Photo‐assembly of reactive liquid crystals by simultaneous diffusion and polymerization can give rise to interesting new polymeric architectures. In this report, the authors summarize recent results, which show how deformation of the molecular helix in a cholesteric network can give rise to interesting new optical properties, such as higher order reflection bands and built‐in optical retardation. When the deformed helix is combined with a pitch gradient over the film thickness, the built‐in retardation can be used for wide‐band cholesteric polarizers that directly generate polarized light.
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