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Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics

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  • A. C. Laforge, Southern Connecticut State University, University of Freiburg
  • ,
  • R. Michiels, University of Freiburg
  • ,
  • Y. Ovcharenko, Technical University of Berlin
  • ,
  • A. Ngai, University of Freiburg
  • ,
  • J. M. Escartín, University of Barcelona
  • ,
  • N. Berrah, Southern Connecticut State University
  • ,
  • C. Callegari, Sincrotrone Trieste
  • ,
  • A. Clark, École Polytechnique Fédérale de Lausanne
  • ,
  • M. Coreno, CNR
  • ,
  • R. Cucini, Sincrotrone Trieste
  • ,
  • M. Di Fraia, Sincrotrone Trieste
  • ,
  • M. Drabbels, École Polytechnique Fédérale de Lausanne
  • ,
  • E. Fasshauer
  • ,
  • P. Finetti, Sincrotrone Trieste
  • ,
  • L. Giannessi, Sincrotrone Trieste, National Institute for Nuclear Physics
  • ,
  • C. Grazioli, National Institute for Nuclear Physics
  • ,
  • D. Iablonskyi, Tohoku University
  • ,
  • B. Langbehn, Technical University of Berlin
  • ,
  • T. Nishiyama, Kyoto University
  • ,
  • V. Oliver, École Polytechnique Fédérale de Lausanne
  • ,
  • P. Piseri, University of Milan
  • ,
  • O. Plekan, Sincrotrone Trieste
  • ,
  • K. C. Prince, Sincrotrone Trieste
  • ,
  • D. Rupp, Technical University of Berlin
  • ,
  • S. Stranges, University of Rome La Sapienza
  • ,
  • K. Ueda, Tohoku University
  • ,
  • N. Sisourat, Sorbonne Université
  • ,
  • J. Eloranta, California State University Northridge
  • ,
  • M. Pi, University of Barcelona
  • ,
  • M. Barranco, University of Barcelona
  • ,
  • F. Stienkemeier, University of Freiburg
  • ,
  • T. Möller, Technical University of Berlin
  • ,
  • M. Mudrich

Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of interatomic Coulombic decay (ICD) in resonantly excited helium nanodroplets using a high-resolution, tunable, extreme ultraviolet free-electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as short as 400 fs, nearly independent of the density of the excited states. Using a combination of time-dependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process, where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles, which drastically accelerates ICD.

OriginalsprogEngelsk
Artikelnummer021011
TidsskriftPhysical Review X
Vol/bind11
Nummer2
ISSN2160-3308
DOI
StatusUdgivet - apr. 2021

Bibliografisk note

Funding Information:
The authors gratefully acknowledge financial support from the Carl-Zeiss-Stiftung, the Deutsche Forschungsgemeinschaft (DFG) under Grant No. MO 719/14-2, within the frame of the Priority Program 1840 “Quantum Dynamics in Tailored Intense Fields” (MU 2347/12-1 and STI 125/22-2), and the Carlsberg Foundation. TDDFT work has been performed under Grant No. FIS2017-87801-P (AEI/FEDER, UE) (M. B. and M. P.). A. C. L. and N. B. acknowledge the support of the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy, Grant No. DE-SC0012376. D. R. acknowledges funding from Leibniz Grant No. SAW/2017/MBI4 and NCCR MUST of the Swiss National Science Foundation (SNF). J. E. acknowledges support from the National Science Foundation Grant No. DMR-1828019. J. M. E. acknowledges support from Ministerio de Ciencia e Innovación of Spain through the Unidades de Excelencia “María de Maeztu” Grant No. MDM-2017-0767.

Publisher Copyright:
© 2021 authors. Published by the American Physical Society.

Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.

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