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

被引：21

作者：

Fukuzawa, Hironobu ^{[1
,2
]}

Takanashi, Tsukasa ^{[1
]}

Kukk, Edwin ^{[3
]}

Motomura, Koji ^{[1
]}

Wada, Shin-iIchi ^{[2
,4
]}

Nagaya, Kiyonobu ^{[2
,5
]}

Ito, Yuta ^{[1
]}

Nishiyama, Toshiyuki ^{[5
]}

Nicolas, Christophe ^{[6
]}

Kumagai, Yoshiaki ^{[1
]}

Iablonskyi, Denys ^{[1
]}

Mondal, Subhendu ^{[1
]}

Tachibana, Tetsuya ^{[1
]}

You, Daehyun ^{[1
]}

Yamada, Syuhei ^{[1
]}

Sakakibara, Yuta ^{[1
]}

Asa, Kazuki ^{[5
]}

Sato, Yuhiro ^{[5
]}

Sakai, Tsukasa ^{[5
]}

Matsunami, Kenji ^{[5
]}

Umemoto, Takayuki ^{[4
]}

Kariyazono, Kango ^{[4
]}

Kajimoto, Shinji ^{[7
]}

Sotome, Hikaru ^{[7
]}

Johnsson, Per ^{[8
]}

Schoffler, Markus S. ^{[9
]}

Kastirke, Gregor ^{[9
]}

Kooser, Kuno ^{[3
]}

Liu, Xiao-Ding ^{[10
]}

Asavei, Theodor ^{[11
]}

Neagu, Liviu ^{[11
,12
]}

Molodtsov, Serguei ^{[13
,14
,15
]}

Ochiai, Kohei ^{[7
]}

Kanno, Manabu ^{[7
]}

Yamazaki, Kaoru ^{[16
]}

Owada, Shigeki ^{[2
]}

Ogawa, Kanade ^{[2
]}

Katayama, Tetsuo ^{[17
]}

Togashi, Tadashi ^{[17
]}

Tono, Kensuke ^{[17
]}

Yabashi, Makina ^{[2
]}

Ghosh, Aryya ^{[18
]}

Gokhberg, Kirill ^{[18
]}

Cederbaum, Lorenz S. ^{[18
]}

Kuleff, Alexander, I ^{[18
,19
]}

Fukumura, Hiroshi ^{[7
]}

Kishimoto, Naoki ^{[7
]}

Rudenko, Artem ^{[20
]}

Miron, Catalin ^{[6
,11
,21
]}

Kono, Hirohiko ^{[7
]}

机构：

[1] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Sendai, Miyagi 9808577, Japan

[2] RIKEN SPring 8 Ctr, Sayo, Hyogo 6795148, Japan

[3] Univ Turku, Dept Phys & Astron, FI-20014 Turku, Finland

[4] Hiroshima Univ, Dept Phys Sci, Higashihiroshima 7398526, Japan

[5] Kyoto Univ, Dept Phys, Kyoto 6068502, Japan

[6] Synchrotron SOLEIL, Orme Merisiers, BP 48, FR-91192 Gif Sur Yvette, France

[7] Tohoku Univ, Grad Sch Sci, Dept Chem, Sendai, Miyagi 9808578, Japan

[8] Lund Univ, Dept Phys, SE-22100 Lund, Sweden

[9] Goethe Univ Frankfurt, Inst Kernphys, Max von Laue Str 1, D-60438 Frankfurt, Germany

[10] Beihang Univ, Sch Phys & Nucl Energy Engn, Beijing 100191, Peoples R China

[11] Horia Hulubei Natl Inst Phys & Nucl Engn, ELI NP, Reactorului St, RO-07712530 Magurele, Jud Ilfov, Romania

[12] Natl Inst Laser Plasma & Radiat Phys, 409 Atomistilor,POB MG 36, Magurele 077125, Jud Ilfov, Romania

[13] European XFEL GmbH, Holzkoppel 4, D-22869 Schenefeld, Germany

[14] ITMO Univ, Kronverksky Pr 49, St Petersburg 197101, Russia

[15] Tech Univ Bergakad Freiberg, Inst Expt Phys, D-09599 Freiberg, Germany

[16] Tohoku Univ, Inst Mat Res, Sendai, Miyagi 9808577, Japan

[17] Japan Synchrotron Radiat Res Inst, Sayo, Hyogo 6795198, Japan

[18] Heidelberg Univ, PCI, Theoret Chem, D-69120 Heidelberg, Germany

[19] ELI ALPS, Budapesti Ut 5, H-6728 Szeged, Hungary

[20] Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA

[21] Univ Paris Saclay, CNRS, CEA, LIDYL,CEA Saclay, F-91191 Gif Sur Yvette, France

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

基金：

日本学术振兴会; 欧洲研究理事会; 芬兰科学院; 瑞典研究理事会;

关键词：

GREENS-FUNCTION; FEMTOSECOND; DYNAMICS; ENERGY; FRAGMENTATION; IONIZATION; MOLECULES; CHARGE; ATOMS;

D O I：

10.1038/s41467-019-10060-z

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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 realtime. 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 (similar to 20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (similar to 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.

引用

页数：8