Tunable Bandgap in Cobalt-Doped FeS₂ Thin Films for Enhanced Solar Cell Performance

Cobalt-doped iron disulfide (FeS₂) thin films were synthesized via chemical bath deposition (CBD) followed by annealing at 450 °C, yielding phase-pure pyrite structures with multifunctional properties. A deposition temperature of 95 °C is critical for promoting Co incorporation, suppressing sulphur vacancies, and achieving structural stabilization of the film. After annealing, the dendritic morphologies transformed into compact quasi-spherical nanoparticles (~100 nm), which enhanced the crystallinity and optoelectronic performance of the films. The films exhibited strong absorption (>50%) in the visible and near-infrared regions and tunable direct bandgaps (1.14 to 0.96 eV, within the optimal range for single-junction solar cells. Electrical characterization revealed a fourth-order increase in conductivity after annealing (up to 4.78 Ω^-1 cm^-1) and confirmed stable p-type behavior associated with Co²⁺-induced acceptor states and defect passivation. These results demonstrate that CBD enabled the fabrication of Co-doped FeS₂ thin films with synergistic structural, electrical, and optical properties. The integration of earth-abundant elements and tunable electronic properties makes these films promising absorber materials for the next-generation photovoltaic devices.