Aurivillius Halide Perovskite: A New Family of Two-Dimensional Materials for Optoelectronic Applications

Abstract

Layered perovskites have attracted considerable attention in optoelectronic applications due to their excellent electronic properties and stability. In this work, the quasi-2D aurivillius halide perovskites are investigated using density functional theory. The single-layer aurivillius perovskite Ba2PbI6 is predicted to have a direct bandgap of 1.89 eV, which is close to that of the Ruddlesden–Popper perovskite Cs2PbI4. The electronic structures near the Fermi level are mainly governed by the [PbX6] octahedra, which leads to similar electronic properties to that of Cs2PbI4. Decomposition energies reveal that these aurivillius perovskites exhibit thermal instability. Increasing the number of [PbX6] octahedra layer can enhance the stability and reduce the bandgap. Bi- and In-based aurivillius perovskites are also calculated to evaluate the Pb-free alternatives. These calculations can serve as a theoretical support in exploring novel layered perovskites.<br>

Navigating the Site-Distinct Energy Conversion Properties of Perovskite Quantum Wells

“…To the best of our knowledge, guanidinium (Gua + ) is the only cation reported to form the ACI 2D HP structure, 13 and the Aurivillius type HP has only been predicted but never experimentally obtained. 14 The hydrophobic spacer molecules in 2D HPs assemble into atomically dense layers to cap the HP skeleton so that moisture could be effectively isolated. Besides, the spacers couple to each other with van der Waals interaction, which further reduces the Gibbs energy of the entire 2D HP system.…”

2D Graphene-Like Pb-Free Perovskite Semiconductor CsSb(Br1–xIx)4 with Quasi-linear Electronic Dispersion and Direct Bandgap Close to Germanium

“…Generally, perovskites show a 3D structure (AMX 3 ) or five 2D layered structures, which include the Ruddlesden−Popper (RP) phase (A′ 2 [A n − 1 M n X 3 n + 1 ]), Dion−Jacobson (DJ) phase ( A ′ [ A n − 1 M n X 3 n + 1 ] ) , A u r i v i l l i u s ( A V ) p h a s e (A′ 2 X 2 [A n−1 M n X 3n+1 ]), 111 phase (A′ 2 A n−1 M n X 3n+3 ), and 110 phase (A n M n X 3n+2 ) (n = positive integer). 13 Here, A′ and A are 12-coordinated organic or inorganic cations with a large ionic radius. M represents the nontoxic metal cation with a stable valence, which is the central ion adopting a six-coordination number and forming an [MX 6 ] octahedral geometry, where X is a halogen or chalcogen anion.…”

Understanding of Layer-Dependent Stability and Rashba Spin Splitting of Two-Dimensional Organic–Inorganic Halide Perovskites α-FABX3 (B = Ge, Sn, and Pb; X = Cl, Br, and I)

“…Furthermore, it is also crucial to find ways to effectively manipulate the Rashba effect of perovskites for their optoelectronic applications, such as applying strain, electric field, lattice vibrations, and composition engineering. 24,28,29 In this work, we carry out a systematically theoretical study on the 2D Ruddlesden−Popper (RP) phase of α-FABX 3 perovskites, 30 in the form of FA n+1 B n X 3n+1 , from first-principles using density functional theory (DFT) calculations. reveals the physics behind the experimental observations that the stability of 2D FAX-terminated α-FABX 3 perovskites is enhanced as the number of layers decrease.…”