In this study, we developed an ink using hexanethiol and Cu(In,Ga)Se2 microcrystals (CIGSe MCs) to make thin films via doctor blade coating. Besides, crack-free thin films were obtained by optimizing CIGSe MC powder concentration and annealing temperature. Subsequently, single-step selenization was performed with and without sodium chloride (NaCl) surface treatment by carefully tuning the temperature. A crack-free surface with densely packed grains was obtained at 500 °C after NaCl treatment. Moreover, the structural parameters of the thin film (annealed at 350 °C) were significantly modified via selenization with NaCl at 500 °C. For instance, the FWHM of the prominent (112) plane reduced from 1.44° to 0.47°, the dislocation density minimized from 13.10 to 1.40 × 1015 lines per m2, and the microstrain decreased from 4.14 to 1.35 × 10-3. Remarkably, these thin films exhibited a high mobility of 26.7 cm2 V-1 s-1 and a low resistivity of 0.03 Ω cm. As a proof of concept, solar cells were engineered with a device structure of SLG/Mo/CIGSe/CdS/i-ZnO/Al-ZnO/Ag, wherein a power conversion efficiency (PCE) of 5.74% was achieved with exceptional reproducibility. Consequently, the outcomes of this investigation revealed the impact of selenization temperature and NaCl treatment on the physical properties and PCE of hexanethiol-based crack-free CIGSe MC ink-coated absorbers, providing new insights into the groundwork of cost-effective solar cells.
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