Simulating fluorine K -edge resonant inelastic x-ray scattering of sulfur hexafluoride and the effect of dissociative dynamics
(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
- Banerjee, Ambar ; Da Cruz, Vinícius Vaz ; Ekholm, Victor LU ; Såthe, Conny LU ; Rubensson, Jan Erik ; Ignatova, Nina ; Gel'mukhanov, Faris and Odelius, Michael
- organization
- publishing date
- 2023-08
- 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}}, }