The self-assembly of cellulose nanocrystals is a powerful method for the fabrication of biosourced photonic films with a chiral optical response. While various techniques have been exploited to tune the optical properties of such systems, the presence of external fields has yet to be reported to significantly modify their optical properties. In this work, by using small commercial magnets (≈ 0.5–1.2 T) the orientation of the cholesteric domains is enabled to tune in suspension as they assemble into films. A detailed analysis of these films shows an unprecedented control of their angular response. This simple and yet powerful technique unlocks new possibilities in designing the visual appearance of such iridescent films, ranging from metallic to pixelated or matt textures, paving the way for the development of truly sustainable photonic pigments in coatings, cosmetics, and security labeling.

Biopolymer-based composites enable to combine different functionalities using renewable materials and cost-effective routes. Here we fabricate novel thermoresponsive photonic films combining cellulose nanocrystals (CNCs) with a polydiolcitrate elastomer exhibiting shape memory properties, known as hydroxyl-dominant poly(dodecanediol-co-citrate) (PDDC-HD). Iridescent films of CNCs are first made by evaporation-induced self-assembly, then embedded in the PDDC-HD prepolymer, and finally cured to obtain a cross-linked composite with shape memory properties. The fabricated samples are characterized by polarized optical microscopy, scanning electron microscopy, and thermomechanical cycling. The obtained hybrid material combines both intense structural coloration and shape memory effect. The association of stiff cellulose nanocrystals and soft polydiolcitrate elastomer enhances the overall mechanical properties (increased modulus and reduced brittleness). This hybrid nanocomposite takes advantage of two promising materials and expands their possibilities to cover a wide range of potential applications as multiresponsive devices and sensors. As they perform from room to body temperatures, they could be also good candidates for biomedical applications.Keywords: biomimetic; cellulose nanocrystals; cholesteric; polydiolcitrates; shape memory

Complex hierarchical architectures are ubiquitous in nature. By designing and controlling the interaction between elementary building blocks, nature is able to optimize a large variety of materials with multiple functionalities. Such control is, however, extremely challenging in man-made materials, due to the difficulties in controlling their interaction at different length scales simultaneously. Here, hierarchical cholesteric architectures are obtained by the self-assembly of cellulose nanocrystals within shrinking, micron-sized aqueous droplets. This confined, spherical geometry drastically affects the colloidal self-assembly process, resulting in concentric ordering within the droplet, as confirmed by simulation. This provides a quantitative tool to study the interactions of cellulose nanocrystals beyond what has been achieved in a planar geometry. Our developed methodology allows us to fabricate truly hierarchical solid-state architectures from the nanometer to the macroscopic scale using a renewable and sustainable biopolymer.Keywords: cellulose nanocrystals; colloidal self-assembly; hierarchical architecture; liquid crystals; microfluidics

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.Keywords: cellulose nanocrystals; chiral-nematic films; iridescence; self-assembly; structural color

The insertion of a metal-coated tip on the surface of a photonic crystal microcavity is used for simultaneous near field imaging of electric and magnetic fields in photonic crystal nanocavities, via the radiative emission of embedded semiconductor quantum dots (QD). The photoluminescence intensity map directly gives the electric field distribution, to which the electric dipole of the QD is coupled. The magnetic field generates, via Faraday's law, a circular current in the apex of the metallized probe that can be schematized as a ring. The resulting magnetic perturbation of the photonic modes induces a blue shift, which can be used to map the magnetic field, within a single near-field scan.Highlights► A metallic coated tip for scanning near-field microscopy interacts with the magnetic field of a photonic crystal cavity. ► The interaction results in a sizeable high frequency shift of its eigenmodes. ► By constructing near field maps of this shift one obtains with high spatial resolution the spatial distribution of the magnetic field intensity.

A local tuning of the modes of photonic crystal systems both to blue and to red sides of the resonance is implemented by nano-infiltration/evaporation of water and laser micro-oxidation. This technology is used to completely control coupled photonic nanocavities (photonic crystal molecules). Beside the standard condition of zero detuning between identical modes of the two cavities (homoatomic molecule), we are also able to produce coupling between two modes of different polarization and spatial distribution (heteroatomic molecule).Highlights► A continuously tunable photonic molecule is obtained. ► The tuning method is implemented by infiltration of water and laser assisted evaporation and microoxidation. ► Both homo-atomic and hetero-atomic molecule configurations are realized.