A Scalable Microstructure Photonic Coating Fabricated by Roll-to-Roll "Defects" for Daytime Subambient Passive Radiative Cooling.

The deep space's coldness (∼4 K) provides a ubiquitous and inexhaustible thermodynamic resource to suppress the cooling energy consumption. However, it is nontrivial to achieve subambient radiative cooling during daytime under strong direct sunlight, which requires rational and delicate photonic design for simultaneous high solar reflectivity (>94%) and thermal emissivity. A great challenge arises when trying to meet such strict photonic microstructure requirements while maintaining manufacturing scalability. Herein, we demonstrate a rapid, low-cost, template-free roll-to-roll method to fabricate spike microstructured photonic nanocomposite coatings with Al2O3 and TiO2 nanoparticles embedded that possess 96.0% of solar reflectivity and 97.0% of thermal emissivity. When facing direct sunlight in the spring of Chicago (average 699 W/m2 solar intensity), the coatings show a radiative cooling power of 39.1 W/m2. Combined with the coatings' superhydrophobic and contamination resistance merits, the potential 14.4% cooling energy-saving capability is numerically demonstrated across the United States.

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.

S/Mo ratio and petal size controlled MoS2 nanoflowers with low temperature metal organic chemical vapor deposition and their application in solar cells.

Vertically aligned two-dimensional (2D) molybdenum disulfide nanoflowers (MoS2 NFs) have drawn considerable attention as a novel functional material with potential for next-generation applications owing to their inherently distinctive structure and extraordinary properties. We report a simple metal organic chemical vapor deposition (MOCVD) method that can grow high crystal quality, large-scale and highly homogeneous MoS2 NFs through precisely controlling the partial pressure ratio of H2S reaction gas, P SR, to Mo(CO)6 precursor, P MoP, at a substrate temperature of 250 °C. We investigate microscopically and spectroscopically that the S/Mo ratio, optical properties and orientation of the grown MoS2 NFs can be controlled by adjusting the partial pressure ratio, P SR/P MoP. It is also shown that the low temperature MOCVD (LT-MOCVD) growth method can regulate the petal size of MoS2 NFs through the growth time, thereby controlling photoluminescence intensity. More importantly, the MoS2 NFs/GaAs heterojunction flexible solar cell exhibiting a power conversion efficiency of ∼1.3% under air mass 1.5 G illumination demonstrates the utility of the LT-MOCVD method that enables the direct growth of MoS2 NFs on the flexible devices. Our work can pave the way for practical, easy-to-fabricate 2D materials integrated flexible devices in optical and photonic applications.

Enhancement of Magneto-Mechanical Actuation of Micropillar Arrays by Anisotropic Stress Distribution.

Magnetically active shape-reconfigurable microarrays undergo programmed actuation according to the arrangement of magnetic dipoles within the structures, achieving complex twisting and bending deformations. Cylindrical micropillars have been widely used to date, whose circular cross-sections lead to identical actuation regardless of the actuating direction. In this study, micropillars with triangular or rectangular cross-sections are designed and fabricated to introduce preferential actuation directions and explore the limits of their actuation. Using such structures, controlled liquid wetting is demonstrated on micropillar surfaces. Liquid droplets pinned on magnetic micropillar arrays undergo directional spreading when the pillars are actuated as depinning of the droplets is enabled only in certain directions. The enhanced deformation due to direction dependent magneto-mechanical actuation suggests that micropillar arrays can be fundamentally tailored to possess application specific responses and opens up opportunities to exploit more complex designs such as micropillars with polygonal cross sections. Such tunable wetting of liquids on microarray surfaces has potential to improve printing technologies via contactless reconfiguration of stamp geometry by magnetic field manipulation.

Polarization-Sensitive and Wide Incidence Angle-Insensitive Fabry-Perot Optical Cavity Bounded by Two Metal Grating Layers.

Infrared (IR) polarimetric imaging has attracted attention as a promising technology in many fields. Generally, superpixels consisting of linear polarizer elements at different angles plus IR imaging array are used to obtain the polarized target signature by using the detected polarization-sensitive intensities. However, the spatial arrangement of superpixels across the imaging array may lead to an incorrect polarimetric signature of a target, due to the range of angles from which the incident radiation can be collected by the detector. In this article, we demonstrate the effect of the incident angle on the polarization performance of an alternative structure where a dielectric layer is inserted between the nanoimprinted subwavelength grating layers. The well-designed spacer creates the Fabry-Perot cavity resonance, and thereby, the intensity of transverse-magnetic I-polarized light transmitted through two metal grating layers is increased as compared with a single-layer metal grating, whereas transverse-electric (TE)-transmitted light intensity is decreased. TM-transmittance and polarization extinction ratio (PER) of normally incident light of wavelength 4.5 µm are obtained with 0.49 and 132, respectively, as the performance of the stacked subwavelength gratings. The relative change of the PERs for nanoimprint-lithographically fabricated double-layer grating samples that are less than 6% at an angle of incidence up to 25°, as compared to the normal incidence. Our work can pave the way for practical and efficient polarization-sensitive elements, which are useful for many IR polarimetric imaging applications.

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.

Enhanced transmission due to antireflection coating layer at surface plasmon resonance wavelengths.

We present experiments and analysis on enhanced transmission due to dielectric layer deposited on a metal film perforated with two-dimensional periodic array of subwavelength holes. The Si3N4 overlayer is applied on the perforated gold film (PGF) fabricated on GaAs substrate in order to boost the transmission of light at the surface plasmon polariton (SPP) resonance wavelengths in the mid- and long-wave IR regions, which is used as the antireflection (AR) coating layer between two dissimilar media (air and PGF/GaAs). It is experimentally shown that the transmission through the perforated gold film with 1.8 µm (2.0 µm) pitch at the first-order (second-order) SPP resonance wavelengths can be increased up to 83% (110%) by using a 750 nm (550 nm) thick Si3N4 layer. The SPP resonance leads to a dispersive resonant effective permeability (µeff ≠ 1) and thereby the refractive index matching condition for the conventional AR coating on the surface of a dielectric material cannot be applied to the resonant PGF structure. We develop and demonstrate the concept of AR condition based on the effective parameters of PGF. In addition, the maximum transmission (zero reflection) condition is analyzed numerically by using a three-layer model and a transfer matrix method is employed to determine the total reflection and transmission. The numerically calculated total reflection agrees very well with the reflection obtained by 3D full electromagnetic simulations of the entire structure. Destructive interference conditions for amplitude and phase to get zero reflection are well satisfied.

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.

Heteronanostructured Field-Effect Transistors for Enhancing Entropy and Parameter Space in Electrical Unclonable Primitives.

Hardware security is not a new problem but is ever-growing in consumer and medical domains owing to hyperconnectivity. A physical unclonable function (PUF) offers a promising hardware security solution for cryptographic key generation, identification, and authentication. However, electrical PUFs using nanomaterials or two-dimensional (2D) transition metal dichalcogenides (TMDCs) often have limited entropy and parameter space sources, both of which increase the vulnerability to attacks and act as bottlenecks for practical applications. We report an electrical PUF with enhanced entropy as well as parameter space by incorporating 2D TMDC heteronanostructures into field-effect transistors (FETs). Lateral heteronanostructures of 2D molybdenum disulfide and tungsten disulfide serve as a potent entropy source. The variable feature of FETs is further leveraged to enhance the parameter space that provides multiple challenge-response pairs, which are essential for PUFs. This combination results in stably repeatable yet highly variable FET characteristics as alternative electrical PUFs. Comprehensive PUF performance analyses validate the bit uniformity, reproducibility, uniqueness, randomness, false rates, and encoding capacity. The 2D material heteronanostructure-driven electrical PUFs with strong FET-to-FET variability can potentially be augmented as an immediately deployable and scalable security solution for various hardware devices.

Analysis of subwavelength metal hole array structure for the enhancement of back-illuminated quantum dot infrared photodetectors.

This paper is focused on analyzing the impact of a two-dimensional metal hole array structure integrated to the back-illuminated quantum dots-in-a-well (DWELL) infrared photodetectors. The metal hole array consisting of subwavelength-circular holes penetrating gold layer (2D-Au-CHA) provides the enhanced responsivity of DWELL infrared photodetector at certain wavelengths. The performance of 2D-Au-CHA is investigated by calculating the absorption of active layer in the DWELL structure using a finite integration technique. Simulation results show that the performance of the DWELL focal plane array (FPA) is improved by enhancing the coupling to active layer via local field engineering resulting from a surface plasmon polariton mode and a guided Fabry-Perot mode. Simulation method accomplished in this paper provides a generalized approach to optimize the design of any type of couplers integrated to infrared photodetectors. Experimental results demonstrate the enhanced signal-to-noise ratio by the 2D-Au-CHA integrated FPA as compared to the DWELL FPA. A comparison between the experiment and the simulation shows a good agreement.

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.

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.

On-Demand Dynamic Chirality Selection in Flower Corolla-like Micropillar Arrays.

Chiral morphology has been intensively studied in various fields including biology, organic chemistry, pharmaceuticals, and optics. On-demand and dynamic chiral inversion not only cannot be realized in most intrinsically chiral materials but also has mostly been limited to chemical or light-induced methods. Herein, we report reversible real-time magneto-mechanical chiral inversion of a three-dimensional (3D) micropillar array between achiral, clockwise, and counterclockwise chiral arrangements. Inspired by the flower corolla, achiral arrays of five and six radially arranged semicylindrical micropillars were employed as model systems to investigate the dynamic symmetry properties of arrays consisting of odd and even numbers of micropillars, respectively. Each micropillar underwent twisting actuation with a different twisting angle depending on the angle with the magnetic field direction and magnetic flux density, thereby collectively changing the chirality from the achiral to chiral state. Importantly, the morphological handedness of the micropillars was inverted within a few seconds by manipulating the direction of the magnetic field. A chiral morphology consisting of magnetically twisted micropillars was shape-fixed by the introduction of a polymeric binder. This binder could be simply washed off to return the shape-fixed twisted micropillars to their initial straight state. Magnetically programmable and reproducible 3D flower corolla-like micropillar arrays are expected to expand the potential of shape-reconfigurable devices that require real-time chiral manipulation in ambient environments.

Ultrafast nonlinear optical spectroscopy of a dual-band negative index metamaterial all-optical switching device.

We study the nonlinear optical response of a fishnet structure-metamaterial all-optical switching device that exhibits two near-infrared negative-index resonances. We study and compare the nonlinear optical response at both resonances and identify transient spectral features associated with the negative index resonance. We see a significantly stronger response at the longer wavelength resonance, but identical temporal dynamics at both resonances, providing insight into separately engineering the switching time and switching ratio of such a fishnet structure metamaterial all-optical switch. We also numerically reproduce the nonlinear behavior of our device using the Drude conductivity model and a finite integration technique over wide spectral and pump fluence ranges. Thereby, we show that beyond the linear properties of the device, the magnitude of the pump-probe response is completely described by only two material parameters. These results provide insight into engineering various aspects of the nonlinear response of fishnet structure metamaterials.

Tuning Hierarchical Order and Plasmonic Coupling of Large-Area, Polymer-Grafted Gold Nanorod Assemblies via Flow-Coating.

Solution-based printing of anisotropic nanostructures is foundational to many emerging technologies, such as energy storage devices, photonic elements, and sensors. Methods to rapidly (>mm/s) manufacture large area assemblies (≫cm2) with simultaneous control of thickness (<10 nm), nanoparticle spacing (<5 nm), surface roughness (<5 nm), and global and local orientational order are still lacking. Herein, we demonstrate such capability using flow-coating to fabricate robust, self-supporting mono- and bilayer films of polystyrene-grafted gold nanorods (PS-AuNRs) onto solid substrates. The relationship among solvent evaporation, deposition speed, substrate surface energy, concentration, and film thickness for solutions of such hairy hybrid nanoparticles spans the Landau-Levich and evaporative film formation regimes. In the Landau-Levich regime, solvent evaporation rapidly concentrates the PS-AuNRs, leading to the formation of thin films with distinct, randomized side-by-side domains. Alternatively, processing at slower velocities in the evaporative regime results in the global alignment of PS-AuNRs. Processing speed and substrate surface energy afford tuning of the film's optical extinction of a given PS-AuNR via fine control of inter-rod distance and subsequent plasmonic coupling between neighboring nanorods. Because the concept of the polymer-grafted nanorod can be expanded to a variety of different polymer canopies, shapes, and core materials, the processing-structure relationships established in this work will have important implications on the future development of anisotropic nanostructure-based applications.

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.

Subpicosecond optical switching with a negative index metamaterial.

We demonstrate a nanoscale, subpicosecond (ps) metamaterial device capable of terabit/second all-optical communication in the near-IR. The 600 fs response, 2 orders of magnitude faster than previously reported, is achieved by accessing a previously unused regime of high-injection level, subpicosecond carrier dynamics in the alpha-Si dielectric layer of the metamaterial. Further, we utilize a previously unrecognized, higher-order, shorter-wavelength negative-index resonance in the fishnet structure, thereby extending device functionality (via structural tuning of device dimensions) over 1.0-2.0 microm. The pump energy required to modulate a single bit is only 3 nJ over our current 700 microm(2) area device and can be easily scaled into the picoJoule regime with smaller cross sectional areas.

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.

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.

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.