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  Combined Experimental and Ab Initio Multireference Configuration Interaction Study of the Resonant Inelastic X-ray Scattering Spectrum of CO2

Maganas, D., Kristiansen, P., Duda, L.-C., Knop-Gericke, A., DeBeer, S., Schlögl, R., et al. (2014). Combined Experimental and Ab Initio Multireference Configuration Interaction Study of the Resonant Inelastic X-ray Scattering Spectrum of CO2. The Journal of Physical Chemistry C, 118(35), 20163-20175. doi:10.1021/jp505628y.

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Maganas, Dimitrios1, Author              
Kristiansen, Paw2, 3, Author
Duda, Laurent-Claudius3, Author
Knop-Gericke, Axel2, Author
DeBeer, Serena1, 4, Author              
Schlögl, Robert2, 5, Author              
Neese, Frank1, Author              
Affiliations:
1Research Department Neese, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023886              
2Inorganic Chemistry Department, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4−6, 14195 Berlin, Germany, ou_persistent22              
3Department of Physics and Astronomy, Division of Molecular and Condensed Matter Physics, Uppsala University, Box 516, S-751 20 Uppsala, Sweden, ou_persistent22              
4Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, United States, ou_persistent22              
5Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              

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 Abstract: The fundamental problem of the symmetry breaking in the resonant inelastic X-ray scattering (RIXS) of the CO2 gas molecule is studied. The measurements were performed under catalytically relevant conditions within an in-house constructed reaction cell. The experimental RIXS plane is constructed from a sequence of resonances, covering the near-edge X-ray absorption fine structure (NEXAFS) spectrum up to 539 eV. The spectra show significant sensitivity with respect to the excitation frequency. The NEXAFS absorption spectrum, as well as the corresponding RIXS spectra, is interpreted with the aid of multireference configuration interaction (MRCI) theory. In this framework, the configuration interaction space spans the space of the intermediate and final states with single and single–double excitations. The dynamic character of the RIXS spectra is investigated by considering the electronic–nuclear vibrational coupling with the bending and antisymmetric stretching vibrations in the important intermediate excited states. In addition, the vibronic coupling mechanism involving the Renner–Teller effect and the core–hole localization pseudo-Jahn–Teller effect of the intermediate states is fully considered. The physical origin of the observed spectral features is discussed qualitatively and quantitatively in terms of individual core-to-valence excitations and valence-to-core decays, respectively. The computational protocol presented here, based on multireference wave function ab initio theory, serves as an important reference for future theoretical and experimental applications of RIXS spectroscopy.

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Language(s): eng - English
 Dates: 2014-06-062014-08-202014-09-04
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jp505628y
 Degree: -

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Title: The Journal of Physical Chemistry C
  Abbreviation : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 118 (35) Sequence Number: - Start / End Page: 20163 - 20175 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766