锥形交叉点产生的电子动力学及其在水溶液中的消相现象

IF 17.6 1区 物理与天体物理 Q1 PHYSICS, MULTIDISCIPLINARY
Yi-Ping Chang, Tadas Balciunas, Zhong Yin, Marin Sapunar, Bruno N. C. Tenorio, Alexander C. Paul, Shota Tsuru, Henrik Koch, Jean-Pierre Wolf, Sonia Coriani, Hans Jakob Wörner
{"title":"锥形交叉点产生的电子动力学及其在水溶液中的消相现象","authors":"Yi-Ping Chang, Tadas Balciunas, Zhong Yin, Marin Sapunar, Bruno N. C. Tenorio, Alexander C. Paul, Shota Tsuru, Henrik Koch, Jean-Pierre Wolf, Sonia Coriani, Hans Jakob Wörner","doi":"10.1038/s41567-024-02703-w","DOIUrl":null,"url":null,"abstract":"<p>A dynamical rearrangement in the electronic structure of a molecule can be driven by different phenomena, including nuclear motion, electronic coherence or electron correlation. Recording such electronic dynamics and identifying its fate in an aqueous solution has remained a challenge. Here, we reveal the electronic dynamics induced by electronic relaxation through conical intersections in both isolated and solvated pyrazine molecules using X-ray spectroscopy. We show that the ensuing created dynamics corresponds to a cyclic rearrangement of the electronic structure around the aromatic ring. Furthermore, we found that such electronic dynamics were entirely suppressed when pyrazine was dissolved in water. Our observations confirm that conical intersections can create electronic dynamics that are not directly excited by the pump pulse and that aqueous solvation can dephase them in less than 40 fs. These results have implications for the investigation of electronic dynamics created during light-induced molecular dynamics and shed light on their susceptibility to aqueous solvation.</p>","PeriodicalId":19100,"journal":{"name":"Nature Physics","volume":"12 1","pages":""},"PeriodicalIF":17.6000,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electronic dynamics created at conical intersections and its dephasing in aqueous solution\",\"authors\":\"Yi-Ping Chang, Tadas Balciunas, Zhong Yin, Marin Sapunar, Bruno N. C. Tenorio, Alexander C. Paul, Shota Tsuru, Henrik Koch, Jean-Pierre Wolf, Sonia Coriani, Hans Jakob Wörner\",\"doi\":\"10.1038/s41567-024-02703-w\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>A dynamical rearrangement in the electronic structure of a molecule can be driven by different phenomena, including nuclear motion, electronic coherence or electron correlation. Recording such electronic dynamics and identifying its fate in an aqueous solution has remained a challenge. Here, we reveal the electronic dynamics induced by electronic relaxation through conical intersections in both isolated and solvated pyrazine molecules using X-ray spectroscopy. We show that the ensuing created dynamics corresponds to a cyclic rearrangement of the electronic structure around the aromatic ring. Furthermore, we found that such electronic dynamics were entirely suppressed when pyrazine was dissolved in water. Our observations confirm that conical intersections can create electronic dynamics that are not directly excited by the pump pulse and that aqueous solvation can dephase them in less than 40 fs. These results have implications for the investigation of electronic dynamics created during light-induced molecular dynamics and shed light on their susceptibility to aqueous solvation.</p>\",\"PeriodicalId\":19100,\"journal\":{\"name\":\"Nature Physics\",\"volume\":\"12 1\",\"pages\":\"\"},\"PeriodicalIF\":17.6000,\"publicationDate\":\"2024-11-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Physics\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1038/s41567-024-02703-w\",\"RegionNum\":1,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"PHYSICS, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Physics","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1038/s41567-024-02703-w","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"PHYSICS, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

分子电子结构的动态重排可以由不同的现象驱动,包括核运动、电子相干性或电子相关性。记录这种电子动力学并确定其在水溶液中的命运一直是一个挑战。在这里,我们利用 X 射线光谱揭示了孤立的吡嗪分子和溶解的吡嗪分子中通过锥形交叉点的电子弛豫引起的电子动力学。我们发现,随之产生的动态与围绕芳香环的电子结构的循环重排相对应。此外,我们还发现,当吡嗪溶于水时,这种电子动力学完全被抑制。我们的观察结果证实,锥形交叉点可以产生不被泵脉冲直接激发的电子动力学,而水溶解可以在不到 40 fs 的时间内消除这些电子动力学。这些结果对研究光诱导分子动力学过程中产生的电子动力学具有重要意义,并揭示了它们对水溶解的敏感性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Electronic dynamics created at conical intersections and its dephasing in aqueous solution

Electronic dynamics created at conical intersections and its dephasing in aqueous solution

A dynamical rearrangement in the electronic structure of a molecule can be driven by different phenomena, including nuclear motion, electronic coherence or electron correlation. Recording such electronic dynamics and identifying its fate in an aqueous solution has remained a challenge. Here, we reveal the electronic dynamics induced by electronic relaxation through conical intersections in both isolated and solvated pyrazine molecules using X-ray spectroscopy. We show that the ensuing created dynamics corresponds to a cyclic rearrangement of the electronic structure around the aromatic ring. Furthermore, we found that such electronic dynamics were entirely suppressed when pyrazine was dissolved in water. Our observations confirm that conical intersections can create electronic dynamics that are not directly excited by the pump pulse and that aqueous solvation can dephase them in less than 40 fs. These results have implications for the investigation of electronic dynamics created during light-induced molecular dynamics and shed light on their susceptibility to aqueous solvation.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Nature Physics
Nature Physics 物理-物理:综合
CiteScore
30.40
自引率
2.00%
发文量
349
审稿时长
4-8 weeks
期刊介绍: Nature Physics is dedicated to publishing top-tier original research in physics with a fair and rigorous review process. It provides high visibility and access to a broad readership, maintaining high standards in copy editing and production, ensuring rapid publication, and maintaining independence from academic societies and other vested interests. The journal presents two main research paper formats: Letters and Articles. Alongside primary research, Nature Physics serves as a central source for valuable information within the physics community through Review Articles, News & Views, Research Highlights covering crucial developments across the physics literature, Commentaries, Book Reviews, and Correspondence.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信