We demonstrate experimental data to elucidate the reason for the discrepancies of reported band gap energy (Eg) of Cu2ZnSnSe4 (CZTSe) thin films, i.e., 1.0 or 1.5 eV. Eg of the coevaporated CZTSe film synthesized at substrate temperature (Tsub) of 370 °C, which was apparently phase pure CZTSe confirmed by x-ray diffraction (XRD) and Raman spectroscopy, is found to be around 1 eV regardless of the measurement techniques. However, depth profile of the same sample reveals the formation of ZnSe at CZTSe/Mo interface. On the other hand, Eg of the coevaporated films increases with Tsub due to the ZnSe formation, from which we suggest that the existence of ZnSe, which is hardly distinguishable from CZTSe by XRD, is the possible reason for the overestimation of overall Eg.

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CuInSe2 (CIS) absorber layer was formed by a direct nonvacuum coating and a subsequent selenization of precursor solutions of Cu(NO3)2 and InCl3 dissolved in methanol. The viscosity of precursor solutions was adjusted by adding ethyl-cellulose (EC) to be suitable for the doctor-blade coating. During the coating and drying process Cu2+ ions in the starting solution were reduced to Cu+, resulting in precursor films consisting of CuCl crystals and amorphous In compound embedded in EC matrix. Selenization of the precursor films with Se vapor at elevated temperature generated double-layered films with an upper layer of chalcopyrite CIS and a carbon residue bottom layer. Significant In loss was observed during the selenization, which was attributed to the evaporation of the In2Se binary phase, confirmed by investigating the change in the Cu/In ratio of the selenized film as a function of Se flux and substrate temperature. As a proof-of-concept, thin film solar cells were fabricated with the double-layered absorber film and the devices exhibited reproducible conversion efficiency as high as about 2%.

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