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

Abstract

Both experiments and theoretical studies have demonstrated that the interaction between the current carrying electrons and the induced polarization charge in single-molecule junctions leads to a strong renormalization of molecular charging energies. However, the effect on electronic excitations and molecular symmetries remain unclear. Using a theoretical framework developed for semiconductor nanostructure based single-electron transistors (SETs), we demonstrate that the image charge interaction breaks the molecular symmetries in a benzene based single-molecule transistor operating in the Coulomb blockade regime. This results in the appearance of a so-called blocking state, which gives rise to negative differential resistance (NDR). We show that the appearance of NDR and its magnitude in the symmetry-broken benzene SET depends in a complicated way on the interplay between the many-body matrix elements, the lead tunnel coupling asymmetry, and the bias polarity. In particular, the current reducing property of the blocking state causing the NDR, is shown to vanish under strongly asymmetric tunnel couplings, when the molecule is coupled stronger to the drain electrode. The calculated IV characteristic may serve as an indicator for image charge broken molecular symmetries in experimental situations.

Accepted version (Phys. Rev. B), 16 pages, 8 figures

References in corpus (16)

• Renormalization of Molecular Electronic Levels at Metal-Molecule Interfaces
• Kinetic Equations for Transport Through Single-Molecule Transistors
• Renormalization of Molecular Quasiparticle Levels at Metal-Molecule Interfaces: Trends Across Binding Regimes
• Electronic excitations of a single molecule contacted in a three-terminal configuration
• A benzene interference single-electron transistor
• A Generic Model for Current Collapse in Spin Blockaded Transport
• Symmetry fingerprints of a benzene single-electron transistor
• First-principles modelling of molecular single-electron transistors
• Dynamic Jahn-Teller effect in electron transport through single C60 molecules
• Electronic and optical properties of electromigrated molecular junctions
• Cotunneling through a magnetic single-molecule transistor based on N\atC60
• Interaction-induced negative differential resistance in asymmetric molecular junctions
• Gate Coupling to Nanoscale Electronics
• Inelastic cotunneling in quantum dots and molecules with weakly broken degeneracies
• Transport signature of pseudo-Jahn-Teller dynamics in a single-molecule transistor
• Berry-phase effects in transport through single Jahn-Teller molecules

Cited by in corpus (18)

• Advances and challenges in single-molecule electron transport
• Large tunable image-charge effects in single-molecule junctions
• Irreversibility and hysteresis in redox molecular conduction junctions
• Zero-energy pinning from interactions in Majorana nanowires
• Full counting statistics and shot noise of cotunneling in quantum dots and single-molecule transistors
• Transport Through Self-Assembled Monolayer Molecular Junctions: Role of In-Plane Dephasing
• Image charge dynamics in time-dependent quantum transport
• Transport mirages in single-molecule devices
• Apparent Reversal of Molecular Orbitals Reveals Entanglement
• Nonequilibrium conductance through a benzene molecule in the Kondo regime
• Effective Field Theory of Interacting π-Electrons
• Non-equilibrium spin-crossover in copper phthalocyanine
• Quantum Transport With Two Interacting Conduction Channels
• Sharp negative differential resistance from vibrational mode softening in molecular junctions
• Negative differential conductance in molecular junctions: an overview of experiment and theory
• Dynamical coupling and negative differential resistance from interactions across the molecule-electrode interface in molecular junctions
• Spin-orbit interaction induces charge beatings in a lightwave-STM single molecule junction
• Multipeak Negative Differential Resistance from Interplay between Nonlinear Stark Effect and Double-Branch Current Flow