Formation and Evolution of Single-Molecule Junctions

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M. Kamenetska,^1,2 M. Koentopp,² A. C. Whalley,³ Y. S. Park,³ M. L. Steigerwald,^3,2 C. Nuckolls,^3,2 M. S. Hybertsen,⁴ and L. Venkataraman¹
¹Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York, USA
²Center for Electron Transport in Molecular Nanostructures, Columbia University, New York, New York, USA
³Department of Chemistry, Columbia University, New York, New York, USA
⁴Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York, USA

Received 22 December 2008; published 24 March 2009

Weanalyze the formation and evolution statistics of single-molecule junctions bondedto gold electrodes using amine, methyl sulfide, and dimethyl phosphinelink groups by measuring conductance as a function of junctionelongation. For each link, the maximum elongation and formation probabilityincrease with molecular length, strongly suggesting that processes other thanjust metal-molecule bond breakage play a key role in junctionevolution under stress. Density functional theory calculations of adiabatic trajectoriesshow sequences of atomic-scale changes in junction structure, including shiftsin the attachment point, that account for the long conductanceplateau lengths observed.

URL:	http://link.aps.org/doi/10.1103/PhysRevLett.102.126803
DOI:	10.1103/PhysRevLett.102.126803
PACS:	73.63.Rt; 61.46.-w; 81.07.Nb; 85.65.+h 73.63.Rt Nanoscale contacts (electronic transport) 61.46.-w Structure of nanoscale materials 81.07.Nb Molecular nanostructures: fabrication and characterization 85.65.+h Molecular electronic devices YEAR: 2009