An ab initio non-equilibrium Green's function approach to charge transport: dithiolethine

TL;DR

This paper introduces a new ab initio non-equilibrium Green's function method combining wave function and tight binding approaches to accurately compute charge transport in molecular junctions, demonstrated on a dithiolethine molecule.

Contribution

It develops a novel ab initio non-equilibrium approach integrating wave function methods with tight binding for molecular junction transport calculations.

Findings

Identified the main conducting channel in dithiolethine.

Calculated the full current-voltage characteristic.

Validated the method on a molecular junction with silver electrodes.

Abstract

We present a novel ab initio non-equilibrium approach to calculate the current across a molecular junction. The method rests on a wave function based full ab initio description of the central region of the junction combined with a tight binding approximation for the electrodes in the frame of the Keldysh Green's function formalism. Our procedure is demonstrated for a dithiolethine molecule between silver electrodes. The main conducting channel is identified and the full current-voltage characteristic is calculated.