Significant THz absorption in CH₃NH₂ molecular defect-incorporated organic-inorganic hybrid perovskite thin film

The valid strong THz absorption at 1.58 THz was probed in the organic-inorganic hybrid perovskite thin film, CH₃NH₃PbI₃, fabricated by sequential vacuum evaporation method. In usual solution-based methods such as 2-step solution and antisolvent, we observed the relatively weak two main absorption peaks at 0.95 and 1.87 THz. The measured absorption spectrum is analyzed by density-functional theory calculations. The modes at 0.95 and 1.87 THz are assigned to the Pb-I vibrations of the inorganic components in the tetragonal phase. By contrast, the origin of the 1.58 THz absorption is due to the structural deformation of Pb-I bonding at the grain boundary incorporated with a CH₃NH₂ molecular defect.