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DOI | 10.1126/science.aaj2198 |
Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction | |
Attar, Andrew R.1,2; Bhattacherjee, Aditi1,2; Pemmaraju, C. D.3,4; Schnorr, Kirsten1,2; Closser, Kristina D.3; Prendergast, David3; Leone, Stephen R.1,2,5 | |
2017-04-07 | |
发表期刊 | SCIENCE |
ISSN | 0036-8075 |
EISSN | 1095-9203 |
出版年 | 2017 |
卷号 | 356期号:6333页码:54-58 |
文章类型 | Article |
语种 | 英语 |
国家 | USA |
英文摘要 | The ultrafast light-activated electrocyclic ring-opening reaction of 1,3-cyclohexadiene is a fundamental prototype of photochemical pericyclic reactions. Generally, these reactions are thought to proceed through an intermediate excited-state minimum (the so-called pericyclic minimum), which leads to isomerization via nonadiabatic relaxation to the ground state of the photoproduct. Here, we used femtosecond (fs) soft x-ray spectroscopy near the carbon K-edge (similar to 284 electron volts) on a table-top apparatus to directly reveal the valence electronic structure of this transient intermediate state. The core-to-valence spectroscopic signature of the pericyclic minimum observed in the experiment was characterized, in combination with time-dependent density functional theory calculations, to reveal overlap and mixing of the frontier valence orbital energy levels. We show that this transient valence electronic structure arises within 60 +/- 20 fs after ultraviolet photoexcitation and decays with a time constant of 110 +/- 60 fs. |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000398689100035 |
WOS关键词 | ABSORPTION-SPECTROSCOPY ; REACTION-PATH ; MOLECULAR-STRUCTURE ; STATE ; 1,3-CYCLOHEXADIENE ; TRANSITION ; PHOTOIRRADIATION ; DYNAMICS ; SYMMETRY |
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/195771 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA; 2.Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA; 3.Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA; 4.Theory Inst Mat & Energy Spectroscopies, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA; 5.Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA |
推荐引用方式 GB/T 7714 | Attar, Andrew R.,Bhattacherjee, Aditi,Pemmaraju, C. D.,et al. Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction[J]. SCIENCE,2017,356(6333):54-58. |
APA | Attar, Andrew R..,Bhattacherjee, Aditi.,Pemmaraju, C. D..,Schnorr, Kirsten.,Closser, Kristina D..,...&Leone, Stephen R..(2017).Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction.SCIENCE,356(6333),54-58. |
MLA | Attar, Andrew R.,et al."Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction".SCIENCE 356.6333(2017):54-58. |
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