超分辨率飞秒电子衍射揭示了锥形交叉点的电子和核动力学

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Hui Jiang, Juanjuan Zhang, Tianyu Wang, Jiawei Peng, Cheng Jin, Xiao Zou, Pengfei Zhu, Tao Jiang, Zhenggang Lan, Haiwang Yong, Feng He, Dao Xiang
{"title":"超分辨率飞秒电子衍射揭示了锥形交叉点的电子和核动力学","authors":"Hui Jiang, Juanjuan Zhang, Tianyu Wang, Jiawei Peng, Cheng Jin, Xiao Zou, Pengfei Zhu, Tao Jiang, Zhenggang Lan, Haiwang Yong, Feng He, Dao Xiang","doi":"10.1038/s41467-025-61975-9","DOIUrl":null,"url":null,"abstract":"<p>Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We overcome this by combining the enhanced temporal resolution of mega-electron-volt ultrafast electron diffraction with a super-resolution real-space inversion algorithm, enabling visualization of nuclear and electronic motions at conical intersections with sub-angstrom resolution, surpassing the diffraction limit. We apply this technique to the textbook example of the ring-opening reaction of 1,3-cyclohexadiene, which proceeds through two conical intersections within 100 femtoseconds. The super-resolved transient structures near conical intersections reveal a C-C bond length difference of less than 0.4 Å and an approximately 30-femtosecond traversal time of the nuclear wave packet between them. These findings establish super-resolution ultrafast scattering as a transformative tool for uncovering quantum dynamics in molecules and open new avenues for studying light-matter interactions at the most fundamental level.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"53 1","pages":""},"PeriodicalIF":15.7000,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections\",\"authors\":\"Hui Jiang, Juanjuan Zhang, Tianyu Wang, Jiawei Peng, Cheng Jin, Xiao Zou, Pengfei Zhu, Tao Jiang, Zhenggang Lan, Haiwang Yong, Feng He, Dao Xiang\",\"doi\":\"10.1038/s41467-025-61975-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We overcome this by combining the enhanced temporal resolution of mega-electron-volt ultrafast electron diffraction with a super-resolution real-space inversion algorithm, enabling visualization of nuclear and electronic motions at conical intersections with sub-angstrom resolution, surpassing the diffraction limit. We apply this technique to the textbook example of the ring-opening reaction of 1,3-cyclohexadiene, which proceeds through two conical intersections within 100 femtoseconds. The super-resolved transient structures near conical intersections reveal a C-C bond length difference of less than 0.4 Å and an approximately 30-femtosecond traversal time of the nuclear wave packet between them. These findings establish super-resolution ultrafast scattering as a transformative tool for uncovering quantum dynamics in molecules and open new avenues for studying light-matter interactions at the most fundamental level.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"53 1\",\"pages\":\"\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-07-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-61975-9\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-61975-9","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0

摘要

圆锥交叉在激发态量子动力学中起着关键作用。由于快速的时间尺度和微妙的结构变化,捕获锥形交叉点附近的瞬态分子结构仍然具有挑战性。我们通过将超高速电子衍射的增强时间分辨率与超分辨率实空间反演算法相结合来克服这一问题,从而实现了亚埃分辨率的锥形交叉点核和电子运动的可视化,超过了衍射极限。我们将该技术应用于1,3-环己二烯开环反应的教科书示例,该反应在100飞秒内通过两个锥形相交。锥形交点附近的超分辨瞬态结构显示C-C键长差小于0.4 Å,它们之间的核波包的穿越时间约为30飞秒。这些发现确立了超分辨率超快散射作为揭示分子量子动力学的变革性工具,并为在最基本的水平上研究光-物质相互作用开辟了新的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections

Super-resolution femtosecond electron diffraction reveals electronic and nuclear dynamics at conical intersections

Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We overcome this by combining the enhanced temporal resolution of mega-electron-volt ultrafast electron diffraction with a super-resolution real-space inversion algorithm, enabling visualization of nuclear and electronic motions at conical intersections with sub-angstrom resolution, surpassing the diffraction limit. We apply this technique to the textbook example of the ring-opening reaction of 1,3-cyclohexadiene, which proceeds through two conical intersections within 100 femtoseconds. The super-resolved transient structures near conical intersections reveal a C-C bond length difference of less than 0.4 Å and an approximately 30-femtosecond traversal time of the nuclear wave packet between them. These findings establish super-resolution ultrafast scattering as a transformative tool for uncovering quantum dynamics in molecules and open new avenues for studying light-matter interactions at the most fundamental level.

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 Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
×
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:604180095
Book学术官方微信