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Linker dependent bond rupture force measurements in single-molecule junctions.

Michael Frei1, Sriharsha V Aradhya, Mark S Hybertsen

  • 1Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, USA.

Journal of the American Chemical Society
|February 18, 2012
PubMed
Summary

We measured single-molecule junction conductance and rupture forces for different chemical link groups. Thiol link groups showed unique behavior due to strong gold-sulfur bonds, yet still ruptured at lower forces than gold-gold bonds.

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Area of Science:

  • Molecular electronics
  • Nanotechnology
  • Surface science

Background:

  • Understanding single-molecule junction properties is crucial for molecular electronics.
  • The choice of linking group significantly influences junction stability and conductance.
  • Atomic force microscopy (AFM) is a key technique for probing molecular junctions.

Purpose of the Study:

  • To investigate the relationship between linking group chemistry and the mechanical and electrical properties of single-molecule junctions.
  • To compare the rupture forces and conductance signatures of different linking groups (amine, methylsulfide, diphenylphosphine, thiol) to gold electrodes.
  • To elucidate the role of electrode-molecule interactions, particularly strong covalent bonding, on junction behavior.

Main Methods:

  • Utilized a modified conducting atomic force microscope (CAFM) to simultaneously measure conductance and rupture force.
  • Fabricated single-molecule junctions using alkanes with four distinct terminal linking groups.
  • Analyzed conductance traces and force-distance curves during junction formation and rupture.

Main Results:

  • Junctions with amine, methylsulfide, and diphenylphosphine linkers exhibited distinct conductance and ruptured at forces lower than single-atom gold contacts.
  • Thiol-terminated alkanes formed strong gold-sulfur bonds, leading to electrode structural rearrangements and significant conductance changes.
  • Despite strong Au-S bonding and electrode disruption, thiol-linked junctions also ruptured at forces lower than pristine single-atom gold contacts on average.

Conclusions:

  • The binding strength and mechanism of linking groups critically affect single-molecule junction stability and conductance.
  • Strong covalent interactions, like Au-S bonds, can induce electrode modifications, altering junction properties.
  • Molecular junction rupture force is generally lower than that of the bare metal contact, irrespective of the linking group's binding strength.