Modeling elastic and photoassisted transport in organic molecular wires: length dependence and current-voltage characteristics

TL;DR

This paper investigates how the length of organic molecular wires affects their elastic and photoassisted electron transport properties, revealing length-dependent conductance, thermopower, and light-induced current features in metal-molecule-metal junctions.

Contribution

It provides analytical and numerical analysis of transport in oligophenylene junctions under light, highlighting length-dependent effects and current-voltage characteristics with photoassistance.

Findings

Conductance decreases exponentially with length in off-resonant transport.

Light enhances conductance and induces current steps at low voltages.

Longer molecules show more pronounced photoinduced effects.

Abstract

Using a pi-orbital tight-binding model, we study the elastic and photoassisted transport properties of metal-molecule-metal junctions based on oligophenylenes of varying lengths. The effect of monochromatic light is modeled with an ac voltage over the contact. We first show how the low-bias transmission function can be obtained analytically, using methods previously employed for simpler chain models. In particular, the decay coefficient of the off-resonant transmission is extracted by considering both a finite-length chain and infinitely extended polyphenylene. Based on these analytical results, we discuss the length-dependence of the linear-response conductance, the thermopower, and the light-induced enhancement of the conductance in the limit of weak intensity and low frequency. In general the conductance-enhancement is calculated numerically as a function of the light frequency. Finally, we compute the current-voltage characteristics at finite dc voltages, and show that in the low-voltage regime, the effect of low-frequency light is to induce current steps with a voltage separation determined by twice the frequency. These effects are more pronounced for longer molecules. We study two different profiles for the dc and ac voltages, and it is found that the results are robust with respect to such variations. Although we concentrate here on the specific model of oligophenylenes, the results should be qualitatively similar for many other organic molecules with a large enough electronic gap.