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Simulating fluorine K -edge resonant inelastic x-ray scattering of sulfur hexafluoride and the effect of dissociative dynamics

Banerjee, Ambar ; Da Cruz, Vinícius Vaz ; Ekholm, Victor LU ; Såthe, Conny LU ; Rubensson, Jan Erik ; Ignatova, Nina ; Gel'mukhanov, Faris and Odelius, Michael (2023) In Physical Review A 108(2).
Abstract

We report on a computational study of resonant inelastic x-ray scattering (RIXS), at different fluorine K-edge resonances of the SF6 molecule, and corresponding nonresonant x-ray emission. Previously measured polarization dependence in RIXS is reproduced and traced back to the local σ and π symmetry of the molecular orbitals and corresponding states involved in the RIXS process. Also electron-hole coupling energies are calculated and related to experimentally observed spectator shifts. The role of dissociative S-F bond dynamics is explored to model detuning of RIXS spectra at the |F1s-16a1g1) resonance, which shows challenges to accurately reproduce the required steepness for core-excited potential energy surface. We show that the RIXS... (More)

We report on a computational study of resonant inelastic x-ray scattering (RIXS), at different fluorine K-edge resonances of the SF6 molecule, and corresponding nonresonant x-ray emission. Previously measured polarization dependence in RIXS is reproduced and traced back to the local σ and π symmetry of the molecular orbitals and corresponding states involved in the RIXS process. Also electron-hole coupling energies are calculated and related to experimentally observed spectator shifts. The role of dissociative S-F bond dynamics is explored to model detuning of RIXS spectra at the |F1s-16a1g1) resonance, which shows challenges to accurately reproduce the required steepness for core-excited potential energy surface. We show that the RIXS spectra can only be properly described by considering breaking of the global inversion symmetry of the electronic wave function and core-hole localization, induced by vibronic coupling. Due to the core-hole localization we have symmetry forbidden transitions, which lead to additional resonances and changing width of the RIXS profile.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review A
volume
108
issue
2
article number
023103
publisher
American Physical Society
external identifiers
  • scopus:85167865095
ISSN
2469-9926
DOI
10.1103/PhysRevA.108.023103
language
English
LU publication?
yes
id
3435e7fa-7ee5-4a43-b4e0-4f4096cca767
date added to LUP
2023-12-08 11:50:13
date last changed
2023-12-08 11:50:48
@article{3435e7fa-7ee5-4a43-b4e0-4f4096cca767,
  abstract     = {{<p>We report on a computational study of resonant inelastic x-ray scattering (RIXS), at different fluorine K-edge resonances of the SF6 molecule, and corresponding nonresonant x-ray emission. Previously measured polarization dependence in RIXS is reproduced and traced back to the local σ and π symmetry of the molecular orbitals and corresponding states involved in the RIXS process. Also electron-hole coupling energies are calculated and related to experimentally observed spectator shifts. The role of dissociative S-F bond dynamics is explored to model detuning of RIXS spectra at the |F1s-16a1g1) resonance, which shows challenges to accurately reproduce the required steepness for core-excited potential energy surface. We show that the RIXS spectra can only be properly described by considering breaking of the global inversion symmetry of the electronic wave function and core-hole localization, induced by vibronic coupling. Due to the core-hole localization we have symmetry forbidden transitions, which lead to additional resonances and changing width of the RIXS profile.</p>}},
  author       = {{Banerjee, Ambar and Da Cruz, Vinícius Vaz and Ekholm, Victor and Såthe, Conny and Rubensson, Jan Erik and Ignatova, Nina and Gel'mukhanov, Faris and Odelius, Michael}},
  issn         = {{2469-9926}},
  language     = {{eng}},
  number       = {{2}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review A}},
  title        = {{Simulating fluorine K -edge resonant inelastic x-ray scattering of sulfur hexafluoride and the effect of dissociative dynamics}},
  url          = {{http://dx.doi.org/10.1103/PhysRevA.108.023103}},
  doi          = {{10.1103/PhysRevA.108.023103}},
  volume       = {{108}},
  year         = {{2023}},
}