Abstract
SynopsisWe present an experimental and theoretical study of resonant inelastic x-ray scattering (RIXS) in the CS2 molecule near the S 1s edge. We show that localization of the S 1s core-hole occurs in CS2 during the RIXS process due to the orientational dephasing of interference between the waves scattering on the two sulfur atoms. Strong evolution of the RIXS profile with the excitation energy far below the first absorption resonance reflects the onset of electron dynamics triggered by a coherent excitation of multiple electronic states.
Highlights
Excitation of a molecule with a high-energy photon leads to an ultrafast dynamic response involving nuclear and electronic degrees of freedom
Reducing the photon energy in the vicinity of the lowest unoccupied molecular orbital (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
The measured S Kβ RIXS spectra result from the excitation of the S 1s electrons to the unoccupied molecular orbitals (MO) accompanied by the decay of the valence-shell electrons to the S 1s core hole and the emission of an x-ray photon
Summary
Excitation of a molecule with a high-energy photon leads to an ultrafast dynamic response involving nuclear and electronic degrees of freedom. To the time-resolved measurements using ultrafast laser sources, the nuclear and electron dynamics can be successfully studied in the x-ray energy domain using a technique known as “core-hole clock” spectroscopy based on core-level excitation and decay. This method uses the lifetime of the intermediate core-hole state as an internal reference clock for the temporal evolution of different processes like ultrafast dissociation of core-excited. The short lifetime of deep core-hole states, accessible with hard x-ray radiation, prevents molecules from changing their orientation during x-ray scattering, which allows one to obtain detailed information on the anisotropy of molecular orbitals using polarized x-ray fluorescence [3]
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