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 (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.

Authors:

Berrah, N.  ^[1];

• Search DOE PAGES for author "Berrah, N."
• Search DOE PAGES for ORCID "0000-0003-3231-1164"

Sanchez-Gonzalez, A.  ^[2];

• Search DOE PAGES for author "Sanchez-Gonzalez, A."
• Search DOE PAGES for ORCID "0000-0001-5055-5790"

Jurek, Z. ^[3]; Obaid, R.  ^[1];

• Search DOE PAGES for author "Obaid, R."
• Search DOE PAGES for ORCID "0000-0002-1759-4752"

Xiong, H. ^[1]; Squibb, R. J. ^[4]; Osipov, T. ^[5]; Lutman, A. ^[5]; Fang, L. ^[6]; Barillot, T. ^[2]; Bozek, J. D. ^[7]; Cryan, J. ^[8]; Wolf, T. J. A.  ^[8];

• Search DOE PAGES for author "Wolf, T. J. A."
• Search DOE PAGES for ORCID "0000-0002-0641-1279"

Rolles, D. ^[9]; Coffee, R. ^[5]; Schnorr, K. ^[10]; Augustin, S. ^[9]; Fukuzawa, H.  ^[11];

• Search DOE PAGES for author "Fukuzawa, H."
• Search DOE PAGES for ORCID "0000-0002-8283-381X"

Motomura, K. ^[11]; Niebuhr, N.  ^[12]

• Search DOE PAGES for author "Niebuhr, N."
• Search DOE PAGES for ORCID "0000-0003-2692-6461"

more »; Frasinski, L. J. ^[2]; Feifel, R. ^[4]; Schulz, C. P. ^[13]; Toyota, K. ^[3]; Son, S. -K.  ^[3];

• Search DOE PAGES for author "Son, S. -K."
• Search DOE PAGES for ORCID "0000-0001-5395-632X"

Ueda, K. ^[11]; Pfeifer, T. ^[10]; Marangos, J. P.  ^[2];

• Search DOE PAGES for author "Marangos, J. P."
• Search DOE PAGES for ORCID "0000-0001-7169-6955"

Santra, R.  ^[14]

• Search DOE PAGES for author "Santra, R."
• Search DOE PAGES for ORCID "0000-0002-1442-9815"

« less

---

+ Show Author Affiliations

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:

Mon Sep 23 00:00:00 EDT 2019

Research Org.:

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and 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