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

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 $\Sigma_{\rm C}$ of the junction. $\Sigma_{\rm C}$ 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.Comment: 13 pages, 7 figure

Coherent Magnetotransport Through an Artificial Molecule

The conductance in an extended multiband Hubbard model describing linear arrays of up to ten quantum dots is calculated via a Lanczos technique. A pronounced suppression of certain resonant conductance peaks in an applied magnetic field due to a density-dependent spin-polarization transition is predicted to be a clear signature of a coherent ``molecular'' wavefunction in the array. A many-body enhancement of localization is predicted to give rise to a {\em giant magnetoconductance} effect in systems with magnetic scattering.Comment: 4 pages, REVTEX 3.0, 5 figures included as postscript file

Parity-locking effect in a strongly-correlated ring

Orbital magnetism in an integrable model of a multichannel ring with long-ranged electron-electron interactions is investigated. In a noninteracting multichannel system, the response to an external magnetic flux is the sum of many diamagnetic and paramagnetic contributions, but we find that for sufficiently strong correlations, the contributions of all channels add constructively, leading to a parity (diamagnetic or paramagnetic) which depends only on the total number of electrons. Numerical results confirm that this parity-locking effect is robust with respect to subband mixing due to disorder.Comment: part of lecture presented in the conference ``Unconventional quantum liquids", appearing in Z. Phy

Comment on "Density Functional Simulation of a Breaking Nanowire"

In a recent Letter, Nakamura et al. [Phys. Rev. Lett. 82, 1538 (1999)] described first principles calculations for a breaking Na nanocontact. Their system consists of a periodic one-dimensional array of supercells, each of which contains 39 Na atoms, originally forming a straight, crystalline wire with a length of 6 atoms. The system is elongated by increasing the length of the unit cell. At each step, the atomic configuration is relaxed to a new local equilibrium, and the tensile force is evaluated from the change of the total energy with elongation. Aside from a discontinuity of the force occuring at the transition from a crytalline to an amorphous configuration during the early stages of elongation, they were unable to identify any simple correlations between the force and the number of electronic modes transmitted through the contact. An important question is whether their model is realistic, i.e., whether it can be compared to experimental results obtained for a single nanocontact between two macroscopic pieces of metal. In this Comment, we demonstrate that with such a small unit cell, the interference effects between neighboring contacts are of the same size as the force oscillations in a single nanocontact.Comment: 1 pag