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

Hironobu Fukuzawa, Tsukasa Takanashi, Edwin Kukk, Koji Motomura, Shin-ichi Wada, Kiyonobu Nagaya, Yuta Ito, Toshiyuki Nishiyama, Christophe Nicolas, Yoshiaki Kumagai, Denys Iablonskyi, Subhendu Mondal, Tetsuya Tachibana, Daehyun You, Syuhei Yamada, Yuta Sakakibara, Kazuki Asa, Yuhiro Sato, Tsukasa Sakai, Kenji Matsunami, Takayuki Umemoto, Kango Kariyazono, Shinji Kajimoto, Hikaru Sotome, Per Johnsson, Markus S. Schöffler, Gregor Kastirke, Kuno Kooser, Xiao-Jing Liu, Theodor Asavei, Liviu Neagu, Serguei Molodtsov, Kohei Ochiai, Manabu Kanno, Kaoru Yamazaki, Shigeki Owada, Kanade Ogawa, Tetsuo Katayama, Tadashi Togashi, Kensuke Tono, Makina Yabashi, Aryya Ghosh, Kirill Gokhberg, Lorenz S. Cederbaum, Alexander I. Kuleff, Hiroshi Fukumura, Naoki Kishimoto, Artem Rudenko, Catalin Miron, Hirohiko Kono and Kiyoshi Ueda ()
Additional contact information
Hironobu Fukuzawa: Tohoku University
Tsukasa Takanashi: Tohoku University
Edwin Kukk: University of Turku
Koji Motomura: Tohoku University
Shin-ichi Wada: RIKEN SPring-8 Center
Kiyonobu Nagaya: RIKEN SPring-8 Center
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
Serguei Molodtsov: European XFEL GmbH, Holzkoppel 4
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
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
Hirohiko Kono: Tohoku University
Kiyoshi Ueda: Tohoku University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-10060-z

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