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The average width of the molecules was about 0.9 nm for the lowest step (a single molecule) and was much shorter (∼0.3 nm) for higher steps. This width is not the length to which a molecule was stretched. Instead, it measures the distance over which a particular junction can be stretched before losing stability. At least part of the width comes from the stretching of the gold atoms in the contacts and from changes in the atomic configurations of the contacts as individual molecules break away.
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We controlled the potential of the tip and the substrate with respect to a reference electrode (an Ag wire) in the aqueous 4,4′-bipyridine solutions by means of a Pt counter electrode and a bipotentiostat. We coated the tip with Apiezon wax in order to reduce ionic conduction and polarization currents below ∼1 pA.
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We thank S. Lindsay, O. Sankey, A. Nitzan, D. Ferry, L. Nagahara, G. Speyer, S. Boussaad, J: Li, and X. Xiao for discussions and the U.S. Department of Energy, NSF, and the U.S. Environmental Protection Agency for support.
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