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Ultrafast relaxation of photoexcited superfluid He nanodroplets

Journal Article · · Nature Communications
 [1];  [2];  [3];  [4];  [5];  [4];  [5];  [6];  [5];  [7];  [5];  [8];  [9];  [10];  [11];  [12];  [13];  [5];  [5];  [5] more »;  [11];  [14];  [15];  [16];  [17];  [18] « less
  1. Aarhus Univ. (Denmark)
  2. Univ. of Freiburg, Freiburg im Breisgau (Germany); Univ. of Connecticut, Storrs, CT (United States)
  3. Central European Research Infrastructure Consortium (CERIC–ERIC), Trieste (Italy); Italian National Research Council (CNR), Monterotondo Scalo (Italy)
  4. Italian National Research Council (CNR), Monterotondo Scalo (Italy)
  5. Elettra Sincrotrone Trieste (Italy)
  6. Italian National Research Council (CNR), Trieste (Italy); Univ. degli Studi, Milan (Italy)
  7. Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne (Switzerland)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  9. Italian National Research Council (CNR), Trieste (Italy)
  10. Kido Dynamics, Lausanne (Switzerland); Inst. de Fisica Interdisciplinar y Sistemas Complejos, Palma de Mallorca (Spain)
  11. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  12. European X-Ray Free-Electron Laser Facility (XFEL), Schenefeld (Germany); Inst. für Optik und Atomare Physik, Berlin (Germany)
  13. Univ. degli Studi, Milan (Italy)
  14. Inst. für Optik und Atomare Physik, Berlin (Germany)
  15. California State Univ., Northridge, CA (United States)
  16. Univ. de Barcelona (Spain)
  17. Univ. de Barcelona (Spain); Univ. Paul Sabatier-Toulouse (France)
  18. Univ. of Freiburg, Freiburg im Breisgau (Germany)
+ Show Author Affiliations
The relaxation of photoexcited nanosystems is a fundamental process of light-matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He*) within 1 ps. Subsequently, the bubble collapses and releases metastable He* at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
Carl-Zeiss-Stiftung; Deutsche Forschungsgemeinschaft; National Science Foundation (NSF); Swiss National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1599845
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
atomic and molecular interactions with photons
macromolecules and clusters