Applicability of the wide-band limit in DFT-based molecular transport calculations

Applicability of the wide-band limit in DFT-based molecular transport calculations

Verzijl, C.J.O.
Seldenthuis, J.S.
Thijssen, J.M.

Applied Sciences

QN/Quantum Nanoscience

2013-03-01

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.

ab initio calculations
approximation theory
density functional theory
Green's function methods

http://resolver.tudelft.nl/uuid:3dab5b34-d9d7-4f34-9921-a6313c6b9b37

https://doi.org/10.1063/1.4793259

American Institute of Physics

0021-9606

https://doi.org/10.1063/1.4793259

Journal of Chemical Physics, 138 (9), 2013

Institutional Repository

journal article

© 2013 American Institute of Physics