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- Hennies, F., et al.
(author)
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Dynamic interpretation of resonant x-ray Raman scattering : ethylene and benzene
- 2007
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In: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 76:3, s. 032505-
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Journal article (peer-reviewed)abstract
- We present a dynamic interpretation of resonant x-ray Raman scattering where vibrationally selective excitation into molecular resonances has been employed in comparison with excitation into higher lying continuum states for condensed ethylene and benzene as molecular model systems. In order to describe the purely vibrational spectral loss features and coupled electronic and vibrational losses the one-step theory for resonant soft x-ray scattering is applied, taking multiple vibrational modes and vibronic coupling into account. The scattering profile is found to be strongly excitation energy dependent and to reflect the intermediate states dynamics of the scattering process. In particular, the purely vibrational loss features allow one to map the electronic ground state potential energy surface in light of the excited state dynamics. Our study of ethylene and benzene underlines the necessity of an explicit description of the coupled electronic and vibrational loss features for the assignment of spectral features observed in resonant x-ray Raman scattering at polyatomic systems, which can be done in both a time independent and a time dependent picture. The possibility to probe ground state vibrational properties opens a perspective to future applications of this photon-in-photon-out spectroscopy.
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| 3. |
- Hennies, F., et al.
(author)
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Non-Adiabatic effects in Resonant Inelastic x-ray Scattering
- 2005
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In: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 95:16, s. 163002-
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Journal article (peer-reviewed)abstract
- We have studied the spectral features of resonant inelastic x-ray scattering of condensed ethylene with vibrational selectivity both experimentally and theoretically. Purely vibrational spectral loss features and coupled electronic and vibrational losses are observed. The one-step theory for resonant soft x-ray scattering is applied, taking multiple vibrational modes and vibronic coupling into account. Our investigation of ethylene underlines that the assignment of spectral features observed in resonant inelastic x-ray scattering of polyatomic systems requires an explicit description of the coupled electronic and vibrational loss features.
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