Probing Structural Perturbation in a Bent Molecular Crystal with Synchrotron Infrared Microspectroscopy and Periodic Density Functional Theory Calculations.

The range of unit cell orientations generated at the kink of a bent single crystal poses unsurmountable challenges with diffraction analysis and limits the insight into the molecular-scale mechanism of bending. On a plastically bent crystal of hexachlorobenzene, it is demonstrated here that spatiall...

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Publicado en:Journal of the American Chemical Society Vol. 139; no. 6; pp. 2318 - 2329
Autores principales: Pejov, Ljupčo, Panda, Manas K., Taro Moriwaki, Naumov, Panče
Formato: Artículo
Publicado: American Chemical Society 2/15/2017
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 2/15/2017
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      pub: American Chemical Society
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        10.1021/jacs.6b11212
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        atl: Probing Structural Perturbation in a Bent Molecular Crystal with Synchrotron Infrared Microspectroscopy and Periodic Density Functional Theory Calculations.
      aug:
        au:
          Pejov, Ljupčo
          Panda, Manas K.
          Taro Moriwaki
          Naumov, Panče
        affil:
          Institute of Chemistry, Faculty of Natural Sciences and Mathematics, Ss. Cyril and Methodius University, MK-1000 Skopje, Macedonia
          New York University Abu Dhabi, P.O. Box 129188, Abu Dhabi, United Arab Emirates
          Japan Synchrotron Radiation Research Institute, 1-1-1 Kouto, Sayo, Hyogo 679-5198, Japan
      su:
        Molecular crystals
        Perturbation theory
        Crystal structure
        Spectrum analysis
        Density functional theory
        Deformations (Mechanics)
      sug:
        subj:
          Molecular crystals
          Perturbation theory
          Crystal structure
          Spectrum analysis
          Density functional theory
          Deformations (Mechanics)
      ab: The range of unit cell orientations generated at the kink of a bent single crystal poses unsurmountable challenges with diffraction analysis and limits the insight into the molecular-scale mechanism of bending. On a plastically bent crystal of hexachlorobenzene, it is demonstrated here that spatially resolved microfocus infrared spectroscopy using synchrotron radiation can be applied in conjunction with periodic density functional theory calculations to predict spectral changes or to extract information on structural changes that occur as a consequence of bending. The approach reproduces well the observed trends, such as the wall effects, and provides estimations of the vibrational shifts, unit cell deformations, and intramolecular parameters. Generally, expansion of the lattice induces red-shift while compression induces larger blue-shift of the characteristic ν(C-C) and ν(C-Cl) modes. Uniform or non-uniform expansion or contraction of the unit cell of 0.1 Šresults in shifts of several cm, whereas deformation of the cell of 0.5° at the unique angle causes shifts of <0.5 cm. Since this approach does not include parameters related to the actual stimulus by which the deformation has been induced, it can be generalized and applied to other mechanically, photochemically, or thermally bent crystals.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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