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

Author

Listed:
  • Hironobu Fukuzawa

    (Tohoku University
    RIKEN SPring-8 Center)

  • Tsukasa Takanashi

    (Tohoku University)

  • Edwin Kukk

    (University of Turku)

  • Koji Motomura

    (Tohoku University)

  • Shin-ichi Wada

    (RIKEN SPring-8 Center
    Hiroshima University)

  • Kiyonobu Nagaya

    (RIKEN SPring-8 Center
    Kyoto University)

  • Yuta Ito

    (Tohoku University)

  • Toshiyuki Nishiyama

    (Kyoto University)

  • Christophe Nicolas

    (Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, BP 48)

  • Yoshiaki Kumagai

    (Tohoku University)

  • Denys Iablonskyi

    (Tohoku University)

  • Subhendu Mondal

    (Tohoku University)

  • Tetsuya Tachibana

    (Tohoku University)

  • Daehyun You

    (Tohoku University)

  • Syuhei Yamada

    (Tohoku University)

  • Yuta Sakakibara

    (Tohoku University)

  • Kazuki Asa

    (Kyoto University)

  • Yuhiro Sato

    (Kyoto University)

  • Tsukasa Sakai

    (Kyoto University)

  • Kenji Matsunami

    (Kyoto University)

  • Takayuki Umemoto

    (Hiroshima University)

  • Kango Kariyazono

    (Hiroshima University)

  • Shinji Kajimoto

    (Tohoku University)

  • Hikaru Sotome

    (Tohoku University)

  • Per Johnsson

    (Lund University)

  • Markus S. Schöffler

    (Institut für Kernphysik, J.W. Goethe Universität)

  • Gregor Kastirke

    (Institut für Kernphysik, J.W. Goethe Universität)

  • Kuno Kooser

    (University of Turku)

  • Xiao-Jing Liu

    (Beihang University)

  • Theodor Asavei

    (Extreme Light Infrastructure - Nuclear Physics (ELI-NP), “Horia Hulubei” National Institute for Physics and Nuclear Engineering)

  • Liviu Neagu

    (Extreme Light Infrastructure - Nuclear Physics (ELI-NP), “Horia Hulubei” National Institute for Physics and Nuclear Engineering
    National Institute for Laser, Plasma and Radiation Physics, 409 Atomistilor, PO Box MG-36)

  • Serguei Molodtsov

    (European XFEL GmbH, Holzkoppel 4
    ITMO University, Kronverksky pr. 49
    Institute of Experimental Physics, Technische Universität Bergakademie Freiberg)

  • Kohei Ochiai

    (Tohoku University)

  • Manabu Kanno

    (Tohoku University)

  • Kaoru Yamazaki

    (Institute for Materials Research, Tohoku University)

  • Shigeki Owada

    (RIKEN SPring-8 Center)

  • Kanade Ogawa

    (RIKEN SPring-8 Center)

  • Tetsuo Katayama

    (Japan Synchrotron Radiation Research Institute (JASRI), Sayo)

  • Tadashi Togashi

    (Japan Synchrotron Radiation Research Institute (JASRI), Sayo)

  • Kensuke Tono

    (Japan Synchrotron Radiation Research Institute (JASRI), Sayo)

  • Makina Yabashi

    (RIKEN SPring-8 Center)

  • Aryya Ghosh

    (Theoretical Chemistry, PCI, Universität Heidelberg)

  • Kirill Gokhberg

    (Theoretical Chemistry, PCI, Universität Heidelberg)

  • Lorenz S. Cederbaum

    (Theoretical Chemistry, PCI, Universität Heidelberg)

  • Alexander I. Kuleff

    (Theoretical Chemistry, PCI, Universität Heidelberg
    ELI-ALPS)

  • Hiroshi Fukumura

    (Tohoku University)

  • Naoki Kishimoto

    (Tohoku University)

  • Artem Rudenko

    (J. R. Macdonald Laboratory, Department of Physics, Kansas State University)

  • Catalin Miron

    (Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, BP 48
    Extreme Light Infrastructure - Nuclear Physics (ELI-NP), “Horia Hulubei” National Institute for Physics and Nuclear Engineering
    LIDYL, CEA, CNRS, Université Paris-Saclay, CEA Saclay)

  • Hirohiko Kono

    (Tohoku University)

  • Kiyoshi Ueda

    (Tohoku University
    RIKEN SPring-8 Center)

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.

Suggested Citation

  • Hironobu Fukuzawa & Tsukasa Takanashi & Edwin Kukk & Koji Motomura & Shin-ichi Wada & Kiyonobu Nagaya & Yuta Ito & Toshiyuki Nishiyama & Christophe Nicolas & Yoshiaki Kumagai & Denys Iablonskyi & Subh, 2019. "Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-10060-z
    DOI: 10.1038/s41467-019-10060-z
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