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DOI | 10.1038/s41467-019-12491-0 |
Coherent structural trapping through wave packet dispersion during photoinduced spin state switching | |
Lemke, Henrik T.1,2; Kjaer, Kasper S.3,4,5; Hartsock, Robert1,3; van Driel, Tim B.1,4; Chollet, Matthieu1; Glownia, James M.1; Song, Sanghoon1; Zhu, Diling1; Pace, Elisabetta6; Matar, Samir F.7; Nielsen, Martin M.4; Benfatto, Maurizio6; Gaffney, Kelly J.8,9; Collet, Eric10; Cammarata, Marco10 | |
2019-10-11 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2017 |
卷号 | 8 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Switzerland; Denmark; Sweden; Italy; France |
英文摘要 | The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)(3)](2+) compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000401959300001 |
WOS关键词 | RAY-ABSORPTION SPECTROSCOPY ; CROSSOVER DYNAMICS ; FEMTOSECOND ; COMPLEXES ; CHARGE ; XANES |
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/204591 |
专题 | 资源环境科学 |
作者单位 | 1.SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA; 2.Paul Scherrer Inst, SwissFEL, CH-5232 Villigen, Switzerland; 3.Stanford Univ, PULSE Inst, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA; 4.Tech Univ Denmark, Dept Phys, Mol Movies, DK-2800 Lyngby, Denmark; 5.Lund Univ, Dept Chem Phys, Box 124, SE-22100 Lund, Sweden; 6.Lab Nazl Frascati INFN, POB 13, I-00044 Frascati, Italy; 7.Univ Bordeaux, CNRS UPR 9048, ICMCB, F-33608 Pessac, France; 8.SLAC Natl Accelerator Lab, SSRL, Menlo Pk, CA 94025 USA; 9.SLAC Natl Accelerator Lab, PULSE Inst, Menlo Pk, CA 94025 USA; 10.Univ Rennes 1, CNRS, IPR, UBL,UMR 6251, F-35042 Rennes, France |
推荐引用方式 GB/T 7714 | Lemke, Henrik T.,Kjaer, Kasper S.,Hartsock, Robert,et al. Coherent structural trapping through wave packet dispersion during photoinduced spin state switching[J]. NATURE COMMUNICATIONS,2019,8. |
APA | Lemke, Henrik T..,Kjaer, Kasper S..,Hartsock, Robert.,van Driel, Tim B..,Chollet, Matthieu.,...&Cammarata, Marco.(2019).Coherent structural trapping through wave packet dispersion during photoinduced spin state switching.NATURE COMMUNICATIONS,8. |
MLA | Lemke, Henrik T.,et al."Coherent structural trapping through wave packet dispersion during photoinduced spin state switching".NATURE COMMUNICATIONS 8(2019). |
条目包含的文件 | 条目无相关文件。 |
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