Structural Disorder in Layered Hybrid Halide Perovskites: Types of Stacking Faults, Influence on Optical Properties and Their Suppression by Crystallization Engineering

Layered hybrid halide perovskites (LHHPs) are an emerging type of semiconductor with a set of unique optoelectronic properties. However, the solution processing of high-quality LHHPs films with desired optical properties and phase composition is a challenging task, possibly due to the structural disorder in the LHHP phase. Nevertheless, there is still a lack of experimental evidence and understanding of the nature of the structural disorder in LHHPs and its influence on the optical properties of the material. In the current work, using 2D perovskites (C4H9NH3)(2)(CH3NH3)(n-1)PbnI3n+1 (further BA(2)MA(n-1)Pb(n)I(3n+1)) with n = 1-4 as a model system, we demonstrate that deviations in LHHPs optical properties and X-ray diffraction occur due to the presence of continuous defects-Stacking Faults (SFs). Upon analyzing the experimental data and modeled XRD patterns of a possible set of stacking faults (SFs) in the BA(2)MAPb(2)I(7) phase, we uncover the most plausible type of SFs, featured by the thickness variation within one perovskite slab. We also demonstrate the successful suppression of SFs formation by simple addition of BAI excess into BA(2)MA(n-1)Pb(n)I(3n+1) solutions.

Automated summary

The optical properties and X-ray diffraction of layered hybrid halide perovskites deviate due to the presence of continuous defects known as stacking faults. These stacking faults can be suppressed by adding excess BAI into the solutions.