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Marcel Mudrich

Ultrafast relaxation of photoexcited superfluid He nanodroplets

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  • M. Mudrich
  • A. C. LaForge, University of Freiburg, Southern Connecticut State University
  • ,
  • A. Ciavardini, Consiglio Nazionale delle Ricerche, CERIC-ERIC
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  • P. O’Keeffe, Consiglio Nazionale delle Ricerche
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  • C. Callegari, Elettra-Sincrotrone Trieste S.C.p.A.
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  • M. Coreno, Consiglio Nazionale delle Ricerche
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  • A. Demidovich, Elettra-Sincrotrone Trieste S.C.p.A.
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  • M. Devetta, University of Milan, CNR-IFN
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  • M. Di Fraia, Elettra-Sincrotrone Trieste S.C.p.A.
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  • M. Drabbels, École Polytechnique Fédérale de Lausanne
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  • P. Finetti, Elettra-Sincrotrone Trieste S.C.p.A.
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  • O. Gessner, Lawrence Berkeley National Laboratory
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  • C. Grazioli, CNR
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  • A. Hernando, Kido Dynamics, CSIC
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  • D. M. Neumark, Lawrence Berkeley National Laboratory, UC Berkeley
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  • Y. Ovcharenko, Technical University of Berlin, European XFEL
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  • P. Piseri, University of Milan
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  • O. Plekan, Elettra-Sincrotrone Trieste S.C.p.A.
  • ,
  • K. C. Prince, Elettra-Sincrotrone Trieste S.C.p.A.
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  • R. Richter, Elettra-Sincrotrone Trieste S.C.p.A.
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  • M. P. Ziemkiewicz, Lawrence Berkeley National Laboratory, UC Berkeley
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  • T. Möller, Technical University of Berlin
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  • J. Eloranta, California State University Northridge
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  • M. Pi, Universitat Pompeu Fabra, Barcelona, University of Barcelona
  • ,
  • M. Barranco, Universitat Pompeu Fabra, Barcelona, University of Barcelona, Universite Toulouse III - Paul Sabatier
  • ,
  • F. Stienkemeier, University of Freiburg

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.

OriginalsprogEngelsk
Artikelnummer112
TidsskriftNature Communications
Vol/bind11
Nummer1
ISSN2041-1723
DOI
StatusUdgivet - 1 dec. 2020

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