Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization

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  • Kasra Amini, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Evgeny Savelyev, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Felix Brauße, Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, 12489 Berlin, Germany.
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  • Nora Berrah, Department of Physics, University of Connecticut, Storrs, Connecticut 06269, USA.
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  • Cédric Bomme, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Mark Brouard, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Michael Burt, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Lauge Christensen
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  • Stefan Düsterer, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Benjamin Erk, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Hauke Höppner, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Thomas Kierspel, Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Faruk Krecinic, Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, 12489 Berlin, Germany.
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  • Alexandra Lauer, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Jason W L Lee, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Maria Müller, Institut für Optik und Atomare Physik, Technische Universität Berlin, 10623 Berlin, Germany.
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  • Erland Müller, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Terence Mullins, Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Harald Redlin, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Nora Schirmel, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Jan Thøgersen
  • Simone Techert, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Sven Toleikis, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Rolf Treusch, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Sebastian Trippel, Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Anatoli Ulmer, Institut für Optik und Atomare Physik, Technische Universität Berlin, 10623 Berlin, Germany.
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  • Claire Vallance, The Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, United Kingdom.
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  • Joss Wiese, Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.
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  • Per Johnsson, Lund Observatory, Department of Astronomy and Theoretical Physics, Lund University, Box 43, SE-22100 Lund, Sweden
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  • Jochen Küpper, Center for Free-Electron Laser Science, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Artem Rudenko, J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, USA.
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  • Arnaud Rouzée, Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, 12489 Berlin, Germany.
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  • Henrik Stapelfeldt
  • Daniel Rolles, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany., Germany
  • Rebecca Boll, Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany.

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Original languageEnglish
JournalStructural Dynamics
Volume5
Issue1
Pages (from-to)014301, 1-14
Number of pages14
ISSN2329-7778
DOIs
Publication statusPublished - 2018

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