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 on the tunneling electrons is shown to amplify and accelerate this build-up mechanism.
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…
We propose a general framework that unifies the point of view of counting statistics of transmitted (fermionic) charges as it is commonly used in the quantum transport community to the point of view of counting statics of phonons (bosons) as it is known from the field of quantum optics. As a particular example, we study on the same footing the counting statistics of electrons transfered through a molecular junction and the corresponding population dynamics of the associated molecular vibrational mode. In the tunnel limit, non-perturbative results in the electron-phonon interaction are derived …
The interaction between electronic and vibrational degrees of freedom is an important mechanism in nonequilibrium charge transport through molecular nanojunctions. While adiabatic polaron-type coupling has been studied in great detail, new transport phenomena arise for nonadiabatic coupling scenarios corresponding to a breakdown of the Born-Oppenheimer approximation. Employing the numerically exact hierarchical equations of motion approach, we analyze the effect of nonadiabatic electronic-vibrational coupling on electron transport in molecular junctions considering a series of models with incr…
Evidence for atomic-scale vibron-mediated electron bunching
CNRS, Laboratoire de Physique des Solides（法国国家科学研究中心，固体物理实验室）；Moscow Institute of Physics and Technology（莫斯科物理技术学院）；CNRS, LOMA, UMR 5798（法国国家科学研究中心，LOMA实验室）
We analyze how functionality could be obtained within single-molecule devices by using a combination of non-equilibrium Green's functions and ab-initio calculations to study the inelastic transport properties of single-molecule junctions. First we apply a full non-equilibrium Green's function technique to a model system with electron-vibration coupling. We show that the features in the inelastic electron tunneling spectra (IETS) of the molecular junctions are virtually independent of the nature of the molecule-lead contacts. Since the contacts are not easily reproducible from one device to ano…
We study the interplay of polaronic effect and superconductivity in transport through molecular Josephson junctions. The tunneling rates of electrons are dominated by vibronic replicas of the superconducting gap, which show up as prominent features in the differential conductance for the dc and ac current. For relatively large molecule-lead coupling, a features that appears when the Josephson frequency matches the vibron frequency can be identified with an over-the-gap structure observed by Marchenkov et al. [Nat. Nanotech. 2, 481 (2007)]. However, we are more concerned with the weak-coupling …
Understanding current-induced bond rupture in single-molecule junctions is both of fundamental interest and a prerequisite for the design of molecular junctions, which are stable at higher bias voltages. In this work, we use a fully quantum mechanical method based on the hierarchical quantum master equation approach to analyze the dissociation mechanisms in molecular junctions. Considering a wide range of transport regimes, from off-resonant to resonant, non-adiabatic to adiabatic transport, and weak to strong vibronic coupling, our systematic study identifies three dissociation mechanisms. In…
Vibronic effects in resonant electron transport through single-molecule junctions are analyzed. The study is based on generic models for molecular junctions, which include electronic states on the molecular bridge that are vibrationally coupled and exhibit Coulomb interaction. The transport calculations employ a master equation approach. The results, obtained for a series of models with increasing complexity, show a multitude of interesting transport phenomena, including vibrational excitation, rectification, negative differential resistance (NDR) as well as local cooling. While some of these …
We revisit the non-collinear exchange coupling across the trilayer magnetic junction mediated by the diluted-magnetic-semiconductor thin film. By numerical approaches, we investigate the spiral angle between the ferromagnetic layers extensively in the parameter space. In contrast to previous study, we discovered the important role of spin relaxation, which tends to favor spiral exchange over the oscillatory Ruderman-Kittel-Kasuya-Yosida interaction. Finally, we discuss the physics origins of these two types of magnetic interactions.
In the present work, we theoretically analyze the steady-state thermoelectric transport through a single-molecule junction with a vibrating bridge. Thermally induced charge current in the system is explored using a nonequilibrium Green's functions formalism. We study combined effects of Coulomb interactions between charge carriers on the bridge and electron-phonon interactions on the thermocurrent beyond the linear response regime. It is shown that electron-vibron interactions may significantly affect both magnitude and direction of the thermocurrent, and vibrational signatures may appear.
We theoretically analyze the spectrum of a magnetic molecule when its charge and spin can couple to the molecular vibrations. More specifically, we show that the interplay between charge-vibron and spin-vibron coupling leads to a renormalization of the magnetic anisotropy parameters of the molecule. This effect is discussed for a model device consisting of an individual magnetic molecule embedded in a junction. We study the transport properties of the device and illustrate how the differential conductance is affected by the vibrationally induced renormalization of the magnetic anisotropy. Depe…
We consider the interaction between electrons and molecular vibrations in the context of electronic transport in nanoscale devices. We present a method based on non-equilibrium Green's functions to calculate both equilibrium and non-equilibrium electronic properties of a single-molecule junction in the presence of electron-vibron interactions. We apply our method to a model system consisting of a single electronic level coupled to a single vibration mode in the molecule, which is in contact with two electron reservoirs. Higher-order diagrams beyond the usual self-consistent Born approximation …
Understanding the influence of vibrational motion of the atoms on electronic transitions in molecules constitutes a cornerstone of quantum physics, as epitomized by the Franck-Condon principle of spectroscopy. Recent advances in building molecular-electronics devices and nanoelectromechanical systems open a new arena for studying the interaction between mechanical and electronic degrees of freedom in transport at the single-molecule level. The tunneling of electrons through molecules or suspended quantum dots has been shown to excite vibrational modes, or vibrons. Beyond this effect, theory pr…
We investigate bistability and memory effects in a molecular junction weakly coupled to metallic leads with the latter being subject to an adiabatic periodic change of the bias voltage. The system is described by a simple Anderson-Holstein model and its dynamics is calculated via a master equation approach. The controlled electrical switching between the many-body states of the system is achieved due to polaron shift and Franck-Condon blockade in the presence of strong electron-vibron interaction. Particular emphasis is given to the role played by the excited vibronic states in the bistability…
The electronic transport of graphene p-n junctions under perpendicular magnetic field is investigated in theory. Under low magnetic field, the transport is determined by the resonant tunneling of Landau levels and conductance versus magnetic field shows a Shubnikov-de Haas oscillation. At higher magnetic field, the p-n junction subjected to the quasi-classical regime and the formation of snake states results in periodical backscattering and transmission as magnetic field varies. The conductance oscillation pattern is mediated both by magnetic field and the carrier concentration on bipolar regi…
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…
The tunnel magneto-Seebeck effect is the dependence of the thermopower of magnetic tunnel junctions on the magnetic configuration. It is conventionally interpreted in terms of a thermoelectric generalization of the tunnel magnetoresistance. Here, we investigate the heat-driven electron transport in these junctions associated with electron-magnon scattering, using stochastic Landau-Lifshitz phenomenology and quantum kinetic theory. Our findings challenge the widely accepted single-electron picture of the tunneling thermopower in magnetic junctions.
The charge-memory effect, bistability and switching between charged and neutral states of a molecular junction, as observed in recent STM experiments, is considered within a minimal polaron model. We show that in the case of strong electron-vibron interaction the rate of spontaneous quantum switching between charged and neutral states is exponentially suppressed at zero bias voltage but can be tuned through a wide range of finite switching timescales upon changing the bias. We further find that, while junctions with symmetric voltage drop give rise to random switching at finite bias, asymmetri…
We present an application of a new formalism to treat the quantum transport properties of fully interacting nanoscale junctions [Phys. Rev. B {\bf 84}, 235428 (2011)]. We consider a model single-molecule nanojunction in the presence of two kinds of electron-vibron interactions. In terms of electron density matrix, one interaction is diagonal in the central region and the second is off-diagonal in between the central region and the left electrode. We use a non-equilibrium Green's function technique to calculate the system's properties in a self-consistent manner. The interaction self-energies a…
Currently, molecular tunnel junctions are recognized as important active elements of various nanodevices. This gives a strong motivation to study physical mechanisms controlling electron transport through molecules. Electron motion through a molecular bridge is always somewhat affected by the environment, and the interactions with the invironment could change the energy of the traveling electron. Under certain conditions these inelastic effects may significantly modify electron transport characteristics. In the present work we describe inelastic and dissipative effects in the electron transpor…
The Josephson supercurrent through the hybrid Majorana--quantum dot--Majorana junction is investigated. We particularly analyze the effect of spin-selective coupling between the Majorana and quantum dot states, which emerges only in the topological phase and will influence the current through bent junctions and/or in the presence of magnetic fields in the quantum dot. We find that the characteristic behaviors of the supercurrent through this system are quite counterintuitive, remarkably differing from the resonant tunneling, e.g., through the similar (normal phase) superconductor--quantum dot-…
Inelastic tunneling of electrons can generate the emission of photons with energies intuitively limited by the applied bias voltage. However, experiments indicate that more complex processes involving the interaction of electrons with plasmon polaritons lead to photon emission with overbias energies. We recently proposed a model of this observation in Phys. Rev. Lett. \textbf{113}, 066801 (2014), in analogy to the dynamical Coulomb blockade, originally developed for treating the electromagnetic environment in mesoscopic circuits. This model describes the correlated tunneling of two electrons i…
We investigate the quantum heat exchange between a nanojunction and a many-body or electromagnetic environment far from equilibrium. It is shown that the two-temperature energy emission-absorption mechanism gives rise to a giant heat flow between the junction and the environment. We obtain analytical results for the heat flow in an idealized high impedance environment and perform numerical calculations for the general case of interacting electrons and discuss the giant freezing and heating effects in the junction under typical experimental conditions.
The Josephson effect is a kind of macroscopic quantum phenomenon that supercurrent flows through a Josephson junction without any voltage applied. We predict a novel vortex-state-mediated Josephson effect in an SNS Josephson junction supporting vortices. The vortex-state-mediated supercurrent is enhanced or reduced significantly in magnitude depending on the junction length, and exhibits several steps with the number of effective propagating channels in current-phase evolution at zero temperature. At finite temperatures, these supercurrent steps persist in the short junction limit, and develop…
We investigate tunneling in metal-insulator-metal junctions employing few atomic layers of hexagonal boron nitride (hBN) as the insulating barrier. While the low-bias tunnel resistance increases nearly exponentially with barrier thickness, subtle features are seen in the current-voltage curves, indicating marked influence of the intrinsic defects present in the hBN insulator on the tunneling transport. In particular, single electron charging events are observed, which are more evident in thicker-barrier devices where direct tunneling is substantially low. Furthermore, we find that annealing th…
Within a phonon-assisted resonance level model we develop a self-consistent procedure for calculating electron transport currents in molecular junctions with intermediate to strong electron-phonon interaction. The scheme takes into account the mutual influence of the electron and phonon subsystems. It is based on the 2nd order cumulant expansion, used to express the correlation function of the phonon shift generator in terms of the phonon momentum Green function. Equation of motion (EOM) method is used to obtain an approximate analog of the Dyson equation for the electron and phonon Green func…
Magnetoelectric coupling between magnetic and electric dipoles is one of the cornerstones of modern physics towards developing the most energy-efficient magnetic data storage. Conventionally, magnetoelectric coupling is achieved in single-phase multiferroics or in magnetoelectric composite nanostructures consisting of ferromagnetic and ferroelectric/piezoelectric materials. Here, we demonstrate an electric-field-induced strain-mediated magnetoelectric effect in ultrathin CoFeB/MgO magnetic tunnel junction employing non-piezoelectric material, which is a vitally important structure for spintron…
We propose a mechanism which allows one to control the transmission of single electrons through a molecular junction. The principle utilizes the emergence of transmission sidebands when molecular vibrational modes are coupled to the electronic state mediating the transmission. We will show that if a molecule-metal junction is biased just below a molecular resonance one may induce the transmission of a single electron by externally exciting a vibrational mode of the molecule. The analysis is quite general but requires that the molecular orbital does not hybridize strongly with the metallic stat…
The conductance of a molecular junction is commonly determined by either charge-transfer-doping, where alignment of the Fermi energy to the molecular levels is achieved, or tunnelling through the tails of molecular resonances within the highest-occupied and lowest-unoccupied molecular-orbital gap. Here, we present an alternative mechanism where electron transport is dominated by electrode surface states. They give rise to metallization of the molecular bridge and additional, pronounced conductance resonances allowing for substantial tailoring of its electronic properties via, e.g. a gate volta…
We consider a model of a Josephson junction of two topological superconducting wires mediated by an interacting quantum dot. An additional normal electrode coupled to the dot from the top allows to probe its density of states. The Majorana states adjacent to the dot hybridize across the junction and from a bound state in the dot. The dot is subjected to the effective magnetic field arising from the superposition of the fields driving each wire into topological states, which, dependent on the angle between the fields, introduces variable Zeeman splitting of the dot active level. We show that el…
Strain-mediated voltage control of magnetization in piezoelectric/ferromagnetic systems is a promising mechanism to implement energy-efficient spintronic memory devices. Here, we demonstrate giant voltage manipulation of MgO magnetic tunnel junctions (MTJ) on a Pb(Mg1/3Nb2/3)0.7Ti0.3O3 (PMN-PT) piezoelectric substrate with (001) orientation. It is found that the magnetic easy axis, switching field, and the tunnel magnetoresistance (TMR) of the MTJ can be efficiently controlled by strain from the underlying piezoelectric layer upon the application of a gate voltage. Repeatable voltage controlle…
We address the electronically induced anisotropy field acting on a spin moment comprised in a vibrating magnetic molecule located in the junction between ferromagnetic metals. Under weak coupling between the electrons and molecular vibrations, the nature of the anisotropy can be changed from favoring a high spin (easy axis) magnetic moment to a low spin (easy plane) by applying a temperature difference or a voltage bias across the junction. For unequal spin-polarizations in the ferromagnetic metals it is shown that the character of the anisotropy is essentially determined by the properties of …
We theoretically investigate the effective exchange interaction, $J_\mathrm{eff}$, mediated by conductive electrons within a nonmagnetic metal spacer, in the presence of a bias voltage, sandwiched by two ferromagnetic insulators. On the basis of the tight-binding model, we show the voltage and spacer thickness dependences of $J_\mathrm{eff}$, and its contorollability is demonstrated. We also propose a new magnonic device with the functions of both field effect transistor and non-volatile memory.
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.
We calculate the conductances and the tunneling magnetoresistance (TMR) of double magnetic tunnel junctions, taking as a model example junctions composed of Fe/ZnSe/Fe/ZnSe/Fe (001). The calculations are done as a function of the gate voltage applied to the in-between Fe layer slab. We find that the application of a gate voltage to the in-between Fe slab strongly affects the junctions' TMR due to the tuning or untuning of conductance resonances mediated by quantum well states. The gate voltage allows a significant enhancement of the TMR, in a more controllable way than by changing the thicknes…
The quest for molecular structures exhibiting strong quantum interference effects in the transport setting has long been on the forefront of chemical research. Here, we establish theoretically that the unusual geometry of spiro-conjugated systems gives rise to complete destructive interference in the resonant-transport regime. This results in a current blockade of the type not present in meta-connected benzene or similar molecular structures. We further show that these systems can undergo a transport-driven Jahn-Teller distortion which can lift the aforementioned destructive-interference effec…
We describe a method to fabricate clean suspended single-wall carbon nanotube (SWCNT) transistors hosting a single quantum dot ranging in length from a few 10s of nm down to $\approx$ 3 nm. We first align narrow gold bow-tie junctions on top of individual SWCNTs and suspend the devices. We then use a feedback-controlled electromigration to break the gold junctions and expose nm-sized sections of SWCNTs. We measure electron transport in these devices at low temperature and show that they form clean and tunable single-electron transistors. These ultra-short suspended transistors offer the prospe…
The carrier-mediated RKKY interaction between local spins plays an important role for the application of magnetically doped graphene in spintronics and quantum computation. Previous studies largely concentrate on the influence of electronic states of uniform systems on the RKKY interaction. Here we reveal a very different way to manipulate the RKKY interaction by showing that the anomalous focusing - a well-known electron optics phenomenon in graphene P-N junctions - can be utilized to refocus the massless Dirac electrons emanating from one local spin to the other local spin. This gives rise t…
Molecular electronics offers unique scientific and technological possibilities, resulting from both the nanometre scale of the devices and their reproducible chemical complexity. Two fundamental yet different effects, with no classical analogue, have been demonstrated experimentally in single-molecule junctions: quantum interference due to competing electron transport pathways, and the Kondo effect due to entanglement from strong electronic interactions. Here we unify these phenomena, showing that transport through a spin-degenerate molecule can be either enhanced or blocked by Kondo correlati…
Metal-intercalated graphene on Ir(111) exhibits phonon signatures in inelastic elec- tron tunneling spectroscopy with strengths that depend on the intercalant. Extraor- dinarily strong graphene phonon signals are observed for Cs intercalation. Li interca- lation likewise induces clearly discriminable phonon signatures, albeit less pronounced than observed for Cs. The signal can be finely tuned by the alkali metal coverage and gradually disappears upon increasing the junction conductance from tunneling to con- tact ranges. In contrast to Cs and Li, for Ni-intercalated graphene the phonon signal…
Photon emission by tunneling electrons can be encouraged by locating a resonator close to the tunnel junction and applying an appropriate voltage-bias. However, studies of normal metals show that the resonator also affects how the charges flow, facilitating processes in which correlated tunneling of two charges produces one photon. We develop a theory to analyze this kind of behavior in Josephson junctions by deriving an effective Hamiltonian describing processes where two Cooper-pairs generate a single photon. We determine the conditions under which the transport is dominated by incoherent tu…
We study the zero temperature conductance and magnetoconductance of ballistic \textit{p-n} junctions in Weyl semimetals. Electron transport is mediated by Klein tunneling between \textit{n}- and \textit{p}- regions. The chiral anomaly that is realized in Weyl semimetals plays a crucial role in the magnetoconductance of the junction. With the exception of field orientations where the angle between $\mathbf{B}$ and the junction plane is small, magnetoconductance is positive and linear in $B$ at both weak and strong magnetic fields. In contrast, magnetoconductance in conventional \textit{p-n} jun…
We investigate models of molecular junctions which constitute minimal Hamiltonians to account for zero-bias-anomaly and the satellite features of inelastic transport by molecular phonons. Through nonlinear transport calculations with the imaginary-time nonequilibrium formalism, a HOMO-LUMO model with Anderson-Holstein interaction is shown to produce co-tunneling conductance peak in the vicinity of Kondo resonance which is mediated by a re-emergent many-body resonance assisted by phonon excitations at bias equal to the phonon frequency. Destruction of the resonance leads to negative-differentia…
We present a theoretical description of the thermopower due to magnon-assisted tunneling in a mesoscopic tunnel junction between two ferromagnetic metals. The thermopower is generated in the course of thermal equilibration between two baths of magnons, mediated by electrons. For a junction between two ferromagnets with antiparallel polarizations, the ability of magnon-assisted tunneling to create thermopower $S_{AP}$ depends on the difference between the size $Π_{\uparrow, \downarrow}$ of the majority and minority band Fermi surfaces and it is proportional to a temperature dependent factor $(k…
We make a theoretical study of the quantum oscillations of the tunneling magnetoresistance (TMR) as a function of the spacer layer thickness. Such oscillations were recently observed in tunneling junctions with a nonmagnetic metallic spacer at the barrier-electrode interface. It is shown that momentum selection due to the insulating barrier and conduction via quantum well states in the spacer, mediated by diffusive scattering caused by disorder, are essential features required to explain the observed period of oscillation in the TMR ratio and its asymptotic value for thick nonmagnetic spacer.
Scanning tunneling spectroscopy requires the application of a potential difference between the sample and a tip. In metal-vacuum-metal junctions, one can safely assume that the potential is constant along the metallic substrate. Here, we show that the inhomogeneous shape of the electric potential has to be taken into account when probing spatially extended molecules on a decoupling layer. To this end, oligothiophene-based molecules were deposited on a monolayer of molybdenum disulfide (MoS$_2$) on a Au(111) surface. By probing the delocalized molecular orbital along the thiophene-backbone, we …
The renormalization of conductances in a Y junction of spinless Luttinger-liquid wires additionally coupled to acoustic longitudinal phonons is investigated in fermionic representation. This system corresponds to geometry of a tunneling experiment and exhibits the interplay between the Coulomb repulsion and the attractive retarded interaction mediated by phonons. The retardation effects related to the propagation of phonons through the junction with arbitrary transmission and reflection amplitudes are taken into account. The appearing logarithmic corrections to conductances of the junction are…
Spin-crossover (SCO) molecules are versatile magnetic switches with applications in molecular electronics and spintronics. Downscaling devices to the single-molecule level remains, however, a challenging task since the switching mechanism in bulk is mediated by cooperative intermolecular interactions. Here, we report on electron transport through individual Fe-SCO molecules coupled to few-layer graphene electrodes \textit{via} $π- π$ stacking. We observe a distinct bistability in the conductance of the molecule and a careful comparison with density functional theory (DFT) calculations allows t…
A theoretical analysis of inelastic electron tunneling spectroscopy (IETS) experiments conducted on molecular junctions are presented, where the second derivative of the current with respect to voltage is usually plotted as a function of applied bias. Within the nonperturbative computational scheme, adequate for arbitrary parameters of the model, we consider the virtual conduction process in the off-resonance region. Here we study the influence of few crucial factors on the IETS spectra: the strength of the vibronic coupling, the phonon energy, and the device working temperature. It was also s…
Josephson junctions are the most prominent nondissipative and at the same time nonlinear elements in superconducting circuits allowing Cooper pairs to tunnel coherently between two superconductors separated by a tunneling barrier. Due to this, physical systems involving Josephson junctions show highly complex behavior and interesting novel phenomena. Here, we consider an infinite one-dimensional chain of superconducting islands where neighboring islands are coupled by capacitances. We study the effect of Josephson junctions shunting each island to a common ground superconductor. We treat the s…
