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Photon-Modulated Bond Covalency of [Sm(II)(η9-C9H9)2].
Vitova, T; Ramanantoanina, H; Schacherl, B; Münzfeld, L; Hauser, A; Ekanayake, R S K; Reitz, C Y; Prüßmann, T; Neill, T S; Göttlicher, J; Steininger, R; Saveleva, V A; Haverkort, M W; Roesky, P W.
Affiliation
  • Vitova T; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Ramanantoanina H; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Schacherl B; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Münzfeld L; Institute for Inorganic Chemistry, Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Hauser A; Institute for Inorganic Chemistry, Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Ekanayake RSK; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Reitz CY; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Prüßmann T; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Neill TS; Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Göttlicher J; Institute for Photon Science and Synchrotron Radiation, Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Steininger R; Institute for Photon Science and Synchrotron Radiation, Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
  • Saveleva VA; ESRF, The European Synchrotron, 71 Avenue des Martyrs, CS40220, 38043 Grenoble Cedex 9, France.
  • Haverkort MW; Institute for Theoretical Physics, University of Heidelberg, Philosophenweg 19, D-69120 Heidelberg, Germany.
  • Roesky PW; Institute for Inorganic Chemistry, Karlsruhe Institute of Technology, P.O. 3640, D-76021 Karlsruhe, Germany.
J Am Chem Soc ; 2024 Jul 05.
Article in En | MEDLINE | ID: mdl-38968342
ABSTRACT
Lanthanides are widely assumed not to form covalent bonds due to the localized nature of their 4f valence electrons. This work demonstrates that the ionic bond of Sm(II) with cyclononatetraenyl (η9-C9H9-) in [Sm(η9-C9H9)2] can be modulated and becomes more covalent by photon-induced transfer of Sm 4f electrons to Sm 5d orbitals. This photon-induced change in bonding properties facilitates a subsequent reconfiguration of [Sm(η9-C9H9)2]. As a result, Sm-C bond length contraction is detected and the local Sm coordination environment exhibits more extensive disorder. Both Sm 4f and 5d electrons have increased participation in covalent Sm-ligand interactions. The Sm L3-edge valence band resonant inelastic X-ray scattering (VB-RIXS), high-resolution X-ray absorption near-edge structure (HR-XANES), and quantum chemical computations showcase a spectroscopic methodology for in-depth studies of bond covalency of lanthanide atoms.
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Full text: 1 Database: MEDLINE Language: En Year: 2024 Type: Article
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Full text: 1 Database: MEDLINE Language: En Year: 2024 Type: Article