Tuning Conductance in π-σ-π Single-Molecule Wires.

While the single-molecule conductance properties of π-conjugated and σ-conjugated systems have been well-studied, little is known regarding the conductance properties of mixed σ-π backbone wires and the factors that control their transport properties. Here we utilize a scanning tunneling microscope-...

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Publicado en:Journal of the American Chemical Society Vol. 138; no. 24; pp. 7791 - 7796
Autores principales: Su, Timothy A., Li, Haixing, Klausen, Rebekka S., Widawsky, Jonathan R., Batra, Arunabh, Steigerwald, Michael L., Venkataraman, Latha, Nuckolls, Colin
Formato: Artículo
Publicado: American Chemical Society 6/22/2016
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 6/22/2016
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      pub: American Chemical Society
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        10.1021/jacs.6b04394
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        atl: Tuning Conductance in π-σ-π Single-Molecule Wires.
      aug:
        au:
          Su, Timothy A.
          Li, Haixing
          Klausen, Rebekka S.
          Widawsky, Jonathan R.
          Batra, Arunabh
          Steigerwald, Michael L.
          Venkataraman, Latha
          Nuckolls, Colin
        affil:
          Department of Chemistry, Columbia University, New York, New York 10027, United States
          Department of Physics and Applied Math, Columbia University, New York, New York 10027, United States
      su:
        Single molecules
        Density functionals
        Atomic radius
        Electric admittance
        Organic compounds
        Electronegativity
      sug:
        subj:
          Single molecules
          Density functionals
          Atomic radius
          Electric admittance
          Organic compounds
          Electronegativity
      ab: While the single-molecule conductance properties of π-conjugated and σ-conjugated systems have been well-studied, little is known regarding the conductance properties of mixed σ-π backbone wires and the factors that control their transport properties. Here we utilize a scanning tunneling microscope-based break-junction technique to study a series of molecular wires with π-σ-π backbone structures, where the π-moiety is an electrode-binding thioanisole ring and the σ-moiety is a triatomic α-β-α chain composed of C, Si, or Ge atoms. We find that the sequence and composition of group 14 atoms in the α-β-α chain dictates whether electronic communication between the aryl rings is enhanced or suppressed. Placing heavy atoms at the α-position decreases conductance, whereas placing them at the β-position increases conductance: for example, the C-Ge-C sequence is over 20 times more conductive than the Ge-C-Ge sequence. Density functional theory calculations reveal that these conductance trends arise from periodic trends (i.e., atomic size, polarizability, and electronegativity) that differ from C to Si to Ge. The periodic trends that control molecular conductance here are the same ones that give rise to the α and β silicon effects from physical organic chemistry. These findings outline a new molecular design concept for tuning conductance in single-molecule electrical devices.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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