title: Applicability of the wide-band limit in DFT-based molecular transport calculations.
abstract: Transport properties of molecular junctions are notoriously expensive to calculate with ab initio methods, primarily due to the semi-infinite electrodes. This has led to the introduction of different approximation schemes for the electrodes. For the most popular metals used in experiments, such as gold, the wide-band limit (WBL) is a particularly efficient choice. In this paper, we investigate the performance of different WBL schemes relative to more sophisticated approaches including the fully self-consistent non-equilibrium Green's function method. We find reasonably good agreement between all schemes for systems in which the molecule (and not the metal-molecule interface) dominates the transport properties. Moreover, our implementation of the WBL requires negligible computational effort compared to the ground-state density-functional theory calculation of a molecular junction. We also present a new approximate but efficient scheme for calculating transport with a finite bias. Provided the voltage drop occurs primarily inside the molecule, this method provides results in reasonable agreement with fully self-consistent calculations.
authors.affiliation: Kavli Institute of Nanoscience, Delft University of Technology, 2628 CJ Delft, The Netherlands.
authors.forename: C J O
authors.initials: CJ
authors.lastname: Verzijl
authors.forename: J S
authors.initials: JS
authors.lastname: Seldenthuis
authors.forename: J M
authors.initials: JM
authors.lastname: Thijssen