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J Am Chem Soc. 2013 Mar 6;135(9):3319-22. doi: 10.1021/ja3106434. Epub 2013 Feb 25.

Controlling formation of single-molecule junctions by electrochemical reduction of diazonium terminal groups.

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Center for Biosensors and Bioelectronics, The Biodesign Institute, and School of Electrical, Computer and Energy Engineering, Arizona State University, Tempe, Arizona 85287, United States.


We report controlling the formation of single-molecule junctions by means of electrochemically reducing two axialdiazonium terminal groups on a molecule, thereby producing direct Au-C covalent bonds in situ between the molecule and gold electrodes. We report a yield enhancement in molecular junction formation as the electrochemical potential of both junction electrodes approach the reduction potential of the diazonium terminal groups. Step length analysis shows that the molecular junction is significantly more stable, and can be pulled over a longer distance than a comparable junction created with amine anchoring bonds. The stability of the junction is explained by the calculated lower binding energy associated with the direct Au-C bond compared with the Au-N bond.

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