Journal of the American Chemical Society
Journal of the American Chemical Society
4 years ago

Electronically Transparent Au–N Bonds for Molecular Junctions

Electronically Transparent Au–N Bonds for Molecular Junctions
Latha Venkataraman, Andrew Pinkard, Zhen-Fei Liu, Yaping Zang, Jeffrey B. Neaton, Xavier Roy, Michael L. Steigerwald
We report a series of single-molecule transport measurements carried out in an ionic environment with oligophenylenediamine wires. These molecules exhibit three discrete conducting states accessed by electrochemically modifying the contacts. Transport in these junctions is defined by the oligophenylene backbone, but the conductance is increased by factors of ∼20 and ∼400 when compared to traditional dative junctions. We propose that the higher-conducting states arise from in situ electrochemical conversion of the dative Au←N bond into a new type of Au–N contact. Density functional theory-based transport calculations establish that the new contacts dramatically increase the electronic coupling of the oligophenylene backbone to the Au electrodes, consistent with experimental transport data. The resulting contact resistance is the lowest reported to date; more generally, our work demonstrates a facile method for creating electronically transparent metal–organic interfaces.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b08370

DOI: 10.1021/jacs.7b08370

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