Edge States in 2D A2PbBr4 Hybrid Perovskites Enabled by Local Structural Reorganization

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-05-30 DOI:10.1002/adma.202419606

Zhi‐Gang Li, Xiang Li, Xiao‐Hui Dong, Hai‐Peng Song, Zi‐Ying Li, Xiang Wu, Ilya Kupenko, Michael Hanfland, Konstantin Glazyrin, Jacky Even, Wei Li, Xian‐He Bu

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Abstract

The edge states (ES) in two‐dimensional (2D) hybrid lead halide perovskites (LHPs) exhibit distinct electronic characteristics, including lower energy and longer lifetimes compared to the interior states (IS). Though the ES of these 2D LHPs show prospect of facilitating photovoltaic and optoelectronic effects, the underlying mechanism remains elusive. Here, the occurrence of ES in a family of 2D A2PbBr4 (A = organic amine cation) LHPs is attributed to the Rashba/Dresselhaus (RD) spin splitting induced by local structural reorganization on the crystal edge. The experimental and theoretical characterizations reveal that the local structure on the crystal edge is significantly strained, which leads to considerable out‐of‐plane distortion of adjacent PbBr6 octahedra, local loss of inversion symmetry and therefore spin‐splitting energy required for the formation of ES. This findings contribute fresh perspectives to the fundamental comprehension of the RD effect, extending the boundaries of spintronics and opening promising pathways for the conceptualization and refinement of devices centered on ES.

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局部结构重组激活二维A2PbBr4杂化钙钛矿的边缘态

二维（2D）杂化卤化铅钙钛矿（LHPs）的边缘态（ES）表现出明显的电子特性，包括比内部态（IS）更低的能量和更长的寿命。虽然这些二维lhp的ES具有促进光伏和光电子效应的前景，但其潜在机制尚不清楚。本文中，2D A2PbBr4 （a =有机胺阳离子）LHPs家族中ES的发生归因于晶体边缘局部结构重组引起的Rashba/Dresselhaus （RD）自旋分裂。实验和理论表征表明，晶体边缘的局部结构受到了明显的应变，导致相邻PbBr6八面体出现相当大的面外畸变，局部反演对称性损失，从而导致形成ES所需的自旋分裂能损失。这一发现为对RD效应的基本理解提供了新的视角，扩展了自旋电子学的边界，并为以ES为中心的设备的概念化和改进开辟了有希望的途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.