Crystal and electronic structures of substituted halide perovskites based on density functional calculation and molecular dynamics

Abstract Durability of organo-lead halide perovskite are important issue for its practical application in a solar cells. In this study, using density functional theory (DFT) and molecular dynamics, we theoretically investigated a crystal structure, electronic structure, and ionic diffusivity of the partially substituted cubic MA 0.5 X 0.5 PbI 3 (MA = CH 3 NH 3 + , X = NH 4 + or (NH 2 ) 2 CH + or Cs + ). Our calculation results indicate that a partial substitution of MA induces a lattice distortion, resulting in preventing MA or X from the diffusion between A sites in the perovskite. DFT calculations show that electronic structures of the investigated partially substituted perovskites were similar with that of MAPbI 3 , while their bandgaps slightly decrease compared to that of MAPbI 3. Our results mean that partial substitution in halide perovskite is effective technique to suppress diffusion of intrinsic ions and tune the band gap.