In this work, we achieve the preparation of nontoxic and earth-abundant chalcopyrite quaternary compound CuAl (1−X) Fe X S 2 thin films by substituting Al with Fe atoms for photovoltaic application. The present work reports tuning the properties of CuAl (1−X) Fe X S 2 (X = 0, 0.25, 0.50, 0.75, and 1) thin films using the chemical spray pyrolysis technique. The polycrystalline tetragonal crystal structure of the prepared film is confirmed by X-ray diffraction analysis. The Fe-substituted film shows high optical absorption in the visible region compared to pure CuAlS 2 . The optical energy band gap of the material decreases from 3.07 eV (X = 0) to 1.39 eV (X = 1) with a linear increase in Fe concentration. The SEM images show the spherical and microflake-like morphological structure. From I−V measurement, a good ohmic response is observed for all the samples. All the films display single semicircle impedance nature, and lower electrical resistivity is obtained for CuAl 0.25 Fe 0.75 S 2 and CuFeS 2 thin films. The photovoltaic performance of CuAl 0.25 Fe 0.75 S 2 and CuFeS 2 solar cells is evaluated, and efficiencies of 3.65 and 2.33%, respectively, are obtained. The above mentioned results confirm that the CuAl 0.25 Fe 0.75 S 2 composition exhibits good optical, morphological, and electrical properties which have potential application prospect in photovoltaic technology.
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