Rectification by charging -- the physics of contact-induced current asymmetry in molecular conductors

Details Rectification by charging -- the physics of contact-induced current asymmetry in molecular conductors Rectification by charging -- the physics of contact-induced current asymmetry in molecular conductors

2007-07-16

arxiv.org/abs/0707.2367v1

Physics

Condensed Matter

Mesoscale and Nanoscale Physics

12 pages, 10 figures

Scientific paper

10.1103/PhysRevB.77.125427

We outline the qualitatively different physics behind charging-induced current asymmetries in molecular conductors operating in the weakly interacting self-consistent field (SCF) and the strongly interacting Coulomb Blockade (CB) regimes. A conductance asymmetry arises in SCF because of the unequal mean-field potentials that shift a closed-shell conducting level differently for positive and negative bias. A very different current asymmetry arises for CB due to the unequal number of open-shell excitation channels at opposite bias voltages. The CB regime, dominated by single charge effects, typically requires a computationally demanding many-electron or Fock space description. However, our analysis of molecular Coulomb Blockade measurements reveals that many novel signatures can be explained using a {{simpler}} orthodox model that involves an incoherent sum of Fock space excitations and {\it{hence treats the molecule as a metallic dot or an island}}. This also reduces the complexity of the Fock space description by just including various charge configurations only, thus partially underscoring the importance of electronic structure, while retaining the essence of the single charge nature of the transport process. We finally point out, however, that the inclusion of electronic structure and hence well-resolved Fock space excitations is crucial in some notable examples.

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