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Both experiments and theoretical studies have demonstrated that theinteraction between the current carrying electrons and the induced polarizationcharge in single-molecule junctions leads to a strong renormalization ofmolecular charging energies. However, the effect on electronic excitations andmolecular symmetries remain unclear. Using a theoretical framework developedfor semiconductor nanostructure based single-electron transistors (SETs), wedemonstrate that the image charge interaction breaks the molecular symmetriesin a benzene based single-molecule transistor operating in the Coulomb blockaderegime. This results in the appearance of a so-called blocking state, whichgives rise to negative differential resistance (NDR). We show that theappearance of NDR and its magnitude in the symmetry-broken benzene SET dependsin a complicated way on the interplay between the many-body matrix elements,the lead tunnel coupling asymmetry, and the bias polarity. In particular, thecurrent reducing property of the blocking state causing the NDR, is shown tovanish under strongly asymmetric tunnel couplings, when the molecule is coupledstronger to the drain electrode. The calculated IV characteristic may serve asan indicator for image charge broken molecular symmetries in experimentalsituations.

Image charge effects in single-molecule junctions: Breaking of symmetries and negative differential resistance in a benzene transistor