Physical Review X (Jun 2020)

Photoelectron Diffraction Imaging of a Molecular Breakup Using an X-Ray Free-Electron Laser

  • Gregor Kastirke,
  • Markus S. Schöffler,
  • Miriam Weller,
  • Jonas Rist,
  • Rebecca Boll,
  • Nils Anders,
  • Thomas M. Baumann,
  • Sebastian Eckart,
  • Benjamin Erk,
  • Alberto De Fanis,
  • Kilian Fehre,
  • Averell Gatton,
  • Sven Grundmann,
  • Patrik Grychtol,
  • Alexander Hartung,
  • Max Hofmann,
  • Markus Ilchen,
  • Christian Janke,
  • Max Kircher,
  • Maksim Kunitski,
  • Xiang Li,
  • Tommaso Mazza,
  • Niklas Melzer,
  • Jacobo Montano,
  • Valerija Music,
  • Giammarco Nalin,
  • Yevheniy Ovcharenko,
  • Andreas Pier,
  • Nils Rennhack,
  • Daniel E. Rivas,
  • Reinhard Dörner,
  • Daniel Rolles,
  • Artem Rudenko,
  • Philipp Schmidt,
  • Juliane Siebert,
  • Nico Strenger,
  • Daniel Trabert,
  • Isabel Vela-Perez,
  • Rene Wagner,
  • Thorsten Weber,
  • Joshua B. Williams,
  • Pawel Ziolkowski,
  • Lothar Ph. H. Schmidt,
  • Achim Czasch,
  • Florian Trinter,
  • Michael Meyer,
  • Kiyoshi Ueda,
  • Philipp V. Demekhin,
  • Till Jahnke

DOI
https://doi.org/10.1103/PhysRevX.10.021052
Journal volume & issue
Vol. 10, no. 2
p. 021052

Abstract

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A central motivation for the development of x-ray free-electron lasers has been the prospect of time-resolved single-molecule imaging with atomic resolution. Here, we show that x-ray photoelectron diffraction—where a photoelectron emitted after x-ray absorption illuminates the molecular structure from within—can be used to image the increase of the internuclear distance during the x-ray-induced fragmentation of an O_{2} molecule. By measuring the molecular-frame photoelectron emission patterns for a two-photon sequential K-shell ionization in coincidence with the fragment ions, and by sorting the data as a function of the measured kinetic energy release, we can resolve the elongation of the molecular bond by approximately 1.2 a.u. within the duration of the x-ray pulse. The experiment paves the road toward time-resolved pump-probe photoelectron diffraction imaging at high-repetition-rate x-ray free-electron lasers.