Efficient DFT+U calculations of ballistic electron transport: Application to Au monatomic chains with a CO impurity

An efficient method for computing the Landauer-Buttiker conductance of an open quantum system within DFT + U is presented. The Hubbard potential is included in electronic-structure and transport calculations as a simple renormalization of the nonlocal pseudopotential coefficients by restricting the integration for the onsite occupations within the cutoff spheres of the pseudopotential. We apply the methodology to the case of an Au monatomic chain in the presence of a CO molecule adsorbed on it. We show that the Hubbard U correction removes the spurious magnetization in the pristine Au chain at the equilibrium spacing, as well as the unphysical contribution of d electrons to the conductance, resulting in a single (spin-degenerate) transmission channel and a more realistic conductance of 1 G(0). We find that the conductance reduction due to CO adsorption is much larger for the atop site than for the bridge site, so that the general picture of electron transport in stretched Au chains given by the local density approximation remains valid at the equilibrium Au-Au spacing within DFT + U. DOI: 10.1103/PhysRevB.87.085108