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DOI | 10.1038/s41467-017-00890-0 |
Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites | |
Guo, Yinsheng1; Yaffe, Omer2; Hull, Trevor D.1; Owen, Jonathan S.1; Reichman, David R.1; Brus, Louis E.1 | |
2019-03-12 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2019 |
卷号 | 10 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Israel |
英文摘要 | Lead-halide perovskites have emerged as promising materials for photovoltaic and optoelectronic applications. Their significantly anharmonic lattice motion, in contrast to conventional harmonic semiconductors, presents a conceptual challenge in understanding the genesis of their exceptional optoelectronic properties. Here we report a strongly temperature dependent luminescence Stokes shift in the electronic spectra of both hybrid and inorganic lead-bromide perovskite single crystals. This behavior stands in stark contrast to that exhibited by more conventional crystalline semiconductors. We correlate the electronic spectra with the anti-Stokes and Stokes Raman vibrational spectra. Dielectric solvation theories, originally developed for excited molecules dissolved in polar liquids, reproduce our experimental observations. Our approach, which invokes a classical Debye-like relaxation process, captures the dielectric response originating from the incipient anharmonicity of the LO phonon at about 20 meV (160 cm(-1)) in the lead-bromide framework. We reconcile this liquid-like model incorporating thermally-activated dielectric solvation with more standard solid-state theories of the emission Stokes shift in crystalline semiconductors. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000460930600007 |
WOS关键词 | TEMPERATURE-DEPENDENCE ; ELECTRON-TRANSFER ; SINGLE-CRYSTAL ; LIFETIME ; MODEL ; RESONANCE ; EXCITONS ; CDTE ; BR |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203456 |
专题 | 资源环境科学 |
作者单位 | 1.Columbia Univ, Dept Chem, New York, NY 10027 USA; 2.Weizmann Inst Sci, Dept Mat & Interfaces, IL-76100 Rehovot, Israel |
推荐引用方式 GB/T 7714 | Guo, Yinsheng,Yaffe, Omer,Hull, Trevor D.,et al. Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites[J]. NATURE COMMUNICATIONS,2019,10. |
APA | Guo, Yinsheng,Yaffe, Omer,Hull, Trevor D.,Owen, Jonathan S.,Reichman, David R.,&Brus, Louis E..(2019).Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites.NATURE COMMUNICATIONS,10. |
MLA | Guo, Yinsheng,et al."Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites".NATURE COMMUNICATIONS 10(2019). |
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