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Nonlinear spectral dispersion in resonant Auger scattering from SF6 for studying nuclear potentials and dynamics
KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Kemi, Teoretisk kemi och biologi.ORCID-id: 0000-0003-1269-8760
Sorbonne Université, CNRS, UMR 7614, Laboratoire de Chimie Physique-Matiére et Rayonnement, F-75005 Paris, France; Synchrotron SOLEIL, l'Orme des Merisiers, Saint-Aubin, BP 48, F-91192 Gif-sur-Yvette Cedex, France.
International Research Center of Spectroscopy and Quantum Chemistry - IRC SQC, Siberian Federal University, 660041 Krasnoyarsk, Russia.
Sorbonne Université, CNRS, UMR 7614, Laboratoire de Chimie Physique-Matiére et Rayonnement, F-75005 Paris, France.
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2024 (Engelska)Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 110, nr 6, artikel-id 062814Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

In this study, we integrate experimental observations and theoretical models to elucidate the complex phenomena observed in the resonant S K-edge KLL Auger scattering spectra of the SF6 molecule. A two-dimensional spectral map, constructed of incident photon energy and kinetic energy of the emitted Auger electron, is shown to be a versatile tool for understanding a character of the core-excited potential energy surface and change of the molecular geometry. Our findings reveal how the distinct dispersion behavior of multiple spectral lines enables mapping of ultrafast dynamics within the short-lived core-excited states. Our results confirm the presence of nuclear dynamics in the S1s-16a1g1 and S1s-16t1u1 core-excited states, while dynamics is absent in the S1s-17t1u1 state. Using a combination of ab initio analysis, simulations with Coulomb model potentials, and a simple analytical approximation, we qualitatively demonstrate how the varying characteristics of spectral dispersion - classified as Raman, non-Raman, and anti-Raman - mirror the relative gradients of the intermediate and final states in the resonant x-ray scattering process. This insight allows for the effective mapping of molecular potential energy curves, offering a prospective tool on the underlying mechanisms of resonant Auger scattering and its potential for probing molecular dynamics.

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American Physical Society (APS) , 2024. Vol. 110, nr 6, artikel-id 062814
Nationell ämneskategori
Atom- och molekylfysik och optik Teoretisk kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-358230DOI: 10.1103/PhysRevA.110.062814ISI: 001390164100001Scopus ID: 2-s2.0-85213023707OAI: oai:DiVA.org:kth-358230DiVA, id: diva2:1924864
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QC 20250121

Tillgänglig från: 2025-01-07 Skapad: 2025-01-07 Senast uppdaterad: 2025-01-21Bibliografiskt granskad

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Kimberg, VictorGel'mukhanov, Faris

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Physical Review A: covering atomic, molecular, and optical physics and quantum information
Atom- och molekylfysik och optikTeoretisk kemi

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