Multiple origins of lipid-based structural colors contribute to a gradient of fruit colors in Viburnum (Adoxaceae).

Structural color is poorly known in plants relative to animals. In fruits, only a handful of cases have been described, including in Viburnum tinus where the blue color results from a disordered multilayered reflector made of lipid droplets. Here, we examine the broader evolutionary context of fruit structural color across the genus Viburnum. We obtained fresh and herbarium fruit material from 30 Viburnum species spanning the phylogeny and used transmission electron microscopy, optical simulations, and ancestral state reconstruction to identify the presence/absence of photonic structures in each species, understand the mechanism producing structural color in newly identified species, relate the development of cell wall structure to reflectance in Viburnum dentatum, and describe the evolution of cell wall architecture across Viburnum. We identify at least two (possibly three) origins of blue fruit color in Viburnum in species which produce large photonic structures made of lipid droplets embedded in the cell wall and which reflect blue light. Examining the full spectrum of mechanisms producing color in pl, including structural color as well as pigments, will yield further insights into the diversity, ecology, and evolution of fruit color.

The limitations of extending nature's color palette in correlated, disordered systems.

Living organisms have developed a wide range of appearances from iridescent to matte textures. Interestingly, angular-independent structural colors, where isotropy in the scattering structure is present, only produce coloration in the blue wavelength region of the visible spectrum. One might, therefore, wonder if such observation is a limitation of the architecture of the palette of materials available in nature. Here, by exploiting numerical modeling, we discuss the origin of isotropic structural colors without restriction to a specific light scattering regime. We show that high color purity and color saturation cannot be reached in isotropic short-range order structures for red hues. This conclusion holds even in the case of advanced scatterer morphologies, such as core-shell particles or inverse photonic glasses-explaining recent experimental findings reporting very poor performances of visual appearance for such systems.

Disordered wax platelets on Tradescantia pallida leaves create golden shine.

Plants have various strategies to protect themselves from harmful light. An example of such a protective mechanism is the growth of epicuticular nanostructures, such as a layer of hair or wax crystals. Most nanostructures are optimised to screen UV radiation, as UV light is particularly damaging for cellular tissue. We find that, contrary to the commonly found UV reflectance, the epicuticular wax crystals on Tradescantia leaves reflect strongly in the higher visible wavelength regime. Thus, they give the leaves a golden shine. We characterize the optical appearance of Tradescantia pallida 'purpurea' leaves by angularly resolved spectroscopy and compare the results to finite difference time domain simulations. We find that it is the disordered assembly of the wax platelets that is the crucial parameter to obtain the observed reflected intensity increase for higher wavelengths.

Topological invariance in whiteness optimisation.

Maximizing the scattering of visible light within disordered nano-structured materials is essential for commercial applications such as brighteners, while also testing our fundamental understanding of light-matter interactions. The progress in the research field has been hindered by the lack of understanding how different structural features contribute to the scattering properties. Here we undertake a systematic investigation of light scattering in correlated disordered structures. We demonstrate that the scattering efficiency of disordered systems is mainly determined by topologically invariant features, such as the filling fraction and correlation length, and residual variations are largely accounted by the surface-averaged mean curvature of the systems. Optimal scattering efficiency can thus be obtained from a broad range of disordered structures, especially when structural anisotropy is included as a parameter. These results suggest that any disordered system can be optimised for whiteness and give comparable performance, which has far-reaching consequences for the industrial use of low-index materials for optical scattering.

Cellulose-Based Scattering Enhancers for Light Management Applications.

To manipulate the light-matter interaction effectively, we often rely on high refractive index inorganic nanoparticles. Such materials are contained essentially in everything that looks colorful or white: from paints to coatings but also in processed food, toothpaste, and cosmetic products. As these nanoparticles can accumulate in the human body and environment, there is a strong need to replace them with more biocompatible counterparts. In this work, we introduce various types of cellulose-based microparticles (CMPs) of four sizes with optimized dimensions for efficient light scattering that can replace traditional inorganic particles. We demonstrate that the produced materials can be exploited as highly efficient scattering enhancers, with designed optical performance. Finally, exploiting these cellulose colloids, we fabricated scattering materials and high transmittance/haze films with record performances with respect to the state-of-the-art values. The renewable and biocompatible nature of our systems, combined with their excellent optical properties, allows for the use of our cellulose-based particles in paints, LEDs, and solar cell devices and especially in applications where the biocompatibility of the component is essential, such as in food and pharmaceutical coatings.

Light Management with Natural Materials: From Whiteness to Transparency.

The possibility of structuring material at the nanoscale is essential to control light-matter interactions and therefore fabricate next-generation paints and coatings. In this context, nature can serve not only as a source of inspiration for the design of such novel optical structures, but also as a primary source of materials. Here, some of the strategies used in nature to optimize light-matter interaction are reviewed and some of the recent progress in the production of optical materials made solely of plant-derived building blocks is highlighted. In nature, nano- to micrometer-sized structured materials made from biopolymers are at the origin of most of the light-transport effects. How natural photonic systems manage light scattering and what can be learned from plants and animals to produce photonic materials from biopolymers are discussed. Tuning the light-scattering properties via structural variations allows a wide range of appearances to be obtained, from whiteness to transparency, using the same renewable and biodegradable building blocks. Here, various transparent and white cellulose-based materials produced so far are highlighted.

Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors.

Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106 m s-1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons.

Angular-Independent Photonic Pigments via the Controlled Micellization of Amphiphilic Bottlebrush Block Copolymers.

Photonic materials with angular-independent structural color are highly desirable because they offer the broad viewing angles required for application as colorants in paints, cosmetics, textiles, or displays. However, they are challenging to fabricate as they require isotropic nanoscale architectures with only short-range correlation. Here, porous microparticles with such a structure are produced in a single, scalable step from an amphiphilic bottlebrush block copolymer. This is achieved by exploiting a novel "controlled micellization" self-assembly mechanism within an emulsified toluene-in-water droplet. By restricting water permeation through the droplet interface, the size of the pores can be precisely addressed, resulting in structurally colored pigments. Furthermore, the reflected color can be tuned to reflect across the full visible spectrum using only a single polymer (Mn  = 290 kDa) by altering the initial emulsification conditions. Such "photonic pigments" have several key advantages over their crystalline analogues, as they provide isotropic structural coloration that suppresses iridescence and improves color purity without the need for either refractive index matching or the inclusion of a broadband absorber.

Viburnum tinus Fruits Use Lipids to Produce Metallic Blue Structural Color.

Viburnum tinus is an evergreen shrub that is native to the Mediterranean region but cultivated widely in Europe and around the world. It produces ripe metallic blue fruits throughout winter [1]. Despite its limited fleshy pulp [2], its high lipid content [3] makes it a valuable resource to the small birds [4] that act as its seed-dispersers [5]. Here, we find that the metallic blue appearance of the fruits is produced by globular lipid inclusions arranged in a disordered multilayer structure. This structure is embedded in the cell walls of the epicarp and underlaid with a dark layer of anthocyanin pigments. The presence of such large, organized lipid aggregates in plant cell walls represents a new mechanism for structural coloration and may serve as an honest signal of nutritional content.

Complex photonic response reveals three-dimensional self-organization of structural coloured bacterial colonies.

Vivid colours found in living organisms are often the result of scattering from hierarchical nanostructures, where the interplay between order and disorder in their packing defines visual appearance. In the case of Flavobacterium IR1, the complex arrangement of the cells in polycrystalline three-dimensional lattices is found to be a distinctive fingerprint of colony organization. By combining analytical analysis of the angle-resolved scattering response of in vivo bacterial colonies with numerical modelling, we show that we can assess the inter-cell distance and cell diameter with a resolution below 10 nm, far better than what can be achieved with conventional electron microscopy, suffering from preparation artefacts. Retrieving the role of disorder at different length scales from the salient features in the scattering response enables a precise understanding of the structural organization of the bacteria.

Bionic 3D printed corals.

Corals have evolved as optimized photon augmentation systems, leading to space-efficient microalgal growth and outstanding photosynthetic quantum efficiencies. Light attenuation due to algal self-shading is a key limiting factor for the upscaling of microalgal cultivation. Coral-inspired light management systems could overcome this limitation and facilitate scalable bioenergy and bioproduct generation. Here, we develop 3D printed bionic corals capable of growing microalgae with high spatial cell densities of up to 109 cells mL-1. The hybrid photosynthetic biomaterials are produced with a 3D bioprinting platform which mimics morphological features of living coral tissue and the underlying skeleton with micron resolution, including their optical and mechanical properties. The programmable synthetic microenvironment thus allows for replicating both structural and functional traits of the coral-algal symbiosis. Our work defines a class of bionic materials that is capable of interacting with living organisms and can be exploited for applied coral reef research and photobioreactor design.

Retrieving the Coassembly Pathway of Composite Cellulose Nanocrystal Photonic Films from their Angular Optical Response.

Aqueous suspensions of cellulose nanocrystals (CNCs) are known to self-assemble into a chiral nematic liquid crystalline phase, leading to solid-state nanostructured colored films upon solvent evaporation, even in the presence of templating agents. The angular optical response of these structures, and therefore their visual appearance, are completely determined by the spatial arrangement of the CNCs when the drying suspension undergoes a transition from a flowing and liquid crystalline state to a kinetically arrested state. Here, it is demonstrated how the angular response of the final film allows for retrieval of key physical properties and the chemical composition of the suspension at the onset of the kinetic arrest, thus capturing a snapshot of the past. To illustrate this methodology, a dynamically evolving sol-gel coassembly process is investigated by adding various amounts of organosilica precursor, namely, 1,2-bis(trimethoxysilyl)ethane. The influence of organosilica condensation on the kinetic arrest can be tracked and thus explains the angular response of the resulting films. The a posteriori and in situ approach is general; it can be applied to a variety of additives in CNC-based films and it allows access to key rheological information of the suspension without using any dedicated rheological technique.

Coherent backscattering of light by an anisotropic biological network.

The scattering strength of a random medium relies on the geometry and spatial distribution of its components as well as on their refractive index. Anisotropy can, therefore, play a major role in the optimization of the scattering efficiency in both biological and synthetic materials. In this study, we show that, by exploiting the coherent backscattering phenomenon, it is possible to characterize the optical anisotropy in Cyphochilus beetle scales without the need to change their orientation or their thickness. For this reason, such a static and easily accessible experimental approach is particularly suitable for the study of biological specimens. Moreover, estimation of the anisotropy in Cyphochilus beetle scales might provide inspiration for improving the scattering strength of artificial white materials.

Long-Wavelength Reflecting Filters Found in the Larval Retinas of One Mantis Shrimp Family (Nannosquillidae).

Both vertebrates and invertebrates commonly exploit photonic structures adjacent to their photoreceptors for visual benefits. For example, use of a reflecting structure (tapetum) behind the retina increases photon capture, enhancing vision in dim light [1-5]. Colored filters positioned lateral or distal to a photoreceptive unit may also be used to tune spectral sensitivity by selective transmission of wavelengths not absorbed or scattered by the filters [6-8]. Here we describe a new category of biological optical filter that acts simultaneously as both a transmissive spectral filter and narrowband reflector. Discovered in the larval eyes of only one family of mantis shrimp (stomatopod) crustaceans (Nannosquillidae), each crystalline structure bisects the photoreceptive rhabdom into two tiers and contains an ordered array of membrane-bound vesicles with sub-wavelength diameters of 153 ± 5 nm. Axial illumination of the intrarhabdomal structural reflector (ISR) in vivo produces a narrow band of yellow reflectance (mean peak reflectivity, 572 ± 18 nm). The ISR is similar to several synthetic devices, such as bandgap filters, laser mirrors, and (in particular) fiber Bragg gratings used in optical sensors for a wide range of industries. To our knowledge, the stomatopod larval ISR is the first example of a naturally occurring analog to these human-made devices. Considering what is known about these animals' visual ecology, we propose that these reflecting filters may help improve the detection of pelagic bioluminescence in shallow water at night. VIDEO ABSTRACT.

Visual Appearance of Chiral Nematic Cellulose-Based Photonic Films: Angular and Polarization Independent Color Response with a Twist.

Hydroxypropyl cellulose (HPC) is a biocompatible cellulose derivative capable of self-assembling into a lyotropic chiral nematic phase in aqueous solution. This liquid crystalline phase reflects right-handed circular polarized light of a specific color as a function of the HPC weight fraction. Here, it is demonstrated that, by introducing a crosslinking agent, it is possible to drastically alter the visual appearance of the HPC mesophase in terms of the reflected color, the scattering distribution, and the polarization response, resulting in an exceptional matte appearance in solid-state films. By exploiting the interplay between order and disorder, a robust and simple methodology toward the preparation of polarization and angular independent color is developed, which constitutes an important step toward the development of real-world photonic colorants.

Anomalous-Diffusion-Assisted Brightness in White Cellulose Nanofibril Membranes.

The understanding of the interaction between light and complex, random structures is the key for designing and tailoring the optical appearance and performance of many materials that surround us, ranging from everyday consumer products, such as those for personal care, paints, and paper, to light diffusers used in the LED-lamps and solar cells. Here, it is demonstrated that the light transport in membranes of pure cellulose nanofibrils (CNFs) can be controlled to achieve bright whiteness in structures only a few micrometers thick. This is in contrast to other materials, such as paper, which require hundreds of micrometers to achieve a comparable appearance. The diffusion of light in the CNF membranes is shown to become anomalous by tuning the porosity and morphological features. Considering also their strong mechanical properties and biocompatibility, such white coatings are proposed as a new application for cellulose nanofibrils.

Photonic Resins: Designing Optical Appearance via Block Copolymer Self-Assembly.

Despite a huge variety of methodologies having been proposed to produce photonic structures by self-assembly, the lack of an effective fabrication approach has hindered their practical uses. These approaches are typically limited by the poor control in both optical and mechanical properties. Here we report photonic thermosetting polymeric resins obtained through brush block copolymer (BBCP) self-assembly. We demonstrate that the control of the interplay between order and disorder in the obtained photonic structure offers a powerful tool box for designing the optical appearance of the polymer resins in terms of reflected wavelength and scattering properties. The obtained materials exhibit excellent mechanical properties with hardness up to 172 MPa and Young's modulus over 2.9 GPa, indicating great potential for practical uses as photonic coatings on a variety of surfaces.