Enhanced optical absorption in two-dimensional Ruddlesden–Popper (C6H5CH2NH3)2PbI4 perovskites via biaxial strain and surface doping

Abstract

Two-dimensional Ruddlesden–Popper (2D RP) perovskites can form layered protective materials using long organic cations as “barrier” caps, which is expected to solve the problem of instability of perovskites in the working environment. In this work, we systematically studied the 2D Ruddlesden–Popper (C₆H₅CH₂NH₃)₂PbI₄ hybrid perovskites using density functional theory. The results reveal that the 2D (C₆H₅CH₂NH₃)₂PbI₄ perovskites are semiconductors with band gaps of 2.22 eV. The optical absorption peak of the 2D (C₆H₅CH₂NH₃)₂PbI₄ perovskite structure is located at 532 nm in the visible region. Interestingly, the optical absorption spectrum of the 2D (C₆H₅CH₂NH₃)₂PbI₄ perovskite structure enhanced under suitable strains. The highest optical absorption peak appears in 2D (C₆H₅CH₂NH₃)₂PbI₄ under a −2% strain, and its theoretical photoelectric conversion efficiency is 28.5%. More interestingly, the replacement of surface I atoms with Br is another ways to enhance the optical absorption spectrum of the 2D (C₆H₅CH₂NH₃)₂PbI₄ perovskite structure. The optical absorption peak blue-shifts to the high energy region, which has higher solar energy flux density than the low energy region. The good stability, tuneable band gap and excellent theoretical photoelectric conversion efficiency of the 2D (C₆H₅CH₂NH₃)₂PbI₄ perovskite structure make it a promising candidate for novel 2D hybrid perovskite based photoelectronic devices and solar cells.