X-ray Emission Spectroscopy To Study Ligand Valence Orbitals in Mn Coordination Complexes.

We discuss a spectroscopic method to determine the character of chemical bonding and for the identification of metal ligands in coordination and bioinorganic chemistry. It is based on the analysis of satellite lines in X-ray emission spectra that arise from transitions between valence orbitals and t...

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Publicado en:Journal of the American Chemical Society Vol. 131; no. 36; pp. 13161 - 13168
Autores principales: Smolentsev, Grigory, Soldatov, Alexander V., Messinger, Johannes, Merz, Kathrin, Weyhermüller, Thomas, Bergmann, Uwe, Pushkar, Yulia, Junko, Junko, Yachandra, Vittal K., Glatzel, Pieter
Formato: Artículo
Publicado: American Chemical Society 9/16/2009
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 9/16/2009
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      pub: American Chemical Society
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        10.1021/ja808526m
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        atl: X-ray Emission Spectroscopy To Study Ligand Valence Orbitals in Mn Coordination Complexes.
      aug:
        au:
          Smolentsev, Grigory
          Soldatov, Alexander V.
          Messinger, Johannes
          Merz, Kathrin
          Weyhermüller, Thomas
          Bergmann, Uwe
          Pushkar, Yulia
          Junko, Junko
          Yachandra, Vittal K.
          Glatzel, Pieter
        affil:
          Faculty of Physics and Research Center for Nanoscale Structure of Matter, Southern Federal University, 344090 Rostov-on-Don, Russia
          Max-Planck Institute for Bioinorganic Chemistry, Stiftstr. 34-36, 45470 Mülheim, Germany
          Department of Chemistry, Umeå University, S-90187 Umeå, Sweden
          Stanford Synchrotron Radiation Lightsource, P.O. Box 20450 Stanford, California 94309
          Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720
          Department of Physics, Purdue University, West Lafayette, Indiana 47907
          European Synchrotron Radiation Facility, 6, rue Jules Horowitz, 38043 Grenoble, France
      su:
        X-ray spectroscopy
        Ligands (Chemistry)
        Manganese
        Density functionals
        Chemical research
      sug:
        subj:
          X-ray spectroscopy
          Ligands (Chemistry)
          Manganese
          Density functionals
          Chemical research
      ab: We discuss a spectroscopic method to determine the character of chemical bonding and for the identification of metal ligands in coordination and bioinorganic chemistry. It is based on the analysis of satellite lines in X-ray emission spectra that arise from transitions between valence orbitals and the metal ion is level (valence-to-core XES). The spectra, in connection with calculations based on density functional theory (DFT), provide information that is complementary to other spectroscopic techniques, in particular X-ray absorption (XANES and EXAFS). The spectral shape is sensitive to protonation of ligands and allows ligands, which differ only slightly in atomic number (e.g., C, N, O…), to be distinguished. A theoretical discussion of the main spectral features is presented in terms of molecular orbitals for a series of Mn model systems: [Mn(HO)], [Mn(HO)OH], and [Mn(HO)NH]. An application of the method, with comparison between theory and experiment, is presented for the solvated Mn ion in water and three Mn coordination complexes, namely [LMn(acac)N]BPh, [LMn(BOPh)(ClO)], and [LMn(acac)N]BPh, where L represents 1,4,7-trimethyl-1,4,7-triazacyclononane, acac stands for the 2,4-pentanedionate anion, and BOPh represents the 1,3-diphenyl-1,3-dibora-2-oxapropane-1,3-diolato dianion.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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