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  Restricted Open-Shell Configuration Interaction Singles Study on M- and L-edge X-ray Absorption Spectroscopy of Solid Chemical Systems

Kubas, A., Verkamp, M., Vura-Weis, J., Neese, F., & Maganas, D. (2018). Restricted Open-Shell Configuration Interaction Singles Study on M- and L-edge X-ray Absorption Spectroscopy of Solid Chemical Systems. Journal of Chemical Theory and Computation, 14(8), 4320-4334. doi:10.1021/acs.jctc.8b00302.

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 Creators:
Kubas, Adam1, 2, Author
Verkamp, Max3, Author
Vura-Weis, Josh3, Author
Neese, Frank1, 4, Author              
Maganas, Dimitrios1, 5, Author              
Affiliations:
1Max Planck Institute for Chemical Energy Conversion, Stiftstr. 34−36, 45470 Mülheim an der Ruhr, Germany, ou_persistent22              
2Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warsaw, Poland, ou_persistent22              
3Department of Chemistry, University of Illinois, 600 South Matthews Avenue, Urbana, Illinois 61801, United States, ou_persistent22              
4Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              
5Research Group Manganas, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541709              

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 Abstract: In this study the M- and L-edge X-ray absorption spectra of a series of open- and closed-shell solids (TiO2 rutile, α-Fe2O3 hematite, FeS2 pyrite, and the spinel Co3O4) are investigated with the restricted open-shell configuration interaction singles methods (ROCIS/DFT and PNO-ROCIS/DFT) using the embedded cluster approach. ROCIS/DFT type of methods are grounded in wave function-based ab initio electronic structure theory and have shown great performance in the field of X-ray spectroscopy in particular in the field of transition metal L-edge spectroscopy. In this work we show that ROCIS/DFT can be used to calculate and interpret metal M- and L-edge XAS spectra of solids. To this end, clusters with up to 52 metal centers are considered. In all cases good to excellent agreement between theory and experiment is obtained. The experimentally probed local coordination environments are discussed in detail. The physical origin of the observed spectral features is explored through the machinery of natural difference orbitals. This analysis provides valuable information with respect to the core to valence, metal to metal charge transfer, and metal to ligand charge transfer characters of the relativistically corrected many particle states. The influence of the above electronic effects to the spectral shapes and the size of the treated clusters are thoroughly investigated.

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Language(s): eng - English
 Dates: 2018-03-272018-06-272018-08-14
 Publication Status: Published in print
 Pages: 15
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jctc.8b00302
 Degree: -

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Title: Journal of Chemical Theory and Computation
  Other : J. Chem. Theory Comput.
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 14 (8) Sequence Number: - Start / End Page: 4320 - 4334 Identifier: ISSN: 1549-9618
CoNE: https://pure.mpg.de/cone/journals/resource/111088195283832