An inherent instability study using ab initio computational methods and experimental validation of Pb(SCN) 2 based perovskites for solar cell applications.

Perovskite materials with ABX ₃ chemistries are promising candidates for photovoltaic applications, owing to their suitable optoelectronic properties. However, they are highly hydrophilic and unstable in nature, limiting the commercialization of perovskite photovoltaics. Mixed halide ion-doped perovskites are reported to be more stable compared to simple ABX ₃ chemistries. This paper describes ab initio modeling, synthesis, and characterization of thiocyanate doped lead iodide CH ₃ NH ₃ PbI _(3-x) (SCN) _x perovskites. Several perovskite chemistries with an increasing concentration of (SCN) ^- at x = 0, 0.25, 0.49, 1.0, 1.45 were evaluated. Subsequently, 'n-i-p' and 'p-i-n' perovskite solar device architectures, corresponding to x = 0, 0.25, 0.49, 1.0 thiocyanate doped lead halide perovskite chemistry were fabricated. The study shows that among all the devices fabricated for different compositions of perovskites, p-i-n perovskite solar cell fabricated using CH ₃ NH ₃ PbI _(3-x) (SCN) _x perovskite at x = 1.0 exhibited the highest stability and device efficiency was retained until 450 h. Finally, a solar panel was fabricated and its stability was monitored.