Unusual conductance of polyyne-based molecular wires

We report a full self-consistent ab initio calculation of the current-voltage curve and the conductance of thiolate capped polyynes in contact with gold electrodes. We find the conductance of polyynes an order of magnitude larger compared with other conjugated oligomers. The reason lies in the position of the Fermi level deep in the HOMO related resonance. With the conductance weakly dependent on the applied bias and almost independent of the length of the molecular chain, polyynes appear as nearly perfect molecular wires.Comment: 4 pages, 5 figures, 3 table

High-order harmonic generation from polyatomic molecules including nuclear motion and a nuclear modes analysis

We present a generic approach for treating the effect of nuclear motion in the high-order harmonic generation from polyatomic molecules. Our procedure relies on a separation of nuclear and electron dynamics where we account for the electronic part using the Lewenstein model and nuclear motion enters as a nuclear correlation function. We express the nuclear correlation function in terms of Franck-Condon factors which allows us to decompose nuclear motion into modes and identify the modes that are dominant in the high-order harmonic generation process. We show results for the isotopes CH$_4$ and CD$_4$ and thereby provide direct theoretical support for a recent experiment [Baker {\it et al.}, Science {\bf 312}, 424 (2006)] that uses high-order harmonic generation to probe the ultra-fast structural nuclear rearrangement of ionized methane.Comment: 6 pages, 6 figure

Consequences of a Change in the Galactic Environment of the Sun

The interaction of the heliosphere with interstellar clouds has attracted interest since the late 1920's, both with a view to explaining apparent quasi-periodic climate "catastrophes" as well as periodic mass extinctions. Until recently, however, models describing the solar wind - local interstellar medium (LISM) interaction self-consistently had not been developed. Here, we describe the results of a two-dimensional (2D) simulation of the interaction between the heliosphere and an interstellar cloud with the same properties as currently, except that the neutral H density is increased from the present value of n(H) ~ 0.2 cm^-3 to 10 cm^-3. The mutual interaction of interstellar neutral hydrogen and plasma is included. The heliospheric cavity is reduced considerably in size (approximately 10 - 14 AU to the termination shock in the upstream direction) and is highly dynamical. The interplanetary environment at the orbit of the Earth changes markedly, with the density of interstellar H increasing to ~2 cm^-3. The termination shock itself experiences periods where it disappears, reforms and disappears again. Considerable mixing of the shocked solar wind and LISM occurs due to Rayleigh-Taylor-like instabilities at the nose, driven by ion-neutral friction. Implications for two anomalously high concentrations of 10Be found in Antarctic ice cores 33 kya and 60 kya, and the absence of prior similar events, are discussed in terms of density enhancements in the surrounding interstellar cloud. The calculation presented here supports past speculation that the galactic environment of the Sun moderates the interplanetary environment at the orbit of the Earth, and possibly also the terrestrial climate.Comment: 23 pages, 2 color plates (jpg), 3 figures (eps

High Harmonic Generation in SF6_{6}: Raman-excited Vibrational Quantum Beats

In a recent experiment (N. Wagner et al., PNAS v103, p13279) on SF$_{6}$, a high-harmonic generating laser pulse is preceded by a pump pulse which stimulates Raman-active modes in the molecule. Varying the time delay between the two pulses modulates high harmonic intensity, with frequencies equal to the vibration frequencies of the Raman-active modes. We propose an explanation of this modulation as a quantum interference between competing pathways that occur via adjacent vibrational states of the molecule. The Raman and high harmonic processes act as beamsplitters, producing vibrational quantum beats among the Raman-active vibrational modes that are excited by the first pulse. We introduce a rigorous treatment of the electron-ion recombination process and the effect of the ionic Coulomb field in the electron propagation outside the molecule, improving over the widely-used three-step model.Comment: submitted to PR

Universal decay of scalar turbulence

The asymptotic decay of passive scalar fields is solved analytically for the Kraichnan model, where the velocity has a short correlation time. At long times, two universality classes are found, both characterized by a distribution of the scalar -- generally non-Gaussian -- with global self-similar evolution in time. Analogous behavior is found numerically with a more realistic flow resulting from an inverse energy cascade.Comment: 4 pages, 3 Postscript figures, submitted to PR

Energy flux fluctuations in a finite volume of turbulent flow

The flux of turbulent kinetic energy from large to small spatial scales is measured in a small domain B of varying size R. The probability distribution function of the flux is obtained using a time-local version of Kolmogorov's four-fifths law. The measurements, made at a moderate Reynolds number, show frequent events where the flux is backscattered from small to large scales, their frequency increasing as R is decreased. The observations are corroborated by a numerical simulation based on the motion of many particles and on an explicit form of the eddy damping.Comment: 10 Pages, 5 figures, 1 tabl

A Multiresolution Census Algorithm for Calculating Vortex Statistics in Turbulent Flows

The fundamental equations that model turbulent flow do not provide much insight into the size and shape of observed turbulent structures. We investigate the efficient and accurate representation of structures in two-dimensional turbulence by applying statistical models directly to the simulated vorticity field. Rather than extract the coherent portion of the image from the background variation, as in the classical signal-plus-noise model, we present a model for individual vortices using the non-decimated discrete wavelet transform. A template image, supplied by the user, provides the features to be extracted from the vorticity field. By transforming the vortex template into the wavelet domain, specific characteristics present in the template, such as size and symmetry, are broken down into components associated with spatial frequencies. Multivariate multiple linear regression is used to fit the vortex template to the vorticity field in the wavelet domain. Since all levels of the template decomposition may be used to model each level in the field decomposition, the resulting model need not be identical to the template. Application to a vortex census algorithm that records quantities of interest (such as size, peak amplitude, circulation, etc.) as the vorticity field evolves is given. The multiresolution census algorithm extracts coherent structures of all shapes and sizes in simulated vorticity fields and is able to reproduce known physical scaling laws when processing a set of voriticity fields that evolve over time

Stiff polymer in monomer ensemble

We make use of the previously developed formalism for a monomer ensemble and include angular dependence of the segments of the polymer chains thus described. In particular we show how to deal with stiffness when the polymer chain is confined to certain regions. We investigate the stiffness from the perspectives of a differential equation, integral equations, or recursive relations for both continuum and lattice models. Exact analytical solutions are presented for two cases, whereas numerical results are shown for a third case.Comment: 10 pages, including 6 figure

Nontrivial temporal scaling in a Galilean stick-slip dynamics

We examine the stick-slip fluctuating response of a rough massive non-rotating cylinder moving on a rough inclined groove which is submitted to weak external perturbations and which is maintained well below the angle of repose. The experiments presented here, which are reminiscent of the Galileo's works with rolling objects on inclines, have brought in the last years important new insights into the friction between surfaces in relative motion and are of relevance for earthquakes, differing from classical block-spring models by the mechanism of energy input in the system. Robust nontrivial temporal scaling laws appearing in the dynamics of this system are reported, and it is shown that the time-support where dissipation occurs approaches a statistical fractal set with a fixed value of dimension. The distribution of periods of inactivity in the intermittent motion of the cylinder is also studied and found to be closely related to the lacunarity of a random version of the classic triadic Cantor set on the line.Comment: 7 pages including 6 figure

A note on the extension of the polar decomposition for the multidimensional Burgers equation

It is shown that the generalizations to more than one space dimension of the pole decomposition for the Burgers equation with finite viscosity and no force are of the form u = -2 viscosity grad log P, where the P's are explicitly known algebraic (or trigonometric) polynomials in the space variables with polynomial (or exponential) dependence on time. Such solutions have polar singularities on complex algebraic varieties.Comment: 3 pages; minor formatting and typos corrected. Submitted to Phys. Rev. E (Rapid Comm.