Determination of the Temperature Dependence of the H--D Spin--Spin Coupling Constant and the Isotope Effect on the Proton Chemical Shift for the Compressed Dihydride Complex [Cp★Ir(P- P)H].

Complex [Cp*lr(dmpm)H] (dmpm = bis(dimethylphosphino)methane) has been reported to display temperature-dependent spin-spin coupling constant (1 ) and isotope effect on the H NMR chemical shift (Δ&delta). A combined electronic structure density functional theory + quantum nuclear dynamics study is us...

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Publicado en:Journal of the American Chemical Society Vol. 127; no. 15; pp. 5632 - 5641
Autores principales: Gelabert, Ricard, Moreno, Miquel, Liuch, José M., Liedos, Agusti, Heinekey, D. Michael
Formato: Artículo
Publicado: American Chemical Society 4/20/2005
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Acceso en línea:Ver este registro en EBSCOhost
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        atl: Determination of the Temperature Dependence of the H--D Spin--Spin Coupling Constant and the Isotope Effect on the Proton Chemical Shift for the Compressed Dihydride Complex [Cp★Ir(P- P)H].
      aug:
        au:
          Gelabert, Ricard
          Moreno, Miquel
          Liuch, José M.
          Liedos, Agusti
          Heinekey, D. Michael
        affil:
          Departament de Qulmica, Universitat Autbnoma de Barcelona, 08193 Bellaterra, Barcelona, Spain.
          Department of Chemistry, Box 351700, University of Washington, Seattle, Washington 98195-1700.
      su:
        Particles (Nuclear physics)
        Electronic structure
        Density functionals
        Potential energy surfaces
        Quantum chemistry
        Line geometry
      sug:
        subj:
          Particles (Nuclear physics)
          Electronic structure
          Density functionals
          Potential energy surfaces
          Quantum chemistry
          Line geometry
      ab: Complex [Cp*lr(dmpm)H] (dmpm = bis(dimethylphosphino)methane) has been reported to display temperature-dependent spin-spin coupling constant (1 ) and isotope effect on the H NMR chemical shift (Δ&delta). A combined electronic structure density functional theory + quantum nuclear dynamics study is used to determine from first-principles the unusual temperature dependence of the spin-spin coupling constant. It is found that the potential energy surface describing the motion of the lr-H2 unit has a deeper minimum in the dihydride region and is characterized by important anharmonicities. These anomalies affect the nature of the vibrational states of the unit and are the main reason for the unusual temperature dependence of 1 and Δ&delta. These results suggest experimental tests to identify compressed dihydride transition metal complexes.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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