Theoretical study of the charge transport through C60-based single-molecule junctions

We present a theoretical study of the conductance and thermopower of single-molecule junctions based on C60 and C60-terminated molecules. We first analyze the transport properties of gold-C60-gold junctions and show that these junctions can be highly conductive (with conductances above 0.1G0, where G0 is the quantum of conductance). Moreover, we find that the thermopower in these junctions is negative due to the fact that the LUMO dominates the charge transport, and its magnitude can reach several tens of micro-V/K, depending on the contact geometry. On the other hand, we study the suitability of C60 as an anchoring group in single-molecule junctions. For this purpose, we analyze the transport through several dumbbell derivatives using C60 as anchors, and we compare the results with those obtained with thiol and amine groups. Our results show that the conductance of C60-terminated molecules is rather sensitive to the binding geometry. Moreover, the conductance of the molecules is typically reduced by the presence of the C60 anchors, which in turn makes the junctions more sensitive to the functionalization of the molecular core with appropriate side groups.Comment: 9 pages, 7 figure

Field enhancement in subnanometer metallic gaps

Motivated by recent experiments [Ward et al., Nature Nanotech. 5, 732 (2010)], we present here a theoretical analysis of the optical response of sharp gold electrodes separated by a subnanometer gap. In particular, we have used classical finite difference time domain simulations to investigate the electric field distribution in these nanojunctions upon illumination. Our results show a strong confinement of the field within the gap region, resulting in a large enhancement compared to the incident field. Enhancement factors exceeding 1000 are found for interelectrode distances on the order of a few angstroms, which are fully compatible with the experimental findings. Such huge enhancements originate from the coupling of the incident light to the evanescent field of hybrid plasmons involving charge density oscillations in both electrodes.Comment: 4 pages, 3 figures, to appear in Physical Review

Role of electronic structure in photoassisted transport through atomic-sized contacts

We study theoretically quantum transport through laser-irradiated metallic atomic-sized contacts. The radiation field is treated classically, assuming its effect to be the generation of an ac voltage over the contact. We derive an expression for the dc current and compute the linear conductance in one-atom thick contacts as a function of the ac frequency, concentrating on the role played by electronic structure. In particular, we present results for three materials (Al, Pt, and Au) with very different electronic structures. It is shown that, depending on the frequency and the metal, the radiation can either enhance or diminish the conductance. This can be intuitively understood in terms of the energy dependence of the transmission of the contacts in the absence of radiation.Comment: 7 pages, 7 figures; four new figures adde

Effect of the Introduction of Impurities on the Stability Properties of Multibreathers at Low Coupling

sing a theorem dubbed the {\em Multibreather Stabiliy Theorem} [Physica D 180 (2003) 235-255] we have obtained the stability properties of multibreathers in systems of coupled oscillators with on-site potentials, with an inhomogeneity. Analytical results are obtained for 2-site, 3-site breathers, multibreathers, phonobreathers and dark breathers. The inhomogeneity is considered both at the on-site potential and at the coupling terms. All the results have been checked numerically with excellent agreement. The main conclusion is that the introduction of a impurity does not alter the stability properties.Comment: 20 pages, 9 figure

Multibreather and vortex breather stability in Klein--Gordon lattices: Equivalence between two different approaches

In this work, we revisit the question of stability of multibreather configurations, i.e., discrete breathers with multiple excited sites at the anti-continuum limit of uncoupled oscillators. We present two methods that yield quantitative predictions about the Floquet multipliers of the linear stability analysis around such exponentially localized in space, time-periodic orbits, based on the Aubry band method and the MacKay effective Hamiltonian method and prove that their conclusions are equivalent. Subsequently, we showcase the usefulness of the methods by a series of case examples including one-dimensional multi-breathers, and two-dimensional vortex breathers in the case of a lattice of linearly coupled oscillators with the Morse potential and in that of the discrete $\phi^4$ model

Stability of non-time-reversible phonobreathers

Non-time reversible phonobreathers are non-linear waves that can transport energy in coupled oscillator chains by means of a phase-torsion mechanism. In this paper, the stability properties of these structures have been considered. It has been performed an analytical study for low-coupling solutions based upon the so called {\em multibreather stability theorem} previously developed by some of the authors [Physica D {\bf 180} 235]. A numerical analysis confirms the analytical predictions and gives a detailed picture of the existence and stability properties for arbitrary frequency and coupling.Comment: J. Phys. A.:Math. and Theor. In Press (2010

Nonequilibrium Green's function theory for nonadiabatic effects in quantum electron transport

We develop nonequilibribrium Green's function based transport theory, which includes effects of nonadiabatic nuclear motion in the calculation of the electric current in molecular junctions. Our approach is based on the separation of slow and fast timescales in the equations of motion for the Green's functions by means of the Wigner representation. Time derivatives with respect to central time serves as a small parameter in the perturbative expansion enabling the computation of nonadiabatic corrections to molecular Green's functions. Consequently, we produce series of analytic expressions for non-adiabatic electronic Green's functions (up to the second order in the central time derivatives); which depend not solely on instantaneous molecular geometry but likewise on nuclear velocities and accelerations. Extended formula for electric current is derived which accounts for the non-adiabatic corrections. This theory is concisely illustrated by the calculations on a model molecular junction

Opportunities and limitations of transition voltage spectroscopy: a theoretical analysis

In molecular charge transport, transition voltage spectroscopy (TVS) holds the promise that molecular energy levels can be explored at bias voltages lower than required for resonant tunneling. We investigate the theoretical basis of this novel tool, using a generic model. In particular, we study the length dependence of the conducting frontier orbital and of the 'transition voltage' as a function of length. We show that this dependence is influenced by the amount of screening of the electrons in the molecule, which determines the voltage drop to be located at the contacts or across the entire molecule. We observe that the transition voltage depends significantly on the length, but that the ratio between the transition voltage and the conducting frontier orbital is approximately constant only in strongly screening (conjugated) molecules. Uncertainty about the screening within a molecule thus limits the predictive power of TVS. We furthermore argue that the relative length independence of the transition voltage for non-conjugated chains is due to strong localization of the frontier orbitals on the end groups ensuring binding of the rods to the metallic contacts. Finally, we investigate the characteristics of TVS in asymmetric molecular junctions. If a single level dominates the transport properties, TVS can provide a good estimate for both the level position and the degree of junction asymmetry. If more levels are involved the applicability of TVS becomes limited.Comment: 8 pages, 12 figure

Breather Statics and Dynamics in Klein--Gordon Chains with a Bend

In this communication, we examine a nonlinear model with an impurity emulating a bend. We justify the geometric interpretation of the model and connect it with earlier work on models including geometric effects. We focus on both the bifurcation and stability analysis of the modes that emerge as a function of the strength of the bend angle, but we also examine dynamical effects including the scattering of mobile localized modes (discrete breathers) off of such a geometric structure. The potential outcomes of such numerical experiments (including transmission, trapping within the bend as well as reflection) are highlighted and qualitatively explained. Such models are of interest both theoretically in understanding the interplay of breathers with curvature, but also practically in simple models of photonic crystals or of bent chains of DNA.Comment: 14 pages, 16 figure