Electromigrated nanoscale junctions have proven very useful for studying electronic transport at the single-molecule scale. However, confirming that conduction is through precisely the molecule of interest and not some contaminant or metal nanoparticle has remained a persistent challenge, typically requiring a statistical analysis of many devices. We review how transport mechanisms in both purely electronic and optical measurements can be used to infer information about the nanoscale junction configuration. The electronic response to optical excitation is particularly revealing. We briefly discuss surface-enhanced Raman spectroscopy on such junctions, and present new results showing that currents due to optical rectification can provide a means of estimating the local electric field at the junction due to illumination.
We present gate-dependent transport measurements of Kondo impurities in bare gold break junctions, generated with high yield using an electromigration process that is actively controlled. Thirty percent of measured devices show zero-bias conductance peaks. Temperature dependence suggests Kondo temperatures \~7K. The peak splitting in magnetic field is consistent with theoretical predictions for g=2, though in many devices the splitting is offset from 2guB by a fixed energy. The Kondo resonances observed here may be due to atomic-scale metallic grains formed during electromigration.
We report measurements of the electron transport through atomic-scale constrictions and tunnel junctions between ferromagnetic electrodes. Structures are fabricated using a combination of e-beam lithography and controlled electromigration. Sample geometries are chosen to allow independent control of electrode bulk magnetizations. As junction size is decreased to the single channel limit, conventional anisotropic magnetoresistance (AMR) increases in magnitude, approaching the size expected for tunneling magnetoresistance (TMR) upon tunnel junction formation. Significant mesoscopic variations ar…
Noise measurements are a probe beyond simple electronic transport that can reveal additional information about electronic correlations and inelastic processes. Here we report noise measurements in individual electromigrated nanojunctions, examining the evolution from the many channel regime to the tunneling regime, using a radio frequency technique. While we generally observe the dependence of noise on bias expected for shot noise, in approximately 12% of junction configurations we find discrete changes in the bias dependence at threshold values of the bias, consistent with electronic excitati…
In this paper we describe a nonlinear imaging method employed to spatially map the occurrence of constrictions occurring on an electrically-stressed gold nanowire. The approach consists at measuring the influence of a tightly focused ultrafast pulsed laser on the electronic transport in the nanowire. We found that structural defects distributed along the nanowire are efficient nonlinear optical sources of radiation and that the differential conductance is significantly decreased when the laser is incident on such electrically-induced morphological changes. This imaging technique is applied to …
We present a theoretical analysis aimed at understanding electrical conduction in molecular tunnel junctions. We focus on discussing the validity of coherent versus incoherent theoretical formulations for single-level tunneling to explain experimental results obtained under a wide range of experimental conditions, including measurements in individual molecules connecting the leads of electromigrated single-electron transistors and junctions of self-assembled monolayers (SAM) of molecules sandwiched between two macroscopic contacts. We show that the restriction of transport through a single lev…
The interaction between electronic and vibrational degrees of freedom in single-molecule junctions may result from the dependence of the electronic energies or the electronic states of the molecular bridge on the nuclear displacement. The latter mechanism leads to a direct coupling between different electronic states and is referred to as nonadiabatic electronic-vibrational coupling. Employing a perturbative nonequilibrium Green's function approach, we study the influence of nonadiabatic electronic-vibrational coupling in model molecular junctions. Thereby we distinguish between systems with w…
The energy and charge fluxes carried by electrons in a two-terminal junction subjected to a random telegraph noise, produced by a single electronic defect, are analyzed. The telegraph processes are imitated by the action of a stochastic electric field that acts on the electrons in the junction. Upon averaging over all random events of the telegraph process, it is found that this electric field supplies, on the average, energy to the electronic reservoirs, which is distributed unequally between them: the stronger is the coupling of the reservoir with the junction, the more energy it gains. Thus…
The interaction between electronic and nuclear degrees of freedom in single-molecule junctions is an essential mechanism, which may result in the current-induced rupture of chemical bonds. As such, it is fundamental for the stability of molecular junctions and for the applicability of molecular electronic devices. In this publication, we study current-induced bond rupture in molecular junctions using a numerically exact scheme, which is based on the hierarchical quantum master equation (HQME) method in combination with a discrete variable representation for the nuclear degrees of freedom. Empl…
The influence of multiple vibrational modes on current fluctuations in electron transport through single-molecule junctions is investigated. Our analysis is based on a generic model of a molecular junction, which comprises a single electronic state on the molecular bridge coupled to multiple vibrational modes and fermionic leads, and employs a master equation approach. The results reveal that in molecular junctions with multiple vibrational modes already weak to moderate electronic-vibrational coupling may result in high noise levels, especially at the onset of resonant transport, in accordanc…
Electronic Whispering Gallery Modes (EWGMs) have been recently observed in several circular graphene junctions, pn and pp0, created in scanning tunnelling microscope experiments. By computing the local density of states within the Dirac-Weyl formalism for massless fermions we demonstrate that the EWGMs may really be emerged in any type of the electrostatic potential induced circular graphene junctions, including uni-junctions (e.g. np- or pp0-junctions) as well as bipolar-junctions (e.g. pnp-heterojunctions). Surprisingly, quantitative analyses show that for all the EWGMs identified (regardles…
Temperature ($T$) dependent conductance $G = G(T)$ data measured in molecular junctions are routinely taken as evidence for a two-step hopping mechanism. The present paper emphasizes that this is not necessarily the case. A curve of $\ln G$ versus $1/T$ decreasing almost linearly (Arrhenius-like regime) and eventually switching to a nearly horizontal plateau (Sommerfeld regime), or possessing a slope gradually decreasing with increasing $1/T$ is fully compatible with a single-step tunneling mechanism. The results for the dependence of $G$ on $T$ presented include both analytical exact and accu…
The exact ground-state exchange-correlation functional of Kohn-Sham density functional theory yields the exact transmission through an Anderson junction at zero bias and temperature. The exact impurity charge susceptibility is used to construct the exact exchange-correlation potential. We analyze the successes and limitations of various types of approximations, including smooth and discontinuous functionals of the occupation, as well as symmetry-broken approaches.
Using a model comprising a 2-level bridge connecting free electron reservoirs we show that coupling of a molecular bridge to electron-hole excitations in the leads can markedly effect the source-drain current through a molecular junction.In some cases, e.g. molecules that exhibit strong charge transfer transitions, the contribution from electron-hole excitations can exceed the Landauer elastic current and dominate the observed conduction.
We use simultaneous electronic transport and optical characterization measurements to reveal new information about electronic and optical processes in nanoscale junctions fabricated by electromigration. Comparing electronic tunneling and photocurrents allows us to infer the optical frequency potential difference produced by the plasmon response of the junction. Together with the measured tunneling conductance, we can then determine the locally enhanced electric field within the junction. In similar structures containing molecules, anti-Stokes and Stokes Raman emission allow us to infer the eff…
We investigate the conductance of normal-conductor/graphene/normal-conductor (NGN) junctions for arbitrary on-site potentials in the normal and graphitic parts of the system. We find that a ballistic NGN junction can display insulating behavior even when the charge-carrier density in the graphene part is finite. This effect originates in the different k intervals supporting propagating modes in graphene and a normal conductor, and persists for moderate levels of bulk, edge, or interface disorder. The ensuing conductance thresholds could be used as an electronic tool to map out details of the g…
We propose to correlate transmittance maps and spectral-density maps of planar junctions, in order to analyze quantitatively and in detail spin-dependent transport calculations. Since spectral-density maps can be resolved with respect to atom, angular momentum, and spin, the resulting correlation coefficients reveal unequivocally, e.g., which layers or which orbitals determine the tunnel conductances. Our method can be used for transport calculations within the Landauer-Büttiker formalism. Its properties and features will be discussed by means of a pure bcc Fe(001) lead as well as an extensive…
We carry out a layer-by-layer investigation to understand electron transport across metal-insulator-metal junctions. Interfacial structures of junctions were studied and characterized using first-principles density functional theory within the generalized gradient approximation. We found that as a function of the number of crystal layers the calculated transmission coefficients of multilayer silicene junctions decay much slower than for BN-based junctions We revisited the semiclassical Boltzmann theory of electronic transport and applied to multilayer silicene and BN-based junctions. The calcu…
Electronic conduction through single molecules is affected by the molecular electronic structure as well as by other information that is extremely difficult to assess, such as bonding geometry and chemical environment. The lack of an independent diagnostic technique has long hampered single-molecule conductance studies. We report simultaneous measurement of the conductance and the Raman spectra of nanoscale junctions used for single-molecule electronic experiments. Blinking and spectral diffusion in the Raman response of both para-mercaptoaniline and a fluorinated oligophenylyne ethynylene cor…
Fluctuations pose fundamental limitations in making sensitive measurements, yet at the same time, noise unravels properties that are inaccessible at the level of the averaged signal. In electronic devices, shot noise arises from the discrete nature of charge carriers and it increases linearly with the applied voltage according to the celebrated Schottky formula. Nonetheless, measurements of shot noise in atomic-scale junctions at high voltage reveal significant nonlinear (anomalous) behavior, which varies from sample to sample, and has no specific trend. Here, we provide a viable, unifying exp…
Understanding and controlling the flow of heat is a major challenge in nanoelectronics. When a junction is driven out of equilibrium by light or the flow of electric charge, the vibrational and electronic degrees of freedom are, in general, no longer described by a single temperature[1-6]. Moreover, characterizing the steady-state vibrational and electronic distributions {\it in situ} is extremely challenging. Here we show that surface-enhanced Raman emission may be used to determine the effective temperatures for both the vibrational modes and the flowing electrons in a biased metallic nanosc…
The accurate determination of electronic temperatures in metallic nanostructures is essential for many technological applications, like plasmon-enhanced catalysis or lithographic nanofabrication procedures. In this Letter we demonstrate that the electronic temperature can be accurately measured by the shape of the tunnel electroluminescence emission edge in tunnel plasmonic nanocavities, which follows a universal thermal distribution with the bias voltage as the chemical potential of the photon population. A significant deviation between electronic and lattice temperatures is found below 30 K …
We investigate the electronic transport properties of a ferromagnet/normal/ferromagnet junction on the surface of a topological insulator with a gate voltage exerted on the normal segment. It is found that the conductance oscillates with the width of normal segment and gate voltage, and the maximum of conductance gradually decreases while the minimum of conductance approaches zero as the width increases. The conductance can be controlled by tuning the gate voltage like a spin field-effect transistor. It is found that the magnetoresistance ratio can be very large, and can also be negative owing…
Micro-refrigerators that operate in the sub-kelvin regime are a key device in quantum technology. A well-studied candidate, an electronic cooler using Normal metal - Insulator - Superconductor (NIS) tunnel junctions offers substantial performance and power. However, its superconducting electrodes are severely overheated due to exponential suppression of their thermal conductance towards low temperatures, and the cooler performs unsatisfactorily - especially in powerful devices needed for practical applications. We employ a second NIS cooling stage to thermalize the hot superconductor at the ba…
Nanoscale molecular-electronic devices and machines are emerging as promising functional elements, naturally flexible and efficient, for next generation technologies. A deeper understanding of carrier dynamics in molecular junctions is expected to benefit many fields of nanoelectronics and power-devices. We determine time-resolved charge current flowing at donor- acceptor interface in molecular junctions connected to metallic electrodes by means of quantum transport simulations. The current is induced by the interaction of the donor with a Gaussian-shape femtosecond laser pulse. Effects of the…
Spatial manipulation of current flow in graphene could be achieved through the use of a tilted pn junction. We show through numerical simulation that a pseudo-Hall effect (i.e. non-equilibrium charge and current density accumulating along one of the sides of a graphene ribbon) can be observed under these conditions. The tilt angle and the pn transition length are two key parameters in tuning the strength of this effect. This phenomenon can be explained using classical trajectory via ray analysis, and is therefore relatively robust against disorder. Lastly, we propose and simulate a three termi…
We investigate transport through molecular wires whose energy levels are affected by environmental fluctuations. We assume that the relevant fluctuations are so slow that they, within a tight-binding description, can be described by disordered, Gaussian distributed onsite energies. For long wires, we find that the corresponding current distribution can be rather broad even for a small energy variance. Moreover, we analyse with a Floquet master equation the interplay of laser excitations and static disorder. Then the disorder leads to spatial asymmetries such that the laser diving can induce a …
Vibrational nonequilibrium effects in charge transport through single-molecule junctions are investigated. Focusing on molecular bridges with multiple electronic states, it is shown that electronic-vibrational coupling triggers a variety of vibronic emission and absorption processes, which influence the conductance properties and mechanical stability of single-molecule junctions profoundly. Employing a master equation and a nonequilibrium Green's function approach, these processes are analyzed in detail for a generic model of a molecular junction and for benzenedibutanethiolate bound to gold e…
We present a theory of molecular motors based on the Ehrenfest dynamics for the nuclear coordinates and the adiabatic limit of the Kadanoff-Baym equations for the current-induced forces. Electron-electron interactions can be systematically included through many-body perturbation theory, making the nonequilibrium Green's functions formulation suitable for first-principles treatments of realistic junctions. The method is benchmarked against simulations via real-time Kadanoff-Baym equations, finding an excellent agreement. Results on a paradigmatic model of molecular motor show that correlations …
We have developed a device fabrication process to pattern graphene into nanostructures of arbitrary shape and control their electronic properties using local electrostatic gates. Electronic transport measurements have been used to characterize locally gated bipolar graphene $p$-$n$-$p$ junctions. We observe a series of fractional quantum Hall conductance plateaus at high magnetic fields as the local charge density is varied in the $p$ and $n$ regions. These fractional plateaus, originating from chiral edge states equilibration at the $p$-$n$ interfaces, exhibit sensitivity to inter-edge backsc…
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…
Using density functional theory and nonequilibrium Greens functions-based methods we investigated the electronic and transport properties of monolayer TiS3 pn-junction. We constructed a lateral pn-junction in monolayer TiS3 by using Li and F adatoms. An applied bias voltage caused significant variability in the electronic and transport properties of the TiS3 pn-junction. In addition, spin dependent current-voltage characteristics of the constructed TiS3 pn-junction were analyzed. Important device characteristics were found such as negative differential resistance and rectifying diode behaviors…
The sensitivity of superconducting qubits allows for spectroscopy and coherence measurements on individual two-level systems present in the disordered tunnel barrier of an $\mathrm{Al/AlO_x/Al}$ Josephson junction. We report experimental evidence for the decoherence of two-level systems by Bogoliubov quasiparticles leaking into the insulating $\mathrm{AlO_x}$ barrier. We control the density of quasiparticles in the junction electrodes either by the sample temperature or by injecting them using an on-chip dc-SQUID driven to its resistive state. The decoherence rates were measured by observing t…
The description of transport phenomena in devices consisting of arrays of tunnel junctions, and the experimental confirmation of these predictions is one of the great successes of mesoscopic physics. The aim of this paper is to give a self-consistent review of sequential transport processes in such devices, based on the so-called "orthodox" model. We calculate numerically the current-voltage (I-V) curves, the conductance versus bias voltage (G-V) curves, and the associated thermal transport in symmetric and asymmetric two-junction arrays such as Coulomb-blockade thermometers (CBTs), supercondu…
Quantum interference effects and decoherence mechanisms in single-molecule junctions are analyzed employing a nonequilibrium Green's function approach. Electrons tunneling through quasi-degenerate states of a nanoscale molecular junction exhibit interference effects. We show that electronic-vibrational coupling, inherent to any molecular junction, strongly quenches such interference effects. As a result, the electrical current can be significantly larger than without electronic-vibrational coupling. The analysis reveals that the quenching of quantum interference is particularly pronounced if t…
We present electronic transport measurements through thiolated C$_{60}$ molecules in liquid environment. The molecules were placed within a mechanically controllable break junction using a single anchoring group per molecule. When varying the electrode separation of the C$_{60}$-modified junctions, we observed a peak in the conductance traces. The shape of the curves is strongly influenced by the environment of the junction as shown by measurements in two distinct solvents. In the framework of a simple resonant tunneling model, we can extract the electronic tunneling rates governing the transp…
Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this region. With the advent of atomically thin van der Waals (vdW) materials and their heterostructures, we are now able to realize a p-n junction at the ultimate quantum limit. In particular, vdW junction…
We study the ac charge and -spin transport through an orbital of a magnetic molecule with spin precessing in a constant magnetic field. We assume that the source and drain contacts have time-dependent chemical potentials. We employ the Keldysh nonequilibrium Green's functions method to calculate the spin and charge currents to linear order in the time-dependent potentials. The molecular and electronic spins are coupled via exchange interaction. The time-dependent molecular spin drives inelastic transitions between the molecular quasienergy levels, resulting in a rich structure in the transport…
Graphene matter in a strong magnetic field, realizing one-dimensional quantum Hall channels, provides a unique platform for studying electron interference. Here, using the Landauer-Büttiker formalism along with the tight-binding model, we investigate the quantum Hall (QH) effects in unipolar and bipolar monolayer-bilayer graphene (MLG-BLG) junctions. We find that a Hall bar made of an armchair MLG-BLG junction in the bipolar regime results in valley-polarized edge-channel interferences and can operate a fully tunable Mach-Zehnder (MZ) interferometer device. Investigation of the bar-width and m…
The multilayer multiconfiguration time-dependent Hartree theory within second quantization representation of the Fock space is applied to study correlated electron transport in models of single-molecule junctions. Extending previous work, we consider models which include both electron-electron and electronic-vibrational interaction. The results show the influence of the interactions on the transient and the stationary electrical current. The underlying physical mechanisms are analyzed in conjunction with the nonequilibrium electronic population of the molecular bridge.
We show that when a molecular junction is under an external bias, its properties can not be uniquely determined by the total electron density in the same manner as the density functional theory (DFT) for ground state (GS) properties. In order to correctly incorporate bias-induced nonequilibrium effects, we present a dual mean field (DMF) approach. The key idea is that the total electron density together with the density of current-carrying electrons are sufficient to determine the properties of the system. Two mean fields, one for current-carrying electrons and the other one for equilibrium el…
We consider effects of strong light-matter interaction on electronic friction in molecular junctions within generic model of single molecule nano cavity junction. Results of the Hubbard NEGF simulations are compared with mean-field NEGF and generalized Head-Gordon and Tully approaches. Mean-field NEGF is shown to fail qualitatively at strong intra-system interactions, while accuracy of the generalized Head-Gordon and Tully results is restricted to situations of well separated intra-molecular excitations, when bath induced coherences are negligible. Numerical results show effects of bias and ca…
Time-dependent currents in molecular junctions can be caused by structural fluctuations or interaction with external fields. In this publication, we demonstrate how the hierarchical quantum master equation approach can be used to study time-dependent transport in a molecular junction. This reduced density matrix methodology provides a numerically exact solution to the transport problem including time-dependent energy levels, molecule-lead coupling strengths and transitions between electronic states of the molecular bridge. Based on a representative model, the influence of a time-dependent mole…
We investigate on the same footing the time-dependent electronic transport properties and vibrational dynamics of a molecular junction. We show that fluctuations of both the molecular vibron displacement and the electronic current across the junction undergo damped oscillations towards the steady-state. We assign the former to the onset of electron tunneling events assisted by vibron-emission. The time-dependent build-up of electron-hole correlations is revealed as a departure of the charge-transfer statistics from the generalized-binomial one after a critical time tc. The phonon-back action o…
Graphene and other 2D materials give a platform for electromechanical sensing of biomolecules in aqueous, room temperature environments. The electronic current changes in response to mechanical deflection, indicating the presence of forces due to interactions with, e.g., molecular species. We develop illustrative models of these sensors in order to give explicit, compact expressions for the current and signal-to-noise ratio. Electromechanical structures have an electron transmission function that follows a generalized Voigt profile, with thermal fluctuations giving a Gaussian smearing analogou…
Epitaxial spin filter tunnel junctions based on the ferromagnetic semiconductor europium monoxide, EuO, are investigated by means of density functional theory. In particular, we focus on the spin transport properties of Cu(100)/EuO(100)/Cu(100) junctions. The dependence of the transmission coefficient and the current-voltage curves on the interface spacing and on the EuO thickness is explained in terms of the EuO density of states and the complex band structure. Furthermore we also discuss the relation between the spin transport properties and the Cu-EuO interface geometry. The level alignment…
The interplay between spin transport and thermoelectricity offers several novel ways of generating, manipulating, and detecting nonequilibrium spin in a wide range of materials. Here we formulate a phenomenological model in the spirit of the standard model of electrical spin injection to describe the electronic mechanism coupling charge, spin, and heat transport and employ the model to analyze several different geometries containing ferromagnetic (F) and nonmagnetic (N) regions: F, F/N, and F/N/F junctions which are subject to thermal gradients. We present analytical formulas for the spin accu…
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 investigate the effects of phonon scattering on the electronic current noise through nanojunctions using the non-equilibrium Green's functions formalism extended to include the counting field. In the case of weak electron-phonon coupling and a single broad electronic level we derive an analytic expression for the current noise at arbitrary temperature and identify physically distinct contributions based on their voltage dependence. We apply our theory to the experimentally relevant case of a deuterium molecule placed in a break-junction and predict a significant inelastic contribution to th…
We investigate the role of electronic-vibrational coupling in resonant electron transport through single-molecule junctions, taking into account that the corresponding coupling strengths may depend on the charge and excitation state of the molecular bridge. In the presence of multiple electronic states, this requires to extend the commonly used model and include vibrationally dependent electron-electron interaction. We use Born-Markov master equation methods and consider selected models to exemplify the effect of the additional interaction on the transport characteristics of a single-molecule …
We show that the strong coupling of pseudospin orientation and charge carrier motion in bilayer graphene has a drastic effect on transport properties of ballistic p-n-p junctions. Electronic states with zero momentum parallel to the barrier are confined under it for one pseudospin orientation, whereas states with the opposite pseudospin tunnel through the junction totally uninfluenced by the presence of confined states. We demonstrate that the junction acts as a cloak for confined states, making them nearly invisible to electrons in the outer regions over a range of incidence angles. This beha…
We present a theoretical approach to include dynamical aspects of molecular structural fluctuations, such as, for example, forming and breaking hydrogen bonds, isomerizations, and dynamical supramolecular structures, in nonequilibrium Green's functions electron transport calculations. Structural transitions are treated as a stochastic telegraph process, and the primary quantity of interest is a retarded Green's function averaged over realizations of a stochastic process. Using the Novikov-Furutsu functional stochastic calculus method, we derive equations of motion for stochastically averaged r…
Electronic transport in a graphene-based ferromagnetic/normal/ferromagnetic junction is investigated by means of Landauer-Büttiker formulism and the nonequilibrium Green's function technique. For the zigzag edge case, the results show that the conductance is always larger than $e^{2}/h$ for the parallel configuration of lead magnetizations, but for the antiparallel configuration the conductance becomes zero because of the band-selective rule. So a magnetoresistance (MR) plateau emerges with the value 100% when the Fermi energy is located around the Dirac point. Besides, choosing narrower graph…
Heating in nanoscale systems driven out of equilibrium is of fundamental importance, has ramifications for technological applications, and is a challenge to characterize experimentally. Prior experiments using nanoscale junctions have largely focused on heating of ionic degrees of freedom, while heating of the electrons has been mostly neglected. We report measurements in atomic-scale Au break junctions, in which the bias-driven component of the current noise is used as a probe of the electronic distribution. At low biases ($<$ 150~mV) the noise is consistent with expectations of shot noise at…
The effects of water wetting conditions on the transport properties of molecular nano-junctions are investigated theoretically by using a combination of classical molecular dynamics and first principles electronic transport calculations. These are at the level of the non-equilibrium Green's function method implemented for self-interaction corrected density functional theory. We find that water effectively produces electrostatic gating to the molecular junction, with a gating potential determined by the time-averaged water dipole field. Such a field is large for the polar benzene-dithiol molecu…
Here we present a theoretical study of the thermoelectric transport through {[}2,2{]}para\-cyclo\-phane-based single-molecule junctions. Combining electronic and vibrational structures, obtained from density functional theory (DFT), with nonequilibrium Green's function techniques, allows us to treat both electronic and phononic transport properties at a first-principles level. For the electronic part, we include an approximate self-energy correction, based on the DFT+$Σ$ approach. This enables us to make a reliable prediction of all linear response transport coefficients entering the thermoele…
In analogy with light refraction at optical boundary, ballistic electrons also undergo refraction when propagate across a semiconductor junction. Establishing a negative refractive index in conventional optical materials is difficult, but the realization of negative refraction in electronic system is conceptually straightforward, which has been verified in graphene p-n junctions in recent experiments. Here, we propose a model to realize double refraction and double focusing of electric current by a normal-hexagonal semiconductor junction. The double refraction can be either positive or negativ…
In a nanoscale molecular junction at finite bias voltage,the intra-molecular distribution of vibrational energy can strongly deviate from the thermal equilibrium distribution and specific vibrational modes can be selectively excited in a controllable way,regardless of the corresponding mode frequency. This is demonstrated for generic models of asymmetric molecular junctions with localized electronic states, employing a master equation as well as a nonequilibrium Green's function approach. It is shown that the applied bias voltage controls the excitation of specific vibrational modes coupled to…
