Layered/3D Halide Hybrid Perovskite Semiconductors: Advances and Promises
Résumé
Layered halide hybrid organic–inorganic perovskites (HOP) have been intensively studied in the past for applications in optoelectronics and microelectronics before the rise of three-dimensional (3D) HOP and their impressive performance in solar cells. Recently, layered HOP have also been proposed as attractive alternatives for photostable solar cells and revisited for light-emitting devices. The ability to modify the composition and shape of these hybrid heterostructures allows tuning quantum and dielectric confinements of charge carriers. These effects are of prime importance for photovoltaic and optoelectronic applications.
We combine classical solid-state physics concepts with atomistic codes based on the density functional theory to analyze the optoelectronic properties of layered HOP. A detailed comparison between layered and 3D HOP is performed to highlight differences and similarities. It allows for thorough analysis of the spin–orbit coupling effects and structural transitions with corresponding electronic band structure folding. We further investigate the effects of octahedral tilting on the band gap, the loss of inversion symmetry and the related Rashba effect, the quantum confinement, the dielectric confinement related to the organic barrier and finally to the excitonic properties. Finally, our study provides an interpretive and predictive framework for the optoelectronic properties of 3D and 2D layered HOP.