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; Kiyoshi Ueda

doi:10.1038/s41467-019-10060-z

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 MatsunamiTakayuki 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, Kiyoshi Ueda

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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.

Original language	English
Article number	2186
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-10060-z
Publication status	Published - 2019 Dec 1

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10.1038/s41467-019-10060-z

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Fukuzawa, H., Takanashi, T., Kukk, E., Motomura, K., Wada, S. I., Nagaya, K., Ito, Y., Nishiyama, T., Nicolas, C., Kumagai, Y., Iablonskyi, D., Mondal, S., Tachibana, T., You, D., Yamada, S., Sakakibara, Y., Asa, K., Sato, Y., Sakai, T., ... Ueda, K. (2019). Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH₂I₂. Nature Communications, 10(1), Article 2186. https://doi.org/10.1038/s41467-019-10060-z

@article{9e8eb4acce9e415b93b523e212a72a8e,

title = "Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2",

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.",

author = "Hironobu Fukuzawa and Tsukasa Takanashi and Edwin Kukk and Koji Motomura and Wada, {Shin ichi} and Kiyonobu Nagaya and Yuta Ito and Toshiyuki Nishiyama and Christophe Nicolas and Yoshiaki Kumagai and Denys Iablonskyi and Subhendu Mondal and Tetsuya Tachibana and Daehyun You and Syuhei Yamada and Yuta Sakakibara and Kazuki Asa and Yuhiro Sato and Tsukasa Sakai and Kenji Matsunami and Takayuki Umemoto and Kango Kariyazono and Shinji Kajimoto and Hikaru Sotome and Per Johnsson and Sch{\"o}ffler, {Markus S.} and Gregor Kastirke and Kuno Kooser and Liu, {Xiao Jing} and Theodor Asavei and Liviu Neagu and Serguei Molodtsov and Kohei Ochiai and Manabu Kanno and Kaoru Yamazaki and Shigeki Owada and Kanade Ogawa and Tetsuo Katayama and Tadashi Togashi and Kensuke Tono and Makina Yabashi and Aryya Ghosh and Kirill Gokhberg and Cederbaum, {Lorenz S.} and Kuleff, {Alexander I.} and Hiroshi Fukumura and Naoki Kishimoto and Artem Rudenko and Catalin Miron and Hirohiko Kono and Kiyoshi Ueda",

note = "Funding Information: The XFEL experiments were performed at the BL3 of SACLA with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) and the program review committee (No. 2013B8058, 2015A8056, 2015B8057). This study was supported by the X-ray Free-Electron Laser Utilization Research Project and the X-ray Free-Electron Laser Priority Strategy Program of the Ministry of Education, Culture, Sports, Science, and Technology of Japan (MEXT), by the Proposal Program of SACLA Experimental Instruments of RIKEN, by the Japan Society for the Promotion of Science (JSPS) KAKENHI Grant Numbers JP15K17487, JP16H04091, JP18K05022, by “Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials” from the MEXT, by the Research Program of “Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials” in “Network Joint Research Center for Materials and Devices”, by European Research Council Advanced Investigator Grant no. 692657, and by the IMRAM project. T.Ta. gratefully acknowledges support by the JSPS KAKENHI Grant Number JP16J02270, E.K. the financial support by the Academy of Finland, D.Y. support by a Grant-in-Aid of Tohoku University Institute for Promoting Graduate Degree Programs Division for Interdisciplinary Advanced Research and Education. P.J. acknowledges support from the Swedish Research Council and the Swedish Foundation for Strategic Research, and A.I.K. by the DFG through QUTIF Priority Programme. K.Y. is grateful for the financial supports from Building of Consortia for the Development of Human Resources in Science and Technology by the MEXT. N.K. appreciates the support of the Cross-ministerial Strategic Innovation Promotion Program. A.R. was supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy under Grant No. DE-FG02-86ER13491. Publisher Copyright: {\textcopyright} 2019, The Author(s).",

year = "2019",

month = dec,

day = "1",

doi = "10.1038/s41467-019-10060-z",

language = "English",

volume = "10",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

number = "1",

}

Fukuzawa, H, Takanashi, T, Kukk, E, Motomura, K, Wada, SI, Nagaya, K, Ito, Y, Nishiyama, T, Nicolas, C, Kumagai, Y, Iablonskyi, D, Mondal, S, Tachibana, T, You, D, Yamada, S, Sakakibara, Y, Asa, K, Sato, Y, Sakai, T, Matsunami, K, Umemoto, T, Kariyazono, K, Kajimoto, S, Sotome, H, Johnsson, P, Schöffler, MS, Kastirke, G, Kooser, K, Liu, XJ, Asavei, T, Neagu, L, Molodtsov, S, Ochiai, K, Kanno, M, Yamazaki, K, Owada, S, Ogawa, K, Katayama, T, Togashi, T, Tono, K, Yabashi, M, Ghosh, A, Gokhberg, K, Cederbaum, LS, Kuleff, AI, Fukumura, H, Kishimoto, N, Rudenko, A, Miron, C, Kono, H & Ueda, K 2019, 'Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH₂I₂', Nature Communications, vol. 10, no. 1, 2186. https://doi.org/10.1038/s41467-019-10060-z

TY - JOUR

T1 - Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2

AU - Fukuzawa, Hironobu

AU - Takanashi, Tsukasa

AU - Kukk, Edwin

AU - Motomura, Koji

AU - Wada, Shin ichi

AU - Nagaya, Kiyonobu

AU - Ito, Yuta

AU - Nishiyama, Toshiyuki

AU - Nicolas, Christophe

AU - Kumagai, Yoshiaki

AU - Iablonskyi, Denys

AU - Mondal, Subhendu

AU - Tachibana, Tetsuya

AU - You, Daehyun

AU - Yamada, Syuhei

AU - Sakakibara, Yuta

AU - Asa, Kazuki

AU - Sato, Yuhiro

AU - Sakai, Tsukasa

AU - Matsunami, Kenji

AU - Umemoto, Takayuki

AU - Kariyazono, Kango

AU - Kajimoto, Shinji

AU - Sotome, Hikaru

AU - Johnsson, Per

AU - Schöffler, Markus S.

AU - Kastirke, Gregor

AU - Kooser, Kuno

AU - Liu, Xiao Jing

AU - Asavei, Theodor

AU - Neagu, Liviu

AU - Molodtsov, Serguei

AU - Ochiai, Kohei

AU - Kanno, Manabu

AU - Yamazaki, Kaoru

AU - Owada, Shigeki

AU - Ogawa, Kanade

AU - Katayama, Tetsuo

AU - Togashi, Tadashi

AU - Tono, Kensuke

AU - Yabashi, Makina

AU - Ghosh, Aryya

AU - Gokhberg, Kirill

AU - Cederbaum, Lorenz S.

AU - Kuleff, Alexander I.

AU - Fukumura, Hiroshi

AU - Kishimoto, Naoki

AU - Rudenko, Artem

AU - Miron, Catalin

AU - Kono, Hirohiko

AU - Ueda, Kiyoshi

N1 - Funding Information: The XFEL experiments were performed at the BL3 of SACLA with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) and the program review committee (No. 2013B8058, 2015A8056, 2015B8057). This study was supported by the X-ray Free-Electron Laser Utilization Research Project and the X-ray Free-Electron Laser Priority Strategy Program of the Ministry of Education, Culture, Sports, Science, and Technology of Japan (MEXT), by the Proposal Program of SACLA Experimental Instruments of RIKEN, by the Japan Society for the Promotion of Science (JSPS) KAKENHI Grant Numbers JP15K17487, JP16H04091, JP18K05022, by “Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials” from the MEXT, by the Research Program of “Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials” in “Network Joint Research Center for Materials and Devices”, by European Research Council Advanced Investigator Grant no. 692657, and by the IMRAM project. T.Ta. gratefully acknowledges support by the JSPS KAKENHI Grant Number JP16J02270, E.K. the financial support by the Academy of Finland, D.Y. support by a Grant-in-Aid of Tohoku University Institute for Promoting Graduate Degree Programs Division for Interdisciplinary Advanced Research and Education. P.J. acknowledges support from the Swedish Research Council and the Swedish Foundation for Strategic Research, and A.I.K. by the DFG through QUTIF Priority Programme. K.Y. is grateful for the financial supports from Building of Consortia for the Development of Human Resources in Science and Technology by the MEXT. N.K. appreciates the support of the Cross-ministerial Strategic Innovation Promotion Program. A.R. was supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy under Grant No. DE-FG02-86ER13491. Publisher Copyright: © 2019, The Author(s).

PY - 2019/12/1

Y1 - 2019/12/1

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85065804889&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85065804889&partnerID=8YFLogxK

U2 - 10.1038/s41467-019-10060-z

DO - 10.1038/s41467-019-10060-z

M3 - Article

C2 - 31097703

AN - SCOPUS:85065804889

SN - 2041-1723

VL - 10

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 2186

ER -

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

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