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A facile improved successive ionic-layer adsorption and reaction (SILAR) sequence is described for the fabrication of Cu 2 ZnSn(S,Se) 4 (CZTSSe) thin-film solar cells (TFSCs) via the selenization of a precursor film. The precursor films were fabricated using a modified SILAR sequence to overcome compositional inhomogeneity due to different adsorptivities of the cations (Cu + , Sn 4+ , and Zn 2+ ) in a single cationic bath. Rapid thermal annealing of the precursor films under S and Se vapor atmospheres led to the formation of carbon-free Cu 2 ZnSnS 4 (CZTS) and CZTSSe absorber layers, respectively, with single large-grained layers. The best devices based on CZTS and CZTSSe absorber layers showed total area (∼0.30 cm 2 ) power conversion efficiencies (PCEs) of 1.96 and 3.74%, respectively, which are notably the first-demonstrated efficiencies using a modified SILAR sequence. Detailed diode analyses of these solar cells revealed that a high shunt conductance ( G  sh ), reverse saturation current density ( J  o ), and ideality factor ( n  d ) significantly affected the PCE, open-circuit voltage ( V  oc ), and fill factor (FF), whereas the short-circuit current density ( J  sc ) was dominated by the series resistance ( R  s ) and G  sh . However, the diode analyses combined with the compositional and interface microstructural analyses shed light on further improvements to the device efficiency. The facile layer-by-layer growth of the kesterite CZTS-based thin films in aqueous solution provides a great promise as an environmentally benign pathway to fabricate a variety of multielement-component compounds with high compositional homogeneities.

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Aqueous-Solution-Processed Cu<sub>2</sub>ZnSn(S,Se)<sub>4</sub> Thin-Film Solar Cells via an Improved Successive Ion-Layer-Adsorption–Reaction Sequence

Aqueous-Solution-Processed Cu2ZnSn(S,Se)4 Thin-Film Solar Cells via an Improved Successive Ion-Layer-Adsorption–Reaction Sequence

Aqueous-Solution-Processed Cu₂ZnSn(S,Se)₄ Thin-Film Solar Cells via an Improved Successive Ion-Layer-Adsorption–Reaction Sequence