Synthesis and characterization of earth-abundant Cu₂MnSnS₄ thin films using a non-toxic solution-based technique

Earth-abundant Cu₂MnSnS₄ (CMTS) thin films were fabricated through a non-toxic spin-coating technique. The precursor solution is based on a 2-methoxyethanol solvated thiourea complex with acetyl-acetone used as an additive agent, and the spin-coated films were post-annealed at 570 °C under a N₂ atmosphere. The influence of annealing time on the structure, composition, morphology, and optical properties of the processed precursor films has been studied in detail. We found that a longer annealing time during CMTS growth can improve the phase purity, promote the preferred orientation along the (112) direction, and enhance grain growth in the micrometer range. Film annealed for 10 min gives a pure CMTS phase, whereas other films annealed for lower and/or higher than 10 min (especially 13 min) can form secondary phases (i.e., SnS, MnS). The band gap energy is estimated as 1.63-1.18 eV for post-annealed films depending on the heat treatment, compared to 1.69 eV for as-prepared film. An efficiency of 0.49% for the device fabricated here has been achieved with an open-circuit voltage of 308.4 mV, a short-circuit current density of 4.7 mA cm^-2, and a fill factor of 33.9%. It offers a new research direction for the application of a CMTS absorber layer in low-cost solar cells.