of standard microfabrication processes that are traditionally designed for planar, rigid substrates (e.g., Si wafers). Here, a fractal web design of a hemispherical photodetector array that contains an organic-dye-sensitized graphene hybrid composite is reported to serve as an effective photoactive component with enhanced light-absorbing capabilities. The device is first fabricated on a planar Si wafer at the microscale and then transferred to transparent hemispherical domes with different curvatures in a deterministic manner. The unique structural property of the fractal web design provides protection of the device from damage by effectively tolerating various external loads. Comprehensive experimental and computational studies reveal the essential design features and optoelectronic properties of the device, followed by the evaluation of its utility in the measurement of both the direction and intensity of incident light.

Microconical silicon mid-IR concentrators: spectral, angular and polarization response.

It is widely discussed in the literature that a problem of reduction of thermal noise of mid-wave and long-wave infrared (MWIR and LWIR) cameras and focal plane arrays (FPAs) can be solved by using light-concentrating structures. The idea is to reduce the area and, consequently, the thermal noise of photodetectors, while still providing a good collection of photons on photodetector mesas that can help to increase the operating temperature of FPAs. It is shown that this approach can be realized using microconical Si light concentrators with (111) oriented sidewalls, which can be mass-produced by anisotropic wet etching of Si (100) wafers. The design is performed by numerical modeling in a mesoscale regime when the microcones are sufficiently large (several MWIR wavelengths) to resonantly trap photons, but still too small to apply geometrical optics or other simplified approaches. Three methods of integration Si microcone arrays with the focal plane arrays are proposed and studied: (i) inverted microcones fabricated in a Si slab, which can be heterogeneously integrated with the front illuminated FPA photodetectors made from high quantum efficiency materials to provide resonant power enhancement factors (PEF) up to 10 with angle-of-view (AOV) up to 10°; (ii) inverted microcones, which can be monolithically integrated with metal-Si Schottky barrier photodetectors to provide resonant PEFs up to 25 and AOVs up to 30° for both polarizations of incident plane waves; and iii) regular microcones, which can be monolithically integrated with near-surface photodetectors to provide a non-resonant power concentration on compact photodetectors with large AOVs. It is demonstrated that inverted microcones allow the realization of multispectral imaging with ∼100 nm bands and large AOVs for both polarizations. In contrast, the regular microcones operate similar to single-pass optical components (such as dielectric microspheres), producing sharply focused photonic nanojets.

Plasmonic-Layered InAs/InGaAs Quantum-Dots-in-a-Well Pixel Detector for Spectral-Shaping and Photocurrent Enhancement.

The algorithmic spectrometry as an alternative to traditional approaches has the potential to become the next generation of infrared (IR) spectral sensing technology, which is free of physical optical filters, and only a very small number of data are required from the IR detector. A key requirement is that the detector spectral responses must be engineered to create an optimal basis that efficiently synthesizes spectral information. Light manipulation through metal perforated with a two-dimensional square array of subwavelength holes provides remarkable opportunities to harness the detector response in a way that is incorporated into the detector. Instead of previous experimental efforts mainly focusing on the change over the resonance wavelength by tuning the geometrical parameters of the plasmonic layer, we experimentally and numerically demonstrate the capability for the control over the shape of bias-tunable response spectra using a fixed plasmonic structure as well as the detector sensitivity improvement, which is enabled by the anisotropic dielectric constants of the quantum dots-in-a-well (DWELL) absorber and the presence of electric field along the growth direction. Our work will pave the way for the development of an intelligent IR detector, which is capable of direct viewing of spectral information without utilizing any intervening the spectral filters.

Shape-Programmed Fabrication and Actuation of Magnetically Active Micropost Arrays.

Micro- and nanotextured surfaces with reconfigurable textures can enable advancements in the control of wetting and heat transfer, directed assembly of complex materials, and reconfigurable optics, among many applications. However, reliable and programmable directional shape in large scale is significant for prescribed applications. Herein, we demonstrate the self-directed fabrication and actuation of large-area elastomer micropillar arrays, using magnetic fields to both program a shape-directed actuation response and rapidly and reversibly actuate the arrays. Specifically, alignment of magnetic microparticles during casting of micropost arrays with hemicylindrical shapes imparts a deterministic anisotropy that can be exploited to achieve the prescribed, large-deformation bending or twisting of the pillars. The actuation coincides with the finite element method, and we demonstrate reversible, noncontact magnetic actuation of arrays of tens of thousands of pillars over hundreds of cycles, with the bending and twisting angles of up to 72 and 61°, respectively. Moreover, we demonstrate the use of the surfaces to control anisotropic liquid spreading and show that the capillary self-assembly of actuated micropost arrays enables highly complex architectures to be fabricated. The present technique could be scaled to indefinite areas using cost-effective materials and casting techniques, and the principle of shape-directed pillar actuation can be applied to other active material systems.

Nature-Inspired Emerging Chiral Liquid Crystal Nanostructures: From Molecular Self-Assembly to DNA Mesophase and Nanocolloids.

Liquid crystals (LCs) are omnipresent in living matter, whose chirality is an elegant and distinct feature in certain plant tissues, the cuticles of crabs, beetles, arthropods, and beyond. Taking inspiration from nature, researchers have recently devoted extensive efforts toward developing chiral liquid crystalline materials with self-organized nanostructures and exploring their potential applications in diverse fields ranging from dynamic photonics to energy and safety issues. In this review, an account on the state of the art of emerging chiral liquid crystalline nanostructured materials and their technological applications is provided. First, an overview on the significance of chiral liquid crystalline architectures in various living systems is given. Then, the recent significant progress in different chiral liquid crystalline systems including thermotropic LCs (cholesteric LCs, cubic blue phases, achiral bent-core LCs, etc.) and lyotropic LCs (DNA LCs, nanocellulose LCs, and graphene oxide LCs) is showcased. The review concludes with a perspective on the future scope, opportunities, and challenges in these truly advanced functional soft materials and their promising applications.

Visible-Light-Induced Self-Organized Helical Superstructure in Orientationally Ordered Fluids.

Light-induced phenomena occurring in nature and in synthetic materials are fascinating and have been exploited for technological applications. Here visible-light-induced formation of a helical superstructure is reported, i.e., a cholesteric liquid crystal phase, in orientationally ordered fluids, i.e., nematic liquid crystals, enabled by a visible-light-driven chiral molecular switch. The cyclic-azobenzene-based chiral molecular switch exhibits reversible photoisomerization in response to visible light of different wavelengths due to the band separation of n-π* transitions of its trans- and cis-isomers. Green light (530 nm) drives the trans-to-cis photoisomerization whereas the cis-to-trans isomerization process of the chiral molecular switch can be caused by blue light (440 nm). It is observed that the helical twisting power of this chiral molecular switch increases upon irradiation with green light, which enables reversible induction of helical superstructure in nematic liquid crystals containing a very small quantity of the molecular switch. The occurrence of the light-induced helical superstructure enables the formation of diffraction gratings in cholesteric films.

Deterministic Nanoassembly of Quasi-Three-Dimensional Plasmonic Nanoarrays with Arbitrary Substrate Materials and Structures.

Guided manipulation of light through periodic nanoarrays of three-dimensional (3D) metal-dielectric patterns provides remarkable opportunities to harness light in a way that cannot be obtained with conventional optics yet its practical implementation remains hindered by a lack of effective methodology. Here we report a novel 3D nanoassembly method that enables deterministic integration of quasi-3D plasmonic nanoarrays with a foreign substrate composed of arbitrary materials and structures. This method is versatile to arrange a variety of types of metal-dielectric composite nanoarrays in lateral and vertical configurations, providing a route to generate heterogeneous material compositions, complex device layouts, and tailored functionalities. Experimental, computational, and theoretical studies reveal the essential design features of this approach and, taken together with implementation of automated equipment, provide a technical guidance for large-scale manufacturability. Pilot assembly of specifically engineered quasi-3D plasmonic nanoarrays with a model hybrid pixel detector for deterministic enhancement of the detection performances demonstrates the utility of this method.

Reversible Circularly Polarized Reflection in a Self-Organized Helical Superstructure Enabled by a Visible-Light-Driven Axially Chiral Molecular Switch.

Development of light-driven functional materials capable of displaying reversible properties is currently a vibrant frontier from both scientific and technological points of view. Here a new visible-light-driven chiral molecular switch is synthesized and characterized. To the best of our knowledge, this is the first example of a chiral molecular switch in which the visible-light-driven azobenzene motif is directly linked to an axially chiral scaffold through a C-C bond. The chiral molecular switch exhibits trans-to- cis photoisomerization upon 530 nm irradiation and cis-to- trans isomerization upon 450 nm irradiation. The switch can thus be photoisomerized in both directions using visible light of different wavelengths, a promising attribute for device applications. It was found that this relatively rigid molecular switch exhibited a high helical twisting power (HTP) in liquid crystal hosts and a large change of HTP value upon photoisomerization. We achieved dynamic reflection tuning across the visible spectrum through incorporation into a self-organized helical superstructure, i.e., a cholesteric liquid crystal. We also demonstrated patterned photodisplays reflecting red, green, and blue circularly polarized light using these cholesteric films. Phototunable color displays were fabricated by selective light irradiation where the information can be reversibly hidden by applying an electric field and restored by applying either a mechanical force or an electric field of higher voltage.

The Halogen Bond: An Emerging Supramolecular Tool in the Design of Functional Mesomorphic Materials.

Owing to their dynamic attributes, non-covalent supramolecular interactions have enabled a new paradigm in the design and fabrication of multifunctional material systems with programmable properties, performances, and reconfigurable traits. Recently, the "halogen bond" has become an enticing supramolecular synthetic tool that displays a plethora of promising and advantageous characteristics. Consequently, this versatile and dynamic non-covalent interaction has been extensively harnessed in various fields such as crystal engineering, self-assembly, materials science, polymer chemistry, biochemistry, medicinal chemistry and nanotechnology. In recent years, halogen bonding has emerged as a tunable supramolecular synthetic tool in the design of functional liquid-crystalline materials with adjustable phases and properties. In this Concept article, the use of halogen bond in the field of stimuli-responsive smart soft materials, that is, liquid crystals is discussed. The design, synthesis and characterization of molecular and macromolecular liquid crystalline materials are described and the modulation of their properties has been emphasized. The power of halogen bonding in offering a large variety of functional liquid crystalline materials from readily accessible mesomorphic and non-mesomorphic complementary building blocks is highlighted. The article concludes with a perspective on the challenges and opportunities in this emerging endeavor towards the realization of enabling and elegant dynamic functional materials.

Bright and Ultrafast Photoelectron Emission from Aligned Single-Wall Carbon Nanotubes through Multiphoton Exciton Resonance.

Ultrashort bunches of electrons, emitted from solid surfaces through excitation by ultrashort laser pulses, are an essential ingredient in advanced X-ray sources, and ultrafast electron diffraction and spectroscopy. Multiphoton photoemission using a noble metal as the photocathode material is typically used but more brightness is desired. Artificially structured metal photocathodes have been shown to enhance optical absorption via surface plasmon resonance but such an approach severely reduces the damage threshold in addition to requiring state-of-the-art facilities for photocathode fabrication. Here, we report ultrafast photoelectron emission from sidewalls of aligned single-wall carbon nanotubes. We utilized strong exciton resonances inherent in this prototypical one-dimensional material, and its excellent thermal conductivity and mechanical rigidity leading to a high damage threshold. We obtained unambiguous evidence for resonance-enhanced multiphoton photoemission processes with definite power-law behaviors. In addition, we observed strong polarization dependence and ultrashort photoelectron response time, both of which can be quantitatively explained by our model. These results firmly establish aligned single-wall carbon nanotube films as novel and promising ultrafast photocathode material.

Dynamic Control of Light Direction Enabled by Stimuli-Responsive Liquid Crystal Gratings.

The ability to control light direction with tailored precision via facile means is long-desired in science and industry. With the advances in optics, a periodic structure called diffraction grating gains prominence and renders a more flexible control over light propagation when compared to prisms. Today, diffraction gratings are common components in wavelength division multiplexing devices, monochromators, lasers, spectrometers, media storage, beam steering, and many other applications. Next-generation optical devices, however, demand nonmechanical, full and remote control, besides generating higher than 1D diffraction patterns with as few optical elements as possible. Liquid crystals (LCs) are great candidates for light control since they can form various patterns under different stimuli, including periodic structures capable of behaving as diffraction gratings. The characteristics of such gratings depend on several physical properties of the LCs such as film thickness, periodicity, and molecular orientation, all resulting from the internal constraints of the sample, and all of these are easily controllable. In this review, the authors summarize the research and development on stimuli-controllable diffraction gratings and beam steering using LCs as the active optical materials. Dynamic gratings fabricated by applying external field forces or surface treatments and made of chiral and nonchiral LCs with and without polymer networks are described. LC gratings capable of switching under external stimuli such as light, electric and magnetic fields, heat, and chemical composition are discussed. The focus is on the materials, designs, applications, and future prospects of diffraction gratings using LC materials as active layers.