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

2022; Nature Portfolio; Volume: 18; Issue: 4 Linguagem: Inglês

10.1038/s41567-022-01507-0

1745-2481

Rebecca Boll, Julia Schäfer, Benoît Richard, K. Fehre, Gregor Kastirke, Zoltán Jurek, M. S. Schöffler, Malik Muhammad Abdullah, N. Anders, T. Baumann, S. Eckart, Benjamin Erk, A. De Fanis, R. Dörner, Sven Grundmann, Patrik Grychtol, Alexander Hartung, M. Hofmann, Markus Ilchen, Ludger Inhester, Christian Jänke, Rui Jin, M. Kircher, Katharina Kubiček, M. Kunitski, Xiang Li, Tommaso Mazza, Severin Meister, N. Melzer, J. Montaño, Valerija Music, G. Nalin, Yevheniy Ovcharenko, Christopher Passow, A. Pier, Nils Rennhack, J. Rist, Daniel E. Rivas, Daniel Rolles, Ilme Schlichting, Lothar Schmidt, Philipp Schmidt, J. Siebert, N. Strenger, D. Trabert, Florian Trinter, Isabel Vela-Peréz, R. Wagner, Peter Walter, M. Weller, Pawel Ziółkowski, Sang-Kil Son, Artem Rudenko, Michael Meyer, Robin Santra, T. Jahnke,

Ion-surface interactions and analysis

Abstract 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.