X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C60), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C60 is considerably delayed. This work uncovers the persistence of the molecular structure of C60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.
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The data that support the findings of this study are available from the corresponding author on reasonable request.
The released version of the software underlying the findings of this study is available from Z.J. and R.S (at email@example.com). and more information is available at http://www.desy.de/~xraypac.
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This work was funded by the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy, grant nos. DE-SC0012376 (N.B., R.O. and H.X.) and DE-FG02-86ER13491 (D.R.). Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. We thank the Knut and Alice Wallenberg Foundation and the Swedish Research Council for support. This work was supported in part by the Hamburg Centre for Ultrafast Imaging centre of excellence of the Deutsche Forschungsgemeinschaft, EXC 1074, project ID 194651731 (Z.J., K.T., S.-K.S. and R.S.). A.S.-G. was funded by the Science and Technolgy Facilities Council (STFC). K.M., H.F. and K.U. acknowledge support by XFEL priority strategy program of MEXT. K.U. and H.F. acknowledge support by the Five-Star Alliance of the Network Joint Research Center of Materials and Devices, and by the TAGEN project. We thank A. LaForge for helpful discussions.
The authors declare no competing interests.
Peer review information Nature Physics thanks Carl Caleman and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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