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Nonlinear spectral dispersion in resonant Auger scattering from SF6 for studying nuclear potentials and dynamics
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Theoretical Chemistry and Biology.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 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 110, no 6, article id 062814Article in journal (Refereed) 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.

Place, publisher, year, edition, pages
American Physical Society (APS) , 2024. Vol. 110, no 6, article id 062814
National Category
Atom and Molecular Physics and Optics Theoretical Chemistry
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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

Available from: 2025-01-07 Created: 2025-01-07 Last updated: 2025-01-21Bibliographically approved

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Kimberg, VictorGel'mukhanov, Faris

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