Layered hybrid organic-inorganic halide perovskites (OIHPs) are receiving increased attention for optoelectronic applications, including photovoltaics, light-emitting diodes, and nonlinear optics. However, investigations on the effects of incorporating a larger chromophore as the ammonium cation in the two-dimensional (2D) OIHP inorganic framework are mostly lacking. To elucidate the role of the organic cation type in tuning the optical properties, we studied herein 2D OIHPs with 14 organic cations, which range from aliphatic molecules to chromophores, by a first-principles analysis. We examined the effects of the structural distortion in the 2D OIHPs, which is correlated to the band gaps in some cases. Band alignments indicated variability in the quantum-well types and were modified for organic cations with functional groups, as compared to the more inert cations. The absorption spectra demonstrated tunability in the optical response, including enhanced absorption. The absorption spectrum for a two-layer OIHP incorporating a cyanostilbene derivative was qualitatively consistent with experimental data. This work can provide guidelines in the choice of the organic cation in 2D OIHPs and motivate further experimental synthesis and characterization.
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Physical and Theoretical Chemistry
- Surfaces, Coatings and Films