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How the Structures and Properties of Two-Dimensional Layered Perovskites MAPbI 3 and CsPbI 3 Vary with the Number of Layers.

This work aims to explore the intrinsic properties of two-dimensional (2D)-layered perovskites, (PEA)2 PbI4 (N) and Cs2 PbI4 (N), and demonstrating how their structures and properties vary with N. The results reveal that both (PEA)2 PbI4 (N) and Cs2 PbI4 (N) are direct bandgap semiconductors, their band/optical gaps and exciton-binding energies vary linearly with 1/N at N ≥ 3, and the effective masses slowly vary with N. Compared to the bulk phases, the structures of ultrathin (PEA)2 PbI4 (N) are more flexible and deformable than Cs2 PbI4 (N). The giant spin-coupling effect greatly decreases the band gaps of both 2D materials; however, it only induces the spin splitting in the bands of (PEA)2 PbI4 (N). This work suggests that the ultrathin 2D materials can be a potential candidate for nano-optoelectronic devices, and that the nanoplates with N ≥ 3 could have similar performances with bulk materials in the carrier migration and exciton separation so that they can be effectively applied in photovoltaic cells.

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