Wang Ailin, Zhang Chengshu, Guan Qianwen, Ye Huang, Li Ruiqing, Li Hang, Geng Yaru, Qu Chang, Wang Zirui, Ji Chengmin, Luo Junhua
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Mater, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.
College of Chemistry and Materials Science, Fujian Normal University, Fuzhou, Fujian, 350007, China.
Small. 2024 Nov 27:e2407843. doi: 10.1002/smll.202407843.
Polar 3D organic-inorganic hybrid perovskites (OIHPs) with the bulk photovoltaic effect (BPVE) have important application value in self-driven X-ray detection, due to their excellent semiconductor properties. However, A-site cations are limited by the tolerance factor, making it difficult to construct ABX-type polar 3D perovskites. Therefore, it is necessary to explore polar 3D perovskitiods with excellent semiconductor properties for self-driven X-ray detection. Herein, by introducing an asymmetric diamine 3-methylaminopropylamine (3-MAPA) cation, a polar 3D perovskitiod, (3-MAPA)PbBr (1) is successfully constructed. Specifically, the dipole-oriented arrangement and intrinsic polarity of 3-MAPA cations endow a non-centrosymmetric structure of 1 single crystal (SC). Notably, under X-ray irradiation, the polar 1 SC exhibits a remarkable bulk photovoltaic of 0.8 V, which is beneficial for self-driven X-ray detection. Consequently, the 1-based detector shows a sensitivity of 101 µC Gy s and a low detection limit of 189 nGy s at 0 V bias. Meanwhile, 1 SC-based X-ray detector exhibits less ion migration due to the abundant N─H···Br hydrogen bonding interaction within the structure, leading to a smaller dark current drift, which supports stable X-ray detection. This study attains stable self-driven X-ray detection based on polar 3D perovskitiods, which enriches the candidates for self-driven X-ray detectors.
具有体光伏效应（BPVE）的极性三维有机-无机杂化钙钛矿（OIHPs）因其优异的半导体性能在自驱动X射线检测中具有重要的应用价值。然而，A位阳离子受容差因子限制，难以构建ABX型极性三维钙钛矿。因此，有必要探索具有优异半导体性能的极性三维类钙钛矿用于自驱动X射线检测。在此，通过引入不对称二胺3-甲基氨基丙胺（3-MAPA）阳离子，成功构建了一种极性三维类钙钛矿（3-MAPA）PbBr（1）。具体而言，3-MAPA阳离子的偶极取向排列和固有极性赋予了单晶（SC）1非中心对称结构。值得注意的是，在X射线照射下，极性的1 SC表现出0.8 V的显著体光伏，这有利于自驱动X射线检测。因此，基于1的探测器在0 V偏压下显示出101 µC Gy s的灵敏度和189 nGy s的低检测限。同时，基于1 SC的X射线探测器由于结构内丰富的N─H···Br氢键相互作用而表现出较少的离子迁移，导致较小的暗电流漂移，从而支持稳定的X射线检测。本研究实现了基于极性三维类钙钛矿的稳定自驱动X射线检测，丰富了自驱动X射线探测器的候选材料。
