Electronic and Optical Properties of van der Waals Heterostructures Based on Two-Dimensional Perovskite (PEA)₂PbI₄ and Black Phosphorus

Abstract

Combining two-dimensional (2D) perovskites with other 2D materials to form a van der Waals (vdW) heterostructure has emerged as an intriguing way of designing electronic and optoelectronic devices. The structural, electronic, and optical properties of the 2D (PEA) 2 PbI 4 /black phosphorus (BP) [PEA:(C 4 H 9 NH 3 ) + ] vdW heterostructure have been investigated using first-principles calculations. We found that the (PEA) 2 PbI 4 /BP heterostructure shows a high stability at room temperature. It is demonstrated that the (PEA) 2 PbI 4 /BP heterostructure exhibits a type-I band arrangement with high carrier mobility. Moreover, the band gap and band offset of (PEA) 2 PbI 4 /BP can be effectively modulated by an external electric field, and a transition from semiconductor to metal is observed. The band edges of (PEA) 2 PbI 4 and BP in the (PEA) 2 PbI 4 /BP heterostructure, which show significant changes with the external electric field, provide further support. Furthermore, the BP layers can enhance the light absorption of the (PEA) 2 PbI 4 /BP heterostructures. Our results indicate that the 2D perovskite and BP vdW heterostructures are competitive candidates for the application of low-dimensional photovoltaic and optoelectronic devices.

Two Dimensional Perovskites/Transition Metal Dichalcogenides Heterostructures: Puzzles and Challenges

“…Similar to the case of perovskite solar cells, [84] the development of optoelectronic devices based on 2DP/TMD stacks significantly outpaced the understanding of their fundamental properties. Despite successful demonstrations of photodetectors or photovoltaic devises based on van der Waals heterostructures composed of 2DPs and TMDs or other layered materials, [23,24,27,[85][86][87][88][89] still very little is know about the fundamental mechanisms standing behind their operation. Most published work focuses on the device performance and only a few publications attempt to provide a more detailed understanding of the photophysics, excitation transfer mechanism and mutual impact of the layers.…”

Impact of AlOx Dielectric Layer on Performance in Two-Dimensional Perovskite Photovoltaic Devices

“…Photovoltaic devices based on ITO/NiO x /perovskite/PCBM/Al structure are fabricated to explore the influence of AlO x layer at Al/PCBM interface on device performance. The commonly studied 2D perovskite (PEA) 2 PbI 4 with excellent stability is used in this work (Figure S4a shows the band gap) . Detailed experimental procedures can be found in the experimental section of the Supporting Information.…”

“…The commonly studied 2D perovskite (PEA) 2 PbI 4 with excellent stability is used in this work (Figure S4a shows the band gap). 41 Detailed experimental procedures can be found in the experimental section of the Supporting Information. The J−V curve of the 2D perovskite photovoltaic device under 1.5 AM filter with an irradiation intensity of 100 mW/cm 2 is shown in Figure S4b.…”

Defect-Induced Inhomogeneous Phase Transition in 2D Perovskite Single Crystals at Low Temperatures

“… 1 − 3 Compared to their three-dimensional (3D) analogues, layered 2D perovskites exhibit better moisture resistance, higher photostability, larger exciton binding energies, and tunable bandgaps due to the presence of the hydrophobic and length-adjustable organic ligands. 1 − 10 These properties make 2D perovskites display great potential in the fabrication of solar cells, light-emitting diodes, and other optoelectronic devices. 11 − 16 …”

“…Two-dimensional (2D) layered Ruddlesden–Popper lead-halide perovskites are a class of semiconductor materials with a general formula of (RNH 3 ) 2 (A) n −1 M n X 3 n +1 , where RNH 3 + is an ammonium cation with a long hydrophobic side chain, A + is a small cation like CH 3 NH 3 + , M 2+ is a metal cation, and X – is a halide anion. They are naturally formed multiple-quantum wells, which are composed of n layers of lead halide octahedrons segregated by insulating ligands. − Compared to their three-dimensional (3D) analogues, layered 2D perovskites exhibit better moisture resistance, higher photostability, larger exciton binding energies, and tunable bandgaps due to the presence of the hydrophobic and length-adjustable organic ligands. − These properties make 2D perovskites display great potential in the fabrication of solar cells, light-emitting diodes, and other optoelectronic devices. − …”