Molecule-electrode interfaces in molecular electronic junctions are prone to chemical reactions, structural changes, and localized heating effects caused by electric current. These can be exploited for device functionality or may be degrading processes that limit performance and device lifetime. We develop a nonequilibrium Green's function based transport theory in which the central region atoms and, more importantly, atoms on molecule-electrode interfaces are allowed to move. The separation of time-scales of slow nuclear motion and fast electronic dynamics enables the algebraic solution of the Kadanoff-Baym equations in the Wigner space. As a result, analytical expressions for dynamical corrections to the adiabatically computed Green's functions are produced. These dynamical corrections depend not only on the instantaneous molecular geometry but also on the nuclear velocities. To make the theoretical approach fully self-consistent, the same time-separation approach is used to develop expressions for the adiabatic, dissipative, and stochastic components of current-induced forces in terms of adiabatic Green's functions. Using these current induced forces, the equation of motion for the nuclear degrees of freedom is cast in the form of a Langevin equation. The theory is applied to model molecular electronic junctions. We observe that the interplay between the value of the spring constant for the molecule-electrode chemical bond and electronic coupling strength to the corresponding electrode is critical for the appearance of structural instabilities and, consequently, telegraphic switching in the electric current. The range of model parameters is identified to observe structurally stable molecular junctions as well as various different kinds of current-induced telegraphic switching. The interfacial structural instabilities are also quantified based on current noise calculations.
We present quantum electron transport theory that incorporates dynamical effects of motion of atoms on electrode-molecule interfaces in the calculations of the electric current. The theory is based on non-equilibrium Green's functions. We separate time scales in the Green's functions on fast relative time and slow central time. The derivative with respect to the central time serves as a small parameter in the theory. We solve the real-time Kadanoff-Baym equations for molecular Green's functions using Wigner representation and keep terms up to the second order with respect to the central time d…
We measure electronic conductance through single conjugated molecules bonded to Au metal electrodes with direct Au-C covalent bonds using the scanning tunneling microscope based break-junction technique. We start with molecules terminated with trimethyltin end groups that cleave off in situ resulting in formation of a direct covalent sigma bond between the carbon backbone and the gold metal electrodes. The molecular carbon backbone used in this study consist of a conjugated pi-system that has one terminal methylene group on each end, which bonds to the electrodes, achieving large electronic co…
We report on a method to fabricate and measure gateable molecular junctions which are stable at room temperature. The devices are made by depositing molecules inside a few-layer graphene nanogap, formed by feedback controlled electroburning. The gaps have separations on the order of 1-2 nm as estimated from a Simmons model for tunneling. The molecular junctions display gateable IV-characteristics at room temperature.
We study electron transport through single-molecule junctions formed by an octanethiol molecule bonded with the thiol anchoring group to a gold electrode and the opposing methyl endgroup to a carbon tip. Using the scanning tunneling microscope based break junction technique, we measure the electrical conductance of such molecular junctions. We observe the presence of well-defined conductance plateaus during the stretching of the molecular bridge, which is the signature of the formation of a molecular junction.
We investigate charge transport in C$_{60}$-based single-molecule junctions with graphene electrodes employing a combination of density functional theory (DFT) electronic structure calculations and Landauer transport theory. In particular, the dependence of the transport properties on the conformation of the molecular bridge and the type of termination of the graphene electrodes is investigated. Furthermore, electron pathways through the junctions are analyzed using the theory of local currents. The results reveal, in agreement with previous experiments, a pronounced dependence of the transpor…
A quantum effect at ambient conditions is presented. A benzene dithiol (BDT) molecule or a tetrahydrofuran (THF) molecule is used as a barrier molecule bridging the gold electrodes from a Mechanically Controllable Break junction. It has been known for a long time that the environment of a junction couples to the conduction. With a microscopic layer of fluid it is actually possible to influence this coupling. The electrode-molecule-electrode configuration is lined with a microscopic layer of THF fluid, also known as the partially wet phase. This is effectively decoupling the electrode-molecule-…
Highly conductive molecular junctions were formed by direct binding of benzene molecules between two Pt electrodes. Measurements of conductance, isotopic shift in inelastic spectroscopy and shot noise compared with calculations provide indications for a stable molecular junction where the benzene molecule is preserved intact and bonded to the Pt leads via carbon atoms. The junction has a conductance comparable to that for metallic atomic junctions (around 0.1-1 Go), where the conductance and the number of transmission channels are controlled by the molecule's orientation at different inter-ele…
We consider plane junctions with graphene electrodes, which are formed by a single-level system ("molecule") placed between the edges of two single-layer graphene half planes. We calculate the edge Green functions of the electrodes and the corresponding lead self-energies for the molecular levels in the cases of semi-infinite single-layer electrodes with armchair and zigzag edges. We show two main effects: first, a peculiar energy-dependent level broadening, reflecting at low energies the linear energy dependence of the bulk density of states in graphene, and, second, the shift and splitting o…
Two recent experimental (Li, J.~\emphj{et al}, \emph{Proc.\ Natl.\ Acad.\ Sci.\ U.~S.~A.} {\bf 2014}, 111, 1282-1287) and theoretical studies (Bâldea, I, \emph{Phys.\ Chem.\ Chem.\ Phys.}\ {\bf 2014}, 16, 25942-25949) have addressed the problem of tuning molecular charge and vibrational properties of single molecules embedded in nanojunctions. These are molecular characteristics escaping so far to an efficient experimental control in broad ranges. Here, we present a general argument demonstrating why, out of various experimental platforms possible, those wherein active molecules are asymmetric…
We analyze various limits of vibrationally coupled resonant electron transport in single-molecule junctions. Based on a master equation approach, we discuss analytic and numerical results for junctions under a high bias voltage or weak electronic-vibrational coupling. It is shown that in these limits the vibrational excitation of the molecular bridge increases indefinitely, i.e. the junction exhibits a vibrational instability. Moreover, our analysis provides analytic results for the vibrational distribution function and reveals that these vibrational instabilities are related to electron-hole …
In this study, we electroplate Cu electrode on Si substrate to realize a large-area vacuum nanogap for electron tunneling. We used cathode coating, cathode rotation, asymmetric current regime, and electrolyte temperature stabilization to obtain the regular geometry of the Cu electrode and reduce its internal tension. Subsequently, internal tension was altered to achieve the predefined surface curvature (concave or convex). For 12-mm diameter Ag/Cu electrode, we achieve the curvature of 40 nm/mm from the Ag side. Reduction of the electrode diameter to 3 mm allowed curvature as low as of 2.5 nm/…
Graphene electrodes provide a suitable alternative to metal contacts in molecular conduction nanojunctions. Here, we propose to use graphene electrodes as a platform for effective photon assisted tunneling through molecular conduction nanojunctions. We predict dramatic increasing currents evaluated at side-band energies $\sim n\hbarω$ ($n$ is a whole number) related to the modification of graphene gapless spectrum under the action of external electromagnetic field of frequency $ω$. A side benifit of using doped graphene electrodes is the polarization control of photocurrent related to the proc…
Estimating the relative alignment between the frontier molecular orbitals that dominates the charge transport through single-molecule junctions represents a challenge for theory. This requires approaches beyond the widely employed framework provided by the density functional theory, wherein the Kohn-Sham "orbitals" are treated as if they were real molecular orbitals, which is not the case. In this paper, we report results obtained by means of quantum chemical calculations, including the EOM-CCSD (equation-of-motion coupled-cluster singles and doubles), which is the state-of-the-art of quantum …
The quantum interaction between molecules and electrode s material at molecules-electrode interfaces is a major ingredient in the electronic transport properties of organic junctions. Driven by the coupling strength between the two materials, it results mainly in a broadening and an energy shift of the interacting molecular orbitals. Using new electrodes materials, such as the recent semi-conducting two-dimensional nanomaterials, has become a recent challenge in the field of molecular-organic electronics that opens new possibilities for controlling the interfacial electronic properties and thu…
Controlling the magnetization reversal process of magnetic elements is important for a wide range of applications that make use of magnetoresistive effects, but is difficult to achieve for devices that require adjacent thin film structures capable of contacting an individual molecule or quantum dot. We report on the fabrication and measurement of ferromagnetic break junction devices with planar, elliptical leads to address the particular challenge of controlling the relative magnetization alignment between neighboring electrodes. Low temperature transport measurements, supported by finite-elem…
Destructive quantum interference (QI) has been a source of interest as a new paradigm for molecular electronics as the electronic conductance is widely dependent on the occurrence or absence of destructive QI effects. In order to interpret experimentally observed transmission features, it is necessary to understand the effects of all components of the junction on electron transport. We perform non-equilibrium Green's function calculations within the framework of density functional theory to assess the structure-function relationship of transport through pyrene molecular junctions with distinct…
We demonstrate shadow evaporation-based fabrication of high-quality ultrasmall normal metal -- insulator -- superconductor tunnel junctions where the thickness of the superconducting electrode is not limited by the requirement of small junction size. The junctions are formed between a film of manganese-doped aluminium acting as the normal conducting electrode, covered by a thicker, superconducting layer of pure Al. We characterize the junctions by sub-gap current--voltage measurements and charge pumping measurements in a gate-driven hybrid single-electron transistor, operated as a turnstile fo…
This paper reports our Monte Carlo (MC) studies aiming to explain the experimentally observed paramagnetic molecule induced antiferromagnetic coupling between the ferromagnetic (FM) electrodes. Recently developed magnetic tunnel junction based molecular spintronics devices (MTJMSDs), which were prepared by chemically bonding the paramagnetic molecules between the FM electrodes along the exposed side edges of magnetic tunnel junctions, exhibited molecule induced strong antiferromagnetic coupling. Our MC studies focused on the atomic model analogous to the MTJMSD and studied the effect of molecu…
We present studies of ballistic transport in three terminal T-shaped junction in a linear and non-linear regime. The floating electrode acts as a scatterer and modifies the conductance in a direct channel (between source and drain electrode). In the low voltage limit, the conductance shows the Wigner threshold effect and the bend resistance. A specific shape of the Wigner singularities can be changed by applied voltage to the floating electrode as well as by a shift of the Fermi level. The system also exhibits filtering properties with current distribution between different modes propagating i…
Negative differential resistance - a decrease in current with increasing bias voltage - is a counter-intuitive effect that is observed in various molecular junctions. Here, we present a novel mechanism that may be responsible for such an effect, based on strong Coulomb interaction between electrons in the molecule and electrons on the atoms closest to the molecule. The Coulomb interaction induces electron-hole binding across the molecule-electrode interface, resulting in a renormalized and enhanced molecule-electrode coupling. Using a self-consistent non-equilibrium Green's function approach, …
The interplay between groups of water molecules and single-atom contacts, as reflected in the electrical conductances and mechanical forces of copper atomic junctions, is explored by means of first-principles theory and semi-empirical calculations. We study the influence of the atomic geometries of copper electrodes with pyramidal and non-crystalline structures in the presence and absence of water on the conductance profiles as the electrodes approach each other. It is shown that the atomic arrangements of nano-contacts have crucial effects on the formation of plateaus and the conductance valu…
The magnetic and spin transport properties of a carbon chain between two armchair graphene nanoribbon (AGNR) electrodes were studied using tight-binding Hamiltonian, mean-field Hubbard model and Landauer-Butikker formalism. The results showed that only odd-numbered carbon chains show intrinsic magnetic moments in chain-graphene junctions. It was also found that the electronic, magnetic and spin transport properties of carbon chain-graphene junctions strongly depend on the position and the length of the carbon chains between AGNR electrodes. Interestingly, we found a fully spin-polarized transm…
The tunnel current and magnetoresistance (TMR) are investigated in magnetic tunnel junctions consisting of a spin-filter tunnel barrier, sandwiched between a ferromagnetic (FM) electrode and a nonmagnetic (NM) electrode. The investigations are based on the transfer matrix method and the free-electron approximation. The numerical results show that the spin transport depends on the relative magnetization orientation of the FM electrode and the spin-filter barrier, such that the tunnel current reaches its maximum when the magnetic moments of the FM electrode and the magnetic barrier are parallel.…
We assess the performances of the transition voltage spectroscopy (TVS) method to determine the energies of the molecular orbitals involved in the electronic transport though molecular junctions. A large number of various molecular junctions made with alkyl chains but with different chemical structure of the electrode-molecule interfaces are studied. In the case of molecular junctions with clean, unoxidized electrode-molecule interfaces, i.e. alkylthiols and alkenes directly grafted on Au and hydrogenated Si, respectively, we measure transition voltages in the range 0.9 - 1.4 V. We conclude th…
Whether at phenomenological or microscopic levels, most theoretical approaches to charge transport through molecular junctions postulate or attempt to justify microscopically the existence of a dominant molecular orbital (MO). Within such single level descriptions, experimental current-voltage I-V curves are sometimes/often analyzed by using analytical formulas expressing the current as a cubic expansion in terms of the applied voltage V, and relate possible V-driven shifts of the level energy offset relative to the metallic Fermi energy \varepsilon_{0} to an asymmetry of molecule-electrode co…
We demonstrate large rectification ratios (> 100) in single-molecule junctions based on a metal-oxide cluster (polyoxometalate), using a scanning tunneling microscope (STM) both at ambient conditions and at low temperature. These rectification ratios are the largest ever observed in a single-molecule junction, and in addition these junctions sustain current densities larger than 10^5 A/cm^2. By following the variation of the I-V characteristics with tip-molecule separation we demonstrate unambiguously that rectification is due to asymmetric coupling to the electrodes of a molecule with an asym…
The stationary Josephson current in a ballistic graphene system is theoretically studied with focus on a planar junction consisting of a monolayer graphene sheet on top of which a pair of superconducting electrodes is deposited. To characterize such a planar junction, we employ two parameters: the coupling strength between the graphene sheet and the superconducting electrodes, and a potential drop induced in the graphene sheet by direct contact with the electrodes. We derive a general formula for the Josephson current by taking these parameters into account in addition to other basic parameter…
Using the tight-binding model and the generalized Green's function formalism, the effect of quantum interference on the electron transport through the benzene molecule in a semiconductor/benzene/semiconductor junction is numerically investigated. We show how the quantum interference sources, different contact positions and local gate, can control the transmission characteristics of the electrode/molecule/electrode junction. We also study the occurrence of anti-resonant states in the transmission probability function using a simple graphical scheme (introduced in Ref.[Phys. Chem. Chem. Phys, 20…
A multilayer edge molecular electronics device (MEMED), which utilize the two metal electrodes of a metal-insulator-metal tunnel junction as the two electrical leads to molecular channels, can overcome the long standing fabrication challenges for developing futuristic molecular devices. However, producing ultrathin insulator is the most challenging step in MEMED fabrication. A simplified molecular device approach was developed by avoiding the need of depositing a new materiel on the bottom electrode for growing ultrathin insulator. This paper discuss the approach for MEMED's insulator growth b…
It is widely believed that when a molecule with thiol (S-H) end groups bridges a pair of gold electrodes, the S atoms bond to the gold and the thiol H atoms detach from the molecule. However, little is known regarding the details of this process, its time scale, and whether molecules with and without thiol hydrogen atoms can coexist in molecular junctions. Here we explore theoretically how inelastic tunneling spectroscopy (IETS) can shed light on these issues. We present calculations of the geometries, low bias conductances and IETS of propanedithiol and propanedithiolate molecular junctions w…
This letter presents experiments on junctions fabricated by a new technique that enables the use of high quality aluminum oxide tunnel barriers with normal metal electrodes at low temperatures. Inverse proximity effect is applied to diminish the superconductivity of an aluminum dot through a clean lateral connection to a normal metal electrode. To demonstrate the effectiveness of this method, fully normal-state single electron transistors (SET) and normal metal-insulator-superconductor (NIS) junctions applying proximized Al junctions were fabricated. The transport characteristics of the juncti…
We present a theoretical study of the heat dissipation in single-molecule junctions. In order to investigate the heat dissipation in the electrodes and the relationship between the transmission spectra and the electronic structures, we consider a toy model that in which electrodes linked by a two-level molecular bridge. By using of the Landauer approach, we show how heat dissipation in the electrodes of a molecular junction is related to its transmission characteristics. We show that in general heat is not equally dissipated in the left and right electrodes of the junction and it depends on th…
The spin-torque in magnetic tunnel junctions possesses two components that both depend on the applied voltage. Here, we develop a new method for the accurate extraction of this bias-dependence from experiments over large voltage ranges. We study several junctions with different magnetic layer structures of the top electrode. Our results obtained on junctions with symmetric CoFeB electrodes agree well with theoretical calculations. The bias-dependences of asymmetric samples, with top electrodes containing NiFe, however, are twisted compared to the quadratic form generally assumed. Our measureme…
Micromagnetic instabilities and non-uniform magnetization states play a significant role in spin transfer induced switching of nanometer scale magnetic elements. Here we model domain wall mediated switching dynamics in perpendicularly magnetized magnetic tunnel junction nanopillars. We show that domain wall surface tension always leads to magnetization oscillations and instabilities associated with the disk shape of the junction. A collective coordinate model is developed that captures aspects of these instabilities and illustrates their physical origin. Model results are compared to those of …
When an electron tunnels between two metal contacts it temporarily induces an image charge (IC) in the electrodes which acts back on the tunneling electron. It is usually assumed that the IC forms instantaneously such that a static model for the image potential applies. Here we investigate how the finite IC formation time affects charge transport through a molecule suspended between two electrodes. For a single level model, an analytical treatment shows that the conductance is suppressed by a factor $Z^2$ (compared to the static IC approximation) where $Z$ is the quasiparticle renormalization …
Anomalous and spin Hall effects are investigated theoretically for a magnetic tunnel junction where the applied voltage produces a Rashba spin-or bit coupling within the tunneling barrier layer. The ferromagnetic electrodes are the source of the spin-polarized current. The tunneling electrons experience a spin-orbit coupling inside the barrier due to the applied electrical field. Charge and spin Hall currents are calculated as functions of the position inside the barrier and the angle between the magnetizations of the electrodes. We find that both charge and spin Hall currents are located insi…
We explore the thermoelectric properties of gold atomic chains bridging gold electrodes by means of \textit{ab initio} and semi-empirical calculations, and heuristic reasoning. We predict the thermoelectric voltage induced by a temperature difference across such junctions to oscillate, repeatedly changing sign, as a function of the number of atoms $N$ making up the atomic chain. We also predict the amplitude of the oscillations to be proportional to $N$ for long atomic chains. Further we predict the thermoelectric voltage to change sign, in some cases, if the junction is stretched without chan…
We calculate the conductance through double junctions of the type M(inf.)-Sn-Mm-Sn-M(inf.) and triple junctions of the type M(inf.)-Sn-Mm-Sn-Mm-Sn-M(inf.), where M(inf.) are semi-infinite metallic electrodes, Sn are 'n' layers of semiconductor and Mm are 'm' layers of metal (the same as the electrodes), and compare the results with the conductance through simple junctions of the type M(inf.)-Sn-M(inf.). The junctions are bi-dimensional and their parts (electrodes and 'active region') are periodic in the direction perpendicular to the transport direction. To calculate the conductance we use the…
We determine the zero-bias anomaly of the conductance of tunnel junctions by an approach unifying the conventional Coulomb blockade theory for ultrasmall junctions with the diffusive anomalies in disordered conductors. Both, electron-electron interactions within the electrodes and electron-hole interactions between the electrodes are taken into account nonperturbatively. Explicit results are given for one- and two-dimensional junctions, and the crossover to ultrasmall junctions is discussed.
Obtaining highly spin-polarized currents in molecular junctions is crucial and desirable for nanoscale spintronics devices. Motivated by our recent symmetry-based theoretical argument for complete blocking of one spin conductance channel in atomic-scale junctions [A. Smogunov and Y. J. Dappe, Nano Lett. 15, 3552 (2015)], we explore the generality of the proposed mechanism and the degree of achieved spin-polarized current for various ferromagnetic electrodes (Ni, Co, Fe) and two different molecules, quaterthiophene and p-quaterphenyl. A simple analysis of the spin-resolved local density of stat…
A ferroelectric tunnel barrier in between two ferromagnetic electrodes (multiferroic tunnel junction, MFTJ), is one of the most promising concepts for future microelectronic devices. In parallel, Hafnia based ferroelectrics are showing great potential for device miniaturization down to the nanoscale. Here we utilize ferroelectric Hf0.5Zr0.5O2 (HZO) with thickness of only 2 nm, epitaxially grown on La0.7Sr0.3MnO3 (LSMO) ferromagnetic electrodes, as a large band-gap insulating barrier integrated in MFTJs with cobalt top electrodes. As previously reported for other MFTJs with similar electrodes, …
Amine terminated molecules show well behaved conductance in the scanning tunneling microscope break-junction experimental measurements. We performed density functional theory based electron transport calculations to explain the nature of this phenomenon. We find that amines can be adsorbed only on apex Au atom, while thiolate group can be attached equally well to undercoordinated and clean Au surfaces. Our calculations show that only one adsorption geo metry is sterically and energetically possible for amine anchored junction whereas three different adsorption geometries with very distinct tra…
We demonstrate the reversible in situ photoreduction of molecular junctions of phosphomolybdate [PMo12O40]3- monolayer self-assembled on flat gold electrodes, connected by the tip of a conductive atomic force microscope. The conductance of the one electron reduced [PMo12O40]4- molecular junction is increased by ca. 10, this open-shell state is stable in the junction in air at room temperature. The analysis of a large current-voltage dataset by unsupervised machine learning and clustering algorithms reveals that the electron transport in the pristine phosphomolybdate junctions leads to symmetri…
Double tunneling junctions of ferromagnet-superconductor-ferromagnet electrodes (FSF) show a jump in the conductance when a parallel magnetic field reverses the magnetization of one of the ferromagnetic electrodes. This change is generally attributed to the spin-valve effect or to pair breaking in the superconductor because of spin accumulation. In this paper it is shown that the Meservey-Tedrov effect causes a similar change in the conductance since the magnetic field changes the energy spectrum of the quasi-particles in the superconductor. A reversal of the bias reverses the sign in the cond…
We investigate the Josephson effect in a bilayer graphene flake contacted by two monolayer sheet deposited by superconducting electrodes. It is found that when the electrodes are attached to the different layers of the bilayer, the Josephson current is in a $π$ state when the bilayer region is undoped and in the absence of vertical bias. Applying doping or bias to the junction reveals $π-0$ transitions which can be controlled by varying the temperature and the junction length. The supercurrent reversal here is very different from the ferromagnetic Josephson junctions where the spin degree of f…
A first-principles approach is presented for the thermoelectricity in molecular junctions formed by a single molecule contact. The study investigates the Seebeck coefficient considering the source-drain electrodes with distinct temperatures and chemical potentials in a three-terminal geometry junction. We compare the Seebeck coefficient in the amino-substituted and unsubstituted butanethiol junction and observe interesting thermoelectric properties in the amino-substituted junction. Due to the novel states around the Fermi levels introduced by the amino-substitution, the Seebeck coefficient co…
A Josephson tunnel junction transistor based on quasiparticle injection is proposed. Its operation relies on the manipulation of the electron distribution in one of the junction electrodes. This is accomplished by injecting quasiparticle current through the junction electrode by two additional tunnel coupled superconductors. Both large supercurrent enhancement and fast quenching can be achieved with respect to equilibrium by varying quasiparticle injection for proper temperature regimes and suitable superconductor combinations. Joined with large power gain this makes the device attractive for …
Despite its fundamental importance for nano physics and chemistry and potential device applications, the relationship between atomic structure and electronic transport in molecular nanostructures is not well understood. Thus the experimentally observed increase of the conductance of some molecular nano junctions when they are stretched continues to be counterintuitive and controversial. Here we explore this phenomenon in propanedithiolate molecules bridging gold electrodes by means of {\em ab initio} computations and semi-empirical modeling. We show that in this system it is due to changes in …
Based on the non-equilibrium Green's function (NEGF) technique and the Landauer-Büttiker theory, the possibility of a molecular spin-electronic device, which consists of a single C$_{60}$ molecule attached to two ferromagnetic electrodes with finite cross sections, is investigated. By studying the coherent spin-dependent transport through the energy levels of the molecule, it is shown that the tunnel magnetoresistance (TMR) of the molecular junction depends on the applied voltages and the number of contact points between the device electrodes and the molecule. The TMR values more than 60% are …
We have applied the Numerical Renormalization Group method to study a mesoscopic system consisting of two samples of metal separated by an insulating barrier, with nanometer dimensions, which allows the tunnelling of a single electron from one to the other side of the junction. The junction is represented by a generalized orthodox model, taking into account the electronic scattering interaction due the hole and the tunnelling electrons, localized in the source and in the drain electrode, respectively. We have calculated the static properties (charge transference, charge average, quadractic cha…
We propose a model for a molecular junction with internal anharmonic torsional vibrations interacting with an electric current. The Wangsness-Bloch-Redfield master equation approach is used to determine the stationary reduced density matrix of the molecule. The dependence of the current, excitation energy and angular momentum of the junction on the applied voltage is studied. Negative differential conductance is observed in the current-voltage characteristics. It is shown that a model with vibrationally dependent coupling to the electrodes, asymmetric with respect to the interchanging of elect…
We report detailed atomistic simulations combined with high-fidelity conductance calculations to probe the structural origins of conductance fluctuations in thermally evolving Au-benzene-1,4-dithiolate-Au junctions. We compare the behavior of structurally ideal junctions (electrodes with flat surfaces) to structurally realistic, experimentally representative junctions resulting from break junction simulations. The enhanced mobility of metal atoms in structurally realistic junctions results in significant changes to the magnitude and origin of the conductance fluctuations. Fluctuations are larg…
We investigate theoretically the interplay of current-induced forces (CIF), Joule heating, and heat transport inside a current-carrying nano-conductor. We find that the CIF, due to the electron-phonon coherence, can control the spatial heat dissipation in the conductor. This yields a significant asymmetric concentration of excess heating (hot-spot) even for a symmetric conductor. When coupled to the electrode phonons, CIF drive different phonon heat flux into the two electrodes. First-principles calculations on realistic biased nano-junctions illustrate the importance of the effect.
On the elementary level, electronic current consists of individual electron tunnelling events that are separated by random time intervals. The waiting time distribution is a probability to observe the electron transfer in the detector electrode at time $t+τ$ given that an electron was detected in the same electrode at earlier time $t$. We study waiting time distribution for quantum transport in a vibrating molecular junction. By treating the electron-vibration interaction exactly and molecule-electrode coupling perturbatively, we obtain master equation and compute the distribution of waiting t…
The influence of vibrational motion on electron conduction through single molecules bound to metal electrodes is investigated employing first-principles electronic-structure calculations and projection-operator Green's function methods. Considering molecular junctions where a central phenyl ring is coupled via (alkane)thiol-bridges to gold electrodes, it is shown that -- depending on the distance between the electronic $π$-system and the metal -- electronic-vibrational coupling may result in pronounced vibrational substructures in the transmittance, a significantly reduced current as well as a…
