Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics

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 n...

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Autores principales: A. C. LaForge, R. Michiels, Y. Ovcharenko, A. Ngai, J. M. Escartín, N. Berrah, C. Callegari, A. Clark, M. Coreno, R. Cucini, M. Di Fraia, M. Drabbels, E. Fasshauer, P. Finetti, L. Giannessi, C. Grazioli, D. Iablonskyi, B. Langbehn, T. Nishiyama, V. Oliver, P. Piseri, O. Plekan, K. C. Prince, D. Rupp, S. Stranges, K. Ueda, N. Sisourat, J. Eloranta, M. Pi, M. Barranco, F. Stienkemeier, T. Möller, M. Mudrich
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Lenguaje:EN
Publicado: American Physical Society 2021
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spelling oai:doaj.org-article:d4ee68ea54634871b1ba75b6c4e767d82021-12-02T14:22:59ZUltrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics10.1103/PhysRevX.11.0210112160-3308https://doaj.org/article/d4ee68ea54634871b1ba75b6c4e767d82021-04-01T00:00:00Zhttp://doi.org/10.1103/PhysRevX.11.021011http://doi.org/10.1103/PhysRevX.11.021011https://doaj.org/toc/2160-3308Interatomic 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.A. C. LaForgeR. MichielsY. OvcharenkoA. NgaiJ. M. EscartínN. BerrahC. CallegariA. ClarkM. CorenoR. CuciniM. Di FraiaM. DrabbelsE. FasshauerP. FinettiL. GiannessiC. GrazioliD. IablonskyiB. LangbehnT. NishiyamaV. OliverP. PiseriO. PlekanK. C. PrinceD. RuppS. StrangesK. UedaN. SisouratJ. ElorantaM. PiM. BarrancoF. StienkemeierT. MöllerM. MudrichAmerican Physical SocietyarticlePhysicsQC1-999ENPhysical Review X, Vol 11, Iss 2, p 021011 (2021)
institution DOAJ
collection DOAJ
language EN
topic Physics
QC1-999
spellingShingle Physics
QC1-999
A. C. LaForge
R. Michiels
Y. Ovcharenko
A. Ngai
J. M. Escartín
N. Berrah
C. Callegari
A. Clark
M. Coreno
R. Cucini
M. Di Fraia
M. Drabbels
E. Fasshauer
P. Finetti
L. Giannessi
C. Grazioli
D. Iablonskyi
B. Langbehn
T. Nishiyama
V. Oliver
P. Piseri
O. Plekan
K. C. Prince
D. Rupp
S. Stranges
K. Ueda
N. Sisourat
J. Eloranta
M. Pi
M. Barranco
F. Stienkemeier
T. Möller
M. Mudrich
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
description 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.
format article
author A. C. LaForge
R. Michiels
Y. Ovcharenko
A. Ngai
J. M. Escartín
N. Berrah
C. Callegari
A. Clark
M. Coreno
R. Cucini
M. Di Fraia
M. Drabbels
E. Fasshauer
P. Finetti
L. Giannessi
C. Grazioli
D. Iablonskyi
B. Langbehn
T. Nishiyama
V. Oliver
P. Piseri
O. Plekan
K. C. Prince
D. Rupp
S. Stranges
K. Ueda
N. Sisourat
J. Eloranta
M. Pi
M. Barranco
F. Stienkemeier
T. Möller
M. Mudrich
author_facet A. C. LaForge
R. Michiels
Y. Ovcharenko
A. Ngai
J. M. Escartín
N. Berrah
C. Callegari
A. Clark
M. Coreno
R. Cucini
M. Di Fraia
M. Drabbels
E. Fasshauer
P. Finetti
L. Giannessi
C. Grazioli
D. Iablonskyi
B. Langbehn
T. Nishiyama
V. Oliver
P. Piseri
O. Plekan
K. C. Prince
D. Rupp
S. Stranges
K. Ueda
N. Sisourat
J. Eloranta
M. Pi
M. Barranco
F. Stienkemeier
T. Möller
M. Mudrich
author_sort A. C. LaForge
title Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
title_short Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
title_full Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
title_fullStr Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
title_full_unstemmed Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
title_sort ultrafast resonant interatomic coulombic decay induced by quantum fluid dynamics
publisher American Physical Society
publishDate 2021
url https://doaj.org/article/d4ee68ea54634871b1ba75b6c4e767d8
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