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Observation of nuclear wave-packet interference in ultrafast interatomic energy transfer

We report the experimental observation of quantum interference in the nuclear wave-packet dynamics driving ultrafast excitation-energy transfer in argon dimers below the threshold of interatomic Coulombic decay (ICD). Using time-resolved photoion-photoion coincidence spectroscopy and quantum dynamic...

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Bibliographic Details
Main Authors: Han, Meng (Author) , Fedyk, Jacqueline (Author) , Ji, Jia-Bao (Author) , Despré, Victor (Author) , Kuleff, Alexander I. (Author) , Wörner, Hans Jakob (Author)
Format: Article (Journal)
Language:English
Published: 23 June 2023
In: Physical review letters
Year: 2023, Volume: 130, Issue: 25, Pages: 1-6
ISSN:1079-7114
DOI:10.1103/PhysRevLett.130.253202
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1103/PhysRevLett.130.253202
Verlag, lizenzpflichtig, Volltext: https://link.aps.org/doi/10.1103/PhysRevLett.130.253202
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Author Notes:Meng Han, Jacqueline Fedyk, Jia-Bao Ji, Victor Despré, Alexander I. Kuleff, and Hans Jakob Wörner
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Summary:We report the experimental observation of quantum interference in the nuclear wave-packet dynamics driving ultrafast excitation-energy transfer in argon dimers below the threshold of interatomic Coulombic decay (ICD). Using time-resolved photoion-photoion coincidence spectroscopy and quantum dynamics simulations, we reveal that the electronic relaxation dynamics of the inner-valence 3s hole on one atom leading to a 4s or 4p excitation on the other one is influenced by nuclear quantum dynamics in the initial state, giving rise to a deep, periodic modulation on the kinetic-energy-release (KER) spectra of the coincident Ar+−Ar+ ion pairs. Moreover, the time-resolved KER spectra show characteristic fingerprints of quantum interference effects during the energy-transfer process. Our findings pave the way to elucidating quantum-interference effects in ultrafast charge- and energy-transfer dynamics in more complex systems, such as molecular clusters and solvated molecules.
Item Description:Gesehen am 06.12.2023
Physical Description:Online Resource
ISSN:1079-7114
DOI:10.1103/PhysRevLett.130.253202

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