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

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

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

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

Theory of metastability in simple metal nanowires

Thermally induced conductance jumps of metal nanowires are modeled using stochastic Ginzburg-Landau field theories. Changes in radius are predicted to occur via the nucleation of surface kinks at the wire ends, consistent with recent electron microscopy studies. The activation rate displays nontrivial dependence on nanowire length, and undergoes first- or second-order-like transitions as a function of length. The activation barriers of the most stable structures are predicted to be universal, i.e., independent of the radius of the wire, and proportional to the square root of the surface tension. The reduction of the activation barrier under strain is also determined.Comment: 5 pages, 3 figure