Dynamical Mean-Field Theory for Molecular Electronics: Electronic Structure and Transport Properties

TL;DR

This paper introduces a combined density functional theory and dynamical mean-field theory approach to accurately compute electronic structures and transport properties of nanoscopic conductors with strongly correlated electrons, exemplified by Ni nanocontacts.

Contribution

It develops a novel method integrating DFT and DMFT for nanostructures with strong electron correlations, providing more accurate transport predictions.

Findings

Dynamical correlations produce quasi-particle resonances at the Fermi level.

Resonances lead to Fano lineshapes in conductance, matching experimental observations.

Method successfully applied to Ni nanocontacts between Cu electrodes.

Abstract

We present an approach for calculating the electronic structure and transport properties of nanoscopic conductors that takes into account the dynamical correlations of strongly interacting d- or f-electrons by combining density functional theory calculations with the dynamical mean-field theory. While the density functional calculation yields a static mean-field description of the weakly interacting electrons, the dynamical mean-field theory explicitly takes into account the dynamical correlations of the strongly interacting d- or f-electrons of transition metal atoms. As an example we calculate the electronic structure and conductance of Ni nanocontacts between Cu electrodes. We find that the dynamical correlations of the Ni 3d-electrons give rise to quasi-particle resonances at the Fermi-level in the spectral density. The quasi-particle resonances in turn lead to Fano lineshapes in the conductance characteristics of the nanocontacts similar to those measured in recent experiments of magnetic nanocontacts.