Triplet Excimer Formation in Platinum-Based Phosphors: A Theoretical Study of the Roles of Pt-Pt Bimetallic Interactions and Interligand π-π Interactions.

We have used density functional theory (DFT) and time-dependent DFT to investigate the geometric and electronic structure and the optical properties of the phosphorescent platinum compounds: Pt(II) (2-(4′,6′-difluorophenyl)pyridinato-N, C)(2,4-pentanedionato-O,O) (FPt1) and Pt(II) (2-(4′,6′-difluoro...

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Publicado en:Journal of the American Chemical Society Vol. 131; no. 32; pp. 11371 - 11381
Autores principales: Dongwook Kim, Brédas, Jean-Luc
Formato: Artículo
Publicado: American Chemical Society 8/19/2009
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 8/19/2009
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        atl: Triplet Excimer Formation in Platinum-Based Phosphors: A Theoretical Study of the Roles of Pt-Pt Bimetallic Interactions and Interligand π-π Interactions.
      aug:
        au:
          Dongwook Kim
          Brédas, Jean-Luc
        affil: School of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400
      su:
        Density functionals
        Functional analysis
        Electronic structure
        Optical properties
        Platinum compounds
        Phosphors
        Monomers
        Phosphorescence
      sug:
        subj:
          Density functionals
          Functional analysis
          Electronic structure
          Optical properties
          Platinum compounds
          Phosphors
          Monomers
          Phosphorescence
      ab: We have used density functional theory (DFT) and time-dependent DFT to investigate the geometric and electronic structure and the optical properties of the phosphorescent platinum compounds: Pt(II) (2-(4′,6′-difluorophenyl)pyridinato-N, C)(2,4-pentanedionato-O,O) (FPt1) and Pt(II) (2-(4′,6′-difluorophenyl)pyridinato-N,C)(1,3-propanedionato-O,O) (FPt0). We first examined isolated compounds (monomers) and evaluated their photophysical properties at the ground-state and lowest triplet excited-state (T) geometries; the characteristics of the S - T transitions are nearly identical in both compounds. Dimers of FPt0 and of FPt1 were then studied in order to shed light, at least qualitatively, on the respective role of Pt-Pt bimetallic interactions and interligand π-π interactions in the formation of excimer structures. While the Pt-Pt interactions are critical for excimer formation, the interligand π-π interactions also play a significant role in determining the optimal excimer geometry and the magnitude of the phosphorescence energy lowering in going from the monomer to the aggregated dimer. The distorted cofacial-type excimer structures found for FPt1, with a Pt-Pt distance around 2.9 A and interligand distances around 3.5-3.8 Å, lead to phosphorescence energy lowerings with respect to the monomer on the order of 0.7-0.96 eV, in very good agreement with experiment.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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