Polarization-sensitive media based on polymers and functional chromophores have deservedly occupied their niche among photonic materials that are increasingly contributing to the possibilities of richer light sensing, in the field of optical communications, information transfer, its storage, display, etc. within a wide range of applications. The media considered here are represented by multiple highly polar compositions based on functional azo dyes doped in a compatible biopolymer as a matrix. This paper presents our specific studies on the influence of molecular-structural factors on the photoanisotropic properties of polarization-sensitive compositions. The illustrative examples show evidence of the finding of one of the factors that work out the light sensitivity of the materials for multiple times. This factor was the molecular aggregation of the chromophoric component. Quite accurate comparisons are shown of the improvement in photoresponsibility of various compositions with the mutual combination of their chromophoric molecules, in particular as a result of their component dimerization. In the overwhelming majority of azochromophoric dimers demonstrate greater sensitivity to actinic polarized light rather than their predecessor versions. The paper also demonstrates an example of going beyond the framework of dimerization towards the further development of the aggregation of molecules with the formation of azopolymers. The latter turned out to be promising in the case of the correct implementation of increasing integration of the components of the studied materials.
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