The physical and cellular mechanism of structural color change in zebrafish.

Many animals exhibit remarkable colors that are produced by the constructive interference of light reflected from arrays of intracellular guanine crystals. These animals can fine-tune their crystal-based structural colors to communicate with each other, regulate body temperature, and create camouflage. While it is known that these changes in color are caused by changes in the angle of the crystal arrays relative to incident light, the cellular machinery that drives color change is not understood. Here, using a combination of 3D focused ion beam scanning electron microscopy (FIB-SEM), micro-focused X-ray diffraction, superresolution fluorescence light microscopy, and pharmacological perturbations, we characterized the dynamics and 3D cellular reorganization of crystal arrays within zebrafish iridophores during norepinephrine (NE)-induced color change. We found that color change results from a coordinated 20° tilting of the intracellular crystals, which alters both crystal packing and the angle at which impinging light hits the crystals. Importantly, addition of the dynein inhibitor dynapyrazole-a completely blocked this NE-induced red shift by hindering crystal dynamics upon NE addition. FIB-SEM and microtubule organizing center (MTOC) mapping showed that microtubules arise from two MTOCs located near the poles of the iridophore and run parallel to, and in between, individual crystals. This suggests that dynein drives crystal angle change in response to NE by binding to the limiting membrane surrounding individual crystals and walking toward microtubule minus ends. Finally, we found that intracellular cAMP regulates the color change process. Together, our results provide mechanistic insight into the cellular machinery that drives structural color change.

Surface Coloring and Plasmonic Information Encryption at 50000 dpi Enabled by Direct Femtosecond Laser Printing.

Femtosecond (fs) laser pulses drive matter into a highly nonequilibrium state, allowing precise sculpturing of irradiated surface sites with sophisticated nanomorphologies. Here, we used fs-laser patterning to create diverse plasmonic morphologies on the top Au layer of the metal-insulator-metal sandwich. Mutual action of laser-driven thermomechanical effects and ultrafast solid-to-liquid transition allows control of the morphology resulting in pronounced surface reflectivity modulation, i.e., in a structural color effect. This enables template-free high-resolution color printing at a superior lateral resolution up to 50000 dots per inch and facile tunability of the color tone and saturation. Moreover, precise control over the orientation of the printed nanostructures within subwavelength lattices allows modulation of their local plasmonic response encrypting the optical information within the colorful images. The hidden information can be unveiled using a facile cross-polarized optical visualization scheme, rendering the proposed method with extra modalities combining high resolution information encryption, coloring, and security labeling.

Mie Magnetic Structural Colors from Short Chains of TiO2 Nanospheres.

We demonstrate distinctive structural colors within a small footprint by using a short chain of nanospheres. Rather than using high-index materials like Si (n ∼ 4), which ensure strong modal confinement, TiO2 is employed. TiO2 has an intermediate index (n ∼ 2), promoting stronger modal coupling between the magnetic dipoles of each particle. This approach enables selective engineering of the magnetic response and yields larger spectral changes compared to that of Si. Despite the lower refractive index, the absence of absorption in TiO2 also produces higher scattering intensities than Si. We develop a quasistatic analytical model that describes the dipolar modal coupling in a trimer and use it to reveal distinct magnetic field strengths in the outer or central particle depending on the polarization of incident light. These results suggest pathways to manipulate the magnetic field in chains of particles and create vibrant structural colors with simple configurations.

Arrays of Bowl-Shaped Janus Particle Film with Structured Colors.

Structural colors generated via total internal reflection (TIR) using nanostructure-free micro-concave shapes have garnered increasing attention. However, the application of large micro-concave structures for structural coloration remains limited. Herein, a flexibly tunable structural color film fabricated by casting polydimethylsiloxane (PDMS) on an array of large poly(glycidyl methacrylate) (PGMA) bowl-shaped particles is reported. The resultant film exhibits tunable red to green structural colors with changing observation angles. Moreover, the color can be further tailored by altering the shape of the film itself. The incorporation of the PDMS layer not only facilitates a shift in the locus of TIR from the bottom surface to the top concave surface of the particles, thereby enabling the generation of structural color, but also confers enhanced flexibility to the film. Further decoration with silver nanoparticles imparts antimicrobial properties, yielding a novel antimicrobial coating material with structural colors. The simple and cost-effective strategy for the production of structural color films provides potential applications in antimicrobial coatings, enabling accessible and customizable structural coloration using big-size micro-concave particles.

Bionic Structural Coloration of Textiles Using the Synthetically Prepared Liquid Photonic Crystals.

The structural coloration of textiles with bionic photonic crystals (PCs) is expected to become a critical approach to the ecological coloration of textiles. Rapid and large-area preparation of PC structurally colored textiles can be achieved via self-assembly of high mass fractions of liquid photonic crystals (LPCs). However, the rapid and large-scale manufacturing of LPCs remains a challenge. In this work, the pH regulator is added in the process of emulsion polymerization to solve the problem of phase transformation caused by the thermal decomposition of the initiator to produce H+ , directly achieving 40 wt.% PS nanospheres in the dispersion. Then oligomers and small-molecule salts are removed from the system via dialysis, and the pre-crystallized LPC system is efficiently prepared. Adjusting the particle size and the mass fraction of nanospheres is shown to be an efficient way to control the optical properties of LPCs. The rapid and large-area preparation of PC structural color fabric and the patterned PC structural color fabric with an iridescent effect is implemented by using LPCs as the assembly intermediate. By constructing the encapsulation layer on the surface of the PC structural color fabric, the consistency of high structural stability and high color saturation of the PC is realized.

Anti-UV Passive Radiative Cooling Chiral Nematic Liquid Crystal Films for Thermal Management.

Passive radiative cooling (PRC) can spontaneously dissipate heat to outer space through atmospheric transparent windows, providing a promising path to meet sustainable development goals. However, achieving simultaneously high transparency, color-customizable, and thermal management of PRC anti ultraviolet (anti-UV) films remains a challenge. Herein, a simple strategy is proposed to utilize liquid crystalline polymer, with high mid-infrared emissive, forming customizable structural color film by molecular self-assembly and polymerization-induced pitch gradient, which guarantees the balance of transparency in visible spectrum and sunlight reflection, rendering anti-UV colored window for thermal management. By performing tests, temperature fall of 5.4 and 7.9 °C are demonstrated at noon with solar intensity of 717 W m-2 and night, respectively. Vivid red-, green-, blue-structured colors, and colorless films are designed and implemented to suppress the solar input and control the effective visible light transmissivity considering the efficiency function of human vision. In addition, temperature rise of 11.1 °C is achieved by applying an alternating current field on the PRC film. This study provides a new perspective on the thermal management and aesthetic functionalities of smart windows and wearables.

Cell wall composition determines handedness reversal in helicoidal cellulose architectures of Pollia condensata fruits.

Chiral asymmetry is important in a wide variety of disciplines and occurs across length scales. While several natural chiral biomolecules exist only with single handedness, they can produce complex hierarchical structures with opposite chiralities. Understanding how the handedness is transferred from molecular to the macroscopic scales is far from trivial. An intriguing example is the transfer of the handedness of helicoidal organizations of cellulose microfibrils in plant cell walls. These cellulose helicoids produce structural colors if their dimension is comparable to the wavelength of visible light. All previously reported examples of a helicoidal structure in plants are left-handed except, remarkably, in the Pollia condensata fruit; both left- and right-handed helicoidal cell walls are found in neighboring cells of the same tissue. By simultaneously studying optical and mechanical responses of cells with different handednesses, we propose that the chirality of helicoids results from differences in cell wall composition. In detail, here we showed statistical substantiation of three different observations: 1) light reflected from right-handed cells is red shifted compared to light reflected from left-handed cells, 2) right-handed cells occur more rarely than left-handed ones, and 3) right-handed cells are located mainly in regions corresponding to interlocular divisions. Finally, 4) right-handed cells have an average lower elastic modulus compared to left-handed cells of the same color. Our findings, combined with mechanical simulation, suggest that the different chiralities of helicoids in the cell wall may result from different chemical composition, which strengthens previous hypotheses that hemicellulose might mediate the rotations of cellulose microfibrils.

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.

Brush-Like Polymeric Gels Enabled Photonic Crystals toward Ultrasensitive Cosolvent Chromism.

Responsive photonic crystals (RPCs) exhibit dynamic chromism upon trigger by various solvents, showing potential applications in qualitative identification and quantitative analysis of multicomponent solvents. However, distinguishing similar solvents, especially traces of cosolvents, remains challenging due to the limited sensitivity of RPCs. To address this, we herein introduce brush-like polymeric gels inside photonic crystals, forming a brush-like polymeric photonic gel (BPPG) that can trace tiny component changes. In this BPPG system, the acrylate backbones and PEG side-chains stretch incrementally due to the cosolvency of ethanol-water mixtures, resulting in highly sensitive chromatic responses within ethanol-rich concentrations. With water content varying slightly from 0 to 1 vol%, the reflection wavelength of BPPG can sharply redshift over 30 nm, leading to very noticeable changes in structural color. This enhanced sensitivity makes BPPG suitable for real-time, in-situ purity monitoring of absolute ethanol during storage, transportation, and other applications.

Cholesteric Liquid Crystal Polymeric Coatings for Colorful Artificial Muscles and Motile Humidity Sensor Skin Integrated with Magnetic Composites.

Structural colorful cholesterics show impressive susceptibility to external stimulation, leading to applications in electro/mechano-chromic devices. However, out-of-plane actuation of structural colorful actuators based on cholesterics and the integration with other stimulation remains underdeveloped. Herein, colorful actuators and motile humidity sensors are developed using humidity-responsive cholesteric liquid crystal networks (CLCNs) and magnetic composites. The developed colorful actuator can exhibit synergistic out-of-plane shape morphing and color change in response to humidity, with CLCNs as colorful artificial muscles. Through the integration with magnetic control, the motile sensor can be navigated to open and confined spaces with the aid of friction to detect local relative humidity. The integration of multi-stimulation actuation of cholesteric magnetic actuators will expand the research frontier of structural colorful actuators and motile sensors for confined spaces.

Influence of Sphericity on Surface Termination of Icosahedral Colloidal Clusters.

Colloids self-organize into icosahedral clusters composed of a Mackay core and an anti-Mackay shell under spherical confinement to minimize the free energy. This study explores the variation of surface arrangements of colloids in icosahedral clusters, focusing on the determining factors behind the surface arrangement. To efficiently assemble particles in emulsion droplets, droplet-to-droplet osmotic extraction from particle-laden droplets to salt-containing droplets is used, where the droplets are microfluidically prepared to guarantee a high size uniformity. The icosahedral clusters are optimally produced during a 24-h consolidation period at a 0.04 m salt concentration. The findings reveal an increase in the number of particle layers from 10 to 15 in the icosahedral clusters as the average number of particles increases from 3300 to 11 000. Intriguingly, the number of layers in the anti-Mackay shells, or surface termination, appears to more strongly depend on the sphericity of the clusters than on the deviation in the particle count from an ideal icosahedral cluster. This result suggests that the sphericity of the outermost layer, formed by the late-stage rearrangement of particles to form an anti-Mackay shell near the droplet interface, may play a pivotal role in determining the surface morphology to accommodate a spherical interface.

Refractive Index-Adaptive Nanoporous Chiral Photonic Crystal Film for Chemical Detection Visualized via Selective Reflection.

Photonic crystals (PC) are of great importance in technology, especially in optics and photonics. In general, the structural color of PCs responds to external stimuli primarily by changing their periodicity. Herein, the authors report on refractive index (RI) adaptive PCs. Cross-linked cholesteric films with interconnected nanopores exhibit a very low RI without light scattering. Transparent PC films with maximum reflectance in the ultravoilet (UV) region respond to various chemicals by changing the reflective color of the PC. The authors demonstrate its unique colorimetric chemical detections of hazardous organic liquids. Loading various chemicals into nanopores significantly shifts the structural color into the visible range depending on the chemical's RI. These results are unique in that the structural color of photonic films is mediated by RI changes rather than periodicity changes. In principle, nanoporous photonic crystal films can detect the RI of a chemical substance by its unique color. In contrast to volumetric changes, this sensing mechanism offers several advantages, including durability, excellent sensitivity, fast response time, and wide detection range. These results provide useful insight into stimulus-responsive PCs. The structural color of PC films can be effectively tuned by adjusting average RIs instead of changing periodicity.

Asymmetric Pairing of Cholesteric Liquid Crystal Droplets for Programmable Photonic Cross-Communication.

The photonic cross-communication between photonic droplets has provided complex color patterns through multiple reflections, potentially serving as novel optical codes. However, the cross-communication is mostly restricted to symmetric pairs of identical droplets. Here, a design rule is reported for the asymmetric pairing of two distinct droplets to provide bright color patterns through strong cross-communication and enrich a variety of optical codes. Cholesteric liquid crystal (CLC) droplets with different stopband positions and sizes are paired. The brightness of corresponding color patterns is maximized when the pairs are selected to effectively guide light along the double reflection path by stopbands of two droplets. The experimental results are in good agreement with a geometric model where the blueshift of stopbands is better described by the angles of refraction rather than reflection. The model predicts the effectiveness of pairing quantitatively, which serves as a design rule for programming the asymmetric photonic cross-communication. Moreover, three distinct droplets can be paired in triangular arrays, where all three cross-communication paths yield bright color patterns when three droplets are selected to simultaneously satisfy the rule. It is believed that asymmetric pairing of distinct CLC droplets opens new opportunities for programmable optical encoding in security and anti-counterfeiting applications.

Two-Color Cholesteric Liquid Crystalline Gels for Reversible Writing and Erasing Information Encryption.

Bright structural color derived from the unique helical superstructure of cholesteric liquid crystals (CLCs) has attracted much attention. In addition, fluorescence color is an intrinsic emission upon excitation, which can be observed often under UV light. However, it is a challenge to combine the fluorescence and structural colors to construct a self-supporting system at the same time. In this work, a photoresponsive cyanostilbene-based gelator (CSpy-C10) is synthesized, which emits blue fluorescence in LC. CSpy-C10 can gel LCs and further construct thermo-/photoresponsive CLC physical gels. The structural color of the CLCs, fluorescence, and mechanical properties of the gels can be independently regulated due to the separation of the chiral unit and photoresponsive unit with aggregation-induced emission behavior. Finally, the reversible information encryption including writing and erasing based on the changes in fluorescence are explored. This kind of two-color material can be applied in the fields ranging from information encryption, fluorescent display to high-tech anticounterfeiting.

Reversible Mechanochromisms via Manipulating Surface Wrinkling.

Mechanochromic structural-colored materials have promising applications in various domains. In this Letter, we report three types of reversible mechanochromisms in simple material systems by harnessing mechano-responsive wrinkling dynamics including (i) brightness mechanochromism (BM), (ii) hue change mechanochromism (HCM), and (iii) viewable angle mechanochromism (VAM). Upon stretching, the BM device exhibits almost a constant hue but reduces light brightness due to the postbuckling mechanics-controlled deformation, while the HCM device can change the hue from blue to red with almost constant intensity because of the linear elastic mechanics-controlled deformation. The VAM device shows a constant hue because of the thin film interference effect. However, the viewable angles decrease with increasing applied strain owing to the light scattering of wrinkles. All of the mechanochromic behaviors exhibit good reversibility and durability. We clearly elucidated the underlying mechanisms for different mechanochromisms and demonstrated their potential applications in smart displays, stretchable strain sensors, and antipeeping/anticounterfeiting devices.

One-Pot Self-Assembly of Dual-Color Domes Using Mono-Sized Silica Nanoparticles.

Spots with dual structural colors on the skin of some organisms in nature are of tremendous interest due to the unique function of their dye-free colors. However, imitation of them requires complicated manufacturing processes, expensive equipment, and multiple predesigned building blocks. In this work, a one-pot strategy based on the phase-separation-assisted nonuniform self-assembly of monosized silica nanoparticles is developed to construct domes with dual structural colors. In drying poly(ethylene glycol)-dextran-based (PEG-DEX) droplets, monosized nanoparticles distribute nonuniformly in two compartments due to the droplet inner flow and different nanoparticle compatibility with the two phases. The dome colors are derived from the self-assembled nanoparticles and are programmable by regulating the assembly conditions. The one-pot strategy enables the preparation of multicolor using only one type of building block. With the dual-color domes, encrypted patterns with a high volume of contents are designed, showing promising applications in information delivery.

Full Geometric Control of Hidden Color Information in Diffraction Gratings under Angled White Light Illumination.

Under white light illumination, gratings produce an angular distribution of wavelengths dependent on the diffraction order and geometric parameters. However, previous studies of gratings are limited to at least one geometric parameter (height, periodicity, orientation, angle of incidence) kept constant. Here, we vary all geometric parameters in the gratings using a versatile nanofabrication technique, two-photon polymerization lithography, to encode hidden color information through two design approaches. The first approach hides color information by decoupling the effects of grating height and periodicity under normal and oblique incidence. The second approach hides multiple sets of color information by arranging gratings in sectors around semicircular pixels. Different images are revealed with negligible crosstalk under oblique incidence and varying sample rotation angles. Our analysis shows that an angular separation of ≥10° between adjacent sectors is required to suppress crosstalk. This work has potential applications in information storage and security watermarks.

Dual-Colored Janus Microspheres with Photonic and Plasmonic Faces.

Photonic and plasmonic colors, stemming from nanostructures of dielectric materials and metals, are promising for pigment-free coloration. In particular, nanostructures with structural colors have been employed in stimuli-responsive Janus microparticles to provide active color pixels. Here, the authors report a simple strategy to produce electro-responsive Janus microspheres composed of photonic and plasmonic faces for active color change. The photonic microspheres are first prepared by self-assembly of silica particles in emulsion droplets of photocurable resin. The silica particles form 3D crystalline arrays in the interior and 2D hexagonal arrays on the interface. The emulsion droplets are photocured and the silica particles are selectively removed to make porous photonic microspheres with hexagonal arrays of dimples on the surface. Directional deposition of gold or aluminum on the photonic microsphere develops plasmonic color on the top hemisphere while maintaining photonic color on the bottom hemisphere. Moreover, the metal deposited on one side renders the Janus microspheres electro-responsive. Therefore, the photonic and plasmonic colors are switchable by the orientation control of the Janus microspheres with an external electric field. The photonic and plasmonic colors are independently adjustable by employing two different sizes of silica particles in core-shell emulsion drops.

Photonic Microbeads Templated by Oil-in-Oil Emulsion Droplets for High Saturation of Structural Colors.

Photonic microbeads containing crystalline colloidal arrays are promising as a key component of structural-color inks for various applications including printings, paintings, and cosmetics. However, structural colors from microbeads usually have low color saturation and the production of the beads requires delicate and time-consuming protocols. Herein, elastic photonic microbeads are designed with enhanced color saturation through facile photocuring of oil-in-oil emulsion droplets. Dispersions of highly-concentrated silica particles in elastomer precursors are microfluidically emulsified into immiscible oil to produce monodisperse droplets. The silica particles spontaneously form crystalline arrays in the entire volume of the droplets due to interparticle repulsion which is unperturbed by the diffusion of the surrounding oil whereas weakened for oil-in-water droplets. The crystalline arrays are permanently stabilized by photopolymerization of the precursor, forming elastic photonic microbeads. The microbeads are transferred into the refractive-index-matched biocompatible oil. The high crystallinity of colloidal arrays increases the reflectivity at stopband and the index matching reduces incoherent scattering at the surface of the microbeads, enhancing color saturation. The colors can be adjusted by mixing two distinctly colored microbeads. Also, low stiffness and high elasticity reduce foreign-body sensation and enhance fluidity, potentially serving as pragmatic structural colorants for photonic inks.

Highly Tough, Stretchable, and Solvent-Resistant Cellulose Nanocrystal Photonic Films for Mechanochromism and Actuator Properties.

Cellulose nanocrystals (CNCs)-derived photonic materials have confirmed great potential in producing renewable optical and engineering areas. However, it remains challenging to simultaneously possess toughness, strength, and multiple responses for developing high-performance sensors, intelligent coatings, flexible textiles, and multifunctional devices. Herein, the authors report a facile and robust strategy that poly(ethylene glycol) dimethacrylate (PEGDMA) can be converged into the chiral nematic structure of CNCs by ultraviolet-triggered free radical polymerization in an N,N-dimethylformamide solvent system. The resulting CNC-poly(PEGDMA) composite exhibits impressive strength (42 MPa), stretchability (104%), toughness (31 MJ m-3 ), and solvent resistance. Notably, it preserves vivid optical iridescence, displaying stretchable variation from red, yellow, to green responding to the applied mechanical stimuli. More interestingly, upon exposure to spraying moisture, it executes sensitive actuation (4.6° s-1 ) and multiple complex 3D deformation behaviors, accompanied by synergistic iridescent appearances. Due to its structural anisotropy of CNC with typical left-handedness, the actuation shows the capability to generate a high probability (63%) of right-handed helical shapes, mimicking a coiled tendril. The authors envision that this versatile system with sustainability, robustness, mechanochromism, and specific actuating ability will open a sustainable avenue in mechanical sensors, stretchable optics, intelligent actuators, and soft robots.