Jie Yang, Xiaolei Zhu, Thomas J. A. Wolf, Zheng Li, João Pedro Figueira Nunes, Ryan Coffee, James P. Cryan, Markus Gühr, Kareem Hegazy, Tony F. Heinz, Keith Jobe, Renkai Li, Xiaozhe Shen, Theodore Veccione, Stephen Weathersby, Kyle J. Wilkin, Charles Yoneda, Qiang Zheng, Todd J. Martinez, Martin Centurion, Xijie Wang
- Conical intersections play a critical role in excited-state dynamics of polyatomic molecules because they govern the reaction pathways of many nonadiabatic processes. However, ultrafast probes have lacked sufficient spatial resolution to image wave-packet trajectories through these intersections directly. Here, we present the simultaneous experimental characterization of one-photon and two-photon excitation channels in isolated CF3I molecules using ultrafast gas-phase electron diffraction. In the two-photon channel, we have mapped out the real-space trajectories of a coherent nuclear wave packet, which bifurcates onto two potential energy surfaces when passing through a conical intersection. In the one-photon channel, we have resolved excitation of both the umbrella and the breathing vibrational modes in the CF3 fragment in multiple nuclear dimensions. These findings benchmark and validate ab initio nonadiabatic dynamics calculations.
MetadatenAuthor details: | Jie YangORCiD, Xiaolei ZhuORCiD, Thomas J. A. WolfORCiD, Zheng Li, João Pedro Figueira NunesORCiD, Ryan CoffeeORCiD, James P. Cryan, Markus GührORCiDGND, Kareem HegazyORCiD, Tony F. HeinzORCiD, Keith Jobe, Renkai LiORCiD, Xiaozhe ShenORCiD, Theodore Veccione, Stephen Weathersby, Kyle J. Wilkin, Charles Yoneda, Qiang Zheng, Todd J. MartinezORCiD, Martin Centurion, Xijie Wang |
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DOI: | https://doi.org/10.1126/science.aat0049 |
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ISSN: | 0036-8075 |
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ISSN: | 1095-9203 |
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Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/29976821 |
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Title of parent work (English): | Science |
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Publisher: | American Assoc. for the Advancement of Science |
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Place of publishing: | Washington |
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Publication type: | Article |
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Language: | English |
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Date of first publication: | 2018/07/06 |
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Publication year: | 2018 |
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Release date: | 2021/11/02 |
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Volume: | 361 |
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Issue: | 6397 |
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Number of pages: | 4 |
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First page: | 64 |
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Last Page: | 67 |
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Funding institution: | U.S. Department of Energy (DOE) Office of Basic Energy Sciences (BES) SUE Division Accelerator and Detector RD program; LCLS Facility; SLAG [DE-AC02-05-CH11231, DE-AC02-76SF00515]; AMOS program within Ye Chemical Sciences, Geosciences, and Biosciences Division, BES of the DOE [DE-AC02-76SF00515]; Office of Naval ResearchOffice of Naval Research [N00014-E-1-0828]; Global Climate and Energy Project; National Science Foundation, Major Research Instrumentation pmgram [ACI4429830]; Wolkswagen Foundation; DOE Office of Science, BESUnited States Department of Energy (DOE) [DE-SC0014170] |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
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DDC classification: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
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Peer review: | Referiert |
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Publishing method: | Open Access / Bronze Open-Access |
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