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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. The handedness of circular polarization of light is reversed by a modular device comprised of a dip-coated birefringent cellulose nanocrystal (CNC) film sandwiched by two CNC/polyethylene glycol composite films. Asymmetric forward and backward propagation of circular propagation resembles an optical diode at wavelengths of selective Bragg reflection.image (c) 2023 WILEY-VCH GmbH, Funding Agencies|Conacyt-Mexico for doctoral studies; Swedish Government Strategic Research Area in Materials Science on Advanced Functional Materials at Linkoeping University [782810]; Conacyt [2009-00971, N-295261]; [LN-254119]

Featured Application The analysis of the transmission of Mueller matrices facilitates studies of optical activity in samples that also exhibit linear anisotropy and depolarization and may have a multilayered structure. Such studies are important for the development of applications in chiroptics. 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, alpha-quartz, liquid crystals, beetle cuticle, and films of cellulose nanocrystals., Funding Agencies|Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]

Chiral nanocrystalline cellulose (NCC) free-standing films were prepared through slow evaporation of aqueous suspensions of cellulose nanocrystals in a nematic chiral liquid crystal phase. Mueller matrix (MM) spectroscopic ellipsometry is used to study the polarization and depolarization properties of the chiral films. In the reflection mode, the MM is similar to the matrices reported for the cuticle of some beetles reflecting near circular left-handed polarized light in the visible range. The polarization properties of light transmitted at normal incidence for different polarization states of incident light are discussed. By using a differential decomposition of the MM, the structural circular birefringence and dichroism of a NCC chiral film are evaluated., Funding Agencies|Knut and Alice Wallenberg foundation; Swedish Research Council; Carl Tryggers foundation; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]; Brazilian agency FAPESP; Brazilian agency CNPq; FAPESP [2014/12424-2]