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We provide experimental evidence for the influence of the molecular structure of the nematic liquid crystal (NLC) on the photoalignment process in three dimensions at the interface with a polymer layer. In particular, the experimental findings are explained through the presence (or absence) of the π-π aromatic interactions between the NLC and the polymer. The influence of the nematic-to-smectic A phase transition on the photocontrol is also addressed. Furthermore, we demonstrate that the photo-induced reorientation scenarios can be eventually connected to c
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