University of Oulu

Kukk, E., Fukuzawa, H., Niskanen, J., Nagaya, K., Kooser, K., You, D., Peschel, J., Maclot, S., Niozu, A., Saito, S., Luo, Y., Pelimanni, E., Itälä, E., Bozek, J. D., Takanashi, T., Berholts, M., Johnsson, P., & Ueda, K. (2021). Formative period in the x-ray-induced photodissociation of organic molecules. Physical Review Research, 3(1).

Formative period in the x-ray-induced photodissociation of organic molecules

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Author: Kukk, E.1; Fukuzawa, H.2,3; Niskanen, J.1;
Organizations: 1Department of Physics and Astronomy, University of Turku, FI-20014 Turku, Finland
2Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan
3RIKEN SPring-8 Center, Kouto 1-1-1, Sayo, Hyogo 679-5148, Japan
4Department of Physics, Kyoto University, Kyoto 606-8502, Japan
5Institute of Physics, University of Tartu, Wilhelm Ostwaldi 1, EE-50411 Tartu, Estonia
6Department of Physics, Lund University, SE-22100 Lund, Sweden
7Nano and Molecular Systems Research Unit, Faculty of Science, University of Oulu, FI-90014 Oulu, Finland
8Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, BP 48, FR-91192 Gif-sur-Yvette Cedex, France
Format: article
Version: published version
Access: open
Online Access: PDF Full Text (PDF, 4.3 MB)
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Language: English
Published: American Physical Society, 2021
Publish Date: 2021-05-14


Absorption of x-ray photons by atomic inner shells of light-element organics and biomolecules often leads to formation of dicationic electronic states and to molecular fragmentation. We investigated the x-ray-induced dissociation landscape of a representative medium-sized organic molecule, thiophene, by femtosecond x-ray pulses from the Super Photon Ring-8 GeV (SPring-8) Angstrom Compact Free-Electron Laser (SACLA). Holes, created in the sulfur 2p orbital by photoemission, were filled by the Auger process that created dicationic molecular states within a broad range of internal energies—a starting point particular to x-ray-induced dynamics. The evolution of the ionized molecules was monitored by a pump-probe experiment using a near-infrared (800 nm) laser pulse. Ion-ion coincidence and ion momentum analysis reveals enhanced yields of ionic fragments from multibody breakup of the ring, attributed to additional ionization of the highly excited fraction of the dicationic parent molecular states. The transient nature of the enhancement and its decay with about a 160-fs time constant indicate formation of an open-ring parent geometry and the statistical survival time of the parent species before the dissociation events. By probing specific Auger final states of transient, highly excited nature by near-infrared light, we demonstrate how pump-probe signatures can be related to the key features in dynamics during the early period of the x-ray-induced damage of organic molecules and biomolecules.

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Series: Physical review research
ISSN: 2643-1564
ISSN-E: 2643-1564
ISSN-L: 2643-1564
Volume: 3
Issue: 1
Article number: 013221
DOI: 10.1103/PhysRevResearch.3.013221
Type of Publication: A1 Journal article – refereed
Field of Science: 114 Physical sciences
Funding: 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 research program “Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials” at the Network Joint Research Center for Materials and Devices, by the IMRAM project, and by the Japan Society for the Promotion of Science (JSPS). E.K., J.N., and E.P. acknowledge financial support from the Academy of Finland, and D.Y. was supported by a grant-in-aid from Tohoku University Institute for Promoting Graduate Degree Programs, Division for Interdisciplinary Advanced Research and Education. J.P. and P.J. acknowledge support from the Swedish Research Council and the Swedish Foundation for Strategic Research.
Copyright information: © 2021 The Authors. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.