학술논문
Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization
Document Type
Author
Berrah, N.; Sanchez-Gonzalez, A.; Jurek, Z.; Obaid, R.; Xiong, H.; Squibb, Richard 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, Raimund; Schulz, C.P.; Toyota, K.; Son, S.-K.; Ueda, K.; Pfeifer, T.; Marangos, J.P.; Santra, R.
Source
Nature Physics. 15:1279-1283
Subject
Language
English
ISSN
1745-2473
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 (C60), exposed to 640eV 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 (20fs) 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.