Self-interaction errors in density functional calculations of electronic transport

TL;DR

This paper addresses the limitations of continuous exchange-correlation functionals in density functional theory, demonstrating that atomic self-interaction corrections significantly improve the accuracy of electronic transport predictions in molecular junctions.

Contribution

It introduces a simple atomic self-interaction correction method that enhances the accuracy of density functional calculations for molecular electronic transport.

Findings

Self-interaction errors cause incorrect metallic transport predictions.

Atomic self-interaction correction aligns calculations better with experimental results.

The method is computationally efficient and improves existing models.

Abstract

All density functional calculations of single-molecule transport to date have used continuous exchange-correlation approximations. The lack of derivative discontinuity in such calculations leads to the erroneous prediction of metallic transport for insulating molecules. A simple and computationally undemanding atomic self-interaction correction greatly improves the agreement with experiment for the prototype Au/dithiolated-benzene/Au junction.