N. Berrah, Álvaro Sánchez-González, Zoltan Jurek, Razib Obaid, H. Xiong, R. J. Squibb, T. Osipov, A. Lutman, L. Fang, T. Barillot, J. D. Bozek, J. Cryan, T. J. A. Wolf, Daniel Rolles, R. Coffee, Kirsten Schnorr, S. Augustin, Hironobu Fukuzawa, K. Motomura, Nina Isabelle Niebuhr, L. J. Frasinski, Raimund Feifel, Claus-Peter Schulz, Kenji Toyota, Sang-Kil Son, K. Ueda, T. Pfeifer, J. P. Marangos, Robin Santra
- 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.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. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.…
MetadatenAuthor details: | N. Berrah, Álvaro Sánchez-GonzálezGND, Zoltan JurekGND, Razib ObaidORCiDGND, H. XiongORCiD, R. J. Squibb, T. Osipov, A. Lutman, L. Fang, T. Barillot, J. D. Bozek, J. Cryan, T. J. A. Wolf, Daniel RollesORCiDGND, R. Coffee, Kirsten SchnorrORCiDGND, S. Augustin, Hironobu FukuzawaORCiDGND, K. Motomura, Nina Isabelle NiebuhrORCiDGND, L. J. Frasinski, Raimund FeifelORCiDGND, Claus-Peter SchulzGND, Kenji ToyotaGND, Sang-Kil SonGND, K. Ueda, T. Pfeifer, J. P. Marangos, Robin SantraORCiDGND |
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DOI: | https://doi.org/10.1038/s41567-019-0665-7 |
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ISSN: | 1745-2473 |
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ISSN: | 1745-2481 |
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Title of parent work (English): | Nature physics |
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Publisher: | Nature Publ. Group |
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Place of publishing: | London |
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Publication type: | Article |
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Language: | English |
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Year of first publication: | 2019 |
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Publication year: | 2019 |
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Release date: | 2020/09/28 |
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Volume: | 15 |
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Issue: | 12 |
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Number of pages: | 7 |
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First page: | 1279 |
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Last Page: | 1301 |
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Funding institution: | Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of EnergyUnited States Department of Energy (DOE) [DE-SC0012376, DE-FG02-86ER13491]; US Department of Energy, Office of Science, Office of Basic Energy SciencesUnited States Department of Energy (DOE) [DE-AC02-76SF00515]; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation; Swedish Research CouncilSwedish Research Council; Hamburg Centre for Ultrafast Imaging centre of excellence of the Deutsche Forschungsgemeinschaft [EXC 1074, 194651731]; Science and Technolgy Facilities Council (STFC)Science & Technology Facilities Council (STFC); XFEL priority strategy program of MEXT; Five-Star Alliance of the Network Joint Research Center of Materials and Devices; TAGEN project |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
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DDC classification: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
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Peer review: | Referiert |
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