Atomic-Scale Visualization of Ultrafast Bond Breaking in X-Ray-Excited Diamond

Ichiro Inoue, Yuka Deguchi, Beata Ziaja, Taito Osaka, Malik M. Abdullah, Zoltan Jurek, Nikita Medvedev, Victor Tkachenko, Yuichi Inubushi, Hidetaka Kasai, Kenji Tamasaku, Toru Hara, Eiji Nishibori, and Makina Yabashi

Phys. Rev. Lett. 126, 117403 – Published 19 March 2021

Abstract

Ultrafast changes of charge density distribution in diamond after irradiation with an intense x-ray pulse (photon energy, 7.8 keV; pulse duration, 6 fs; intensity, $3 \times 10^{19} W / {cm}^{2}$ ) have been visualized with the x-ray pump–x-ray probe technique. The measurement reveals that covalent bonds in diamond are broken and the electron distribution around each atom becomes almost isotropic within $\sim 5 fs$ after the intensity maximum of the x-ray pump pulse. The 15 fs time delay observed between the bond breaking and atomic disordering indicates nonisothermality of electron and lattice subsystems on this timescale. From these observations and simulation results, we interpret that the x-ray-induced change of the interatomic potential drives the ultrafast atomic disordering underway to the following nonthermal melting.

Received 1 June 2020
Revised 9 December 2020
Accepted 23 January 2021

DOI:https://doi.org/10.1103/PhysRevLett.126.117403

Physics Subject Headings (PhySH)

Atomic & molecular processes in external fields Ultrafast phenomena

Free-electron lasers Warm-dense matter

X-ray diffraction

Plasma PhysicsCondensed Matter, Materials & Applied PhysicsAtomic, Molecular & Optical

Authors & Affiliations

Ichiro Inoue^1,*,†, Yuka Deguchi^2,†, Beata Ziaja ^3,4,‡, Taito Osaka¹, Malik M. Abdullah³, Zoltan Jurek³, Nikita Medvedev^5,6, Victor Tkachenko^4,7,3, Yuichi Inubushi^8,1, Hidetaka Kasai^2,9, Kenji Tamasaku¹, Toru Hara¹, Eiji Nishibori ^2,9,§, and Makina Yabashi^1,8

¹RIKEN SPring-8 Center, 1-1-1 Kouto, Sayo, Hyogo 679-5148, Japan
²Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan
³Center of Free-Electron Laser Science, Deutsches Elektronen-Synchrotron, Notkestraße 85, 22607, Germany
⁴Institute of Nuclear Physics, Polish Academy of Sciences, Radzikowskiego 152, 31-342 Krakow, Poland
⁵Institute of Physics, Czech Academy of Sciences, Na Slovance 2, Prague 8, 18221, Czech Republic
⁶Institute of Plasma Physics, Czech Academy of Sciences, Za Slovankou 3, 182 00 Prague 8, Czech Republic
⁷European XFEL GmbH, Holzkoppel 4, 22869 Schenefeld, Germany
⁸Japan Synchrotron Radiation Research Institute, Kouto 1-1-1, Sayo, Hyogo 679-5198, Japan
⁹Faculty of Pure and Applied Sciences and Tsukuba Research Center for Energy Materials Science, University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan

^*inoue@spring8.or.jp
^†These authors contributed equally to this Letter.
^‡beata.ziaja-motyka@cfel.de
^§nishibori.eiji.ga@u.tsukuba.ac.jp

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Vol. 126, Iss. 11 — 19 March 2021

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