Many-body theory of electronic transport in single-molecule heterojunctions

Abstract

A many-body theory of molecular junction transport based on nonequilibrium Green's functions is developed, which treats coherent quantum effects and Coulomb interactions on an equal footing. The central quantity of the many-body theory is the Coulomb self-energy matrix ${\Sigma }_{\mathrm{C}}$ of the junction. ${\Sigma }_{\mathrm{C}}$ is evaluated exactly in the sequential tunneling limit, and the correction due to finite tunneling width is evaluated self-consistently using a conserving approximation based on diagrammatic perturbation theory on the Keldysh contour. Our approach reproduces the key features of both the Coulomb blockade and coherent transport regimes simultaneously in a single unified transport theory. As a first application of our theory, we have calculated the thermoelectric power and differential conductance spectrum of a benzenedithiol-gold junction using a semi-empirical $\pi$-electron Hamiltonian that accurately describes the full spectrum of electronic excitations of the molecule up to 8--10eV.

13 pages, 7 figures

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Cited by in corpus (8)

• Giant Thermoelectric Effect from Transmission Supernodes
• Resonant Electron Transport in Single-Molecule Junctions: Vibrational Excitation, Rectification, Negative Differential Resistance and Local Cooling
• Local temperatures of strongly-correlated quantum dots out of equilibrium
• Spin-dependent thermoelectric effects in transport through a nanoscopic junction involving spin impurity
• The thermodynamic meaning of local temperature of nonequilibrium open quantum systems
• The number of transmission channels through a single-molecule junction
• Quantum interference and electron correlation in charge transport through triangular quantum dot molecules
• Kondo effect given exactly by density functional theory