Electric field breakdown in single molecule junctions

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[1] Li, Haixing
[2] Su, Timothy A.
[3] Zhang, Vivian
[4] Steigerwald, Michael L.
[5] Nuckolls, Colin
[6] Venkataraman, Latha
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Steigerwald, Michael L. (mls2064@columbia.edu) | 1600年 / American Chemical Society卷 / 137期
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Here we study the stability and rupture of molecular junctions under high voltage bias at the single molecule/single bond level using the scanning tunneling microscope-based break-junction technique. We synthesize carbon-; silicon-; and germanium-based molecular wires terminated by aurophilic linker groups and study how the molecular backbone and linker group affect the probability of voltage-induced junction rupture. First; we find that junctions formed with covalent S-Au bonds are robust under high voltage and their rupture does not demonstrate bias dependence within our bias range. In contrast; junctions formed through donor-acceptor bonds rupture more frequently; and their rupture probability demonstrates a strong bias dependence. Moreover; we find that the junction rupture probability increases significantly above ∼1 V in junctions formed from methylthiol-terminated disilanes and digermanes; indicating a voltage-induced rupture of individual Si-Si and Ge-Ge bonds. Finally; we compare the rupture probabilities of the thiol-terminated silane derivatives containing Si-Si; Si-C; and Si-O bonds and find that Si-C backbones have higher probabilities of sustaining the highest voltage. These results establish a new method for studying electric field breakdown phenomena at the single molecule level. © 2015 American Chemical Society;
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