Influence of structural disorder and large-scale geometric fluctuations on the Coherent Transport of Metallic Junctions and Molecular Wires

TL;DR

This study introduces an efficient recursive Green function method to analyze how structural disorder and geometric fluctuations affect electronic conductance in metallic and molecular nano-junctions, aligning well with experimental data.

Contribution

The paper presents a computationally efficient recursive Green function approach that accurately models conductance in large, disordered nano-junctions, enabling analysis of complex molecular systems.

Findings

Conductance variations of about 20% in weakly disordered gold and silver wires.

Silver junction conductance is mainly determined by the narrowest point.

Distorted conformations significantly influence molecular wire conductance.

Abstract

Structural disorder is present in almost all experimental measurements of electronic transport through single molecules or molecular wires. To assess its influence on the conductance is computationally demanding, because a large number of conformations must be considered. Here we analyze an approximate recursive layer Green function approach for the ballistic transport through quasi one-dimensional nano-junctions. We find a rapid convergence of the method with its control parameter, the layer thickness, and good agreement with existing experimental and theoretical data. Because the computational effort rises only linearly with system size, this method permits treatment of very large systems. We investigate the conductance of gold- and silver wires of different sizes and conformations. For weak electrode disorder and imperfect coupling between electrode and wire we find conductance variations of approximately 20%. Overall we find the conductance of silver junctions well described by the immediate vicinity of narrowest point in the junction, a result that may explain the observation of well-conserved conductance plateaus in recent experiments on silver junctions. In an application to flexible oligophene wires, we find that strongly distorted conformations that are sterically forbidden at zero temperature, contribute significantly to the observed average zero-bias conductance of the molecular wire.