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

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

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

Fluctuational Instabilities of Alkali and Noble Metal Nanowires

We introduce a continuum approach to studying the lifetimes of monovalent metal nanowires. By modelling the thermal fluctuations of cylindrical nanowires through the use of stochastic Ginzburg-Landau classical field theories, we construct a self-consistent approach to the fluctuation-induced `necking' of nanowires. Our theory provides quantitative estimates of the lifetimes for alkali metal nanowires in the conductance range 10 < G/G_0 < 100 (where G_0=2e^2/h is the conductance quantum), and allows us to account for qualitative differences in the conductance histograms of alkali vs. noble metal nanowires

Correlated charge polarization in a chain of coupled quantum dots

Coherent charge transfer in a linear array of tunnel-coupled quantum dots, electrostatically coupled to external gates, is investigated using the Bethe ansatz for a symmetrically biased Hubbard chain. Charge polarization in this correlated system is shown to proceed via two distinct processes: formation of bound states in the metallic phase, and charge transfer processes corresponding to a superposition of antibound states at opposite ends of the chain in the Mott-insulating phase. The polarizability in the insulating phase of the chain exhibits a universal scaling behavior, while the polarization charge in the metallic phase of the model is shown to be quantized in units of $e/2$.Comment: 9 pages, 3 figures, 1 tabl

Comment on "Nonlinear current-voltage curves of gold quantum point contacts" [Appl. Phys. Lett. 87, 103104 (2005)]

In a recent Letter [Appl. Phys. Lett. 87, 103104 (2005)], Yoshida et al. report that nonlinearities in current-voltage curves of gold quantum point contacts occur as a result of a shortening of the distance between electrodes at finite bias, presumably due to thermal expansion. For short wires, the electrode displacement induces a thickening of the wire, as well as nonlinearities of the IV curve, while the radius of long wires is left unchanged, thus resulting in a linear IV curve. We argue here that electron shell effects, which favor wires with certain "magic radii," prevent the thickening of long wires under compression, but have little effect on wires below a critical length.Comment: Version accepted for publication in Applied Physics Letter