Dataset Information

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.

SUBMITTER: Fukuzawa H

PROVIDER: S-EPMC6522627 | biostudies-literature | 2019 May

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH<sub>2</sub>I<sub>2</sub>.

Fukuzawa Hironobu H Takanashi Tsukasa T Kukk Edwin E Motomura Koji K Wada Shin-Ichi SI Nagaya Kiyonobu K Ito Yuta Y Nishiyama Toshiyuki T Nicolas Christophe C Kumagai Yoshiaki Y Iablonskyi Denys D Mondal Subhendu S Tachibana Tetsuya T You Daehyun D Yamada Syuhei S Sakakibara Yuta Y Asa Kazuki K Sato Yuhiro Y Sakai Tsukasa T Matsunami Kenji K Umemoto Takayuki T Kariyazono Kango K Kajimoto Shinji S Sotome Hikaru H Johnsson Per P Schöffler Markus S MS Kastirke Gregor G Kooser Kuno K Liu Xiao-Jing XJ Asavei Theodor T Neagu Liviu L Molodtsov Serguei S Ochiai Kohei K Kanno Manabu M Yamazaki Kaoru K Owada Shigeki S Ogawa Kanade K Katayama Tetsuo T Togashi Tadashi T Tono Kensuke K Yabashi Makina M Ghosh Aryya A Gokhberg Kirill K Cederbaum Lorenz S LS Kuleff Alexander I AI Fukumura Hiroshi H Kishimoto Naoki N Rudenko Artem A Miron Catalin C Kono Hirohiko H Ueda Kiyoshi K

Nature communications 20190516 1

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 femtos ...[more]

PMID: 31097703

Similar Datasets

Project description:The spontaneous crystal surface reconstruction of M-plane α-Al2O3 is employed for nanopatterning and nanofabrication in various fields of research including, among others, magnetism, superconductivity, and optoelectronics. In this reconstruction process the crystalline surface transforms from a planar morphology to one with a nanoscale ripple patterning. However, the high sample temperature required to induce surface reconstruction made in situ studies of the process seem unfeasible. The kinetics of ripple pattern formation therefore remained uncertain, and thus production of templates for nanofabrication could not advance beyond a trial-and-error stage. We present an approach combining in situ real-time grazing incidence small-angle X-ray scattering experiments (GISAXS) with model-based analysis and with ex situ atomic force microscopy (AFM) to observe this morphological transition in great detail. Our approach provides time-resolved information about all relevant morphological parameters required to trace the surface topography on the nanometer scale during reconstruction, i.e., the time dependence of the pattern wavelength, the ripple length, width, and height, and thus their facet angles. It offers a comprehensive picture of this process exemplified by a M-plane α-Al2O3 surface annealed at 1325 °C for 930 min. Fitting the model parameters to the experimental GISAXS data revealed a Johnson-Mehl-Avrami-Kolmogorov type of behavior for the pattern wavelength and a predominantly linear time dependence of the other parameters. In this case the reconstruction resulted in a crystalline surface fully patterned with asymmetric ripple-shaped nanostructures of 75 nm periodicity, 15 nm in height, and 630 nm in length. By elucidating the time dependence of these morphological parameters, this study shows a powerful way to significantly advance the predictability of annealing outcome and thus to efficiently customize nanopatterned α-Al2O3 templates for improved nanofabrication routines.

Dataset Information

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

Publications

Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH<sub>2</sub>I<sub>2</sub>.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Dataset Information

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

Publications

Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH<sub>2</sub>I<sub>2</sub>.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

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