期刊
NATURE PHYSICS
卷 15, 期 12, 页码 1279-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41567-019-0665-7
关键词
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资金
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy [DE-SC0012376, DE-FG02-86ER13491]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- Knut and Alice Wallenberg Foundation
- Swedish Research Council
- Hamburg Centre for Ultrafast Imaging centre of excellence of the Deutsche Forschungsgemeinschaft [EXC 1074, 194651731]
- Science and Technolgy Facilities Council (STFC)
- XFEL priority strategy program of MEXT
- Five-Star Alliance of the Network Joint Research Center of Materials and Devices
- TAGEN project
- EPSRC [EP/R019509/1, EP/I032517/1] Funding Source: UKRI
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.
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