一维[(CH3)2NH2]PbI3 Hybrid Perovskite 中的强电子-鹭鸶耦合和晶格动力学

A. Nonato, Juan S. Rodríguez-Hernández, D. S. Abreu, C. C. S. Soares, Mayra A. P. Gómez, Alberto García-Fernández, María A. Señarís-Rodríguez, Manuel Sánchez andújar, A. P. Ayala, C. W. A. Paschoal, Rosivaldo Xavier da Silva
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Particularly, DMAPbI3 has attracted attention due to other\ninteresting behaviors and properties, such as thermally induced order-disorder\nprocesses, dielectric transition, and cooperative electric ordering of DMA\ndipole moments. In this paper, we investigated the interplay between\nlow-temperature SPT undergone by the low-dimensional (1D) hybrid halide\nperovskite-like material DMAPbI3 and its optoelectronic properties. Our\napproach combines synchrotron X-ray powder diffraction, Raman spectroscopy,\nthermo-microscopy, differential scanning calorimetry (DSC), and\nphotoluminescence (PL) techniques. Temperature-dependent Synchrotron powder\ndiffraction and Raman Spectroscopy reveal that the modes associated with I-Pb-I\nand DMA+ ion play a crucial role in the order-disorder SPT in DMAPbI3. The\nreversible SPT modifies its optoelectronic properties, notably affecting its\nthermochromic behavior and PL emission. 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引用次数: 0

摘要

混合卤化物包光体(HHPs)结合了有机-无机材料低成本高效制备方法的优点,具有显著的光电特性,因而备受关注。值得注意的是,包括二维(2D)层和一维(1D)链在内的低维混合卤化物过氧化物因其卓越的稳定性和防潮性而备受认可,这使它们在实际应用中极具吸引力。尤其是 DMAPbI3 由于其他有趣的行为和性质,如热诱导的有序-无序过程、介电常数转变和 DMA 双极矩的协同电有序化而备受关注。在本文中,我们研究了低维(1D)混合卤代磷灰石类物质 DMAPbI3 经历的低温 SPT 与其光电特性之间的相互作用。我们的研究方法结合了同步辐射 X 射线粉末衍射、拉曼光谱、热显微镜、差示扫描量热法(DSC)和光致发光(PL)技术。与温度相关的同步辐射粉末衍射和拉曼光谱显示,与 I-Pb-I 和 DMA+ 离子相关的模式在 DMAPbI3 的有序-无序 SPT 中起着关键作用。可逆的 SPT 改变了其光电特性,尤其影响了其hermochromic 行为和 PL 发射。聚光现象的起源与自俘获激子(STEs)有关,这种自俘获激子是通过黄-瑞斯因子(Huang-Rhys factor,S = 97+-1)量化的强电子-声子耦合作用产生的。我们的研究结果表明,这些 STE 不仅在较低温度下增强了聚光光谱,而且还引起了颜色发射的偏移,使其从浅橙红色转变为强烈的亮红色。
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Strong Electron-Phonon Coupling and Lattice Dynamics in One-Dimensional [(CH3)2NH2]PbI3 Hybrid Perovskite
Hybrid halide perovskites (HHPs) have attracted significant attention due to their remarkable optoelectronic properties that combine the advantages of low cost-effective fabrication methods of organic-inorganic materials. Notably, low-dimensional hybrid halide perovskites including two-dimensional (2D) layers and one-dimensional (1D) chains, are recognized for their superior stability and moisture resistance, making them highly appealing for practical applications. Particularly, DMAPbI3 has attracted attention due to other interesting behaviors and properties, such as thermally induced order-disorder processes, dielectric transition, and cooperative electric ordering of DMA dipole moments. In this paper, we investigated the interplay between low-temperature SPT undergone by the low-dimensional (1D) hybrid halide perovskite-like material DMAPbI3 and its optoelectronic properties. Our approach combines synchrotron X-ray powder diffraction, Raman spectroscopy, thermo-microscopy, differential scanning calorimetry (DSC), and photoluminescence (PL) techniques. Temperature-dependent Synchrotron powder diffraction and Raman Spectroscopy reveal that the modes associated with I-Pb-I and DMA+ ion play a crucial role in the order-disorder SPT in DMAPbI3. The reversible SPT modifies its optoelectronic properties, notably affecting its thermochromic behavior and PL emission. The origin of the PL phenomenon is associated to self-trapped excitons (STEs), which are allowed due to a strong electron-phonon coupling quantified by the Huang-Rhys factor (S = 97+-1). Notably, we identify the longitudinal optical (LO) phonon mode at 84 cm-1 which plays a significant role in electron-phonon interaction. Our results show these STEs not only intensify the PL spectra at lower temperatures but also induce a shift in the color emission, transforming it from a light orange-red to an intense bright strong red.
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