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V. Geskin, R. Stadler, J. Cornil:
"Partial vs. integer electron transfer in molecular assemblies: On the importance of multideterminant theoretical description and the necessity to find a solution within DFT";
AIP Conference Proceedings, 1642 (2015), S. 249 - 252.

Nonequilibrium Green´s function techniques (NEGF) combined with density functional theory (DFT)
calculations have become a standard tool for the description of electron transport through single molecule nanojunctions
in the coherent tunneling (CT) regime. However, the applicability of these methods for transport in the Coulomb
blockade (CB) regime is questionable. For a molecular assembly model, with multideterminant calculations as a
benchmark, we show how a closed-shell ansatz, the usual ingredient of mean-field methods, fails to properly describe the
step like electron-transfer characteristic in weakly coupled systems. Detailed analysis of this misbehavior allows us to
propose a practical scheme to extract the addition energies in the CB regime for single-molecule junctions from NEGF
DFT within the local-density approximation (closed shell). We show also that electrostatic screening effects are taken
into account within this simple approach.

http://dx.doi.org/10.1063/1.4906664

Projektleitung Robert Stadler:
Elektrochemische Interferenz