Self-Association and Nitroaromatic-Induced Deaggregation of Pyrene Substituted Pyridine Amides.

The self-assembly features of the bis-pyrene methyl amide functionalized pyridine and benzene "tweezers" 1 and 2 were studied in organic solution and in the solid state. These systems were found to display remarkably different selfassociation features and optical properties, which was rationalized b...

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Publicado en:Journal of the American Chemical Society Vol. 136; no. 1; pp. 495 - 506
Autores principales: Sung Kuk Kim, Jong Min Lim, Tuhin Pradhan, Hyo Sung Jung, Lynch, Vincent M., Jong Seung Kim, Dongho Kim, Sessler, Jonathan L.
Formato: Artículo
Publicado: American Chemical Society 1/8/2014
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Acceso en línea:Ver este registro en EBSCOhost
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        00027863
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      dt: 1/8/2014
      vid: 136
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      pub: American Chemical Society
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        10.1021/ja411672f
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        atl: Self-Association and Nitroaromatic-Induced Deaggregation of Pyrene Substituted Pyridine Amides.
      aug:
        au:
          Sung Kuk Kim
          Jong Min Lim
          Tuhin Pradhan
          Hyo Sung Jung
          Lynch, Vincent M.
          Jong Seung Kim
          Dongho Kim
          Sessler, Jonathan L.
        affil:
          Department of Chemistry, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
          Department of Chemistry, Yonsei University, Seoul 120-749, Korea
          Department of Chemistry, Korea University, Seoul 136-701, Korea
      su:
        Density functionals
        Chlorohydrocarbons
        Trihalomethanes
        Aromatic compounds
        Organic compounds
      sug:
        subj:
          Density functionals
          Chlorohydrocarbons
          Trihalomethanes
          Aromatic compounds
          Organic compounds
      ab: The self-assembly features of the bis-pyrene methyl amide functionalized pyridine and benzene "tweezers" 1 and 2 were studied in organic solution and in the solid state. These systems were found to display remarkably different selfassociation features and optical properties, which was rationalized by control experiments using compounds bearing pyrenemethyl esters, alkyl groups, or a single pyrene substituent (3-6). As dilute solutions in chloroform, tweezers 1 displays both pyrene monomer and excimer emission features reflecting intramolecular contacts between the pyrene subunits. At higher concentrations in chloroform, as well as in the solid state, tweezers 1 self-assembles to form a linear supramolecular polymer. In contrast, tweezers 2 does not interact in an intermolecular fashion and photoexcitation produces emission features characteristic of a pyrene monomer. DFT (density functional theory) and TDDFT (time dependent density functional theory) calculations revealed that the lowest vertical transitions are forbidden and that S of 1 is an emissive state. In contrast to 1 and 2, both pyrene-free control systems 5 and 6 were found to form linearly self-assembled supramolecular arrays in the solid state, albeit of differing structure. Upon exposure to trinitrobenzene (TNB), the self-assembled structures formed from 1 undergo deaggregation to form TNB complexes. This change is reflected in both an easily discernible color change and a quenching of the fluorescence emission intensity. Changes in the optical features were also seen in the case of 2. However, notable differences between these two ostensibly similar systems were seen.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2014
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