In this work, we present the innovative synthesis of salophen (acetaminosalol) derivatives in a solvent-free environment by high-speed ball milling, using a non-conventional activation method, which allowed obtaining compounds in a shorter time and with a better yield. Furthermore, for the first time, the salophen derivatives were deposited as composite films, using a matrix of poly 3,4-ethylene dioxythiophene:polystyrene sulfonate (PEDOT:PSS) polymer. Significant findings include the transformation from the benzoid to the quinoid form of PEDOT post-IPA treatment, as evidenced by Raman spectroscopy. SEM analysis revealed the formation of homogeneous films, and AFM provided insights into the changes in surface roughness and morphology post-IPA treatment, which may be crucial for understanding potential applications in electronics. The optical bandgap ranges between 2.86 and 3.2 eV for PEDOT:PSS-salophen films, placing them as organic semiconductors. The electrical behavior of the PEDOT:PSS-salophen films undergoes a transformation with the increase in voltage, from ohmic to space charge-limited conduction, and subsequently to constant current, with a maximum of 20 mA. These results suggest the possible use of composite films in organic electronics.

Zinc(II) bis(8-hydroxyquinolinate) (Zn(HQ)₂) and 1,10-phenanthroline (phen) were combined to fabricate an organic semiconductor in a bulk heterojunction architecture and subsequently embedded in a poly 3,4-ethylene dioxythiophene–polystyrene sulfonate (PEDOT–PSS) matrix. The resulting Zn(HQ)₂-phen/PEDOT–PSS was deposited as a film upon tin-oxide-coated glass and graphite-covered Tetra Pak (TP)-recycled substrates for the manufacture of organic photoconductive devices. The topographical and micromechanical characteristics of the hybrid films were assessed by atomic force microscopy, with an average roughness of 5.6 nm, maximum tensile strength of 7.95 MPa, and Knoop microhardness of 14.7. The fundamental energy gap (E_g) was determined employing the Kubelka–Munk function, with E_g of 3.5–3.8 eV. These results were complemented with a computational DFT molecular orbital analysis of the species involved in the hybrid semiconductor. The devices were electrically characterized under UV irradiation conditions, obtaining the current–voltage and power–voltage relationships. The maximum current in the TP–graphite device is 1.8 × 10⁻² A and 1.1 × 10⁻² A in the device on glass–ITO. Zn(HQ)₂-phen/PEDOT–PSS film presents its own operating regimes relating to a photoconductor or flexible photoresistor. The power in the device on glass–ITO is 120 mW and 113 mW for shortwave and longwave, respectively, and in the device on TP–graphite, it is 198 mW and 139 mW.