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Acetylene's scission visualized by selfie

Can molecules take pictures of themselves? That is more or less the principle underlying laser-induced electron diffraction (LIED): A laser field strips an electron from a molecule and then sends it back to report on the structure of the remaining ion. Wolter et al. applied this technique to acetylene to track the cleavage of its C–H bond after double ionization (see the Perspective by Ruan). They imaged the full structure of the molecule and also distinguished more rapid dissociative dynamics when it was oriented parallel rather than perpendicular to the LIED field.
Science, this issue p. 308; see also p. 283

Abstract

Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (C2H2) 9 femtoseconds after ionization. Using mid-infrared laser–induced electron diffraction (LIED), we obtained snapshots as a proton departs the [C2H2]2+ ion. By introducing an additional laser field, we also demonstrate control over the ultrafast dissociation process and resolve different bond dynamics for molecules oriented parallel versus perpendicular to the LIED field. These measurements are in excellent agreement with a quantum chemical description of field-dressed molecular dynamics.

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Published In

Science
Volume 354 | Issue 6310
21 October 2016

Submission history

Received: 13 June 2016
Accepted: 19 September 2016
Published in print: 21 October 2016

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Acknowledgments

We acknowledge financial support from the Spanish Ministry of Economy and Competitiveness (MINECO), through the “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV-2015-0522), grants FIS2014-56774-R and FIS2014-51478-ERC; the Catalan Institució Catalana de Recerca I Estudis Avançats; Agencia de Gestió d’Ajuts Universitaris i de Recerca (AGAUR) with grant SGR 2014-2016; the Fundació Cellex Barcelona; the European Union’s Horizon 2020 research and innovation program under LASERLAB-EUROPE (EU-H2020 654148); COST Actions MP1203, XUV/X-ray light and fast ions for ultrafast chemistry (XLIC); the Marie Sklodowska-Curie grant agreement 641272; and the European Research Council through ERC-2013 Advanced Grant 338580. B.W. was supported by AGAUR (FI-DGR 2013–2015). M.G.P. was supported by the ICFONEST+ program, partially funded by the Marie Curie cofunding of Regional, National and International Programs—COFUND (FP7-PEOPLE-2013-COFUND) action of the European Commission. A.-T.L. and C.D.L. are supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, under grant DE-FG02-86ER13491. We thank D. Zalvidea, M. Sclafani, and A. Stolow for helpful and inspiring discussions.

Authors

Affiliations

B. Wolter*
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
M. G. Pullen*
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
A.-T. Le
J. R. Macdonald Laboratory, Physics Department, Kansas State University, Manhattan, KS 66506-2604, USA.
M. Baudisch
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
K. Doblhoff-Dier
Leiden Institute of Chemistry, Gorlaeus Laboratories, Leiden University, Post Office Box 9502, 2300 RA Leiden, Netherlands.
A. Senftleben
Universität Kassel, Institut für Physik und CINSaT, Heinrich-Plett-Str. 40, 34132 Kassel, Germany.
M. Hemmer
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron (DESY), Centre for Ultrafast Imaging (CUI), 22607 Hamburg, Germany.
C. D. Schröter
Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany.
J. Ullrich
Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany.
Physikalisch-Technische Bundesanstalt (PTB), Bundesallee 100, 38116 Braunschweig, Germany.
T. Pfeifer
Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany.
R. Moshammer
Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany.
S. Gräfe
Institute for Physical Chemistry, Friedrich-Schiller University Jena, 07743 Jena, Germany.
Abbe Center of Photonics, Friedrich-Schiller-University Jena, 07743 Jena, Germany.
O. Vendrell
Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron (DESY), Centre for Ultrafast Imaging (CUI), 22607 Hamburg, Germany.
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark.
C. D. Lin
J. R. Macdonald Laboratory, Physics Department, Kansas State University, Manhattan, KS 66506-2604, USA.
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
Institució Catalana de Recerca i Estudis Avançats (ICREA), Pg. Lluís Companys 23, 08010 Barcelona, Spain.

Notes

*
These authors contributed equally to this work.
Corresponding author. Email: [email protected]

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