Tunable Structural Color Research Articles

Deformation-Induced Photoprogrammable Pattern of Polyurethane Elastomers Based on Poisson Effect.

Elastomers with high aspect ratio surface patterns are a promising class of materials for designing soft machines in the future. Here, a facile method for fabricating surface patterns on polyurethane elastomer by subtly utilizing the Poisson effect and gradient photocrosslinking is demonstrated. By applying uniaxial tensile strains, the aspect ratio of the surface patterns can be optionally manipulated. At prestretched state, the pattern on the polyurethane elastomer can be readily constructed through compressive stress, resulting from the gradient photocrosslinking via selective photodimerization of an anthracene-functionalized polyurethane elastomer (referred to as ANPU). The macromolecular aggregation structures during stretching deformation significantly contribute to the fabrication of high aspect ratio surface patterns. The insightful finite element analysis well demonstrates that the magnitude and distribution of internal stress in the ANPU elastomer can be regulated by selectively gradient crosslinking, leading to polymer chains migrate from the exposed region to the unexposed region, thereby generating a diverse array of surface patterns. Additionally, the periodic surface patterns exhibit tunable structural color according to the different stretching states and are fully reversible over multiple cycles, opening up avenues for diverse applications such as smart displays, stretchable strain sensors, and anticounterfeiting devices.

Thermoresponsive Lamellar Hydrogels with Tunable Turbidity, Structural Color, and Anisotropic Swelling.

We report a thermoresponsive anisotropic photonic hydrogel: poly(dodecyl glyceryl itaconate)/polyacrylamide-poly(N-isopropylacrylamide) hydrogel (PDGI/PAAm-PNIPAM hydrogel). Hydrogels with uniaxially aligned lamellar bilayers possess bright structural color and swelling anisotropy, while PNIPAM-based hydrogels exhibit distinct thermoresponsive properties around a lower critical solution temperature (LCST). Hybridization of thermoresponsive PNIPAM with the lamellar hydrogel can give the anisotropic photonic hydrogel various fascinating thermoresponsive properties, such as structural color/turbid transition, thermoresponsive structural color, and anisotropic deswelling/reswelling behavior by temperature stimuli. The temperature-induced changes in turbidity, structural color, and anisotropic swelling of the gel around the LCST can be tuned by controlling the incorporated PNIPAM density. PNIPAM can be regioselectively incorporated into the specific region of the lamellar hydrogels by photomasking during UV polymerization. The PDGI/PAAm-PNIPAM hydrogel can find diverse promising applications such as smart windows and smart displays.

A confined self-assembly approach towards chiral photonic materials with circularly polarized structural colors for information storage and encryption

Chiroptical materials with tunable circular polarization performances have gained wide interest because of promising applications in optical devices and information communication. However, limited by their intrinsic chirality, such materials suffer from serious deficiencies in dynamical manipulation on circularly polarized light (CPL). Here, we demonstrate a kinetic trapping approach to capture multi-domain cholesteric mesophases for polarization-dependent structural coloration. The resultant photonic structures depicted by limited solvent evaporation display light control from selective left-handed circularly polarized light reflection to dual reflection, as a result of forming highly tilted and distorted domains with a phase-retardation effect. Notably, a positive linear correlation is established between the circular polarization behavior and structural orientation regulated by the solvent evaporation. The tunable circular polarization structural colors enable the application of the photonic materials for complex encryption in terms of polychromatic coding arrays. The confined-anisotropic-fabrication method of photonic structures paves a foundation toward advanced functional materials with promising applications in light science and technology.

Artificial Skin with Patterned Stripes for Color Camouflage and Thermoregulation.

Chameleons are famous for their quick color changing abilities, and it is commonly assumed that they do this for camouflage. However, recent reports revealed that chameleons also change color for body temperature regulation. Inspired by the structure of the panther chameleon's skin, a stripe-patterned poly(N-isopropylacrylamide) (PNIPAM) and polyacrylamide (PAM) hydrogel film with a laminated structure is fabricated in this work; thus, both camouflage and thermoregulation can be achieved through controlling Vis and NIR light effectively. For the PNIPAM stripe, the upper layer is the native PNIPAM hydrogel and the lower layer is the carbon nanotube-composited PNIPAM hydrogel. Thus, the PNIPAM stripe is capable of reaching 28 °C at a low environmental temperature (12 °C) and a low radiation intensity (20 mW cm-2), while preventing the body temperature from rising by changing to white under a strong radiation intensity (100 mW cm-2). For the PAM stripe, the upper layer combines colloidal photonic crystals and displays a tunable structural color by stretching, and the lower layer is mixed with PNIPAM microgels for thermal regulation. Through the fabrication of multifunctional patterns, the film can achieve both dynamic structural color and thermoregulation by precisely controlling solar radiation absorption, scattering, and reflection. More importantly, in the stripe-patterned system, the shrinkage of the PNIPAM stripes can effectively trigger the elongation of the PAM stripe, which endows the structural color changing process to be self-powered completely. The performances show that the stripe-patterned film may have potential applications in intelligent coatings, especially in areas with large temperature differences during the day such as high plains.

Multicolor Electrochromic Display and Patterned Device Based on Hollow-SiO2-Supported WO3 Photonic Crystals.

Electrochromic photonic crystals (PCs) have been intensively studied in the field of display, sensors, and intelligent materials due to their tunable brilliant structural colors. The mostly studied electrochromic PCs are based on the tunable lattice parameter after electrifying; namely, the electrochromic process is caused by the structural change of PCs. Besides the lattice parameter, the refractive index is another key factor to determine the structural color of PCs. Here, a kind of hollow-SiO2-supported WO3 (H-SiO2/WO3) PCs is designed, where the refractive index of the WO3 portion is changeable under charging. Benefiting from the support effect and tunable thickness of H-SiO2, large-area PC samples with good surface morphology and bright multicolor output are prepared. The reflection peaks of these composite PCs can shift by 30-90 nm, and their corresponding colors changed obviously after the voltage was applied. After being pixelated by laser-marking, the H-SiO2/WO3 PCs can dynamically display different numeric and alphabetic patterns in an electric-driven writing and erasing process. Not only does this composite PC structure broaden the color change range of WO3-based materials but also avoids the structural change in the electrochromic process. This work provides more possibilities for electrochromic PCs in the field of color-changing pattern displays.

Trackable and highly fluorescent nanocellulose-based printable bio-resins for image-guided tissue regeneration

Dynamic tracking of cell migration during tissue regeneration remains challenging owing to imaging techniques that require sophisticated devices, are often lethal to healthy tissues. Herein, we developed a 3D printable non-invasive polymeric hydrogel based on 2,2,6,6-(tetramethylpiperidin-1-yl) oxyl (TEMPO)-oxidized nanocellulose (T-CNCs) and carbon dots (CDs) for the dynamic tracking of cells. The as-prepared T-CNC@CDs were used to fabricate a liquid bio-resin containing gelatin methacryloyl (GelMA) and polyethylene glycol diacrylate (GPCD) for digital light processing (DLP) bioprinting. The shear-thinning properties of the GPCD bio-resin were further improved by the addition of T-CNC@CDs, allowing high-resolution 3D printing and bioprinting of human cells with higher cytocompatibility (viability ∼95 %). The elastic modulus of the printed GPCD hydrogel was found to be ∼13 ± 4.2 kPa, which is ideal for soft tissue engineering. The as-fabricated hydrogel scaffold exhibited tunable structural color property owing to the addition of T-CNC@CDs. Owing to the unique fluorescent property of T-CNC@CDs, the human skin cells could be tracked within the GPCD hydrogel up to 30 days post-printing. Therefore, we anticipate that GPCD bio-resin can be used for 3D bioprinting with high structural stability, dynamic tractability, and tunable mechanical stiffness for image-guided tissue regeneration.

Eco-friendly cellulosic photonic pigments with tunable structural color for anti-counterfeiting and decorative applications

Cholesteric cellulose films exhibiting an adjustable reflection wavelength across the entire visible range were obtained through the application of ultrasound treatment to a suspension of cellulose nanocrystals (CNCs) prior to casting. The influence of both low and high intensity ultrasound power on the structural color of iridescent films was systematically investigated, along with an elucidation of the mechanism behind helical pitch regulation. The findings reveal that low ultrasonic power applied to the CNC suspension has minimal impact on the structural color of the CNC film, primarily enhancing the dispersion of CNC. On the other hand, high ultrasonic power applied to the CNC suspension can effectively adjust the structural color thanks to not only improving the dispersion of CNCs suspensions, but also altering the morphology and size of the CNCs. More importantly, co-friendly cellulosic photonic pigments with tunable structural color can be easily obtained utilizing the fragility of iridescent films for applications such as anti-counterfeiting labels, nail modification and decorative coatings and so on, thereby demonstrating considerable potential for practical utilization.

Design of Reflective Tunable Structural Color Metasurface Based on Guided-Mode Resonance Filter and Sb2S3

In recent years, dynamically tunable structural color has attracted great interest. Here, we introduce the guided-mode resonance (GMR) filter and the phase-change material Sb2S3 to design a reflective optical metasurface to produce tunable structural color, in which the combination of the GMR filter, with narrow resonant wavelength, and the Sb2S3, with a much larger bandgap and higher refractive index, helps to produce high-quality tunable structural color. The simulation results indicate that through the phase transition between the amorphous and crystalline states of Sb2S3, the proposed metasurface can generate tunable structural color that can be perceived by the naked eye. Furthermore, the metasurface can sensitively sense environmental changes through changes in structural color. This work provides a new method for realizing dynamically tunable structural color, and paves the way for the application of controllable structural color in dynamic displays, optical stealth, colorimetric sensing, and other fields.

Video-Rate Switching of High-Reflectivity Hybrid Cavities Spanning All Primary Colors.

Dynamically tunable reflective structural colors are attractive for reflective displays (electronic paper). However, it is challenging to tune a thin layer of structural color across the full red-green-blue (RGB) basis set of colors at video rates and with long-term stability. In this work, this is achieved through a hybrid cavity built from metal-insulator-metal (MIM) "nanocaves" and an electrochromic polymer (PProDOTMe2 ). The reflective colors are modulated by electrochemically doping/dedoping the polymer. Compared with traditional subpixel-based systems, this hybrid structure provides high reflectivity (>40%) due to its "monopixel" nature and switches at video rates. The polymer bistability helps deliver ultralow power consumption (≈2.5mWcm-2 ) for video display applications and negligible consumption (≈3µWcm-2 ) for static images, compatible with fully photovoltaic powering. In addition, the color uniformity of the hybrid material is excellent (over cm-2 ) and the scalable fabrication enables large-area production.

Thermally Tunable Structural Color Based on Patterned Ultra-Thin Asymmetric Fabry–Perot Cavity with Phase-Change Material

Tunable structural color has gained significant attention due to its dynamic characteristics. However, conventional devices are usually regulated only in their color capabilities by structural parameters, restricting real-time dynamic applications. In this study, we propose an ultra-thin asymmetric Fabry–Perot cavity patterned with phase-change materials (MPMP). The reversible phase transition of VO2 induces changes in the MPMP’s optical performance, enabling color mode switching through temperature control and resulting in rapid color conversion and low-temperature regulation. By adjusting relevant structural parameters of the VO2 layer and nanodiscs, the color performance range can be tailored. Through numerical investigations, we demonstrate that MPMP can produce stable transformation of dynamic structural colors by harnessing the phase-change effect. Our research unveils new possibilities for applications such as anti-counterfeiting, bio/chemical sensing, and temperature sensing.

Highly Stable Microcapsules of Colloidal Photonic Ink in Nonpolar Medium for Full Color E‐Skin Device

AbstractThe colloidal dispersion in a nonpolar medium is an essential material for electrophoretic displays (EPD) with low‐power consumption. A uniform‐sized superparamagnetic iron oxide nanoparticle (SPION) is a promising candidate for EPD, which exhibits tunable structural color by Bragg diffraction. In this study, the surface of SPION is charged in a nonpolar medium by inverse micelles of Solsperse‐17k, an oil‐soluble polymeric surfactant. A photonic ink of SPION dispersion exhibits simultaneous magnetochromism and electrochromism. The photonic ink is encapsulated via a complex coacervation process, in which double layers of gelatin/gum Arabic form a stable shell for µ‐capsule. The µ‐capsules show tunable structural colors, which depends upon the size of SPION in photonic ink. The increased surfactant content in photonic ink brings about a decrease in µ‐capsule size due to a reduced surface tension. A lowered gelatin concentration during coacervation results in a smaller µ‐capsule, which exhibits an electrical color tunability. Optical characterization using a confocal microscopy enables 3D visualization of the inner structure of µ‐capsules and the formation of particle chain structure of SPION in H‐field. The encapsulated photonic ink exhibits magnetochromism for 1 year, illuminating the long‐term stability of µ‐capsules developed in this study.

Photo‐Responsive Azobenzene‐Containing Inverse Opal Films for Information Security

AbstractStimuli‐responsive photonic crystals (PCs) have attracted increasing attentions owing to the unique optical feature in regulating the propagation of light and tunable structural colors in response to external stimuli, emerging application potential on diverse fields. However, the development of stimuli‐responsive PCs with wide visible light range, broad shift of bandgaps, and adjustable responsive rates for counterfeiting remains challenging. Herein, a simple strategy for the preparation of photo‐responsive azobenzene‐containing inverse opal (AzoIO) films is reported. First, azobenzene‐containing composites are generated by filling functional monomers into voids of silica colloids crystals. Followed by the thermal polymerization and subsequent etching, a series of AzoIO films are successfully fabricated with adjustable structural colors in wide visible wavelength. Upon irradiation with linearly polarized visible light (LPVL), a slowly broad blueshift of bandgaps (≈138 nm, 3200 s) is observed due to the anisotropic shrinkage of the periodic PC structures. However, UV light irradiation contributed to a fast broad blueshift of bandgaps (≈131 nm, 10 s), owing to the photoisomerization merit of azobenzene moiety. The proof‐of‐concept study on the applications in light‐modulated multicolored writable paper, encryption films, and fast writing/erasing demonstrated the potential for information security. This work paves an avenue for developing promising optical anti‐counterfeiting materials.

Bio-Inspired Highly Brilliant Structural Colors and Derived Photonic Superstructures for Information Encryption and Fluorescence Enhancement.

Inspired by the brilliant and tunable structural colors based on the large refractive index contrast (Δn) and non-close-packing structures of chameleon skins, ZnS-silica photonic crystals (PCs) with highly saturated and adjustable colors are fabricated. Due to the large Δn and non-close-packing structure, ZnS-silica PCs show 1) intense reflectance (maximal: 90%), wide photonic bandgaps, and large peak areas, 2.6-7.6, 1.6, and 4.0 times higher than those of silica PCs, respectively; 2) tunable colors by simply adjusting the volume fraction of particles with the same size, more convenient than the conventional way of altering particle sizes; and 3) a relatively low threshold of PC's thickness (57 µm) possessing maximal reflectance compared to that (>200 µm) of the silica PCs. Benefiting from the core-shell structure of the particles, various derived photonic superstructures are fabricated by co-assembling ZnS-silica and silica particles into PCs or by selectively etching silica or ZnS of ZnS-silica/silica and ZnS-silica PCs. A new information encryption technique is developed based on the unique reversible "disorder-order" switch of water-responsive photonic superstructures. Additionally, ZnS-silica PCs are ideal candidates for enhancing fluorescence (approximately tenfold), approximately six times higher than that of silica PC.

Dynamically Tunable Structural Colors Enabled by Pixelated Programming of Soft Materials on Thickness

AbstractStructural colors are widespread in nature and have become an important component of the lives. Considerable efforts have been made toward reversible color tuning, which underpins intriguing applications, including color displays, anti‐counterfeiting, and information encryption. However, the limited size, complicated fabrication processes, and low modulation speeds of structural colors are the main obstacles to their further development. Herein, a facile method to realize dynamically tunable structural colors is presented, which are enabled by the pixelated programming of soft materials on thickness. Pixelated photoresist microarrays with different heights are obtained using a digitalized lithography technique, enabling delicate control over the thickness of the liquid crystal (LC) layers. Stimuli‐responsive LCs endow structural colors with dynamic and reversible tunability and exhibit remarkable switching speeds with external stimuli. The proposed strategy sheds new light on dynamically tunable structural colors and promotes the development of optical anti‐counterfeiting, thermal sensors, and advanced information encryption.

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.

Inside Cover Picture

The cover picture shows three‐dimensional ordered porous photonic microspheres prepared by BBCP/homopolymer binary blend. The interfacial curvature of the internal droplets increases with the increase of hPS content realized through swelling of the PS domain of the BBCP. Consequently, pore diameter of the porous structure can be precisely tailored leading to the tunable structural colors. More details are given in the article by Song et al. on page 1566—1574.image

Tunable structural transmissive color in fano-resonant optical coatings employing phase-change materials

Reversible, nonvolatile, and pronounced refractive index modulation is an unprecedented combination of properties enabled by chalcogenide phase-change materials (PCMs). This combination of properties makes PCMs a fast-growing platform for active, low-energy nanophotonics, including tunability to otherwise passive thin-film optical coatings. Here, we integrate the PCM Sb2Se3 into a novel four-layer thin-film optical coating that exploits photonic Fano resonances to achieve tunable structural colors in both reflection and transmission. We show, contrary to traditional coatings, that Fano-resonant optical coatings (FROCs) allow for achieving transmissive and reflective structures with narrowband peaks at the same resonant wavelength. Moreover, we demonstrate asymmetric optical response in reflection, where Fano resonance and narrow-band filtering are observed depending upon the light incidence side. Finally, we use a multi-objective inverse design via machine learning (ML) to provide a wide range of solution sets with optimized structures while providing information on the performance limitations of the PCM-based FROCs. Adding tunability to the newly introduced Fano-resonant optical coatings opens various applications in spectral and beam splitting, and simultaneous reflective and transmissive displays, diffractive objects, and holograms.

Tough and Transparent Photonic Hydrogel Nanocomposites for Display, Sensing, and Actuation Applications

Thermosensitive hydrogels with periodic dielectric structures displaying tunable structural color by temperature stimuli have attracted much research interest recently. However, reported thermosensitive photonic hydrogels either using the poly(N-isopropylacrylamide) (PNIPAM) bulk hydrogel as the responsive matrix or using PNIPAM microgels as the photonic building blocks have poor mechanical strength. Moreover, the expensive and time-consuming preparation process also limits their further application. In this work, a different strategy for preparing PNIPAM-based photonic hydrogel nanocomposite films with strong mechanical strength is proposed by incorporating a PNIPAM microgel film with the polyacrylamide (PAM) hydrogel. The preparation process is simple but efficient, and the obtained nanocomposite films have tunable mechanical strength by changing the crosslinking degree of the PAM hydrogels. More interestingly, the structural color of the nanocomposite films can be retained up to 80 °C (at least), much higher than those of previously reported PNIPAM-based photonic materials. In addition to being thermochromic, the film is sensitive to humidity, and the structural color-changing process is similar to the molting process of cicadas. Furthermore, the nanocomposite films have synchronous shape deformations and color changes and can be used as color-tunable soft actuators. The microgel film-capped photonic hydrogels provide a new strategy for the preparation of thermoresponsive photonic hydrogels and structural color-tunable actuators.

Polarization-Sensitive Structural Colors Based on Anisotropic Silicon Metasurfaces

Structural colors based on all-dielectric metasurfaces hold great promise for a wide range of applications, including high-density optical storage, ultra-high-resolution 3D displays, imaging security certification, and so on. However, achieving dynamic tunable structural color with a compact and simple Si platform remains a great challenge. Here, we propose a dynamic tunable structural coloration with polarization-sensitive metasurfaces consisting of arrays of Si elliptical nanopillars, enabling full-colored images to be displayed and switched through the control of the polarization of incident light. A distinct feature of our design is that the color phase is independent of the viewing angle, which is fundamental for real applications. Moreover, we demonstrated that dual and multiple colors can be obtained by varying the angle of either the polarizer or the analyzer. Our scheme provides a simple yet general approach for potential applications in the fields of virtual reality, ultra-high-resolution 3D displays, and high-density information storage.

Structural Colors on Al Surface via Capped Cu-Si3N4 Bilayer Structure

Tunable structural colors have a multitude of applications in the beautification of mobile devices, in the decoration of artwork, and in the creation of color filters. In this paper, we describe a Metal-Insulator-Metal (MIM) design that can be used to systematically tune structural colors by altering the thickness of the top metal and intermediate insulator. Cu and Si3N4 were selected as the top metal and intermediate insulator layers, respectively, and various reflection colors were printed on Al. To protect the Cu surface from scratchiness and oxidation, a number of capping layers, including SiO2, LPSQ, PMMA, and the commercially available clear coat ProtectaClear, were applied. In addition to their ability to protect Cu from a humid environment without deteriorating color quality, ProtectaClear and LPSQ coatings have minimal angle dependency. Furthermore, a bilayer of PMMA/SiO2 can protect the Cu surface from the effects of humidity. In addition, the PMMA/SiO2 and ProtectaClear/SiO2 bilayers can also protect against corrosion on the Cu surface. The colors can be tuned by controlling the thickness of either the metal layer or intermediate insulator layer, and vivid structural colors including brown, dark orange, blue, violet, magenta, cyan, green-yellow, and yellow colors can be printed. The measured dielectric functions of Cu thin films do not provide any evidence of the plasmonic effect, and therefore, it is expected that the obtained colors are attributed to thin-film interference.