Electron Dynamics in the Core-ExcitedCS2Molecule Revealed through Resonant Inelastic X-Ray Scattering Spectroscopy
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We present an experimental and theoretical study of resonant inelastic x-ray scattering (RIXS) in the carbon disulphide CS 2 molecule near the sulfur K-absorption edge.We observe a strong evolution of the RIXS spectral profile with the excitation energy tuned below the lowest unoccupied molecular orbital (LUMO) absorption resonance.The reason for this is twofold.Reducing the photon energy in the vicinity of the LUMO absorption resonance leads to a relative suppression of the LUMO contribution with respect to the emission signal from the higher unoccupied molecular orbitals, which results in the modulation of the total RIXS profile.At even larger negative photon-energy detuning from the resonance, the excitationenergy dependence of the RIXS profile is dominated by the onset of electron dynamics triggered by a coherent excitation of multiple electronic states.Furthermore, our study demonstrates that in the hard x-ray regime, localization of the S 1s core hole occurs in CS 2 during the RIXS process because of the orientational dephasing of interference between the waves scattering on the two sulfur atoms.Core-hole localization leads to violation of the symmetry selection rules for the electron transitions observed in the spectra.
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This RIXS spectral evolution is understood as the onset of electron dynamics triggered by a coherent excitation of multiple electronic states.
“With theoretical support, we understood this evolution as the onset of electron dynamics triggered by a coherent excitation of multiple electronic states [31].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [31]
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Roadmap of ultrafast x-ray atomic and molecular physics
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- Authors
- Marchenko, T., Carniato, S., Journel, L., Guillemin, R., Kawerk, E., Žitnik, M., Kavčič, M., Bučar, K., Bohinc, R., Petric, M., Vaz da Cruz, V., Gel’mukhanov, F., & Simon, M.
- Affiliations
- Centre National de la Recherche Scientifique (FR)
- Jožef Stefan Institute (SI)
- Synchrotron SOLEIL (FR)
- ORCID
- Venue
- Physical Review X
- Publisher
- American Physical Society (APS)
- Published
- 2015-08-20
- Volume
- 5
- Issue
- 3
- Pages
- 031021
- ISSN
- 2160-3308 (ISSN-L)
- OpenAlex
- W2176143296
- Cited by
- 20
- References
- 50
- Citations by year
- 2026: 2 · 2025: 3 · 2023: 2 · 2021: 2 · 2019: 2 · 2018: 5 · 2017: 3 · 2016: 1
- FWCI
- 3.11
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Licence
- Locations
- Physical Review X (publishedVersion, cc-by)
- HAL (submittedVersion, cc-by)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- Javna Agencija za Raziskovalno Dejavnost RS (P1-0112)
- Vetenskapsrådet
- Agence Nationale de la Recherche
- Marie Curie ITN project SPRITE (317169)
- Laboratoire d’Excellence Physics Atoms Light Matter
- Investissements d’Avenir (ANR-10-LABX-0039)
- Topics
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Keywords
- carbon disulfide, core-excited states, sulfur K-edge, resonant inelastic X-ray scattering, core-hole localization, hard X-ray spectroscopy, symmetry selection rules, electron dynamics
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