Electron transport through a metal-molecule-metal junction

Molecules of bisthiolterthiophene have been adsorbed on the two facing gold electrodes of a mechanically controllable break junction in order to form metal-molecule(s)-metal junctions. Current-voltage (I-V) characteristics have been recorded at room temperature. Zero bias conductances were measured in the 10-100 nS range and different kinds of non-linear I-V curves with step-like features were reproducibly obtained. Switching between different kinds of I-V curves could be induced by varying the distance between the two metallic electrodes. The experimental results are discussed within the framework of tunneling transport models explicitly taking into account the discrete nature of the electronic spectrum of the molecule.Comment: 12 pages, 12 figures to appear in Phys. Rev. B 59(19) 199

Incoherent charge transport through molecular wires: interplay of Coulomb interaction and wire population

The influence of Coulomb interaction on the electron transport through molecular wires is studied in the regime of incoherent tunneling. In the limit of strong Coulomb repulsion, the current for spinless electrons is determined. It is shown that the voltage profile along the wire crucially influences the dependence of the current on the wire length. Upon inclusion of the spin degree of freedom one finds a blocking effect which depends both on the interaction strength and on the population of the wire. For finite Coulomb interaction, the temperature dependence of the blocking is studied and it is shown that several regimes with different blocking strength may exist.Comment: 18 pages, 8 figures, elsart.cls v2.18 include

Charging induced asymmetry in molecular conductors

We investigate the origin of asymmetry in various measured current-voltage (I-V) characteristics of molecules with no inherent spatial asymmetry, with particular focus on a recent break junction measurement. We argue that such asymmetry arises due to unequal coupling with the contacts and a consequent difference in charging effects, which can only be captured in a self-consistent model for molecular conduction. The direction of the asymmetry depends on the sign of the majority carriers in the molecule. For conduction through highest occupied molecular orbitals (i.e. HOMO or p-type conduction), the current is smaller for positive voltage on the stronger contact, while for conduction through lowest unoccupied molecular orbitals (i.e. LUMO or n-type conduction), the sense of the asymmetry is reversed. Within an extended Huckel description of the molecular chemistry and the contact microstructure (with two adjustable parameters, the position of the Fermi energy and the sulphur-gold bond length), an appropriate description of Poisson's equation, and a self-consistently coupled non-equilibrium Green's function (NEGF) description of transport, we achieve good agreement between theoretical and experimental I-V characteristics, both in shape as well as overall magnitude.Comment: length of the paper has been extended (4 pages to 6 pages), two new figures have been added (3 figures to 5 figures), has been accepted for PR

Stretching dependence of the vibration modes of a single-molecule Pt-H2-Pt bridge

A conducting bridge of a single hydrogen molecule between Pt electrodes is formed in a break junction experiment. It has a conductance near the quantum unit, G_0 = 2e^2/h, carried by a single channel. Using point contact spectroscopy three vibration modes are observed and their variation upon stretching and isotope substitution is obtained. The interpretation of the experiment in terms of a Pt-H_2-Pt bridge is verified by Density Functional Theory calculations for the stability, vibrational modes, and conductance of the structure.Comment: 5 pages, 4 figure

From a local Green function to molecular charge transport

A local-orbital based ab initio approach to obtain the Green function for large heterogeneous systems is developed. First a Green function formalism is introduced based on exact diagonalization. Then the self energy is constructed from an incremental scheme, rendering the procedure feasible, while at the same time physical insight into different local correlation contributions is obtained. Subsequently the Green function is used in the frame of the Landauer theory and the wide band approximation to calculate the electronic transmission coefficient across molecular junctions. The theory is applied to meta- and para-ditholbenzene linked to gold electrodes and various correlation contributions are analyzed

Path-integral Monte-Carlo simulations for electronic dynamics on molecular chains: I. Sequential hopping and super exchange

An improved real-time quantum Monte Carlo procedure is presented and applied to describe the electronic transfer dynamics along molecular chains. The model consists of discrete electronic sites coupled to a thermal environment which is integrated out exactly within the path integral formulation. The approach is numerically exact and its results reduce to known analytical findings (Marcus theory, golden rule) in proper limits. Special attention is paid to the role of superexchange and sequential hopping at lower temperatures in symmetric donor-bridge-acceptor systems. In contrast to previous approximate studies, superexchange turns out to play a significant role only for extremely high lying bridges where the transfer is basically frozen or for extremely low temperatures where for weaker dissipation a description in terms of rate constants is no longer feasible. For bridges with increasing length an algebraic decrease of the yield is found for short as well as for longer bridges. The approach can be extended to electronic systems with more complicated topologies including impurities and in presence of external time dependent forces.Comment: 14 pages, 9 figures submitted to the Journal of Chemical Physic

Generalized Numerical Renormalization Group for Dynamical Quantities

In this paper we introduce a new approach for calculating dynamical properties within the numerical renormalization group. It is demonstrated that the method previously used fails for the Anderson impurity in a magnetic field due to the absence of energy scale separation. The problem is solved by evaluating the Green function with respect to the reduced density matrix of the full system, leading to accurate spectra in agreement with the static magnetization. The new procedure (denoted as DM-NRG) provides a unifying framework for calculating dynamics at any temperature and represents the correct extension of Wilson's original thermodynamic calculation.Comment: 4 pages RevTeX, 6 eps figures include

Coherent charge transport through molecular wires: influence of strong Coulomb repulsion

We derive a master equation for the electron transport through molecular wires in the limit of strong Coulomb repulsion. This approach is applied to two typical situations: First, we study transport through an open conduction channel for which we find that the current exhibits an ohmic-like behaviour. Second, we explore the transport properties of a bridged molecular wire, where the current decays exponentially as a function of the wire length. For both situations, we discuss the differences to the case of non-interacting electrons.Comment: 15 pages, 4 figures, elsart style, accepted at Chem Phy

Landau-Zener transitions in a linear chain

We present an exact asymptotic solution for electron transition amplitudes in an infinite linear chain driven by an external homogeneous time-dependent electric field. This solution extends the Landau-Zener theory for the case of infinite number of states in discrete spectrum. In addition to transition amplitudes we calculate an effective diffusion constant.Comment: 3 figure

Shot noise in tunneling transport through molecules and quantum dots

We consider electrical transport through single molecules coupled to metal electrodes via tunneling barriers. Approximating the molecule by the Anderson impurity model as the simplest model which includes Coulomb charging effects, we extend the ``orthodox'' theory to expand current and shot noise systematically order by order in the tunnel couplings. In particular, we show that a combined measurement of current and shot noise reveals detailed information of the system even in the weak-coupling limit, such as the ratio of the tunnel-coupling strengths of the molecule to the left and right electrode, and the presence of the Coulomb charging energy. Our analysis holds for single-level quantum dots as well.Comment: 8 page