Electron-Phonon Coupling Suppression by Enhanced Lattice Rigidity in 2D Perovskite Single Crystals for High-Performance X-Ray Detection,Advanced Materials

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Electron-Phonon Coupling Suppression by Enhanced Lattice Rigidity in 2D Perovskite Single Crystals for High-Performance X-Ray Detection
Advanced Materials ( IF 27.4 ) Pub Date : 2022-12-02 , DOI: 10.1002/adma.202208875
Bobo Zhang ₁ , Tao Zheng ₂ , Jiaxue You ₁ , Chuang Ma ₁ , Yucheng Liu ₁ , Lu Zhang ₁ , Jun Xi ₃ , Guohua Dong ₄ , Ming Liu ₄ , Shengzhong Frank Liu _{1,

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Affiliation

Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, Shaanxi Key Laboratory for Advanced Energy Devices, Shaanxi Engineering Lab for Advanced Energy Technology, International Joint Research Center of Shaanxi Province for Photoelectric Materials Science, Institute for Advanced Energy Materials, School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, 710119, China.
State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi'an, 710072, China.
Key Laboratory for Physical Electronics and Devices of the Ministry of Education & Shaanxi Key Lab of Information Photonic Technique, School of Electronic Science and Engineering, Xi'an Jiaotong University, No. 28, Xianning West Road, Xi'an, 710049, China.
The Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education & International Center for Dielectric Research, School of Electronic Science and Engineering, State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, 710049, China.
Dalian National Laboratory for Clean Energy, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of the Chinese Academy of Sciences, Beijing, 100039, China.

2D Dion−Jacobson (DJ) perovskite single crystals (PSCs) usually demonstrate better X-ray detection performance than Ruddlesden-Popper (RP) PSCs. However, the mechanism of the improved performance is still elusive. Here, by the aid of strong interactions between dimethylbiguanide (DGA) and PbI₂, a novel DJ-perovskitoid (DGA)PbI₄ is designed. From the comparison of (DGA)PbI₄ to other 2D PSCs, it is discovered that the tiniest lattice distortion and increased hydrogen bonds in the atom-scaled analysis strengthen lattice rigidity and weaken electron-phonon coupling to suppress disordered scattering of carriers, resulting in significantly improved carrier transport and stability. Therefore, high carrier mobility (78.1 cm² V⁻¹ s⁻¹) and a pronounced sensitivity of 4869.0 µC Gy_air⁻¹cm⁻² are achieved using (DGA)PbI₄, which are the best in 2D Pb-based PSC devices to date. Finally, the (DGA)PbI₄ devices exhibit good spatial resolution in X-ray imaging and excellent long-term stability to work as a promising candidate for medical diagnostics and nondestructive determination.

中文翻译：

用于高性能 X 射线检测的二维钙钛矿单晶中增强的晶格刚度抑制电子-声子耦合

二维 Dion-Jacobson (DJ) 钙钛矿单晶 (PSC) 通常表现出比 Ruddlesden-Popper (RP) PSC 更好的 X 射线检测性能。然而，改进性能的机制仍然难以捉摸。在这里，借助二甲基双胍 (DGA) 和 PbI ₂之间的强相互作用，设计了一种新型 DJ-钙钛矿 (DGA)PbI _{4 。}_{从 (DGA)PbI 4}与其他二维 PSC的比较发现，原子尺度分析中最微小的晶格畸变和增加的氢键增强了晶格刚性并削弱了电子 - 声子耦合以抑制载流子的无序散射，导致显着改善载体运输和稳定性。因此，高载流子迁移率 (78.1 cm ² V ^-1s ^{-1 ) 和 4869.0 µC Gy}_air^-1 cm ^-2的显着灵敏度是使用 (DGA)PbI ₄实现的，这是迄今为止二维铅基 PSC 器件中最好的。最后，(DGA)PbI ₄器件在 X 射线成像中表现出良好的空间分辨率和出色的长期稳定性，可作为医学诊断和无损检测的有前途的候选者。

更新日期：2022-12-02

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