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    Area of Science:

    • Molecular electronics
    • Nanotechnology
    • Surface science

    Background:

    • Single molecules offer potential for electronic device miniaturization.
    • Controlling molecular orientation is crucial for optimizing electronic properties.

    Purpose of the Study:

    • To investigate single-molecule junction formation with externally controlled molecular orientation.
    • To measure and compare the conductance of tetrafluoroterephthalic acid (TFTPA) and terephthalic acid (TPA) molecules under different electrode potentials.

    Main Methods:

    • Utilizing scanning tunneling microscopy break junction (STM-BJ) technique.
    • Employing first-principles nonequilibrium Green's function (NEGF) computation.
    • Experimentally measuring single-molecule conductance.

    Main Results:

    • A highly ordered, flat-oriented molecular superstructure forms at negative electrode potentials, enabling direct π-electrode contact.
    • Flat-oriented junctions exhibit conductance 3 orders of magnitude higher than vertically connected molecules.
    • Experimentally measured conductances for flat TFTPA and TPA are 0.24 ± 0.04 G₀ and 0.22 ± 0.02 G₀, respectively.
    • Positive electrode potentials disrupt the ordered structure, eliminating high-conductance states.

    Conclusions:

    • External control of molecular orientation via electrode potential is a viable strategy for forming highly conductive single-molecule junctions.
    • Flat-oriented molecular junctions significantly outperform those connected via anchoring groups.
    • The observed conductance dependence on electrode potential suggests a LUMO-mediated transport mechanism.