In this article, we present a wet ultrasonochemical synthesis of nanocrystalline TiO2 powders in the anatase form in ethanol solution and their surface decoration using uniformly dispersed Ag metallic nanoparticles of about 4 nm at concentration of n = 0.5 to 2.5 wt% and those of 10–20 nm larger at a higher concentration than 1 wt%. The structure of the prepared composites was characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), atomic force microscopy (AFM), Raman and X-ray photoelectron spectroscopy (XPS). Optical properties were determined using UV-vis spectroscopy. Six polymer solar cells with modification by an TiO2/n-Ag hole transporting layer were manufactured and studied under AM 1.5G-simulated solar illumination (100 mW cm−2). The best performance was obtained for a device with the ITO/(PEDOT:PSS):1.5%Ag in TiO2/P3HT:PCBM/Al architectures. Under these conditions, a PCE of 2.07% with open circuit voltage Voc = 0.612 V, short circuit current density Jsc = 5.94 mA cm−2, and fill factor FF = 0.57 was achieved. Additionally, devices were tested by electrochemical impedance spectroscopy under illumination and a well-fitted equivalent circuit was proposed. Finally, our idea of the linkage of TiO2/n-Ag with PEDOT:PSS and P3HT in the constructed devices taking into account the amount of Ag in TiO2 was proposed.
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