Silvia Vignolini

Pointillist structural color in Pollia fruit

Biological communication by means of structural color has existed for at least 500 million years. Structural color is commonly observed in the animal kingdom, but has been little studied in plants. We present a striking example of multilayer-based strong iridescent coloration in plants, in the fruit of Pollia condensata. The color is caused by Bragg reflection of helicoidally stacked cellulose microfibrils that form multilayers in the cell walls of the epicarp. We demonstrate that animals and plants have convergently evolved multilayer-based photonic structures to generate colors using entirely distinct materials. The bright blue coloration of this fruit is more intense than that of any previously described biological material. Uniquely in nature, the reflected color differs from cell to cell, as the layer thicknesses in the multilayer stack vary, giving the fruit a striking pixelated or pointillist appearance. Because the multilayers form with both helicoidicities, optical characterization reveals that the reflected light from every epidermal cell is polarized circularly either to the left or to the right, a feature that has never previously been observed in a single tissue.

Biomimetic layer-by-layer assembly of artificial nacre

Nacre is a technologically remarkable organic-inorganic composite biomaterial. It consists of an ordered multilayer structure of crystalline calcium carbonate platelets separated by porous organic layers. This microstructure exhibits both optical iridescence and mechanical toughness, which transcend those of its constituent components. Replication of nacre is essential for understanding this complex biomineral, and paves the way for tough coatings fabricated from cheap abundant materials. Fabricating a calcitic nacre imitation with biologically similar optical and mechanical properties will likely require following all steps taken in biogenic nacre synthesis. Here we present a route to artificial nacre that mimics the natural layer-by-layer approach to fabricate a hierarchical crystalline multilayer material. Its structure-function relationship was confirmed by nacre-like mechanical properties and striking optical iridescence. Our biomimetic route uses the interplay of polymer-mediated mineral growth, combined with layer-by-layer deposition of porous organic films. This is the first successful attempt to replicate nacre, using CaCO(3).

A 3D Optical Metamaterial Made by Self-Assembly

Optical metamaterials have unusual optical characteristics that arise from their periodic nanostructure. Their manufacture requires the assembly of 3D architectures with structure control on the 10-nm length scale. Such a 3D optical metamaterial, based on the replication of a self-assembled block copolymer into gold, is demonstrated. The resulting gold replica has a feature size that is two orders of magnitude smaller than the wavelength of visible light. Its optical signature reveals an archetypal Pendry wire metamaterial with linear and circular dichroism.

Rewritable photonic circuits

The authors present a technique that allows to modify the local characteristics of two-dimensional photonic crystals by controlled microinfiltration of liquids. They demonstrate experimentally that by addressing and infiltrating each pore with a simple liquid, e.g., water, it is possible to write pixel by pixel optical devices of any geometry and shape. Calculations confirm that the obtained structures indeed constitute the desired resonators and waveguide structures.

Digital Color in Cellulose Nanocrystal Films

Cellulose nanocrystals (CNCs) form chiral nematic phases in aqueous suspensions that can be preserved upon evaporation of water. The resulting films show an intense directional coloration determined by their microstructure. Here, microreflection experiments correlated with analysis of the helicoidal nanostructure of the films reveal that the iridescent colors and the ordering of the individual nematic layers are strongly dependent on the polydispersity of the size distribution of the CNCs. We show how this affects the self-assembly process, and hence multidomain color formation in such bioinspired structural films.

Controlled, bio-inspired self-assembly of cellulose-based chiral reflectors

Layered transparent photonic stacks are known to give rise to highly brilliant color in a variety of living organisms.[1] The biomimetic replication of these structures not only offers a wide range of applications, but can also be used as a tool to gain understanding of the biological processes responsible for the self-assembly of these structures in nature. Recent studies showed that cellulose microfibrils form helicoidal stacks in the plant cell wall, which selectively reflect circularly-polarised light of a specific wavelength.[2]–[5] Such structures are responsible for the bright colors in fruits[2] and leaves[3] of very different species of plants.[4,5] Similar photonic structures can be artificially produced using the same constituent material, cellulose nano-crystals (CNCs).[6,7] Slow evaporation of a CNC suspension gives rise to their spontaneous assembly into a chiral nematic liquid crystalline phase that can be preserved in the dry state.[8,9] The self-assembly process is strongly dependent on the properties of the nanoscale building blocks and on the macroscopic parameters that characterise the assembly.[10]–[12] Many factors influence the optical and mechanical properties of the obtained film, including temperature and pressure[13,15,16] the substrate,[14] and the surface chemistry of the CNCs.[17,18] Nevertheless the self-assembly process is robust and can be coupled with a range of chemical processes.[19]–[21]

Analysing photonic structures in plants

The outer layers of a range of plant tissues, including flower petals, leaves and fruits, exhibit an intriguing variation of microscopic structures. Some of these structures include ordered periodic multilayers and diffraction gratings that give rise to interesting optical appearances. The colour arising from such structures is generally brighter than pigment-based colour. Here, we describe the main types of photonic structures found in plants and discuss the experimental approaches that can be used to analyse them. These experimental approaches allow identification of the physical mechanisms producing structural colours with a high degree of confidence.

Bright-White Beetle Scales Optimise Multiple Scattering of Light

Whiteness arises from diffuse and broadband reflection of light typically achieved through optical scattering in randomly structured media. In contrast to structural colour due to coherent scattering, white appearance generally requires a relatively thick system comprising randomly positioned high refractive-index scattering centres. Here, we show that the exceptionally bright white appearance of Cyphochilus and Lepidiota stigma beetles arises from a remarkably optimised anisotropy of intra-scale chitin networks, which act as a dense scattering media. Using time-resolved measurements, we show that light propagating in the scales of the beetles undergoes pronounced multiple scattering that is associated with the lowest transport mean free path reported to date for low-refractive-index systems. Our light transport investigation unveil high level of optimisation that achieves high-brightness white in a thin low-mass-per-unit-area anisotropic disordered nanostructure.

Tunable 3D Extended Self‐Assembled Gold Metamaterials with Enhanced Light Transmission

The optical properties of metamaterials made by block copolymer self-assembly are tuned by structural and environmental variations. The plasma frequency red-shifts with increasing lattice constant and blue-shifts as the network filling fraction increases. Infiltration with dielectric liquids leads also to a red-shift of the plasma edge. A 300 nm-thick slab of gyroid-structured gold has a remarkable transmission of 20%.

Engineering of light confinement in strongly scattering disordered media

Disordered photonic materials can diffuse and localize light through random multiple scattering, offering opportunities to study mesoscopic phenomena, control light-matter interactions, and provide new strategies for photonic applications. Light transport in such media is governed by photonic modes characterized by resonances with finite spectral width and spatial extent. Considerable steps have been made recently towards control over the transport using wavefront shaping techniques. The selective engineering of individual modes, however, has been addressed only theoretically. Here, we experimentally demonstrate the possibility to engineer the confinement and the mutual interaction of modes in a two-dimensional disordered photonic structure. The strong light confinement is achieved at the fabrication stage by an optimization of the structure, and an accurate and local tuning of the mode resonance frequencies is achieved via post-fabrication processes. To show the versatility of our technique, we selectively control the detuning between overlapping localized modes and observe both frequency crossing and anti-crossing behaviours, thereby paving the way for the creation of open transmission channels in strongly scattering media.