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

• Fukuzawa, Hironobu

• Takanashi, Tsukasa

• Kukk, Edwin

• Motomura, Koji

• Wada, Shin-ichi

• Nagaya, Kiyonobu

• Ito, Yuta

• Nishiyama, Toshiyuki

• Nicolas, Christophe

• Kumagai, Yoshiaki

• Iablonskyi, Denys

• Mondal, Subhendu

• Tachibana, Tetsuya

• You, Daehyun

• Yamada, Syuhei

• Sakakibara, Yuta

• Asa, Kazuki

• Sato, Yuhiro

• Sakai, Tsukasa

• Matsunami, Kenji

• Umemoto, Takayuki

• Kariyazono, Kango

• Kajimoto, Shinji

• Sotome, Hikaru

• Johnsson, Per

• Schöffler, Markus S.

• Kastirke, Gregor

• Kooser, Kuno

• Liu, Xiao-Jing

• Asavei, Theodor

• Neagu, Liviu

• Molodtsov, Serguei

• Ochiai, Kohei

• Kanno, Manabu

• Yamazaki, Kaoru

• Owada, Shigeki

• Ogawa, Kanade

• Katayama, Tetsuo

• Togashi, Tadashi

• Tono, Kensuke

• Yabashi, Makina

• Ghosh, Aryya

• Gokhberg, Kirill

• Cederbaum, Lorenz S.

• Kuleff, Alexander I.

• Fukumura, Hiroshi

• Kishimoto, Naoki

• Rudenko, Artem

• Miron, Catalin

• Kono, Hirohiko

• Ueda, Kiyoshi

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.

Journal

• Nature Communications

  Nature Communications 10 2186-, 2019-05-16

  Springer Science and Business Media LLC

Keywords

• Atomic and molecular interactions with photons
• Chemical physics
• Free-electron lasers

Details

• CRID: 1050001202929855488
• NII Article ID: 120006634627
• ISSN: 20411723
• DOI: 10.1038/s41467-019-10060-z
• HANDLE: 2433/241634
• Web Site: https://www.nature.com/articles/s41467-019-10060-z.pdf
• Web Site: https://www.nature.com/articles/s41467-019-10060-z
• Text Lang: en
• Article Type: journal article
• Data Source:
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  • Crossref
  • CiNii Articles
  • KAKEN