The transport properties of unsubstituted and amino-substituted butanethiol molecules sandwiched between Au electrodes are investigated by using first-principles approaches. New states are observed around the Fermi levels when -NH2 is substituted for -H in the bridging butanethiol. The amino-substituted states lead to a sharp increase of the current which is credited to the resonant tunneling in the junction. We observe a novel conductance peak at VSD = 0.1 V and negative differential resistance (NDR) in a certain range of source-drain bias. In addition to the I-VSD characteristics, we also investigate the current as a function of gate voltage (I-VG) and find that, for a fixed source-drain bias (VSD = 0.01 V), the gate voltage can modulate the conductance by up to 30 times in the amino-substituted butanethiol junction. These I-VG characteristics suggest that the amino-substituted butanethiol molecular junction may be a promising candidate for field-effect transistors.
Asymmetric i/V curves with respect to the polarity of the voltage bias were observed in the Hg-Au junctions containing bilayers of alkanethiols of different chain length. Larger current resulted when a negative bias was applied to the metal carrying a longer chain alkanethiol monolayer. This behavior is simulated using a single molecule junction model, within the frameworks of the extended Huckel (EH) model and the nonequilibrium Green's function formalism at the Hartree Fock level (NEGF-HF). Qualitative agreement with the experimental results with respect to the magnitude and sign of this asy…
Using first-principles approaches we investigate local heating and the inelastic contribution to the current for various alkanethiols sandwiched between metal electrodes. In the absence of good heat dissipation into the bulk electrodes, we find that the local temperature of the alkanethiols is relatively insensitive to their length. This is due to the rates of heating and cooling processes scaling similarly with length. On the other hand, when considering heat dissipation into the bulk electrodes, the local temperature of alkanethiols decreases as their length increases. We also find that the …
Three terminal single-electron transistor devices utilizing Al/Al2O3 gate electrodes were developed for the study of electron transport through individual single-molecule magnets. The devices were patterned via multiple layers of optical and electron beam lithography. Electromigration induced breaking of the nanowires reliably produces 1-3 nm gaps between which the SMM can be situated. Conductance through a single Mn12(3-thiophenecarboxylate) displays the coulomb blockade effect with several excitations within +/- 40 meV.
We use a self-consistent method to study the current of the single molecular transistor modulated by the transverse gate-bias in the level of the first-principles calculations. The numerical results show that both the polyacene-dithiol molecules and the fused-ring oligothiophene molecules are the potential high-frequency molecular transistor controlled by the transverse field. The long molecules of the polyacene-dithiol or the fused-ring thiophene are in favor of realizing the gate-bias controlled molecular transistor. The theoretical results suggest the related experiments.
Devices made of few molecules constitute the miniaturization limit that both inorganic and organic-based electronics aspire to reach. However, integration of millions of molecular junctions with less than 100 molecules each has been a long technological challenge requiring well controlled nanometric electrodes. Here we report molecular junctions fabricated on a large array of sub-10 nm single crystal Au nanodots electrodes, a new approach that allows us to measure the conductance of up to a million of junctions in a single conducting Atomic Force Microscope (C-AFM) image. We observe two peaks …
We explore multi-terminal quantum transport through a benzene molecule threaded by an Aharonov-Bohm flux $ϕ$. A simple tight-binding model is used to describe the system and all the calculations are done based on the Green's function formalism. With a brief description of two-terminal quantum transport, we present a detailed study of three-terminal transport properties through the benzene molecule to reveal the actual mechanism of electron transport. Here we numerically compute the multi-terminal conductances, reflection probabilities and current-voltage characteristics in the aspects of molec…
In a straightforward application of molecular nanospintronics to quantum computing, single-molecule spin transistors can be used to measure and control nuclear spin qubits. A jump in the conductance occurs when the electronic spin inverts its polarization, and this happens at a so-called anticrossing between energy levels, which in turn only takes place at a specific magnetic field determined by the nuclear spin state. So far, this procedure has only been implemented for the terbium(III) bis(phthalocyaninato) complex. Here we explore theoretically whether a similar behavior is expected for a h…
We investigate vibron-assisted electron transport in single-molecule transistors containing an individual Fe4 Single-Molecule Magnet. We observe a strong suppression of the tunneling current at low bias in combination with vibron-assisted excitations. The observed features are explained by a strong electron-vibron coupling in the framework of the Franck-Condon model supported by density-functional theory.
In single-molecule transistors, we observe inelastic cotunneling features that correspond energetically to vibrational excitations of the molecule, as determined by Raman and infrared spectroscopy. This is a form of inelastic electron tunneling spectroscopy of single molecules, with the transistor geometry allowing in-situ tuning of the electronic states via a gate electrode. The vibrational features shift and change shape as the electronic levels are tuned near resonance, indicating significant modification of the vibrational states. When the molecule contains an unpaired electron, we also ob…
Transistors, regardless of their size, rely on electrical gates to control the conductance between source and drain contacts. In atomic-scale transistors, this conductance is exquisitely sensitive to single electrons hopping via individual orbitals. Single-electron transport in molecular transistors has been previously studied using top-down approaches to gating, such as lithography and break junctions. But atomically precise control of the gate - which is crucial to transistor action at the smallest size scales - is not possible with these approaches. Here, we used individual charged atoms, m…
Current-driven vibrational non-equilibrium induces vibrational sidebands in single-molecule transistors which arise from tunneling processes accompanied by absorption of vibrational quanta. Unlike conventional sidebands, these absorption sidebands occur in a regime where the current is nominally Coulomb blockaded. Here, we develop a detailed and analytical theory of absorption sidebands, including current-voltage characteristics as well as shot noise. We discuss the relation of our predictions to recent experiments.
We measure electron tunneling in single-molecule transistors made from C_{140}, a molecule with a mass-spring-mass geometry chosen as a model system to study electron-vibration coupling. We observe vibration-assisted tunneling at an energy corresponding to the stretching mode of C_{140}. Molecular modeling provides explanations for why this mode couples more strongly to electron tunneling than the other internal modes of the molecule. We make comparisons between the observed tunneling rates and those expected from the Franck-Condon model.
Weakly coupled molecular junctions are an active and important field of research as they exhibit various non-linear transport phenomena. We have investigated the carrier transport through weakly coupled B2C2N2H6 molecules using quantum many-body approach coupled with kinetic (master) equations. Interestingly, various types of non-linear current-voltage characteristics, such as, negative differential conductance (NDC), rectifications, Coulomb staircase, which is the hallmark of multistate transport devices, have been obtained. The source-drain voltage induced change in the occupation probabilit…
We report on the observation of Kondo and split Kondo peaks in single-molecule transistors containing a single spin transition molecule with a Fe2+ ion. Coulomb blockade characteristics reveal a double quantum dot behavior in a parallel configuration, making our system a molecular equivalent to a semiconducting double-quantum-dot system. As the gate voltage is increased the charging of the second dot by an additional electron induces a splitting of the Kondo peak. We discuss possible origins of this effect including a spin transition into a high-spin state.
The role of Chemistry in the road towards quantum devices is the design of elementary pieces with a built-in function. A brilliant example is the use of molecular transistors as nuclear spin detectors, which, up to now, has been implemented only on [TbPc$_2$]$^-$. We argue that this is an artificial constraint and critically discuss the limitations of current theoretical approaches to assess the potential of molecules for their use in spintronics. In connection with this, we review the recent progress in the preparation of highly coherent spin qubits based on vanadium dithiolate complexes and …
Platinum diselenide (PtSe_2) field-effect transistors with ultrathin channel regions exhibit p-type electrical conductivity that is sensitive to temperature and environmental pressure. Exposure to a supercontinuum white light source reveals that positive and negative photoconductivity coexists in the same device. The dominance of one type of photoconductivity over the other is controlled by environmental pressure. Indeed, positive photoconductivity observed in high vacuum converts to negative photoconductivity when the pressure is rised. Density functional theory calculations confirm that phys…
We report two examples of transport phenomena based on sharp features in the effective density of states of molecular-scale transistors: Kondo physics in C$_{60}$-based devices, and gate-modulated negative differential resistance (NDR) in ``control'' devices that we ascribe to adsorbed contamination. We discuss the need for a statistical approach to device characterization, and the criteria that must be satisfied to infer that transport is based on single molecules. We describe apparent Kondo physics in C$_{60}$-based single-molecule transistors (SMTs), including signatures of molecular vibrat…
We propose a practical realization of a field-effect transistor for phonons. Our device is based on a single ionic polymeric molecule and it gives modulations as large as -25% in the thermal conductance for feasible temperatures and electric field magnitudes. Such effect can be achieved by reversibly switching the acoustic torsion mode into an optical mode through the coupling of an applied electric field to the dipole moments of the monomers. This device can pave the way to the future development of phononics at the nanoscale or molecular scale.
The Dzyaloshinskii-Moriya interaction is shown to result in a canting of spins in a single molecule transistor. We predict non-linear transport signatures of this effect induced by spin-orbit coupling for the generic case of a molecular dimer. The conductance is calculated using a master equation and is found to exhibit a non-trivial dependence on the magnitude and direction of an external magnetic field. We show how three-terminal transport measurements allow for a determination of the coupling-vector characterizing the Dzyaloshinskii-Moriya interaction. In particular, we show how its orienta…
While Single Molecule Transistors have been employed in laboratory research for a number of years, there remain many details related to charge transport that have yet to be delineated. We have used the technique of electromigration to create a nanometer-size gap for hosting a single molecule in the narrowest portion of a gold wire defined by electron beam lithography. A recently synthesized Borromean Ring complex was used as the active molecular element of the transistor devices. It is well established in Single Molecule Transistors that, for sweeps of source-drain voltage, a region of zero co…
We report Kondo resonances in the conduction of single-molecule transistors based on transition metal coordination complexes. We find Kondo temperatures in excess of 50 K, comparable to those in purely metallic systems. The observed gate dependence of the Kondo temperature is inconsistent with observations in semiconductor quantum dots and a simple single-dot-level model. We discuss possible explanations of this effect, in light of electronic structure calculations.
It is understood that molecular conjugation plays an important role in charge transport through single-molecule junctions. Here, we investigate electron transport through an anthraquinone based single-molecule three-terminal device. With the use of an electric-field induced by a gate electrode, the molecule is reduced resulting into a ten-fold increase in the off-resonant differential conductance. Theoretical calculations link the change in differential conductance to a reduction-induced change in conjugation, thereby lifting destructive interference of transport pathways.
We have used an electromigration technique to fabricate C$_{60}$-based single-molecule transistors. We detail the process statistics and the protocols used to infer the successful formation of a single-molecule transistor. At low temperatures each transistor acts as a single-electron device in the Coulomb blockade regime. Resonances in the differential conductance indicate vibrational excitations consistent with a known mode of C$_{60}$. In several devices we observe conductance features characteristic of the Kondo effect, a coherent many-body state comprising an unpaired spin on the molecule …
Inspired by cotunneling spectroscopy of spin-states in a single OPE5-based molecule, we investigate the prospects for electric control of magnetism in purely organic molecules contacted in a three-terminal geometry. Using the gate electrode, the molecule is reversibly switched between three different redox states, with magnetic spectra revealing both ferromagnetic and antiferromagnetic exchange couplings on the molecule. These observations are shown to be captured by an effective low-energy Heisenberg model, which we substantiate microscopically by a simple valence bond description of the mole…
We present an experimental and theoretical study of a magnetic single-molecule transistor based on N@C60 connected to gold electrodes. Particular attention is paid to the regime of intermediate molecule-lead coupling, where cotunneling effects manifest themselves in the Coulomb-blockade regime. The experimental results for the differential conductance as a function of bias, gate voltage, and external magnetic field are in agreement with our analysis of the tunneling rates and provide evidence of magnetic signatures in single-N@C60 devices arising from an antiferromagnetic exchange interaction …
We have used the electromigration technique to fabricate a $\rm{C_{60}}$ single-molecule transistor (SMT). We present a full experimental study as a function of temperature, down to 35 mK, and as a function of magnetic field up to 8 T in a SMT with odd number of electrons, where the usual spin-1/2 Kondo effect occurs, with good agreement with theory. In the case of even number of electrons, a low temperature magneto-transport study is provided, which demonstrates a Zeeman splitting of the zero-bias anomaly at energies well below the Kondo scale.
Single-molecule transistors provide a unique experimental tool to investigate the coupling between charge transport and the molecular degrees of freedom in individual molecules. One interesting class of molecules for such experiments are the single-molecule magnets, since the intramolecular exchange forces present in these molecules should couple strongly to the spin of transport electrons, thereby providing both new mechanisms for modulating electron flow and also new means for probing nanoscale magnetic excitations. Here we report single-molecule transistor measurements on devices incorporat…
Understanding the intermolecular interactions and utilize these interactions to effectively control the transport behavior of single molecule is the key step from single molecule device to molecular circuits1-6. Although many single molecule detection techniques are used to detect the molecular interaction at single-molecule level1,4,5,7,8, probing and tuning the intermolecular interaction all by electrical approaches has not been demonstrated. In this work, we successful assemble a double molecule transistor incorporating two manganese phthalocyanine molecules, on which we probe and tune the …
Current-voltage characteristics of a single-electron transistor with a vibrating quantum dot were calculated assuming vibrons to be in a coherent (non-equilibrium) state. For a large amplitude of quantum dot oscillations we predict strong suppression of conductance and the lifting of polaronic blockade by bias voltage in the form of steps in $I-V$ curves. The height of the steps differs from the prediction of the Franck-Condon theory (valid for equilibrated vibrons) and the current saturates at lower voltages then for the case, when vibrons are in equilibrium state.
We demonstrate a device geometry for single-molecule electronics experiments that combines both the ability to adjust the spacing between the electrodes mechanically and the ability to shift the energy levels in the molecule using a gate electrode. With the independent in-situ variations of molecular properties provided by these two experimental "knobs", we are able to achieve a much more detailed characterization of electron transport through the molecule than is possible with either technique separately. We illustrate the devices' performance using C60 molecules.
Using first-principles methods we study theoretically the properties of an individual $\{Fe_4\}$ single-molecule magnet (SMM) attached to metallic leads in a single-electron transistor geometry. We show that the conductive leads do not affect the spin ordering and magnetic anisotropy of the neutral SMM. On the other hand, the leads have a strong effect on the anisotropy of the charged states of the molecule, which are probed in Coulomb blockade transport. Furthermore, we demonstrate that an external electric potential, modeling a gate electrode, can be used to manipulate the magnetic propertie…
C$_3$N is a recently discovered 2D layered material structurally similar to graphene, which has demonstrated immense prospect for future nanoelectronics. In this work, we have designed and investigated the operation and performance of a C$_3$N island single electron transistor (SET) for the first time. Using First-principles based calculations, we investigated the effect of various molecular adsorptions on the electronic and conduction behaviour of the SET. C$_3$N was found to be the perfect host material for capturing CO$_2$. The charge stability diagram carries the signature of different mol…
We present a first-principles method for calculating the charging energy of a molecular single-electron transistor operating in the Coulomb blockade regime. The properties of the molecule are modeled using density-functional theory, the environment is described by a continuum model, and the interaction between the molecule and the environment are included through the Poisson equation. The model is used to calculate the charge stability diagrams of a benzene and C$_{60}$ molecular single-electron transistor.
The joint effect of the electron-phonon interaction and Kondo effect on the nonequilibrium transport through the single molecule transistor is investigated by using the improved canonical transformation scheme and extended equation of motion approach. Two types of Kondo phonon-satellites with different asymmetric shapes are fully confirmed in the spectral function, and are related to the electron spin singlet or hole spin singlet, respectively. Moreover, when a moderate Zeeman splitting is caused by a local magnetic field, the Kondo satellites in the spin resolved spectral function are found d…
We develop a theoretical model for how organic molecules can control the electronic and transport properties of an underlying transistor channel to whose surface they are chemically bonded. The influence arises from a combination of long-ranged dipolar electrostatics due to the molecular head-groups, as well as short-ranged charge transfer and interfacial dipole driven by equilibrium band-alignment between the molecular backbone and the reconstructed semiconductor surface atoms.
We calculate the electronic transport through a molecular dimer, in which an excess electron is delocalized over equivalent monomers, which can be locally distorted. In this system the Born-Oppenheimer approximation breaks down resulting in quantum entanglement of the mechanical and electronic motion. We show that pseudo Jahn-Teller (pJT) dynamics of the molecule gives rise to conductance peaks that indicate this violation. Their magnitude, sign and position sharply depend on the electro-mechanical properties of the molecule, which can be varied in recently developed three-terminal junctions w…
The electrostatic behaviour of an 1,3-Cyclobutadiene (C$_{4}$H$_{4}$) based Single Molecular Transistor (SMT) has been investigated using the first principle calculation based on Density functional Theory and non-equilibrium Green's function approach. While the molecule is placed on top of a dielectric layer (backed by a metallic gate) and weakly coupled between the Source/Drain electrodes, the charge stability diagram revealed the presence of individual charge states in the Coulomb Blockade regime. This gets affected significantly on addition of an another gate electrode placed on the top of …
Both experiments and theoretical studies have demonstrated that the interaction between the current carrying electrons and the induced polarization charge in single-molecule junctions leads to a strong renormalization of molecular charging energies. However, the effect on electronic excitations and molecular symmetries remain unclear. Using a theoretical framework developed for semiconductor nanostructure based single-electron transistors (SETs), we demonstrate that the image charge interaction breaks the molecular symmetries in a benzene based single-molecule transistor operating in the Coulo…
We study all-carbon-hydrogen molecular transistors where zigzag graphene nanoribbons play the role of three metallic electrodes connected to a ring-shaped 18-annulene molecule. Using the nonequilibrium Green function formalism combined with density functional theory, recently extended to multiterminal devices, we show that the proposed nanostructures exhibit exponentially small transmission when the source and drain electrodes are attached in a configuration that ensures destructive interference of electron paths around the ring. The third electrode, functioning either as an attached infinite-…
We present a new mechanism for a spin blockade effect associated with a change in the type of magnetic anisotropy over oxidation state in a single molecule transistor, by taking an example of an individual Eu$_{2}$(C$_{8}$H$_{8}$)$_{3}$ molecule weakly coupled to non-magnetic electrodes without linker groups. The molecule switches its magnetization direction from in-plane to out-of-plane when it is charged. In other words, the magnetic anisotropy of the molecule changes from easy plane to easy axis when the molecule is charged. By solving the master equation based on model Hamiltonian, we find…
Kondo effect offers an important paradigm to understand strong correlated many-body physics. Although under intensive study, some of important properties of Kondo effect, in systems where both itinerant coupling and localized coupling play significant roles, are still elusive. Here we report evolution and universality of two stage Kondo effect, the simplest form where both couplings are important using single molecule transistor devices incorporating Manganese phthalocyanine molecules. Kondo temperature T* of two-stage Kondo effect evolves linearly against effective interaction of involved two…
Molecular transistors have the potential for switching with lower gate voltages than conventional field-effect transistors. We have calculated the performance of a single-molecule device in which there is interference between electron transport through the highest occupied molecular orbital and the lowest unoccupied molecular orbital of a single molecule. Quantum interference results in a subthreshold slope that is independent of temperature. For realistic parameters the change in gate potential required for a change in source-drain current of two decades is 20 mV, which is a factor of six sma…
We monitor the Landau-Zener dynamics of a single-ion magnet in a spin-transistor geometry. For increasing field-sweep rates, the spin reversal probability shows increasing deviations from that of a closed system. In the low-conductance limit, such deviations are shown to result from a dephasing process. In particular, the observed behaviors are succesfully simulated by means of an adiabatic master equation, with time averaged dephasing (Lindblad) operators. The time average is tentatively interpeted in terms of the finite time resolution of the continuous measurement.
Tunnel transport of interacting spin-polarized electrons through a single-level vibrating quantum dot in external magnetic field is studied. By using density matrix method, the current-voltage characteristics and the dependence of conductance on temperature of a single-electron transistor were calculated. We found that a lifting of Coulomb blockade in external magnetic field happens in stages. The Franck-Condon steps associated with inelastic electron tunneling in our case are doubled due to contribution of two Zeeman-split levels in electron transport. The doubling of steps can be also observ…
On the basis of the nonequilibrium Green's function and nonperturbative canonical transformation for the local electron-phonon interaction (EPI), the quantum transport through a single-molecule transistor(SMT) has been investigated with a particular attention paid to the joint effect of the EPI and SMT-lead coupling on the spectral function and conductance. In addition to the usual EPI-induced renormalized effects (such as the red-shift, sharpening, and phonon-sidebands of the SMT level), owing to improved disentagling the electron-phonon system, it has been found that, the profile of the spec…
A nanopore based detection methodology was proposed and investigated for the detection of Nicotine. This technique uses a Single Molecular Transistor (SMT) working as a nanopore operational in the Coulomb Blockade regime. When the Nicotine molecule is pulled through the nanopore area surrounded by the Source(S), Drain(D) and Gate electrodes, the charge stability diagram can detect the presence of the molecule and is unique for a specific molecular structure. Due to the weak coupling between the different electrodes which is set by the nanopore size, the molecular energy states stay almost unaf…
We develop a conceptually simple scheme based on a master-equation approach to evaluate the full-counting statistics (FCS) of elastic and inelastic off-resonant tunneling (cotunneling) in quantum dots (QDs) and molecules. We demonstrate the method by showing that it reproduces known results for the FCS and shot noise in the cotunneling regime. For a QD with an excited state, we obtain an analytic expression for the cumulant generating function (CGF) taking into account elastic and inelastic cotunneling. From the CGF we find that the shot noise above the inelastic threshold in the cotunneling r…
We report low-temperature electrical transport studies of molecule-scale silicon nanowires. Individual nanowires exhibit well-defined Coulomb blockade oscillations characteristic of charge addition to a single nanostructure with length scales up to at least 400 nm. Further studies demonstrate coherent charge transport through discrete single particle quantum levels extending the whole device, and show that the ground state spin configuration follows the Lieb-Mattis theorem. In addition, depletion of the nanowires suggests that phase coherent single-dot characteristics are accessible in a regim…
We investigate the possibility of optical current control through single molecules which are weakly coupled to leads. A master equation approach for the transport through a molecule is combined with a Floquet theory for the time-dependent molecule. This yields an efficient numerical approach to the evaluation of the current through time-dependent nano-structures in the presence of a finite external voltage. We propose tunable optical current switching in two- and three-terminal molecular electronic devices driven by properly adjusted laser fields, i.e. a novel class of molecular transistors.
We consider the electron transport in single molecule magnet transistors in the presence of Zeeman spin splitting and magnetic quantum coherence (MQC). The Zeeman interaction is extended along the leads, thereby producing gaps in the energy spectrum which allow electron transport with spin polarized along a certain direction. The MQC induces an effective coupling between localized spin states and continuum spin states in the single molecule magnet and leads, respectively. We investigate the conductance at zero temperature as a function of the applied bias and magnetic field, and show that the …
The spin-configuration of semiconductor artificial molecules consisting of quantum dots and spin field effect transistors is studied theoretically. We find that the antiferromagnetic spin configuration can be changed to the ferromagnetic one by applying a gate voltage to the spin field effect transistors. We show that the square-norm of the total spin of an artificial molecule oscillates with the twist angle $θ$ and has maxima at $θ=$ an odd integer times $π$. We also show that the square-norm of the total spin of the ring-shaped artificial molecule changes drastically at certain values of $θ$…
The present paper gives an elaborate theoretical description of a new molecular charge transport mechanism applying to a single molecule trapped between two macroscopic electrodes in a solid state device. It is shown by a Hubbard type model of the electronic and electrostatic interactions, that the close proximity of metal electrodes may allow electrons to tunnel from the electrode directly into a very localized image charge stabilized states on the molecule. Due to this mechanism, an exceptionally large number of redox states may be visited within an energy scale which would normally not allo…
Extended Huckel theory (EHT) along with NEGF (Non-equilibrium Green's function formalism) has been used for modeling coherent transport through molecules. Incorporating dephasing has been proposed to theoretically reproduce experimental characteristics for such devices. These elastic and inelastic dephasing effects are expected to be important in quantum devices with the feature size around 10nm, and hence an efficient and versatile solver is needed. This model should have flexibility to be applied to a wide range of nano-scale devices, along with 3D electrostatics, for arbitrary shaped contac…
We report electronic transport measurements of single-molecule transistor devices incorporating bipyridyl-dinitro oligophenylene-ethynylene dithiol (BPDN-DT), a molecule known to exhibit conductance switching in other measurement configurations. We observe hysteretic conductance switching in 8% of devices with measurable currents, and find that dependence of the switching properties on gate voltage is rare when compared to other single-molecule transistor devices. This suggests that polaron formation is unlikely to be responsible for switching in these devices. We discuss this and alternative …
Current-voltage characteristics of a spintromechanical device, in which spin-polarized electrons tunnel between magnetic leads with anti-parallel magnetization through a single level movable quantum dot, are calculated. New exchange- and electromechanical coupling-induced (spin-polaronic) effects that determine strongly nonlinear current-voltage characteristics were found. In the low-voltage regime of electron transport the voltage-dependent and exchange field-induced displacement of quantum dot towards the source electrode leads to nonmonotonic behavior of differential conductance that demons…
We present explicit kinetic equations for quantum transport through a general molecular quantum-dot, accounting for all contributions up to 4th order perturbation theory in the tunneling Hamiltonian and the complete molecular density matrix. Such a full treatment describes not only sequential, cotunneling and pair tunneling, but also contains terms contributing to renormalization of the molecular resonances as well as their broadening. Due to the latter all terms in the perturbation expansion are automatically well-defined for any set of system parameters, no divergences occur and no by-hand r…
We present a model of the molecular transistor, operation of which is based on the interplay between two physical mechanisms, peculiar to open quantum systems that act in concert: PT-symmetry breaking corresponding to coalescence of resonances at the exceptional point of the molecule, connected to the leads, and Fano-Feshbach antiresonance. This switching mechanism can be realized in particular in a special class of molecules with degenerate energy levels, i.e. diradicals, which possess mirror symmetry. At zero gate voltage infinitesimally small interaction of the molecule with the leads break…
We present atomistic calculations of quantum coherent electron transport through fulleropyrrolidine terminated molecules bridging a graphene nanogap. We predict that three difficult problems in molecular electronics with single molecules may be solved by utilizing graphene contacts: (1) a back gate modulating the Fermi level in the graphene leads facilitate control of the device conductance in a transistor effect with high on/off current ratio; (2) the size mismatch between leads and molecule is avoided, in contrast to the traditional metal contacts; (3) as a consequence, distinct features in …
