Predicted Lead-Free Perovskites for Solar Cells

Organic–inorganic halide perovskites are quite promising in applications of large scale photovoltaic technology. However, toxicity is one of the crucial issues in these materials, and searching for environmentally friendly perovskite materials for green energy applications is in high demand. Here we present a systematic ab initio study on the replacement of toxic Pb in the perovskite CH3NH3PbI3 (MAPbI3) with possible mono- and a few binary replacements. In the mono-replacements study, Ge and Sn are the best alternatives to Pb. In the binary replacements, we replace Pb by mixing Ca/Si and Zn/Si. In case of Ca/Si, a monotonic decrease in band gaps with a monotonic increase in the optical absorption was observed with increasing the Ca concentration. It is observed for the first time that the substitution of Ca/Si (or Zn/Si) at the B-site with various ratios would lead to remarkably high device absorption efficiencies. The band gaps of the studied mixed replacements are in the ideal ranges for single-junction...