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Many species of beetles from the family Scarabaeidae reflect light with near-circular polarization. In some cases, spectral narrow-band polarization phenomena result in a distinct color with a metallic shine. In other cases, broad-band features are seen, and these beetles have a silvery or goldish appearance. These features in the cuticles originate from helicoidal structures, so-called circular Bragg structures and also referred to as Bouligand structures. In this communication, Protaetia mirifica, exhibiting near-circular polarization properties in dual spectral regions, centered approximately at the wavelengths of 474 and 770 nm, is investigated in considerable detail using Mueller matrix spectroscopic ellipsometry (MMSE). From interference oscillations in the MMSE spectra, the pitch profile of the helicoidal structures in the beetle cuticle is extracted and further used in electromagnetic modeling of the cuticle structure, including the determination of epicuticle and exocuticle thicknesses (280 nm and 8.1 μm, respectively) and anisotropic optical properties. These findings are confirmed by scanning electron microscopy. The analysis shows that the uppermost 4 μm of the cuticle has a nearly constant pitch of 310 nm, which abruptly jumps to 440 nm and then gradually increases up to 575 nm. Sum decompositions of MMSE spectra reveal that the beetle cuticle reflects like a circular polarizer or like a dielectric mirror, depending on the spectral region.

Depending on processing methods and conditions, cellulose nanocrystal (CNC) films exhibit linear birefringence or selective Bragg reflection. The latter means reflection of light with left‐handed circular polarization (LCP) due to CNC in a helicoidal microstructure of the same handedness. Herein, glass‐supported CNC/polyethylene glycol (CNC/PEG) composite films with PEG concentrations in the range of 0–30% w/w with selective Bragg reflection at wavelengths from 440 to 550 nm are prepared. A modular device comprised of a dip‐coated birefringent CNC‐glass sample sandwiched between two CNC/PEG‐glass samples shows different responses to light with LCP and to light with right‐handed circular polarization (RCP). The device suppresses selective Bragg reflection from the rear (front) CNC/PEG sample for incident light with LCP (RCP), even when the birefringent film does not meet the condition for a halfwave plate. This behavior resembles the performance of optical diodes for circular polarization. Polarization properties of composite films and optical diodes in terms of degree of polarization and ellipticity are discussed within the Stokes–Mueller formalism. Electromagnetic simulations of Mueller matrices reveal the equivalence of modular and in‐tandem film approaches of optical diodes.

Nanocelluloses are very attractive materials for creating structured films with unique optical properties using different preparation techniques. Evaporation-induced self-assembly of cellulose nanocrystals (CNC) aqueous suspensions produces iridescent films with selective circular Bragg reflection. Blade coating of sonicated CNC suspensions leads to birefringent CNC films. In this work, fabrication of both birefringent and chiral films from non-sonicated CNC suspensions using a shear-coating method is studied. Polarization optical microscopy and steady-state viscosity profiles show that non-sonicated CNC suspensions (concentration of 6.5 wt%) evolve with storage time from a gel-like shear-thinning fluid to a mixture of isotropic and chiral nematic liquid crystalline phases. Shear-coated films prepared from non-sonicated fresh CNC suspensions are birefringent, whereas films prepared from suspensions stored several weeks show reflection of left-handed polarized light. Quantification of linear and circular birefringence as well circular dichroism in the films is achieved by using a Mueller matrix formalism.

Evaporation-induced-self-assembly is widely used to produce chiral cellulose nanocrystal (CNC) free-standing films reflecting left-handed polarized light. Research on supported chiral CNC films is rather scarce. The reflection and/or transmission of unpolarized light are the most common optical techniques used to characterize the selective reflection of CNC films whereas the use of techniques to quantify chiral properties is limited. Here, the fabrication of chiral CNC films supported on glass substrates by a shear-coating method, as well as a full characterization of their polarization properties, are reported. Optical chirality is evidenced in films, showing a brilliant blue structural color when viewed through a left-handed polarizer and darkness through a right-handed polarizer. Mueller-matrix data in the reflection and transmission modes are used to quantitatively characterize the structural origin of color in the films. The quantification of the linear and circular birefringence, as well as circular dichroism, is performed by analytical inversion of the Mueller matrix data in the transmission mode and regression analysis using Tellegen constitutive equations. The equivalence of the two methods to quantify the structural chirality in CNC films is demonstrated. The swelling of films in water and kinetics during drying is studied by reflection spectroscopy.

Optical chirality, in terms of circular birefringence and circular dichroism, is described by its electromagnetic and magnetoelectric material tensors, and the corresponding optical activity contributes to the Mueller matrix. Here, spectroscopic ellipsometry in the spectral range 210–1690 nm is used to address chiral phenomena by measuring Mueller matrices in transmission. Three approaches to determine chirality parameters are discussed. In the first approach, applicable in the absence of linear polarization effects, circular birefringence and circular dichroism are evaluated directly from elements of a Mueller matrix. In the second method, differential decomposition is employed, which allows for the unique separation of chirality parameters from linear anisotropic parameters as well as from depolarization provided that the sample is homogeneous along the optical path. Finally, electromagnetic modeling using the Tellegen constitutive relations is presented. The last method also allows structural effects to be included. The three methods to quantify optical chirality are demonstrated for selected materials, including sugar solutions, α-quartz, liquid crystals, beetle cuticle, and films of cellulose nanocrystals.

Helicoidal structures of lamellae of nanofibrils constitute the cuticle of some scarab beetles with iridescent metallic-like shine reflecting left-handed polarized light. The spectral and polarization properties of the reflected light depend on the pitch of the helicoidal structures, dispersion of effective refractive indices and thicknesses of layers in the cuticle. By modelling the outer exocuticle of the scarab beetle Cotinis mutabilis as a stack of continuously twisted biaxial slices of transparent materials, we extract optical and structural parameters by nonlinear regression analysis of variable-angle Mueller-matrix spectroscopic data. Inhomogeneities in the beetle cuticle produce depolarization with non-uniformity in cuticle thickness as the dominant effect. The pitch across the cuticle of C. mutabilis decreased with depth in a two-level profile from 380 to 335 nm and from 390 to 361 nm in greenish and reddish specimens, respectively, whereas in a yellowish specimen, the pitch decreased with depth in a three-level profile from 388 to 326 nm.

Transparent films of cellulose nanocrystals (CNC) are prepared by dip-coating on glass substrates from aqueous suspensions of hydrolyzed filter paper. Dragging forces acting during films’ deposition promote a preferential alignment of the rod-shaped CNC. Films that are 2.8 and 6.0 µm in thickness show retardance effects, as evidenced by placing them between a linearly polarized light source and a linear polarizer sheet in the extinction configuration. Transmission Mueller matrix spectroscopic ellipsometry measurements at normal incidence as a function of sample rotation were used to characterize polarization properties. A differential decomposition of the Mueller matrix reveals linear birefringence as the unique polarization parameter. These results show a promising way for obtaining CNC birefringent films by a simple and controllable method.