Temperature Dependence of Blue Phosphorescent Cyclometalated Ir(III) Complexes.

The photophysical properties for a series of facial (fac) cyclometalated Ir(III) complexes (fac-Ir(C^N) (C^N = 2-phenylpyridyl (ppy), 2-(4,6-difluorophenyl)pyridyl (F2ppy), 1 -phenylpyrazolyl (ppz), 1-(2,4-difluorophenyl)pyrazolyl) (F2ppz), and 1-(2-(9,9′-dimethylfluorenyl))pyrazolyl (fIz)), fac-lr(...

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Publicado en:Journal of the American Chemical Society Vol. 131; no. 28; pp. 9813 - 9823
Autores principales: Sajoto, Tissa, Djurovich, Peter I., Tamayo, Arnold B., Oxgaard, Jonas, Goddard III, William A., Thompson, Mark E.
Formato: Artículo
Publicado: American Chemical Society 7/22/2009
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 7/22/2009
      vid: 131
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      pub: American Chemical Society
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        43815288
        10.1021/ja903317w
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      tig:
        atl: Temperature Dependence of Blue Phosphorescent Cyclometalated Ir(III) Complexes.
      aug:
        au:
          Sajoto, Tissa
          Djurovich, Peter I.
          Tamayo, Arnold B.
          Oxgaard, Jonas
          Goddard III, William A.
          Thompson, Mark E.
        affil:
          Department of Chemistry, University of Southern California, Los Angeles, California 90089
          Department of Chemistry, California Institute of Technology, Pasadena, California 91125
      su:
        Photophores
        Density functionals
        Ligands (Chemistry)
        Biochemistry
        Immobilized ligands (Biochemistry)
        Low temperatures
        Mathematical complexes
      sug:
        subj:
          Photophores
          Density functionals
          Ligands (Chemistry)
          Biochemistry
          Immobilized ligands (Biochemistry)
          Low temperatures
          Mathematical complexes
      ab: The photophysical properties for a series of facial (fac) cyclometalated Ir(III) complexes (fac-Ir(C^N) (C^N = 2-phenylpyridyl (ppy), 2-(4,6-difluorophenyl)pyridyl (F2ppy), 1 -phenylpyrazolyl (ppz), 1-(2,4-difluorophenyl)pyrazolyl) (F2ppz), and 1-(2-(9,9′-dimethylfluorenyl))pyrazolyl (fIz)), fac-lr(C^N)(C^N′) (C^N = ppz or F2ppz and C^N′ = ppy or F2ppy), and fac-Ir(C^C′)3 (C^C′ = 1-phenyl-3-methylbenzimidazolyl (pmb)) have been studied in dilute 2-methyltetrahydrofuran (2-MeTHF) solution in a temperature range of 77-378 K. Photoluminescent quantum yields (Φ) for the 10 compounds at room temperature vary between near zero and unity, whereas all emit with high efficiency at low temperature (77 K). The quantum yield for fac-Ir(ppy) (Φ = 0.97) is temperature-independent. For the other complexes, the temperature-dependent data indicates that the luminescent efficiency is primarily determined by thermal deactivation to a nonradiative state. Activation energies and rate constants for both radiative and nonradiative processes were obtained using a Boltzmann analysis of the temperature-dependent luminescent decay data. Activation energies to the nonradiative state are found to range between 1600 and 4800 cm. The pre-exponential factors for deactivation are large for complexes with C^N ligands (10-10 s) and significantly smaller for fac-Ir(pmb) (10 s). The kinetic parameters for decay and results from density functional theory (DFT) calculations of the triplet state are consistent with a nonradiative process involving Ir-N (Ir-C for fac-Ir(pmb)) bond rupture leading to a five-coordinate species that has triplet metal-centered (MC) character. Linear correlations are observed between the activation energy and the energy difference calculated for the emissive and MC states. The energy level for the MC state is estimated to lie between 21 700 and 24 000 cm for the fac-Ir(C^N) complexes and at 28 000 cm for fac-Ir(pmb).
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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