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

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

doi:10.1038/s41567-022-01507-0

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

Journal Article · 21 February 2022 · Nature Physics

DOI: https://doi.org/10.1038/s41567-022-01507-0 · OSTI ID:1868998

^[1]; Schäfer, Julia M. ^[2];

^[3]; Fehre, Kilian ^[4]; Kastirke, Gregor ^[4]; Jurek, Zoltan ^[5]; Schöffler, Markus S. ^[4]; Abdullah, Malik M. ^[6];

^[4]; Baumann, Thomas M. ^[1];

^[4];

^[6]; De Fanis, Alberto ^[1];

^[4];

^[1]; Hartung, Alexander ^[4]; Hofmann, Max ^[4]; Ilchen, Markus ^[7];

^[5] more »

European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Goethe Univ., Frankfurt (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany); Universität Kassel (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Shanghai Jiao Tong Univ. (China)
European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Kansas State Univ., Manhattan, KS (United States)
Max Planck Inst. fuer Kernphysik, Heidelberg (Germany)
Max Planck Inst. fuer Medizinische Forschung, Heidelberg (Germany)
European X-ray Free-Electron Laser (XFEL), Schenefeld (Germany); Goethe Univ., Frankfurt (Germany)
Universität Kassel (Germany)
Goethe Univ., Frankfurt (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Fritz Haber Institute of the Max Planck Society, Berlin (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

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^-15s) 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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-76SF00515; SC0019451; SC0020276

OSTI ID:: 1868998

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 4 Vol. 18; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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