Electron transport characteristics through molecular wires are studied by using the Green's function formalism. Parametric calculations are performed based on the tight-binding model to investigate the transport properties through the wires. The transport characteristics are significantly influenced by (a) the interference effects, (b) chemical substituent group, (c) molecule-to-electrode coupling strength and (d) the gate voltage, and, here we focus our results in these aspects. In this article we also discuss the noise power of current fluctuations. The noise power gives key information about the electron correlation which is obtained by calculating the Fano factor (F) and the complete knowledge of the current fluctuations is very essential to fabricate efficient molecular devices.
Understanding electron transport processes in molecular wires connected between contacts is a central focus in the field of molecular electronics. Especially, the dephasing effect causing tunneling-to-hopping transition has great importance from both applicational and fundamental points of view. We analyzed coherent and incoherent electron transmission through conjugated molecular wires by means of density-functional tight-binding theory within the D'Amato-Pastawski model. Our approach can study explicitly the structure/transport relationship in molecular junctions in a dephasing environmental…
Analytic results for the conductance of a molecular wire attached to mesoscopic tubule leads are obtained. They permit to study linear transport in presence of low dimensional leads in the whole range of parameters. In particular contact effects can be addressed in detail. By focusing on the specificity of the lead-wire contact, we show that the geometry of this hybrid system supports a mechanism of channel selection, which is a distinctive hallmark of the mesoscopic nature of the electrodes.
Recently, rectifying direction inversion has been observed in dipyrimidinyl-diphenyl (PMPH) diblock molecular wire [J. Am. Chem. Soc. (2005) 127, 10456], and a protonation mechanism was suggested to explain this interesting phenomena. In this paper, we study the protonation effect on transport properties of PMPH molecule by first principles calculations. No significant rectification is found for the pristine diblock molecular wire. Protonation leads to conductance enhancement and rectification. However, for all considered junctions with rectifying effect, the preferential current directions ar…
Understanding of charge transport mechanisms in nanoscale structures is essential for the development of molecular electronic devices. Charge transport through 1D molecular systems connected between two contacts is influenced by several parameters such as the electronic structure of the molecule and the presence of disorder and defects. In this work, we have modeled 1D molecular wires connected between electrodes and systematically investigated the influence of both soliton formation and the presence of defects on properties such as the conductance and the density of states. Our numerical calc…
Electrical conduction through a two-terminal molecular device is studied using non-equilibrium Green's functions (NEGF) formalism. Such junction is made of a short linear wire which is connected to the metallic electrodes. Molecule itself is described with the help of Huckel (tight-binding) model with the electron interactions treated within extended Hubbard model (EHM), while the coupling to the electrodes is described with the help of a broad-band theory. Coulomb interactions within molecular wire are treated by means of the restricted Hartree-Fock (RHF) approximation. In particular, the inf…
We study the electronic and transport properties of two novel molecular wires made of atomic chains of carbon atoms (polyynes) capped with either, benzene-thiols or pyridines. While both molecules are structurally similar, the electrical conductance of benzene-thiol-capped chains attached to gold electrodes is found to be much higher than that of pyridine-capped chains. We predict that the conductance is almost independent of molecular length, which suggests that these molecules could be ideal molecular wires for sub-10 nm circuitry. Both systems exhibit negative differential resistance (NDR) …
We study linear electron transport through a molecular wire sandwiched between nanotube leads. We show that the presence of such electrodes strongly influences the calculated conductance. We find that depending on the quality and geometry of the contacts between the molecule and the tubular reservoirs, linear transport can be tuned between an effective Newns spectral behavior and a more structured one. The latter strongly depends on the topology of the leads. We also provide analytical evidence for an anomalous behavior of the conductance as a function of the contact strength.
We discuss the conductance of a molecular bridge between mesoscopic electrodes supporting low-dimensional transport and bearing an internal structure. As an example for such nanoelectrodes we assume semi-infinite (carbon) nanotubes. In the Landauer scattering matrix approach, we show that the conductance of this hybrid is very sensitive to the geometry of the contact unlike the usual behaviour in the presence of bulk electrodes.
We explore electron transport properties in a quantum wire attached to two metallic electrodes. A simple tight-binding model is used to describe the system and the coupling of the wire to the electrodes (source and drain) is treated through Newns-Anderson chemisorption theory. In our present model, the site energies of the wire are characterized by the relation $ε_i=W\cos(i λ^νπ)$ where $W$, $λ$, $ν$ are three positive numbers. For $ν=0$, the threshold bias voltage of electron conduction across the bridge can be controlled very nicely by tuning the strength of the potential $W$. On the other h…
The electronic conduction of a novel, three-terminal molecular architecture, analogous to a heterojunction bipolar transistor is studied. In this architecture, two diode arms consisting of donor-acceptor molecular wires fuse through a ring, while a gate modulating wire is a π-conjugated wire. The calculated results show the enhancement or depletion mode of a transistor by applying a gate field along the positive or negative direction. A small gate field is required to switch on the current in the proposed architecture. The changes in the electronic conduction can be attributed to the intrinsic…
Recent experimental realization [J. Am. Chem. Soc., 127 (2005) 7328] of various dithiocarbamate self assembly on gold surface opens the possibility for use of dithiocarbamate linkers to anchor molecular wires to gold electrodes. In this paper, we explore this hypothesis computationally. We computed the electron transport properties of 4,4'-bipyridine (BP), 4,4'-bipyridinium-1,1'-bis(carbodithioate) (BPBC), 4-(4'-pyridyl)-peridium-1-carbodithioate (BPC) molecule junctions based on the density functional theory and non-equilibrium Green's functions. We demonstrated that the stronger molecule-ele…
We introduce a theoretical approach based on scattering theory and total energy methods that treats transport non-linearities, conformational changes and charging effects in molecular wires in a unified way. We apply this approach to molecular wires consisting of chain molecules with different electronic and structural properties bonded to metal contacts. We show that non-linear transport in all of these systems can be understood in terms of a single physical mechanism and predict that negative differential resistance at high bias should be a generic property of such molecular wires.
The influence of contacts on linear transport through a molecular wire attached to mesoscopic tubule leads is studied. It is shown that low dimensional leads, such as carbon nanotubes, in contrast to bulky electrodes, strongly affect transport properties. By focusing on the specificity of the lead-wire contact, we show, in a fully analytical treatment, that the geometry of this hybrid system supports a mechanism of channel selection and a sum rule, which is a distinctive hallmark of the mesoscopic nature of the electrodes.
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.
We explore electron transport properties in molecular wires made of heterocyclic molecules (pyrrole, furan and thiophene) by using the Green's function technique. Parametric calculations are given based on the tight-binding model to describe the electron transport in these wires. It is observed that the transport properties are significantly influenced by (a) the heteroatoms in the heterocyclic molecules and (b) the molecule-to-electrodes coupling strength. Conductance ($g$) shows sharp resonance peaks associated with the molecular energy levels in the limit of weak molecular coupling, while t…
The electroluminescence of a polythiophene wire suspended between two metallic electrodes is probed using a scanning tunneling microscope. Under positive sample voltage, the spectral and voltage dependencies of the emitted light are consistent with the fluorescence of the wire junction mediated by localized plasmons. This emission is strongly attenuated for the opposite polarity. Both emission mechanism and polarity dependence are similar to what occurs in organic light emitting diodes (OLED) but at the level of a single molecular wire.
Molecular dynamics simulation have shown that after initial surface melting, nanowires can melt via two mechanisms: an interface front moves towards the wire centre; the growth of an instability at the interface can cause the solid to pinch-off and breakup. By perturbing a capillary fluctuation model describing the interface kinetics, we show when each mechanism is preferred and compare the results to molecular dynamics simulation. A Plateau-Rayleigh-type of instability is found, and suggests longer nanowires will melt via a instability mechanism, whereas in shorter nanowires the melting front…
A scanning tunnelling microscope is used to pull a polythiophene wire from a Au(111) surface while measuring the current traversing the junction. Abrupt current increases measured during the lifting procedure are associated to the detachment of molecular sub-units, in apparent contradiction with the expected exponential decrease of the conductance with wire length. \textit{Ab initio} simulations reproduce the experimental data and demonstrate that this unexpected behavior is due to release of mechanical stress in the wire, paving the way to mechanically gated single-molecule electronic devices…
Combining the features of molecular wires and femtosecond laser pulses gives the unique opportunity to optically switch electron currents in molecular devices with very high speed. Based on a weak-coupling approximation between wire and leads a quantum master equation for the population dynamics and the electric current through the molecular wire has been developed which allows for arbitrary time-dependent laser fields interacting with the wire. This formalism is combined with the theory of optimal control. For a tight-binding approximation of the wire we show how to compute the laser pulses t…
We present analytic and numerical studies based on Landauer theory of conductance antiresonances of molecular wires. Our analytic treatment is a solution of the Lippmann-Schwinger equation for the wire that includes the effects of the non-orthogonality of the atomic orbitals on different atoms exactly. The problem of non-orthogonality is treated by solving the transport problem in a new Hilbert space which is spanned by an orthogonal basis. An expression is derived for the energies at which antiresonances should occur for a molecular wire connected to a pair of single-channel 1D leads. From th…
We analyze the low-voltage transport response of large molecular wires bridging graphene electrodes, where the molecules are physisorbed onto the graphene sheets by planar anchor groups. In our study, the sheets are pulled away to vary the gap length and the relative atomic positions. The molecular wires are also translated in directions parallel and perpendicular to the sheets. We show that the energy position of the Breit-Wigner molecular resonances is universal for a given molecule, in the sense that it is independent of the details of the graphene edges, gaps lengths or of the molecule pos…
We derive an explicit expression for the quantum conductivity of a molecular wire containing a redox center, which is embedded in an electrochemical environment. The redox center interacts with the solvent, and the average over the solvent configurations is performed numerically. Explicit calculations have been performed for a chain of three atoms. When the redox center interacts strongly with neighboring electronic levels, the current-potential curves show interesting features like rectification, current plateaus and negative differential resistance. Electronic spectroscopy of intermediate st…
We present a self-consistent method for the evaluation of the electronic current flowing through a multi-terminal molecular wire. The method is based on Buttiker- Landauer theory which relates the current to one-electron scattering probabilities. The scattering problem is solved using a tight-binding form for Schroedinger's equation that incorporates a self-consistent evaluation of the electro-static potential in the region of the molecular wire. We apply the method to a three-terminal molecular wire connected to metallic leads. The molecular wire is a pi-conjugated carbon chain with thiol end…
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 …
We present a theoretical study of spin-dependent transport through molecular wires bridging ferromagnetic metal nanocontacts. We extend to magnetic systems a recently proposed model that provides a em quantitative explanation of the conductance measurements of Reed et al. on Au break-junctions bridged by self-assembled molecular monolayers (SAMs) of 1,4-benzene-dithiolate (BDT) molecules. Based on our calculations, we predict that spin-valve behavior should be observable in nickel break-junctions bridged by SAM's formed from BDT. We also consider spin transport in systems consisting of a clean…
The modified superexchange model is used to derive the expression for nonresonant tunneling conductance mediated by localized and delocalized molecular orbitals associated with the terminal and the interior molecular units respectively. The model is shown to work as long as delocalization of electron density in the chain's molecular orbitals is sustained during the tunneling. The criteria for reduction of the superexchange model of charge tunneling to the flat barrier model are formulated and the parameters of the barrier model (energy gap and effective electron mass) are specified in the term…
A molecular wire coupled to two electron reservoirs is investigated within a tight-binding approach including spin and Coulomb interaction. Under the assumption of weak coupling to the electron reservoirs a quantum master equation can be derived for the electron transport through the wire. Motivated by the phenomenon of coherent destruction of tunneling for monochromatic laser fields, the influence of Gaussian laser pulses on the transport through the wires is studied. For situations in which the maximum amplitude of the electric field fulfills the conditions for the destructive quantum effect…
Here we describe the design, single-molecule transport measurements, and theoretical modeling of a ferrocene-based organometallic molecular wire, whose bias-dependent conductance shows a clear Lorentzian form with magnitude exceeding 70% of the conductance quantum G_0. We attribute this unprecedented level of single-molecule conductance to a manifestation of the low-lying molecular resonance and extended orbital network long-predicted for a conjugated organic system. A similar-in-length, all-organic conjugated phenylethynyl oligomer molecular framework shows much lower conductance.
We have observed tunable negative differential resistance (NDR) in scanning tunneling spectroscopy measurements of a double layer of C60 molecules on a metallic surface. Using a simple model we show that the observed NDR behavior is explained by voltage-dependent changes in the tunneling barrier height.
Computationally inexpensive approximations describing electron-phonon scattering in molecular-scale conductors are derived from the non-equilibrium Green's function method. The accuracy is demonstrated with a first principles calculation on an atomic gold wire. Quantitative agreement between the full non-equilibrium Green's function calculation and the newly derived expressions is obtained while simplifying the computational burden by several orders of magnitude. In addition, analytical models provide intuitive understanding of the conductance including non-equilibrium heating and provide a co…
We study contact effects on electron transport across a molecular wire sandwiched between two semi-infinite (carbon) nanotube leads as a model for nanoelectrodes. Employing the Landauer scattering matrix approach we find that the conductance is very sensitive to parameters such as the coupling strength and geometry of the contact. The conductance exhibits markedly different behavior in the two limiting scenarios of single contact and multiple contacts between the molecular wire and the nanotube interfacial atoms. In contrast to a single contact the multiple-contact configuration acts as a filt…
The influence of Gaussian laser pulses on the transport through molecular wires is investigated within a tight-binding model for spinless electrons including correlation. Motivated by the phenomenon of coherent destruction of tunneling for monochromatic laser fields, situations are studied in which the maximum amplitude of the electric field fulfills the conditions for the destructive quantum effect. It is shown that, as for monochromatic laser pulses, the average current through the wire can be suppressed. For parameters of the model, which do not show a net current without any optical field,…
Well-known conductive molecular wires, like cumulene or polyyne, provide a model for interconnecting molecular electronics circuit. In the recent experiment, the appearance of carbon wire bridging two-dimensional electrodes - graphene sheets - was observed [PRL 102, 205501 (2009)], thus demonstrating a mechanical way of producing the cumulene. In this work, we study the structure and conductance properties of the carbon wire suspended between carbon nanotubes (CNTs) of different chiralities (zigzag and armchair), and corresponding conductance variation upon stretching. We find the geometrical …
Charge transport measurements on flexible Mo$_{6}$S$_{3}$I$_{6}$ (MoSI) nanowires with different diameters in highly imperfect 2-terminal circuits reveal systematic power law behaviour of the conductivity $σ(T,V)$ as a function of temperature and voltage. On the basis of measurements on a number of circuits we conclude that the behaviour in \emph{thin} wires can be most convincingly described by tunneling through Tomonaga-Luttinger liquid (TLL) segments of MoSI wire, which is in some cases modified by environmental Coulomb blockade (ECB). The latter are proposed to arise from deformations or i…
New features of molecular wires can be observed when they are irradiated by laser fields. These effects can be achieved by periodically oscillating fields but also by short laser pulses. The theoretical foundation used for these investigations is a density matrix formalism where the full system is partitioned into a relevant part and a thermal fermionic bath. The derivation of a quantum master equation, either based on a time-convolutionless or time-convolution projection-operator approach, incorporates the interaction with time-dependent laser fields non-perturbatively and is valid at low tem…
The effect of laser fields on the electron transport through a molecular wire being weakly coupled to two leads is investigated. The molecular wire acts as a coherent quantum ratchet if the molecule is composed of periodically arranged, asymmetric chemical groups. This setup presents a quantum rectifier with a finite dc-response in the absence of a static bias. The nonlinear current is evaluated in closed form within the Floquet basis of the isolated, driven wire. The current response reveals multiple current reversals together with a nonlinear dependence (reflecting avoided quasi-energy cross…
We present first principles calculations of current-voltage characteristics (IVC) and conductance of Au(111):S2-cumulene-S2:Au(111) molecular wire junctions with realistic contacts. The transport properties are calculated using full self-consistent ab initio NEGF-DFT methods under external bias. The conductance of the cumulene wires shows oscillatory behavior depending on the number of carbon atoms (double bonds). Among all conjugated oligomers, we find that cumulene wires with odd number of carbon atoms yield the highest conductance with metallic-like ballistic transport behavior. The reason …
With this study we analyze the fluctuations of an electronic only heat current across a molecular wire. The wire is composed of a single energy level which connects to two leads which are held at different temperatures. By use of the Green function method we derive the finite frequency power spectral density (PSD) of the emerging heat current fluctuations. This result assumes a form quite distinct from the power spectral density of the accompanying electric current noise. The complex expression simplifies considerably in the limit of zero frequency, yielding the heat noise intensity. The heat …
We use strain to statically tune the semiconductor band gap of individual InAs quantum dots (QDs) embedded in a GaAs photonic wire featuring very efficient single photon collection efficiency. Thanks to the geometry of the structure, we are able to shift the QD excitonic transition by more than 20 meV by using nano-manipulators to apply the stress. Moreover, owing to the strong transverse strain gradient generated in the structure, we can relatively tune two QDs located in the wire waveguide and bring them in resonance, opening the way to the observation of collective effects such as superradi…
Structural disorder is present in almost all experimental measurements of electronic transport through single molecules or molecular wires. To assess its influence on the conductance is computationally demanding, because a large number of conformations must be considered. Here we analyze an approximate recursive layer Green function approach for the ballistic transport through quasi one-dimensional nano-junctions. We find a rapid convergence of the method with its control parameter, the layer thickness, and good agreement with existing experimental and theoretical data. Because the computation…
We report our investigations on the finite-size effects of the Lorenz number in a molecular wire. Using Landauer-Büttiker formalism, we find that for sufficiently long wires there are two validity regimes of the Wiedemann-Franz (WF) law, the cotunneling and the sequential tunneling regimes, while in small systems only the first regime survives. We compare our results with the standard Kubo formalism and explain its failure to detect the WF law in small systems. Furthermore, our studies on exponentially localized disordered wires show that the Lorenz number value L_0 predicted by the WF law is …
Quantum descriptions of many complex systems are formulated most naturally in bases of states that are not mutually orthogonal. We introduce a general and powerful yet simple approach that facilitates solving such models exactly by embedding the non-orthogonal states in a new Hilbert space in which they are by definition mutually orthogonal. This novel approach is applied to electronic transport in molecular quantum wires and is used to predict conductance antiresonances of a new type that arise solely out of the non-orthogonality of the local orbitals on different sites of the wire.
Photo-induced charge separation in nanowires or molecular wires had been studied in previous experiments and simulations. Most researches deal with the carrier diffusions with the classical phenomenological models, or the static energy levels by quantum mechanics calculations. Here we give a dynamic quantum investigation on the charge separation and dissipation in molecule wires. The method is based on the time-dependent non-equilibrium Green's function theory. Polyacetylene chain and poly-phenylene are used as model systems with a tight-binding Hamiltonian and the wide band limit approximatio…
Measurements of electron transfer rates as well as of charge transport characteristics in DNA produced a number of seemingly contradictory results, ranging from insulating behaviour to the suggestion that DNA is an efficient medium for charge transport. Among other factors, environmental effects appear to play a crucial role in determining the effectivity of charge propagation along the double helix. This chapter gives an overview over charge transfer theories and their implication for addressing the interaction of a molecular conductor with a dissipative environment. Further, we focus on poss…
The potential profile across a biased molecular junction is calculated within the framework of a simple Thomas-Fermi type screening model. In particular, the relationship between this profile and the lateral molecular cross section is examined. We find that a transition from a linear potential profile to a potential that drops mainly near the molecule-metal contacts occurs with increasing cross section width, in agreement with numerical quantum calculations.
Besides active, functional molecular building blocks such as diodes or switches, passive components as, e.g., molecular wires, are required to realize molecular-scale electronics. Incorporating metal centers in the molecular backbone enables the molecular energy levels to be tuned in respect to the Fermi energy of the electrodes. Furthermore, by using more than one metal center and sp-bridging ligands, a strongly delocalized electron system is formed between these metallic "dopants", facilitating transport along the molecular backbone. Here, we study the influence of molecule--metal coupling o…
The influence of an electron-vibrational coupling on the laser control of electron transport through a molecular wire that is attached to several electronic leads is investigated. These molecular vibrational modes induce an effective electron-electron interaction. In the regime where the wire electrons couple weakly to both the external leads and the vibrational modes, we derive within a Hartree-Fock approximation a nonlinear set of quantum kinetic equations. The quantum kinetic theory is then used to evaluate the laser driven, time-averaged electron current through the wire-leads contacts. Th…
Using density functional theory, we investigate TM-cyclopentadienyl-benzene sandwich molecular wires (SMWs) which are composites of TM-cyclopentadienyl and TM-benzene wires (TM = transition metal (V, Fe)). All the SMWs are found to be highly stable ferromagnetic half-metals, showing spin switching behavior. Transport calculations show that finite size clusters display spin filter property when coupled with Au electrodes on either side. I-V characteristics of all systems confirm the spin filter property, with Au-BzVCpVBz-Au displaying exceptionally high performance. In addition to spin filterin…
We present a detailed study of the conduction properties of a molecular wire where hopping processes between electronic sites are coupled to a vibrational mode of the molecule. The latter is sandwiched between two electronic leads at finite temperatures. We show that the electro-mechanical coupling can lead to a strong enhancement of the lead-to-lead conduction. Moreover, under suitable driving of the molecular vibrational mode, the device can act as a transistor passing sharply from enhanced conduction to short-circuit configuration.
We consider circular currents in molecular wires with loop substructures studied within simple tight-binding models. Previous studies of this issue have focused on specific molecular structures. Here we address several general issues. First we consider the quantitative definition of a circular current and adopt a definition that identified the circular component of a loop current as the sole source of the magnetic field induced in the loop. The latter may be associated with the field at the loop center, with the magnetic moment associated with this field or with the total magnetic flux threadi…
The effect of dephasing on electron transport through a benzene molecule is carefully examined using a phenomenological model introduced by Büttiker. Within a tight-binding framework all the calculations are performed based on the Green's function formalism. We investigate the influence of dephasing on transmission probability and current-voltage characteristics for three different configurations ({\em ortho}, {\em meta} and {\em para}) of the molecular system depending on the locations of two contacting leads. The presence of dephasing provides a significant change in the spectral properties …
Freely suspended metallic single-wall carbon nanotubes (SWNTs) exhibit reduced current carrying ability compared to those lying on substrates, and striking negative differential conductance (NDC) at low electric fields. Theoretical analysis reveals significant self-heating effects including electron scattering by hot non-equilibrium optical phonons. Electron transport characteristics under strong self-heating are exploited for the first time to probe the thermal conductivity of individual SWNTs (~ 3600 Wm-1K-1 at T=300 K) up to ~700 K, and reveal a 1/T dependence expected for Umklapp phonon sc…
We study thermal transport through Pt nanowires that bridge planar contacts as a function of wire length and vibrational frequency of the contacts. When phonons in the contacts have lower average frequencies than those in the wires thermal transport occurs under conditions away from local equilibrium with low-frequency phonons experiencing a higher thermal gradient than high-frequency ones. This results in a size-dependent increase in the effective thermal conductivity of the wire with decreasing vibrational frequencies of the contacts. The interfacial resistivity when heat flows from the wire…
Recently [Phys. Rev. B 91, 125433 (2015)] we derived a general formula for the time-dependent quantum electron current through a molecular junction subject to an arbitrary time-dependent bias within the Wide Band Limit Approximation (WBLA) and assuming a single particle Hamiltonian. Here we present an efficient numerical scheme for calculating the current and particle number. Using the Padé expansion of the Fermi function, it is shown that all frequency integrals occurring in the general formula for the current can be removed analytically. Furthermore, when the bias in the reservoirs is assume…
If the factors controlling the decay in single-molecule electrical conductance G with molecular length L could be understood and controlled, then this would be a significant step forward in the design of high-conductance molecular wires. For a wide variety of molecules conducting by phase coherent tunneling, conductance G decays with length following the relationship G = Aexp-\bηL. It is widely accepted that the attenuation coefficient \bη is determined by the position of the Fermi energy of the electrodes relative to the energy of frontier orbitals of the molecular bridge, whereas the termina…
We study Andreev reflection in a normal conductor-molecule-superconductor junction using a first principles approach. In particular, we focus on a family of molecules consisting of a molecular backbone and a weakly coupled side group. We show that the presence of the side group can lead to a Fano resonance in the Andreev reflection. We use a simple theoretical model to explain the results of the numerical calculations and to make predictions about the possible sub-gap resonance structures in the Andreev reflection coefficient.
In a bridge configuration, a single graphene nanoribbon (GNR) is positioned with a picometer precision over a trench in between two monoatomic steps on an Au(111) surface. This GNR molecular wire adopts a deformed conformation towards the down terrace in between the two contact step edges. Using differential conductance dI/dV mapping from a low-temperature scanning tunneling microscope, it is demonstrated how the electronic delocalization along GNR is cut at each contact by its down curvature. It points out the need to bring conductive nanocontacts backside of the support for preserving the fr…
We present a theoretical study of the transport characteristics of molecular junctions, where first-row diatomic molecules are attached to (001) gold and platinum electrodes. We find that the conductance of all of these junctions is of the order of the conductance quantum unit $G_0$, spelling out that they belong to the transparent regime. We further find that the transmission coefficients show wide plateaus as a function of the energy, instead of the usual sharp resonances that signal the molecular levels in the tunneling regime. We use Caroli's model to show that this is a rather generic pro…
We investigate the transport behavior of polyene molecules sandwiched between two metallic contacts using the non-equilibrium Green's function formalism. We calculate both current and noise power as a function of applied voltage and show that they decrease with increasing size of the polyene molecules. We find that even with symmetric connection to metallic contacts, current verus voltage curves can be asymmetric for asymmetrically substituted polyenes. Most importantly, we demonstrate a cross-over from Poissonian to sub-Poissonian behavior in the shot noise as a function of applied voltage. T…
