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Nat Commun. 2019 May 16;10(1):2186. doi: 10.1038/s41467-019-10060-z.

Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2.

Author information

1
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai, 980-8577, Japan.
2
RIKEN SPring-8 Center, Sayo, Hyogo, 679-5148, Japan.
3
Department of Physics and Astronomy, University of Turku, Turku, FI-20014, Finland.
4
Department of Physical Science, Hiroshima University, Higashi-Hiroshima, 739-8526, Japan.
5
Department of Physics, Kyoto University, Kyoto, 606-8502, Japan.
6
Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin, BP 48, FR-91192, Gif-sur-Yvette, Cedex, France.
7
Department of Chemistry, Graduate School of Science, Tohoku University, Sendai, 980-8578, Japan.
8
Department of Physics, Lund University, Lund, SE-22100, Sweden.
9
Institut für Kernphysik, J.W. Goethe Universität, Max-von-Laue-Str. 1, D-60438, Frankfurt, Germany.
10
School of Physics and Nuclear Energy Engineering, Beihang University, Beijing, 100191, P.R. China.
11
Extreme Light Infrastructure - Nuclear Physics (ELI-NP), "Horia Hulubei" National Institute for Physics and Nuclear Engineering, RO-077125, 30 Reactorului Street, Măgurele, Jud Ilfov, Romania.
12
National Institute for Laser, Plasma and Radiation Physics, 409 Atomistilor, PO Box MG-36, 077125, Magurele, Jud Ilfov, Romania.
13
European XFEL GmbH, Holzkoppel 4, Schenefeld, D-22869, Germany.
14
ITMO University, Kronverksky pr. 49, St. Petersburg, 197101, Russia.
15
Institute of Experimental Physics, Technische Universität Bergakademie Freiberg, 09599, Freiberg, Germany.
16
Institute for Materials Research, Tohoku University, Sendai, 980-8577, Japan.
17
Japan Synchrotron Radiation Research Institute (JASRI), Sayo, Hyogo, 679-5198, Japan.
18
Theoretical Chemistry, PCI, Universität Heidelberg, 69120, Heidelberg, Germany.
19
ELI-ALPS, Budapesti út 5, H-6728, Szeged, Hungary.
20
J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS, 66506, USA.
21
LIDYL, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191, Gif-sur-Yvette, France.
22
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai, 980-8577, Japan. kiyoshi.ueda@tohoku.ac.jp.
23
RIKEN SPring-8 Center, Sayo, Hyogo, 679-5148, Japan. kiyoshi.ueda@tohoku.ac.jp.

Abstract

The increasing availability of X-ray free-electron lasers (XFELs) has catalyzed the development of single-object structural determination and of structural dynamics tracking in real-time. Disentangling the molecular-level reactions triggered by the interaction with an XFEL pulse is a fundamental step towards developing such applications. Here we report real-time observations of XFEL-induced electronic decay via short-lived transient electronic states in the diiodomethane molecule, using a femtosecond near-infrared probe laser. We determine the lifetimes of the transient states populated during the XFEL-induced Auger cascades and find that multiply charged iodine ions are issued from short-lived (∼20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (∼100 fs). We identify the mechanisms behind these different time scales: contrary to the short-lived transient states which relax by molecular Auger decay, the long-lived ones decay by an interatomic Coulombic decay between two iodine atoms, during the molecular fragmentation.

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