Rectification effects in coherent transport through single molecules

A minimal model for coherent transport through a donor/acceptor molecular junction is presented. The two donor and acceptor sites are described by single levels energetically separated by an intramolecular tunnel barrier. In the limit of strong coupling to the electrodes a current rectification for different bias voltage polarities occurs. Contacts with recent experiments of molecular rectification are also given.     

Quantum transport through STM-lifted single PTCDA molecules

Using a scanning tunneling microscope we have measured the quantum conductance through a PTCDA molecule for different configurations of the tip–molecule–surface junction. A peculiar conductance resonance arises at the Fermi level for certain tip to surface distances. We have relaxed the molecular junction coordinates and calculated transport by means of the Landauer/Keldysh approach. The zero bias transmission calculated for fixed tip positions in lateral dimensions but different tip–substrate distances show a clear shift and sharpening of the molecular chemisorption level on increasing the STM–surface distance, in agreement with experiment.     

Statistical approach to investigating transport through single molecules

We present a statistical approach that combines comprehensive current-voltage data acquisition during the controlled manipulation of a molecular junction with subsequent statistical analysis. Thereby the most probable transport characteristics can be determined. The excellent sensitivity of this impartial approach to even subnanometer-long molecules is illustrated by benzene-1,4-dithiol and 4,4"-bis(acetylthiol)-2,2',5',2"-tetramethyl-[1,1';4',1"] terphenyl results.     

Effects of atomic-scale contacts on transport properties through single molecules - ab initio study

Using the RTM/NEGF method, which is a first-principles calculation tool for the quantum transport through nanostructures between electrodes, we study the effects of atomic-scale contacts on the transport properties through single molecules. Electronic states and current-voltage (I-V) characteristics are investigated in various contact conditions with and without single molecules between electrodes. We find that similar nonlinear behaviors appear in the I-V characteristics. Such nonlinear behaviors are determined not only by the HOMO-LUMO electronic states of single molecules between electrodes, but also by the atomic-scale contact conditions. We show that the transitions from tunneling to ballistic regimes affect the I-V characteristics significantly.     

Full counting statistics of strongly non-ohmic transport through single molecules

We study analytically the full counting statistics of charge transport through single molecules, strongly coupled to a weakly damped vibrational mode. The specifics of transport in this regime--a hierarchical sequence of avalanches of transferred charges, interrupted by "quiet" periods--make the counting statistics strongly non-Gaussian. We support our findings for the counting statistics as well as for the frequency-dependent noise power by numerical simulations, finding excellent agreement.     

Franck-Condon blockade and giant Fano factors in transport through single molecules

We show that Franck-Condon physics leads to a significant current suppression at low bias voltages (termed Franck-Condon blockade) in transport through single molecules with strong coupling between electronic and vibrational degrees of freedom. Transport in this regime is characterized by remarkably large Fano factors (10(2)-10(3) for realistic parameters), which arise due to avalanchelike transport of electrons. Avalanches occur in a self-similar manner over a wide range of time scales, leading to power-law dependences of the current noise on frequency and vibrational relaxation rate.     

Effects of interbase electronic coupling and electrode on charge transport through short DNA molecules: A numerical study

We report on theoretical results about the coherent charge transport of short DNA molecules using the transmission approach, as a function of interbase electronic coupling and electrodes. A dinucleotide poly(GC) chain is studied as a generic case, and the transmission coefficient as well as I–V$I\text{–}V$ curves are presented. The well-stacked “π  -way” is favorable for conveying charge carriers through short sequences, and the current can be reduced in strong electronic coupling regime. Further, the steplike appearance and threshold voltage in I–V$I\text{–}V$ curves dramatically depend on the coupling strength. The electrodes are shown to dominate charge transport of single band and may contribute to the threshold voltage, and the enhancement of conductance in low contact coupling regime is possible.     

A bond bending model for negative differential resistance in transport through single molecules

We develop a model for transport through benzene-based single molecules with an NO₂ side-group, which incorporates bond bending between the NO₂ and the adjacent benzene ring and successfully reproduces the experimentally observed strong negative differential resistance. Transport through the molecule is assumed to be incoherent and is treated using photon assisted tunnelling.     

Field-assisted spin-polarized electron transport through a single quantum well with spin-orbit coupling

We have investigated theoretically the field-driven electron transport through a single-quantum-well semiconductor heterostructure with spin-orbit coupling.The splitting of the asymmetric Fano-type resonance peaks due to the Dresselhaus spin-orbit coupling is found to be highly sensitive to the direction of the incident electron.The splitting of the Fano-type resonance induces the spin-polarization dependent electron current.The location and the line shape of the Fano-type resonance can be controlled by adjusting the energy and the direction of the incident electron,the oscillation frequency,and the amplitude of the external field.These interesting features may be used to devise tunable spin filters and realize pure spin transmission currents.     

Field-assisted spin-polarized electron transport through a single quantum well with spinben orbit coupling

We have investigated theoretically the field-driven electron transport through a single-quantum-well semiconductor heterostructure with spin-orbit coupling. The splitting of the asymmetric Fano-type resonance peaks due to the Dresselhaus spin-orbit coupling is found to be highly sensitive to the direction of the incident electron. The splitting of the Fano-type resonance induces the spin-polarization dependent electron current. The location and the line shape of the Fano-type resonance can be controlled by adjusting the energy and the direction of the incident electron, the oscillation frequency, and the amplitude of the external field. These interesting features may be used to devise tunable spin filters and realize pure spin transmission currents.     

Dynamical symmetry breaking in transport through molecules

We analyze the interplay between vibrational and electronic degrees of freedom in charge transport across a molecular single-electron transistor. We focus on the wide class of molecules which possess quasidegenerate vibrational eigenstates, while no degeneracy occurs for their anionic configuration. We show that the combined effect of a thermal environment and coupling to leads, involving tunneling events charging and discharging the molecule, leads to a dynamical symmetry breaking where quasidegenerate eigenstates acquire different occupations. This imbalance gives rise to a characteristic asymmetry of the current versus an applied gate voltage.     

Electron transport through asymmetric DNA molecules

We investigate quantum mechanical electron transport along the long axis of the DNA molecule using an effective tight-binding model. The overall contour plot of transmission, the current-voltage characteristics, and the differential conductance are examined for the variation of backbone onsite energy, the energy-dependent hopping strength, and the contact coupling between the leads and the DNA molecule. It is shown that as backbone asymmetry increases, the merging and collapse of the two mini-bands take place and an extra resonance peak in the transmission appears. In addition, we present the modulation of voltage threshold in the current-voltage curves and a double-peak structure in the differential conductance due to the disappearance of the merged mini-band. Finally, in the Coulomb blockade regime of asymmetric contact coupling, a distinct and under-unity resonance in the transmission appears due to the interference effects between the DNA molecular bands and the electronic structure of the leads at the DNA-lead interface.     

Driving current through single organic molecules

We investigate electronic transport through two types of conjugated molecules. Mechanically controlled break junctions are used to couple thiol end groups of single molecules to two gold electrodes. Current-voltage characteristics ( IVs) of the metal-molecule-metal system are observed. These IVs reproduce the spatial symmetry of the molecules with respect to the direction of current flow. We hereby unambiguously detect an intrinsic property of the molecule and are able to distinguish the influence of both the molecule and the contact to the metal electrodes on the transport properties of the compound system.     

Selective spin coupling through a single exciton

We present a novel scheme for performing a conditional phase gate between two spin qubits in adjacent semiconductor quantum dots through delocalized single exciton states, formed through the interdot F?rster interaction. We consider two resonant quantum dots, each containing a single excess conduction band electron whose spin embodies the qubit. We demonstrate that both the two-qubit gate and arbitrary single-qubit rotations may be realized to a high fidelity with current semiconductor and laser technology.     

Controlled transport through a single molecule

We demonstrate how an electrode-molecule-electrode junction can be controllably opened and closed by careful tuning of the contacts' interspace and voltage. The molecule, an octanethiol, flips to bridge a ~1 nm interspace between substrate and scanning tunnelling microscope tip when an electric field exceeds a threshold (switch 'on'). Reducing the field below this threshold value leads to the reproducible detachment of the octanethiol (switch 'off'). Once contacted, a further reduction of the contacts' interspace leads to an increase of the conductance of the molecule.     

Theory of inelastic electric current through single molecules

An electronic structure theory has been developed for an inelastic electric current of electron-intramolecular vibration coupling origin in terms of the Keldysh Green function method and the self-consistent Born approximation. Numerical calculations were made for the benzenedithiol molecule linking the two Au(111) electrodes. The calculations successfully reproduce typical features commonly observed in inelastic tunneling spectroscopy. The vibrational excitation energy due to the inelastic current was estimated. The inelastic electric current is quite important for the structural stability and the switching possibility of the molecular device.     

自旋轨道耦合Su-Schrieffer-Heeger原子链系统的电子输运特性

在Su-Schrieffer-Heeger (SSH)原子链中,电子在胞内和胞间的跳跃依赖于其自旋时,即SSH原子链存在自旋轨道耦合作用时,存在不同缠绕数的非平庸拓扑边缘态.如何探测自旋轨道耦合SSH原子链不同缠绕数的边缘态是一个重要问题.本文在紧束缚近似下研究了自旋轨道耦合SSH原子链的非平庸拓扑边缘态性质及其零能附近的电子输运特性.研究发现四重和二重简并边缘态的缠绕数分别为2和1;并且仅当源极入射电子的自旋被极化(铁磁电极)时,自旋轨道耦合SSH原子链在零能附近的电子输运特性才能反映其边缘态的能谱特性.尤其是,随着自旋轨道耦合SSH原子链与左、右导线之间的耦合强度由弱到强改变,对于缠绕数为2的四重简并边缘态,入射电子在零能附近的透射峰数目将从4个变为0;而对于缠绕数为1的二重简并边缘态情形,其透射峰数目将从2个变为0.因此,在源极为铁磁电极的情形下,通过观察自旋轨道耦合SSH原子链在零能附近电子共振透射峰的数目随着其与左、右导线之间耦合强度的变化,来探测其不同缠绕数的边缘态.上述结果为基于电子输运特性探测自旋轨道耦合SSH原子链不同拓扑性质的边缘态提供了一种可选择的理论方案.     

Single-file transport of water molecules through a carbon nanotube

Recent molecular dynamics simulations of water transport through the interior channel of a carbon nanotube in contact with an aqueous reservoir showed that conduction occurred in bursts with collective water motion. A continuous-time random-walk model is used to describe concerted transport through channels densely filled with molecules in a single-file arrangement, as also found in zeolites, as well as ion channels and aquaporins in biological membranes. Theoretical predictions for different collective properties of the single-file transport agree with the simulation results.     

Negative differential resistance in transport through organic molecules on silicon

Recent scanning tunneling microscopy studies of individual organic molecules on Si(001) reported negative differential resistance (NDR) above a critical applied field, observations explained by a resonant tunneling model proposed prior to the experiments. Here we use both density functional theory and a many-electron GW self-energy approach to quantitatively assess the viability of this mechanism in hybrid junctions with organic molecules on Si. For cyclopentene on p-type Si(001), the frontier energy levels are calculated to be independent of applied electric fields, ruling out the proposed mechanism for NDR. Guidelines for achieving NDR are developed and illustrated with two related molecules, aminocyclopentene and pyrroline.