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Three dye molecules (Dye) of Acid Brilliant Scarlet 3R (AR18), Amido Naphthol Red G (AR1), Indigo Carmine (IC), as well as sodium dodecyl sulfate (SDS) as dopant agents were used for electrochemical synthesis of polypyrrole (PPy) layers onto indium doped tin oxide (ITO) coated polyethylene terephthalate (PET) electrode. The morphology, electrochemical, optical, and spectroelectrochemical properties of the layers were investigated. The study of the electrochemical behavior showed that the presence of each AR18, AR1, or IC with SDS, had shown an excellent synergistic effect on the electrochemical stability of layers. The morphological characterization of the PPy/dopant(s) using atomic force microscopy (AFM) showed that the surface roughness in the PPy/IC-SDS layer was 39% and 32% less than the PPy/AR18-SDS and PPy/AR1-SDS, respectively. The absorption spectrum of PPy/dopant(s) in the UV–Vis …