Theoretical Selection of 2D Perovskite for Constructing Efficient Heterojunction Solar Cells

Abstract

Two-dimensional (2D) metal halide perovskites can co-construct with the state-of-the-art three-dimensional (3D) perovskite analogs to form 2D/3D perovskite heterojunction architectures, which enables the photovoltaic devices to deliver higher energy conversion efficiency and near-commercial stability. However, the question remains as to whether any type of 2D perovskite, i.e., RP, DJ, or ACI perovskites, is workable with a 3D analog to outperform the pristine 3D perovskites. Here, we investigate the structural and electronic properties of distinct types of 2D/3D perovskite heterojunctions based on first-principles calculations. We selected a 3D FAPbI 3 perovskite combined with representative 2D RP, DJ, and ACI perovskites to construct a series of 2D/3D perovskite heterojunctions and analyzed the carrier transport kinetics and charge recombination of each heterojunction. The results indicate that RP-PbI, DJ-FAI, and ACI-FAI heterojunctions exhibited favorable transport and separation of photogenerated carriers, but the RP-PbI and ACI-FAI heterojunctions appear to possess greater potential for photovoltaic applications than the DJ-FAI heterojunction due to relatively fewer recombination losses. Moreover, based on the direction of photogenerated carrier transport at the heterojunction, we predict that RP-PbI would be superior to DJ-FAI for conventional 2D/3D devices and that the ACI-FAI heterojunction is expected to well function in the inverted 2D/3D devices.

An investigation using DFT into the impact of hydrogen on oxygen migration processes during aluminum anodization

“…29 Density functional theory (DFT) has been the most effective tool in condensed matter physics for computing electronic structure and its properties since its inception in the 1960s, when it was initially used to derive the well-known Kohn-Sham (KS) equation under the local density approximation (LDA). Numerous atomic and molecular physics puzzles, including those involving catalytic active sites, 30,31 geometric structure, 32,33 and material electronic structure properties, 34,35 can be resolved with DFT. DFT is also commonly used to calculate the functions of the ions during chemical reactions, 36,37 as it can accurately reveal reaction pathways clearly.…”

High responsivity VIS-NIR photodetector based on (PEA)2PbI4/P3HT heterojunction

“…The 2D RP perovskite material has the general chemical formula A 2 B n−1 M n X 3n+1 [11], (A is a long aliphatic or aromatic alkylammonium cation, B is MA + (CH 3 NH 3 + ), Cs + , or FA + (NH 2 CH 3 NH 3 + ), M is Pb 2+ or Sn 2+ , and X is Cl − , Br − , or I − , and n is the number of [MX 6 ] 4− octahedral monolayers between the A layers of the organic spacer). In the typical RP perovskite structure, the organic ligands' long and hydrophobic alkyl chains protect the inorganic layers from moisture-induced decomposition and exhibit greater stability [12,13]. Dou et al [14] prepared (PEA) 2 PbI 4 by mechanical exfoliation and combined it with graphene to build a channel to prepare a two-color blue-green photodetector, which showed excellent performance at 460 nm and 532 nm.…”

Interfacial Rivet to Fill Structural Defects: A Spacer Engineering Gift for 3D Solar Cells

“…2D perovskites have proven to be effective photovoltaic material in addressing the instability and efficiency issues of PSCs. [ 2,7–9 ] Owing to the presence of organic spacers in their unique structure, 2D perovskites exhibit excellent long‐term stability, the ability to suppress ion migration, and larger formation energy. In addition, 2D perovskites integrate inorganic skeletons and organic molecules to form a natural 2D framework, which can be regarded as a natural quantum well [ 10 ] with adjustable structure and properties [ 11 ] leading to superior electrical and optical characteristics.…”