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  Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction

Yang, J., Zhu, X., Wolf, T. J. A., Li, Z., Nunes, J. P. F., Coffee, R., et al. (2018). Imaging CF3I conical intersection and photodissociation dynamics with ultrafast electron diffraction. Science, 361(6397), 64-67. doi:10.1126/science.aat0049.

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 Urheber:
Yang, J.1, 2, Autor
Zhu, X.2, 3, Autor
Wolf, T. J. A.2, Autor
Li, Z.2, 4, 5, Autor           
Nunes, J. P. F.6, Autor
Coffee, R.2, 7, 8, Autor
Cryan, J. P.2, Autor
Gühr, M.2, 9, Autor
Hegazy, K.2, 8, Autor
Heinz, T. F.2, 10, Autor
Jobe, K.1, Autor
Li, R.1, Autor
Shen, X.1, Autor
Veccione, T.1, Autor
Weathersby, S.1, Autor
Wilkin, K. J.11, Autor
Yoneda, C.1, Autor
Zheng, Q.1, Autor
Martinez, T. J.2, 3, Autor
Centurion, M.11, Autor
Wang, X.1, Autor mehr..
Affiliations:
1SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
2Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
3Department of Chemistry, Stanford University, Stanford, ou_persistent22              
4Center for Free Electron Laser Science, Deutsches Elektronen-Synchrotron (DESY), Hamburg, ou_persistent22              
5Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938286              
6Department of Chemistry, University of York, Heslington, ou_persistent22              
7Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
8Department of Physics, Stanford University, Stanford, ou_persistent22              
9Institut für Physik und Astronomie, Universität Potsdam, Potsdam, ou_persistent22              
10Department of Applied Physics, Stanford University, Stanford, ou_persistent22              
11Department of Physics and Astronomy, University of Nebraska–Lincoln, Lincoln, ou_persistent22              

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 Zusammenfassung: 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.

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Sprache(n): eng - English
 Datum: 2018-05-152018-01-142018-07-06
 Publikationsstatus: Erschienen
 Seiten: 4
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1126/science.aat0049
 Art des Abschluß: -

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Projektname : We thank G. M. Stewart from SLAC National Accelerator Laboratory for the assistance with making movie S1. Funding: The experimental part of this research was performed at SLAC MeV-UED, which is supported in part by the U.S. Department of Energy (DOE) Office of Basic Energy Sciences (BES) SUF Division Accelerator and Detector R&D program, the LCLS Facility, and SLAC under contracts DE-AC02-05-CH11231 and DE-AC02-76SF00515. J.Y., T.F.H., J.P.C., R.C., T.J.A.W., X.Z., and T.J.M. acknowledge support by the AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division, BES of the DOEunder contract DE-AC02-76SF00515. J.P.F.N. acknowledges support by the Wild Overseas Scholars Fund of Department of Chemistry, University of York. T.J.M. acknowledges support from Office of Naval Research grant N00014-12-1-0828 and the Global Climate and Energy Project. This work used the XStream computational resources supported by the National Science Foundation Major Research Instrumentation program (ACI-1429830). Z.L. acknowledges support by the Volkswagen Foundation. M.G. is funded via a Lichtenberg Professorship of the Volkswagen Foundation. K.J.W. and M.C. were supported by the DOE Office of Science, BES under award DE-SC0014170.
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Quelle 1

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Titel: Science
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Washington, D.C. : American Association for the Advancement of Science
Seiten: 4 Band / Heft: 361 (6397) Artikelnummer: - Start- / Endseite: 64 - 67 Identifikator: ISSN: 0036-8075
CoNE: https://pure.mpg.de/cone/journals/resource/991042748276600_1