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.

Hydrogels for active photonics.

Conventional photonic devices exhibit static optical properties that are design-dependent, including the material's refractive index and geometrical parameters. However, they still possess attractive optical responses for applications and are already exploited in devices across various fields. Hydrogel photonics has emerged as a promising solution in the field of active photonics by providing primarily deformable geometric parameters in response to external stimuli. Over the past few years, various studies have been undertaken to attain stimuli-responsive photonic devices with tunable optical properties. Herein, we focus on the recent advancements in hydrogel-based photonics and micro/nanofabrication techniques for hydrogels. In particular, fabrication techniques for hydrogel photonic devices are categorized into film growth, photolithography (PL), electron-beam lithography (EBL), and nanoimprint lithography (NIL). Furthermore, we provide insights into future directions and prospects for deformable hydrogel photonics, along with their potential practical applications.

Radiative Cooling for Energy Sustainability: From Fundamentals to Fabrication Methods Toward Commercialization.

Radiative cooling, a technology that lowers the temperature of terrestrial objects by dissipating heat into outer space, presents a promising ecologically-benign solution for sustainable cooling. Recent years witness substantial progress in radiative cooling technologies, bringing them closer to commercialization. This comprehensive review provides a structured overview of radiative cooling technologies, encompassing essential principles, fabrication techniques, and practical applications, with the goal of guiding researchers toward successful commercialization. The review begins by introducing the fundamentals of radiative cooling and the associated design strategies to achieve it. Then, various fabrication methods utilized for the realization of radiative cooling devices are thoroughly discussed. This discussion includes detailed assessments of scalability, fabrication costs, and performance considerations, encompassing both structural designs and fabrication techniques. Building upon these insights, potential fabrication approaches suitable for practical applications and commercialization are proposed. Further, the recent efforts made toward the practical applications of radiative cooling technology, including its visual appearance, switching capability, and compatibility are examined. By encompassing a broad range of topics, from fundamental principles to fabrication and applications, this review aims to bridge the gap between theoretical research and real-world implementation, fostering the advancement and widespread adoption of radiative cooling technology.

Freestanding, Freeform Metamolecule Fibers Tailoring Artificial Optical Magnetism.

Metamolecule clusters support various unique types of artificial electromagnetism at optical frequencies. However, the technological challenges regarding the freeform fabrication of freestanding metamolecule clusters with programmed geometries and multiple compositions remain unresolved. Here, the freeform, freestanding raspberry-like metamolecule (RMM) fibers based on the directional guidance of a femtoliter meniscus are presented, resulting in the evaporative co-assembly of silica nanoparticles and gold nanoparticles with the aid of 3D nanoprinting. This method offers a facile and universal pathway to shape RMM fibers in 3D, enabling versatile manipulation of near- and far-field characteristics. In particular, the authors demonstrate the ability to decrease the scattering of the millimeter-scale RMM fiber in visible spectrum. In addition, the influence of electric and magnetic dipole modes on the directional scattering of RMM fibers is investigated. These experiments show that the magnetic response of an individual RMM can be controlled by adjusting the filling factor of gold nanoparticles. The authors anticipate that this method will allow for unrestricted design and realization of nanophotonic structures, surpassing the limitations of conventional fabrication processes.

Humidity-Responsive RGB-Pixels via Swelling of 3D Nanoimprinted Polyvinyl Alcohol.

Humidity-responsive structural coloration is actively investigated to realize real-time humidity sensors for applications in smart farming, food storage, and healthcare management. Here, humidity-tunable nano pixels are investigated with a 700 nm resolution that demonstrates full standard RGB (sRGB) gamut coverage with a millisecond-response time. The color pixels are designed as Fabry-Pérot (F-P) etalons which consist of an aluminum mirror substrate, humidity-responsive polyvinyl alcohol (PVA) spacer, and a top layer of disordered silver nanoparticles (NPs). The measured volume change of the PVA reaches up to 62.5% when the relative humidity (RH) is manipulated from 20 to 90%. The disordered silver NP layer permits the penetration of water molecules into the PVA layer, enhancing the speed of absorption and swelling down to the millisecond level. Based on the real-time response of the hydrogel-based F-P etalons with a high-throughput 3D nanoimprint technique, a high-resolution multicolored color print that can have potential applications in display technologies and optical encryption, is demonstrated.

Tunable metasurfaces via the humidity responsive swelling of single-step imprinted polyvinyl alcohol nanostructures.

The application of hydrogels in nanophotonics has been restricted due to their low fabrication feasibility and refractive index. Nevertheless, their elasticity and strength are attractive properties for use in flexible, wearable-devices, and their swelling characteristics in response to the relative humidity highlight their potential for use in tunable nanophotonics. We investigate the use of nanostructured polyvinyl alcohol (PVA) using a one-step nanoimprinting technique for tunable and erasable optical security metasurfaces with multiplexed structural coloration and metaholography. The resolution of the PVA nanoimprinting reaches sub-100 nm, with aspect ratios approaching 10. In response to changes in the relative humidity, the PVA nanostructures swell by up to ~35.5%, providing precise wavefront manipulation of visible light. Here, we demonstrate various highly-secure multiplexed optical encryption metasurfaces to display, hide, or destroy encrypted information based on the relative humidity both irreversibly and reversibly.

Disordered-nanoparticle-based etalon for ultrafast humidity-responsive colorimetric sensors and anti-counterfeiting displays.

The development of real-time and sensitive humidity sensors is in great demand from smart home automation and modern public health. We hereby proposed an ultrafast and full-color colorimetric humidity sensor that consists of chitosan hydrogel sandwiched by a disordered metal nanoparticle layer and reflecting substrate. This hydrogel-based resonator changes its resonant frequency to external humidity conditions because the chitosan hydrogels are swollen under wet state and contracted under dry state. The response time of the sensor is ~104 faster than that of the conventional Fabry-Pérot design. The origins of fast gas permeation are membrane pores created by gaps between the metal nanoparticles. Such instantaneous and tunable response of a new hydrogel resonator is then exploited for colorimetric sensors, anti-counterfeiting applications, and high-resolution displays.

Multilevel Absorbers via the Integration of Undoped and Tungsten-Doped Multilayered Vanadium Dioxide Thin Films.

Reconfigurable light absorbers have attracted much attention by providing additional optical responses and expanding the number of degrees of freedom in security applications. Fabry-Pèrot absorbers based on phase change materials with tunable properties can be implemented over large scales without the need for additional steps such as lithography, while exhibiting reconfigurable optical responses. However, a fundamental limitation of widely used phase change materials such as vanadium dioxide and germanium-antimony-tellurium-based chalcogenide glasses is that they have only two distinct phases; therefore, only two different states of optical properties are available. Here, we experimentally demonstrate active multilevel absorbers that are tuned by controlling the external temperature. This is produced by creating large-scale lithography-free multilayer structures with both undoped and tungsten-doped solution-processed monoclinic-phase vanadium dioxide thin films. The doping of vanadium dioxide with tungsten allows for the modulation of the phase-transition temperature, which results in an extra degree of freedom and therefore an additional step for the tunable properties. The proposed multilevel absorber is designed and characterized both numerically and experimentally. Such large-scale multilevel tunable absorbers realized with nanoparticle-based solution fabrication techniques are expected to open the way for advanced thermo-optical cryptographic devices based on tunable reflective coloration and near-infrared absorption.

Angular selection of transmitted light and enhanced spontaneous emission in grating-coupled hyperbolic metamaterials.

We propose dielectric grating-coupled hyperbolic metamaterials as a functional device that shows angular selection of transmitted light and enhanced radiative emission rate. We numerically demonstrate that the surface plasmon polaritons in the hyperbolic metamaterials can be effectively outcoupled to the surrounding space by using gratings and facilitate control of the light transmission in the visible frequency. We confirm that the high density of states and the effect of outcoupled plasmonic modes of the proposed structure lead to the increase of Purcell factor and radiative emission. This work will provide multifunctionalities in sensing and imaging systems that use hyperbolic metamaterials.

Nanoimprint lithography for high-throughput fabrication of metasurfaces.

Metasurfaces are composed of periodic sub-wavelength nanostructures and exhibit optical properties that are not found in nature. They have been widely investigated for optical applications such as holograms, wavefront shaping, and structural color printing, however, electron-beam lithography is not suitable to produce large-area metasurfaces because of the high fabrication cost and low productivity. Although alternative optical technologies, such as holographic lithography and plasmonic lithography, can overcome these drawbacks, such methods are still constrained by the optical diffraction limit. To break through this fundamental problem, mechanical nanopatterning processes have been actively studied in many fields, with nanoimprint lithography (NIL) coming to the forefront. Since NIL replicates the nanopattern of the mold regardless of the diffraction limit, NIL can achieve sufficiently high productivity and patterning resolution, giving rise to an explosive development in the fabrication of metasurfaces. In this review, we focus on various NIL technologies for the manufacturing of metasurfaces. First, we briefly describe conventional NIL and then present various NIL methods for the scalable fabrication of metasurfaces. We also discuss recent applications of NIL in the realization of metasurfaces. Finally, we conclude with an outlook on each method and suggest perspectives for future research on the high-throughput fabrication of active metasurfaces.