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Title: Ultrafast relaxation of photoexcited superfluid He nanodroplets

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5];  [4];  [5]; ORCiD logo [6]; ORCiD logo [5]; ORCiD logo [7];  [5]; ORCiD logo [8]; ORCiD logo [9];  [10]; ORCiD logo [11];  [12];  [13];  [5];  [5]; ORCiD logo [5] more »;  [11];  [14];  [15]; ORCiD logo [16]; ORCiD logo [17]; ORCiD logo [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)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; German Research Foundation (DFG); National Science Foundation (NSF); Carl-Zeiss-Stiftung; Swiss National Science Foundation (SNSF)
OSTI Identifier:
1599845
Grant/Contract Number:  
[AC02-05CH11231; DMR-1828019; FIS2017-87801-P]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
[ Journal Volume: 11; Journal Issue: 1]; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; atomic and molecular interactions with photons; macromolecules and clusters

Citation Formats

Mudrich, M., LaForge, A. C., Ciavardini, A., O’Keeffe, P., Callegari, C., Coreno, M., Demidovich, A., Devetta, M., Fraia, M. Di, Drabbels, M., Finetti, P., Gessner, O., Grazioli, C., Hernando, A., Neumark, D. M., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Ziemkiewicz, M. P., Möller, T., Eloranta, J., Pi, M., Barranco, M., and Stienkemeier, F. Ultrafast relaxation of photoexcited superfluid He nanodroplets. United States: N. p., 2020. Web. doi:10.1038/s41467-019-13681-6.
Mudrich, M., LaForge, A. C., Ciavardini, A., O’Keeffe, P., Callegari, C., Coreno, M., Demidovich, A., Devetta, M., Fraia, M. Di, Drabbels, M., Finetti, P., Gessner, O., Grazioli, C., Hernando, A., Neumark, D. M., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Ziemkiewicz, M. P., Möller, T., Eloranta, J., Pi, M., Barranco, M., & Stienkemeier, F. Ultrafast relaxation of photoexcited superfluid He nanodroplets. United States. doi:10.1038/s41467-019-13681-6.
Mudrich, M., LaForge, A. C., Ciavardini, A., O’Keeffe, P., Callegari, C., Coreno, M., Demidovich, A., Devetta, M., Fraia, M. Di, Drabbels, M., Finetti, P., Gessner, O., Grazioli, C., Hernando, A., Neumark, D. M., Ovcharenko, Y., Piseri, P., Plekan, O., Prince, K. C., Richter, R., Ziemkiewicz, M. P., Möller, T., Eloranta, J., Pi, M., Barranco, M., and Stienkemeier, F. Wed . "Ultrafast relaxation of photoexcited superfluid He nanodroplets". United States. doi:10.1038/s41467-019-13681-6. https://www.osti.gov/servlets/purl/1599845.
@article{osti_1599845,
title = {Ultrafast relaxation of photoexcited superfluid He nanodroplets},
author = {Mudrich, M. and LaForge, A. C. and Ciavardini, A. and O’Keeffe, P. and Callegari, C. and Coreno, M. and Demidovich, A. and Devetta, M. and Fraia, M. Di and Drabbels, M. and Finetti, P. and Gessner, O. and Grazioli, C. and Hernando, A. and Neumark, D. M. and Ovcharenko, Y. and Piseri, P. and Plekan, O. and Prince, K. C. and Richter, R. and Ziemkiewicz, M. P. and Möller, T. and Eloranta, J. and Pi, M. and Barranco, M. and Stienkemeier, F.},
abstractNote = {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.},
doi = {10.1038/s41467-019-13681-6},
journal = {Nature Communications},
number = [1],
volume = [11],
place = {United States},
year = {2020},
month = {1}
}

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