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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 and Kumagai, Yoshiaki , et al. (2019) In Nature Communications 10(1).
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... (More)
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. © 2019, The Author(s). (Less)
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Nature Communications
volume
10
issue
1
article number
2186
publisher
Nature Publishing Group
external identifiers
  • pmid:31097703
  • scopus:85065804889
ISSN
2041-1723
DOI
10.1038/s41467-019-10060-z
language
English
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yes
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f60b9d16-9e0f-4ae2-98a4-9012665d1233
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2019-05-27 11:32:01
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2020-08-05 05:21:49
@article{f60b9d16-9e0f-4ae2-98a4-9012665d1233,
  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. © 2019, The Author(s).},
  author       = {Fukuzawa, Hironobu and Takanashi, Tsukasa and Kukk, Edwin and Motomura, Koji and Wada, Shin-ichi and Nagaya, Kiyonobu and Ito, Yuta and Nishiyama, Toshiyuki and Nicolas, Christophe and Kumagai, Yoshiaki and Iablonskyi, Denys and Mondal, Subhendu and Tachibana, Tetsuya and You, Daehyun and Yamada, Syuhei and Sakakibara, Yuta and Asa, Kazuki and Sato, Yuhiro and Sakai, Tsukasa and Matsunami, Kenji and Umemoto, Takayuki and Kariyazono, Kango and Kajimoto, Shinji and Sotome, Hikaru and Johnsson, Per and Schöffler, Markus S. and Kastirke, Gregor and Kooser, Kuno and Liu, Xiao-Jing and Asavei, Theodor and Neagu, Liviu and Molodtsov, Serguei and Ochiai, Kohei and Kanno, Manabu and Yamazaki, Kaoru and Owada, Shigeki and Ogawa, Kanade and Katayama, Tetsuo and Togashi, Tadashi and Tono, Kensuke and Yabashi, Makina and Ghosh, Aryya and Gokhberg, Kirill and Cederbaum, Lorenz S. and Kuleff, Alexander I. and Fukumura, Hiroshi and Kishimoto, Naoki and Rudenko, Artem and Miron, Catalin and Kono, Hirohiko and Ueda, Kiyoshi},
  issn         = {2041-1723},
  language     = {eng},
  number       = {1},
  publisher    = {Nature Publishing Group},
  series       = {Nature Communications},
  title        = {Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2},
  url          = {http://dx.doi.org/10.1038/s41467-019-10060-z},
  doi          = {10.1038/s41467-019-10060-z},
  volume       = {10},
  year         = {2019},
}