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Title: Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization

Abstract

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 (C 60), 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 C 60 is considerably delayed. This work uncovers the persistence of the molecular structure of C 60, 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. In conclusion, these findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [1];  [1];  [4];  [5];  [5];  [6];  [2];  [7];  [8]; ORCiD logo [8];  [9];  [5];  [10];  [9]; ORCiD logo [11];  [11]; ORCiD logo [12] more »;  [2];  [4];  [13];  [3]; ORCiD logo [3];  [11];  [10]; ORCiD logo [2]; ORCiD logo [14] « less
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Imperial College, London (United Kingdom)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
  4. Univ. of Gothenburg (Sweden)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  6. Univ. of Texas, Austin, TX (United States). Center for High Energy Density Science
  7. Synchrotron SOLEIL, L’Orme des Merisiers, Saint Aubin, Gif-sur-Yvette (France)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  9. Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab.
  10. Max-Planck-Inst. für Kernphysik, Heidelberg (Germany)
  11. Tohoku Univ., Sendai (Japan). Inst. of Multidisciplinary Research for Advanced Materials
  12. Univ. of Potsdam, Potsdam (Germany). Inst. für Physik und Astronomie
  13. Max Born Inst., Berlin (Germany)
  14. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science; Univ. of Hamburg (Germany)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC); Science and Technolgy Facilities Council (STFC), United Kingdom
OSTI Identifier:
1595137
Grant/Contract Number:  
AC02-76SF00515; FG02-86ER13491; SC0012376
Resource Type:
Accepted Manuscript
Journal Name:
Nature Physics
Additional Journal Information:
Journal Volume: 15; Journal Issue: 12; Journal ID: ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Berrah, N., Sanchez-Gonzalez, A., Jurek, Z., Obaid, R., Xiong, H., Squibb, R. J., Osipov, T., Lutman, A., Fang, L., Barillot, T., Bozek, J. D., Cryan, J., Wolf, T. J. A., Rolles, D., Coffee, R., Schnorr, K., Augustin, S., Fukuzawa, H., Motomura, K., Niebuhr, N., Frasinski, L. J., Feifel, R., Schulz, C. P., Toyota, K., Son, S. -K., Ueda, K., Pfeifer, T., Marangos, J. P., and Santra, R. Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization. United States: N. p., 2019. Web. doi:10.1038/s41567-019-0665-7.
Berrah, N., Sanchez-Gonzalez, A., Jurek, Z., Obaid, R., Xiong, H., Squibb, R. J., Osipov, T., Lutman, A., Fang, L., Barillot, T., Bozek, J. D., Cryan, J., Wolf, T. J. A., Rolles, D., Coffee, R., Schnorr, K., Augustin, S., Fukuzawa, H., Motomura, K., Niebuhr, N., Frasinski, L. J., Feifel, R., Schulz, C. P., Toyota, K., Son, S. -K., Ueda, K., Pfeifer, T., Marangos, J. P., & Santra, R. Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization. United States. doi:10.1038/s41567-019-0665-7.
Berrah, N., Sanchez-Gonzalez, A., Jurek, Z., Obaid, R., Xiong, H., Squibb, R. J., Osipov, T., Lutman, A., Fang, L., Barillot, T., Bozek, J. D., Cryan, J., Wolf, T. J. A., Rolles, D., Coffee, R., Schnorr, K., Augustin, S., Fukuzawa, H., Motomura, K., Niebuhr, N., Frasinski, L. J., Feifel, R., Schulz, C. P., Toyota, K., Son, S. -K., Ueda, K., Pfeifer, T., Marangos, J. P., and Santra, R. Mon . "Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization". United States. doi:10.1038/s41567-019-0665-7.
@article{osti_1595137,
title = {Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization},
author = {Berrah, N. and Sanchez-Gonzalez, A. and Jurek, Z. and Obaid, R. and Xiong, H. and Squibb, R. J. and Osipov, T. and Lutman, A. and Fang, L. and Barillot, T. and Bozek, J. D. and Cryan, J. and Wolf, T. J. A. and Rolles, D. and Coffee, R. and Schnorr, K. and Augustin, S. and Fukuzawa, H. and Motomura, K. and Niebuhr, N. and Frasinski, L. J. and Feifel, R. and Schulz, C. P. and Toyota, K. and Son, S. -K. and Ueda, K. and Pfeifer, T. and Marangos, J. P. and Santra, R.},
abstractNote = {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. In conclusion, these findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.},
doi = {10.1038/s41567-019-0665-7},
journal = {Nature Physics},
number = 12,
volume = 15,
place = {United States},
year = {2019},
month = {9}
}

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