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DOI | 10.1038/s41467-018-05313-2 |
Competition between proton transfer and intermolecular Coulombic decay in water | |
Richter, Clemens1; Hollas, Daniel2; Saak, Clara-Magdalena3; Foerstel, Marko4,7; Miteva, Tsveta5; Mucke, Melanie3; Bjorneholm, Olle3; Sisourat, Nicolas5; Slavicek, Petr2; Hergenhahn, Uwe1,6 | |
2018-11-26 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2018 |
卷号 | 9 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Czech Republic; Sweden; France |
英文摘要 | Intermolecular Coulombic decay (ICD) is a ubiquitous relaxation channel of electronically excited states in weakly bound systems, ranging from dimers to liquids. As it is driven by electron correlation, it was assumed that it will dominate over more established energy loss mechanisms, for example fluorescence. Here, we use electron-electron coincidence spectroscopy to determine the efficiency of the ICD process after 2a(1) ionization in water clusters. We show that this efficiency is surprisingly low for small water clusters and that it gradually increases to 40-50% for clusters with hundreds of water units. Ab initio molecular dynamics simulations reveal that proton transfer between neighboring water molecules proceeds on the same timescale as ICD and leads to a configuration in which the ICD channel is closed. This conclusion is further supported by experimental results from deuterated water. Combining experiment and theory, we infer an intrinsic ICD lifetime of 12-52 fs for small water clusters. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000451176100013 |
WOS关键词 | GAUSSIAN-BASIS SETS ; RELAXATION PROCESSES ; LIQUID WATER ; ELECTRON ; FRAGMENTATION ; IONIZATION ; DYNAMICS ; AMMONIA ; PHOTOEMISSION |
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/203887 |
专题 | 资源环境科学 |
作者单位 | 1.Leibniz Inst Surface Engn IOM, Permoserstr 15, D-04318 Leipzig, Germany; 2.Univ Chem & Technol Prague, Dept Phys Chem, Tech 5, Prague 16628 6, Czech Republic; 3.Uppsala Univ, Dept Phys & Astron, Box 516751 20, Uppsala, Sweden; 4.Max Planck Inst Plasma Phys, Boltzmannstr 2, D-85748 Garching, Germany; 5.Sorbonne Univ, Lab Chim Phys Matiere & Rayonnement, CNRS, UMR 7614, F-75005 Paris, France; 6.Max Planck Inst Plasma Phys, Wendelsteinstr 1, D-17491 Greifswald, Germany; 7.Tech Univ Berlin, Inst Opt & Atom Phys, Hardenbergstr 36, D-10623 Berlin, Germany |
推荐引用方式 GB/T 7714 | Richter, Clemens,Hollas, Daniel,Saak, Clara-Magdalena,et al. Competition between proton transfer and intermolecular Coulombic decay in water[J]. NATURE COMMUNICATIONS,2018,9. |
APA | Richter, Clemens.,Hollas, Daniel.,Saak, Clara-Magdalena.,Foerstel, Marko.,Miteva, Tsveta.,...&Hergenhahn, Uwe.(2018).Competition between proton transfer and intermolecular Coulombic decay in water.NATURE COMMUNICATIONS,9. |
MLA | Richter, Clemens,et al."Competition between proton transfer and intermolecular Coulombic decay in water".NATURE COMMUNICATIONS 9(2018). |
条目包含的文件 | 条目无相关文件。 |
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