TY - JOUR

T1 - Precursor configurations and post-rupture evolution of Ag-CO-Ag single-molecule junctions

AU - Balogh, Zoltan

AU - Visontai, David

AU - Makk, Peter

AU - Gillemot, Katalin

AU - Oroszlany, Laszlo

AU - Posa, Laszlo

AU - Lambert, Colin

AU - Halbritter, Andras

PY - 2014/12/21

Y1 - 2014/12/21

N2 - Experimental correlation analysis and first-principles theory are used to probe the structure and evolution of Ag-CO-Ag single-molecule junctions both before the formation and after the rupture of the junctions. Two dimensional correlation histograms and conditional histograms demonstrate that prior to the single-molecule bridge configuration the CO molecule is already bound parallel to the Ag single-atom contact. This molecular precursor configuration is accompanied by the opening of additional conductance channels compared to the single-channel transport in pure Ag monoatomic junctions. To investigate the post-rupture evolution of the junction we introduce a cross-correlation analysis between the opening and the subsequent closing conductance traces. This analysis implies that the molecule is bound rigidly to the apex of one electrode, and so the same single-molecule configuration is re-established as the junction is closed. The experimental results are confirmed by ab initio simulations of the evolution of contact geometries, transmission eigenvalues and scattering wavefunctions.

AB - Experimental correlation analysis and first-principles theory are used to probe the structure and evolution of Ag-CO-Ag single-molecule junctions both before the formation and after the rupture of the junctions. Two dimensional correlation histograms and conditional histograms demonstrate that prior to the single-molecule bridge configuration the CO molecule is already bound parallel to the Ag single-atom contact. This molecular precursor configuration is accompanied by the opening of additional conductance channels compared to the single-channel transport in pure Ag monoatomic junctions. To investigate the post-rupture evolution of the junction we introduce a cross-correlation analysis between the opening and the subsequent closing conductance traces. This analysis implies that the molecule is bound rigidly to the apex of one electrode, and so the same single-molecule configuration is re-established as the junction is closed. The experimental results are confirmed by ab initio simulations of the evolution of contact geometries, transmission eigenvalues and scattering wavefunctions.

KW - BREAK-JUNCTIONS

KW - CONDUCTANCE

KW - CONTACTS

KW - ELECTRODES

KW - TRANSPORT

KW - MECHANICS

KW - CHAINS

KW - ATOMS

U2 - 10.1039/c4nr04645e

DO - 10.1039/c4nr04645e

M3 - Journal article

VL - 6

SP - 14784

EP - 14791

JO - Nanoscale

JF - Nanoscale

SN - 2040-3364

IS - 24

ER -