Whiteness arises from the random scattering of incident light from disordered structures. [1] Opaque white materials have to contain a sufficiently large number of scatterers and therefore usually require thicker, material-rich nanostructures than structural color arising from the coherent interference of light. [2,3] In nature, bright white appearance arises from the dense arrays of pterin pigments in pierid butterflies, [4] guanine crystals in spiders, [5] or leucophore cells in the flexible skin of cuttlefish. [6] A striking example of such whiteness is found in the chitinous networks of white beetles, e.g., Lepidiota stigma and Cyphochilus sp. [7][8][9] Previous research investigating these beetle structures has shown that the chitinous network is one of the most strongly scattering materials in nature, and therefore the question arises whether this structure is evolutionary optimized for strong scattering while minimizing the Most studies of structural color in nature concern periodic arrays, which through the interference of light create color. The "color" white however relies on the multiple scattering of light within a randomly structured medium, which randomizes the direction and phase of incident light. Opaque white materials therefore must be much thicker than periodic structures. It is known that flying insects create "white" in extremely thin layers. This raises the question, whether evolution has optimized the wing scale morphology for white reflection at a minimum material use. This hypothesis is difficult to prove, since this requires the detailed knowledge of the scattering morphology combined with a suitable theoretical model. Here, a cryoptychographic X-ray tomography method is employed to obtain a full 3D structural dataset of the network morphology within a white beetle wing scale. By digitally manipulating this 3D representation, this study demonstrates that this morphology indeed provides the highest white retroreflection at the minimum use of material, and hence weight for the organism. Changing any of the network parameters (within the parameter space accessible by biological materials) either increases the weight, increases the thickness, or reduces reflectivity, providing clear evidence for the evolutionary optimization of this morphology. amount of employed material, thus reducing the weight of the organism. The brilliant white reflection from Cyphochilus beetles is assumed to be important for camouflage among white fungi and in a shady environment.In contrast to periodic photonic materials, for which the optical response is straightforward to calculate, the reflection of light from such disordered network morphologies requires a detailed knowledge of local geometry. [2,3,9,10] For these complex cases, the validity of the diffusion approximation is limited, since single scattering elements are difficult to be identified. [7] To fully understand the correlation between the structure and (optical) properties of complex materials, the detailed real-space structure in combination with a s...

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.

A common strategy to optimize whiteness in living organisms consists in using 3D random networks with dense and polydisperse scattering elements constituted by relatively low refractive index materials. Inspired by these natural architectures, a fast and scalable method to produce highly scattering porous polymer films via phase separation is developed. By varying the molecular weight of the polymer, the morphology of the porous films is modified, and therefore their scattering properties are tuned. The achieved transport mean free paths are in the micrometer range, improving the scattering strength of analogous low refractive index systems, e.g., standard white paper, by an order of magnitude. The produced porous films show a broadband reflectivity of ≈75% while only 4 µm thick. In addition, the films are flexible and can be readily index-matched with water (i.e., they become transparent when wet), allowing for various applications such as coatings with tunable transmittance and responsive paints. elements must be randomly arranged, typically decreasing the packing efficiency. [5][6][7] To compensate for the non-ideal packing, materials that are very highly scattering strength are generally chosen for industrial applications (i.e., materials with high refractive indexes). DOIA great example of multiple scattering optimization in a low refractive index medium is observed in the scales of Cyphochilus beetles (Figure 1a,c). Here, the anisotropic chitin network inside the scales which cover the insect's body outperforms all man-made low refractive index materials known to date. [3,[8][9][10][11] The key to such optimization lies in the tuning of the filling fraction and in the anisotropic nature of the fibrillar structure in the scales. [3,10] Inspired by these natural design principles, we fabricated highly scattering white networks solely constituted by poly methyl methacrylate (PMMA) (Figure 1b,d). The resulting porous films are flexible and show the shortest transport mean free path reported in the literature for low refractive index materials. We demonstrated that the scattering strength of the network can be enhanced by varying the molecular weight of PMMA to achieve transport mean free paths (l t ) as low as 1 µm for an incident wavelength around 500 nm. Having such a short transport mean free path yields a reflectance of 75% for a 4 µm thick film. Due to their low refractive index (close to 1.5 over the whole visible range) and porosity, the produced free-standing films can be easily index-matched with water and other conventional solvents, providing a tunable response, which transitions from white to transparent upon wetting (Figure 1b; Figure S1 and Movie S1, Supporting Information). This property, in addition with the high flexibility of the films ( Figure S2 and Movie S2, Supporting Information), allows for various coating applications. We demonstrated that the scattering properties are maintained when the porous films are grinded into powders, opening their exploitation as white enhancers in paints, pa...

Cellulose is the most abundant biopolymer on Earth. Cellulose fibers, such as the one extracted form cotton or woodpulp, have been used by humankind for hundreds of years to make textiles and paper. Here we show how, by engineering light–matter interaction, we can optimize light scattering using exclusively cellulose nanocrystals. The produced material is sustainable, biocompatible, and when compared to ordinary microfiber-based paper, it shows enhanced scattering strength (×4), yielding a transport mean free path as low as 3.5 μm in the visible light range. The experimental results are in a good agreement with the theoretical predictions obtained with a diffusive model for light propagation.

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

Structural colours in living organisms have been observed and analysed in a large number of species, however the study of how the micro- and nano-scopic natural structures responsible of such colourations develop has been largely ignored. Understanding the interplay between chemical composition, structural morphology on multiple length scales, and mechanical constraints requires a range of investigation tools able to capture the different aspects of natural hierarchical architectures. Here, we report a developmental study of the most widespread strategy for structural colouration in nature: the cuticular multilayer. In particular, we focus on the exoskeletal growth of the dock leaf beetle Gastrophysa viridula, capturing all aspects of its formation: the macroscopic growth is tracked via synchrotron microtomography, while the submicron features are revealed by electron microscopy and light spectroscopy combined with numerical modelling. In particular, we observe that the two main factors driving the formation of the colour-producing multilayers are the polymerization of melanin during the ecdysis and the change in the layer spacing during the sclerotisation of the cuticle. Our understanding of the exoskeleton formation provides a unique insight into the different processes involved during metamorphosis.

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.

Pachyrhynchus sarcitis weevils are flightless weevils characterized by colored patches of scales on their dark elytra. The vivid colors of such patches result from the reflection of differently oriented 3D photonic crystals within their scales. The results show that hybrid P. sarcitis, the first filial generation of two P. sarcitis populations from Lanyu Island (Taiwan) and Babuyan Island (Philippines), mixes the color of its ancestors by tuning the photonic structure in its scales. A careful spectroscopical and anatomical analysis of the weevils in the phylogeny reveals the hereditary characteristics of the photonic crystals within their scales in terms of lattice constant, orientation and domain size. Monitoring how structural coloration is inherited by offspring highlights the versatility of photonic structures to completely redesign the optical response of living organisms. Such finding sheds light onto the evolution and development mechanisms of structural coloration in Pachyrhynchus weevils and provides inspiration for the design of visual appearance in artificial photonic materials.