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Core-hole coherent spectroscopy in molecules

We study the ultrafast dynamics initiated by a coherent superposition of core-excited states of nitrous oxide molecule. Using high-level ab initio methods, we show that the decoherence caused by the electronic decay and the nuclear dynamics is substantially slower than the induced ultrafast quantum...

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Bibliographic Details
Main Authors: Rodríguez-Cuenca, Emilio (Author) , Picón, Antonio (Author) , Oberli, Solène (Author) , Kuleff, Alexander I. (Author) , Vendrell, Oriol (Author)
Format: Article (Journal)
Language:English
Published: 25 June 2024
In: Physical review letters
Year: 2024, Volume: 132, Issue: 26, Pages: 263202-1-263202-7
ISSN:1079-7114
DOI:10.1103/PhysRevLett.132.263202
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1103/PhysRevLett.132.263202
Verlag, lizenzpflichtig, Volltext: https://link.aps.org/doi/10.1103/PhysRevLett.132.263202
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Author Notes:Emilio Rodríguez-Cuenca, Antonio Picón, Solène Oberli, Alexander I. Kuleff, and Oriol Vendrell
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Summary:We study the ultrafast dynamics initiated by a coherent superposition of core-excited states of nitrous oxide molecule. Using high-level ab initio methods, we show that the decoherence caused by the electronic decay and the nuclear dynamics is substantially slower than the induced ultrafast quantum beatings, allowing the system to undergo several oscillations before it dephases. We propose a proof-of-concept experiment using the harmonic up-conversion scheme available at x-ray free-electron laser facilities to trace the evolution of the created core-excited-state coherence through a time-resolved x-ray photoelectron spectroscopy.
Item Description:Gesehen am 28.04.2025
Physical Description:Online Resource
ISSN:1079-7114
DOI:10.1103/PhysRevLett.132.263202

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