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Abstract of [Boll22]

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X-ray multiphoton-induced Coulomb explosion images complex single molecules

Rebecca Boll, Julia M. Schäfer, Benoît Richard, Kilian Fehre, Gregor Kastirke, Zoltan Jurek, Markus S. Schöffler, Malik M. Abdullah, Nils Anders, Thomas M. Baumann, Sebastian Eckart, Benjamin Erk, Alberto De Fanis, Reinhard Dörner, Lutz Foucar, Sven Grundmann, Patrik Grychtol, Alexander Hartung, Max Hofmann, Markus Ilchen, Ludger Inhester, Christian Janke, Rui Jin, Max Kircher, Katharina Kubicek, Maksim Kunitski, Xiang Li, Tommaso Mazza, Severin Meister, Niklas Melzer, Jacobo Montano, Valerija Music, Giammarco Nalin, Yevheniy Ovcharenko, Christopher Passow, Andreas Pier, Nils Rennhack, Jonas Rist, Daniel E. Rivas, Daniel Rolles, Ilme Schlichting, Lothar Ph.H. Schmidt, Philipp Schmidt, Juliane Siebert, Nico Strenger, Daniel Trabert, Florian Trinter, Isabel Vela-Perez, Rene Wagner, Peter Walter, Miriam Weller, Pawel Ziolkowski, Sang-Kil Son, Artem Rudenko, Michael Meyer, Robin Santra, and Till Jahnke

Nat. Phys. 18, 423–428 (2022)


Following structural dynamics in real time is a fundamental goal towards a better understanding of chemical reactions. Recording snapshots of individual molecules with ultrashort exposure times is a key ingredient towards this goal, as atoms move on femtosecond (10-15 s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem of low target densities, low scattering cross sections and random spatial orientation of the molecules. Therefore, obtaining images of entire, isolated molecules capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense femtosecond pulses from an X-ray free-electron laser trigger rapid and complete Coulomb explosions of 2-iodopyridine and 2-iodopyrazine molecules. We obtain intriguingly clear momentum images depicting ten or eleven atoms, including all the hydrogens, and thus overcome a so-far impregnable barrier for complete Coulomb explosion imaging–its limitation on molecules consisting of three to five atoms. In combination with state-of-the-art multi-coincidence techniques and elaborate theoretical modelling, this allows tracing ultrafast hydrogen emission and obtaining information on the result of intramolecular electron rearrangement. Our work represents an important step towards imaging femtosecond chemistry via Coulomb explosion.

Tags: XMDYN, iodopyridine, Coulomb explosion, CEI, x-ray explosion dynamics, coincidence, experiment, SQS, European XFEL, CFEL, DESY

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