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Electron Dynamics in the Core-Excited CS2 Molecule Revealed through Resonant Inelastic X-Ray Scattering Spectroscopy
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2015 (English)In: Physical Review X, ISSN 2160-3308, Vol. 5, no 3, 031021Article in journal (Refereed) Published
Abstract [en]

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 excitation-energy 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 CS2 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.

Place, publisher, year, edition, pages
2015. Vol. 5, no 3, 031021
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Physical Sciences
URN: urn:nbn:se:kth:diva-173437DOI: 10.1103/PhysRevX.5.031021ISI: 000359870200001ScopusID: 2-s2.0-84946061151OAI: diva2:854899

QC 20150918

Available from: 2015-09-18 Created: 2015-09-11 Last updated: 2015-09-18Bibliographically approved

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da Cruz, V. VazGel'mukhanov, F.
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