Optimization of CuInGaS Nanoparticles and Their Application in the Hole-Transporting Layer of Highly Efficient and Stable Mixed-Halide Perovskite Solar Cells.

Inorganic hole-transport materials (HTMs) have been frequently applied in perovskite solar cells (PSCs) and are a promising solution to improve the poor stability of PSCs. In this study, we investigate solution-processed copper indium gallium disulfide (CIGS) nanocrystals (NCs) as a dopant-free inorganic HTM in n-i-p type PSCs. Moreover, Cs(MA-FA)Pb(IBr) mixed-halide perovskite with proper crystalline quality and long-time stability was utilized as the light-absorbing layer under ambient conditions. To optimize the cell performance and better charge extraction from the perovskite layer, the Ga concentration in the Cu(InGa)S composition was changed, and the value was altered between 0.0 and 0.75. It was shown that the CIGS band gap enhances with increasing Ga content; thus, with tunable band gaps and engineering of the energy level alignment, a better collection of photogenerated holes and a reduced electron-hole recombination rate could be achieved. The maximum power conversion efficiency of 15.6% was obtained for the PSC with Cu(InGa)S hole-transport layer composition, which is the highest efficiency reported so far for CIGS-based dopant-free PSCs. This value is very close to the efficiency of devices fabricated with doped spiro-OMeTAD as an organic HTM. Additionally, the stability of nonencapsulated PSCs was studied, and CIGS-based devices demonstrated 70% retention after 90 days of aging in the dark and in 50% relative humidity conditions. This result is quite better than the similar measurements for the doped spiro-OMeTAD-based devices.