Nanoparticle-Induced Grain Growth of Carbon-Free Solution-Processed CuIn(S,Se)₂ Solar Cell with 6% Efficiency

Chalcopyrite-based solar cell deposited by solution processes is of great research interest because of the ease of fabrication and cost effectiveness. Despite the initial promising results, most of the reported methods encounter challenges such as limited grain growth, carbon-rich interlayer, high thermal budget, and the presence of secondary Cu-rich phases, which limit the power conversion efficiency (PCE). In this paper, we develop a new technique to deposit large grain, carbon-free CISSe absorber layers from aqueous nanoparticle/precursor mixture which resulted in a solar cell with PCE of 6.2%. CuCl2, InCl3, and thiourea were mixed with CuS and In2S3 nanoparticles in water to form the unique nanoparticle/precursor solution. The Carbon layer formation was prevented because organic solvents were not used in the precursor. The copper-rich (CuS) nanoparticles were intentionally introduced as nucleation sites which accelerate grain growth. In the presence of nanoparticles, the grain size of CISSe film increased by a factor of 7 and the power conversion efficiency of the solar cell is 85% higher than the device without nanoparticle. This idea of using nanoparticles as a means to promote grain growth can be further exploited for other types of chalcopyrite thin film deposited by solution methods.