Junctional Conductance Research Articles

Spatial coupling of quantum-anomalous-Hall and chiral-Majorana modes

We calculate density and current spatial distributions of a 2D model junction between a normal QAH contact and a superconducting QAH region hosting propagating (chiral) Majorana modes. We use a simplified Hamiltonian describing the spatial coupling of the modes on each side of the junction, as well as the related junction conductance. We study how this coupling is affected by orbital effects caused by an external magnetic field.

Phononic heat transport in molecular junctions: Quantum effects and vibrational mismatch.

Problems of heat transport are ubiquitous to various technologies such as power generation, cooling, electronics, and thermoelectrics. In this paper, we advocate for the application of the quantum self-consistent reservoir method, which is based on the generalized quantum Langevin equation, to study phononic thermal conduction in molecular junctions. The method emulates phonon-phonon scattering processes while taking into account quantum effects and far-from-equilibrium (large temperature difference) conditions. We test the applicability of the method by simulating the thermal conductance of molecular junctions with one-dimensional molecules sandwiched between solid surfaces. Our results satisfy the expected behavior of the thermal conductance in anharmonic chains as a function of length, phonon scattering rate, and temperature, thus validating the computational scheme. Moreover, we examine the effects of vibrational mismatch between the solids' phonon spectra on the heat transfer characteristics in molecular junctions. Here, we reveal the dual role of vibrational anharmonicity: It raises the resistance of the junction due to multiple scattering processes, yet it promotes energy transport across a vibrational mismatch by enabling phonon recombination and decay processes.

Copper atomic contacts exposed to water molecules.

Monatomic and molecular hydrogen and also oxygen, as well as water molecules and OH that are exposed to atomic copper in intimate contact, have been studied theoretically using computational methods. The authors optimized moderately large structures of Cu/H/Cu, Cu/HCuH/Cu, Cu/H2/Cu, Cu/H2O/Cu, Cu/OH/Cu, Cu/O/Cu, and Cu/O2/Cu and calculated appropriate values for conductance and inelastic tunneling spectroscopy (IETS) properties of the contact junctions, elucidating them as being a possible outcome resulting from the exposure of copper electrodes to the atomic/molecular contaminant species. Here we also demonstrate the IETS properties, by means of ab initio calculations, which can determine the form of the junction geometries. Furthermore, we identify the bonding geometries at the interfaces of the copper electrodes that directly give rise to the specific IETS signatures that have been observed in recent experiments. Based on low-bias conductance and IETS calculations, for the specific case of water exposure of copper electrodes, it was concluded that a single hydrogen or a single oxygen atom bridging the copper electrodes is not responsible for the high conductance peak measurements. Regarding Model 4, where an individual water molecule is considered to be the bridging constituent, our computational results suggest that it has a relatively low probability of being an appropriate candidate. Based upon current computational results, the two hydrogens in Model 3 appear to be in molecular form, although they still form a bond with the adjacent copper atoms. Comparing computational with experimental results indicates that Model 3 is in acceptable agreement with available data.

Long-Range Activationless Photostimulated Charge Transport in Symmetric Molecular Junctions.

Molecular electronic junctions consisting of nitroazobenzene oligomers covalently bonded to a conducting carbon surface using an established "all-carbon" device design were illuminated with UV-vis light through a partially transparent top electrode. Monitoring junction conductance with a DC bias imposed permitted observation of photocurrents while varying the incident wavelength, light intensity, molecular layer thickness, and temperature. The photocurrent spectrum tracked the in situ absorption spectrum of nitroazobenzene, increased linearly with light intensity, and depended exponentially on applied bias. The electronic characteristics of the photocurrent differed dramatically from those of the same device in the dark, with orders of magnitude higher conductance and very weak attenuation with molecular layer thickness (β = 0.14 nm-1 for thickness above 5 nm). The temperature dependence of the photocurrent was opposite that of the dark current, with a 35% decrease in conductance between 80 and 450 K, while the dark current increased by a factor of 4.5 over the same range. The photocurrent was similar to the dark current for thin molecular layers but greatly exceeded the dark current for low bias and thick molecular layers. We conclude that the light and dark mechanisms are additive, with photoexcited carriers transported without thermal activation for a thickness range of 5-10 nm. The inverse temperature dependence is likely due to scattering or recombination events, both of which increase with temperature and in turn decrease the photocurrent. Photostimulated resonant transport potentially widens the breadth of conceivable molecular electronic devices and may have immediate value for wavelength-specific photodetection.

Gate-tuned conductance of graphene-ribbon junctions with nanoscale width variations.

To utilize graphene as interconnection electrodes in high-density nanoelectronic structures, the electrical stability of graphene should be guaranteed under nanometer-scale deviations. Graphene-ribbon (GR) junctions with accessible dimensions (i.e., sub-micrometer widths) are used in diverse interconnection electrode applications and should be characterized properly if they are to be applied in high-density nanoelectronics. Analyzing the effects of nanoscale GR width variations on the conductance of the entire graphene electrode is necessary for their proper characterization. Here, we diagnose the conductance and thermal effect of graphene electrode junctions constructed from GRs of various widths and directions under gate-tuned voltages. On applying partial gate voltages, we identify the effect of local potential variance on the entire graphene electrode junction. As a result, we were able to perceive precise and minute conductance variations for the entire graphene electrode, arising mainly from different sub-micrometer-scale widths of the GRs, which could not be distinguished using conventional global gating methods.

Charge transfer complexation boosts molecular conductance through Fermi level pinning.

Interference features in the transmission spectra can dominate charge transport in metal-molecule-metal junctions when they occur close to the contact Fermi energy (E F). Here, we show that by forming a charge-transfer complex with tetracyanoethylene (TCNE) we can introduce new constructive interference features in the transmission profile of electron-rich, thiophene-based molecular wires that almost coincide with E F. Complexation can result in a large enhancement of junction conductance, with very efficient charge transport even at relatively large molecular lengths. For instance, we report a conductance of 10-3 G 0 (∼78 nS) for the ∼2 nm long α-quaterthiophene:TCNE complex, almost two orders of magnitude higher than the conductance of the bare molecular wire. As the conductance of the complexes is remarkably independent of features such as the molecular backbone and the nature of the contacts to the electrodes, our results strongly suggest that the interference features are consistently pinned near to the Fermi energy of the metallic leads. Theoretical studies indicate that the semi-occupied nature of the charge-transfer orbital is not only important in giving rise to the latter effect, but also could result in spin-dependent transport for the charge-transfer complexes. These results therefore present a simple yet effective way to increase charge transport efficiency in long and poorly conductive molecular wires, with important repercussions in single-entity thermoelectronics and spintronics.

The importance of intramolecular conductivity in three dimensional molecular solids.

Recent years have seen tremendous progress towards understanding the relation between the molecular structure and function of organic field effect transistors. The metrics for organic field effect transistors, which are characterized by mobility and the on/off ratio, are known to be enhanced when the intermolecular interaction is strong and the intramolecular reorganization energy is low. While these requirements are adequate when describing organic field effect transistors with simple and planar aromatic molecular components, they are insufficient for complex building blocks, which have the potential to localize a carrier on the molecule. Here, we show that intramolecular conductivity can play a role in controlling device characteristics of organic field effect transistors made with macrocycle building blocks. We use two isomeric macrocyclic semiconductors that consist of perylene diimides linked with bithiophenes and find that the trans-linked macrocycle has a higher mobility than the cis-based device. Through a combination of single molecule junction conductance measurements of the components of the macrocycles, control experiments with acyclic counterparts to the macrocycles, and analyses of each of the materials using spectroscopy, electrochemistry, and density functional theory, we attribute the difference in electron mobility of the OFETs created with the two isomers to the difference in intramolecular conductivity of the two macrocycles.

Conduction in cardiac tissue. Historical reflections.

Two hypotheses have been proposed to explain propagation of the action potential in heart. According to the gap junction hypothesis local short‐circuit currents pass from the proximal depolarized cell to the distal inactive cell via gap junctions and are responsible for the depolarization of the distal cell. In the ephapse hypothesis the depolarization of the proximal cell generates an electrical field in the narrow cleft between cells resulting in depolarization beyond threshold of the distal cell. Measurements of length constant, free diffusion of 42K, local currents between cells, existence of high‐conductance gap junctions led to the conclusion that heart muscle is a functional syncytium. Propagation of the action potential, however, is not uniform but anisotropic and discontinuous; it can be also unidirectional. These findings are strong arguments in favor of the gap junction thesis. They do not exclude, as predicted by theoretical calculations, that in conditions of an abnormal fall in gap junction conductance ephaptic conduction takes over. In this last case, definitive experimental confirmation is still required. See also: https://doi.org/10.14814/phy2.13861 & https://doi.org/10.14814/phy2.13862

Control over Near-Ballistic Electron Transport through Formation of Parallel Pathways in a Single-Molecule Wire.

This paper reports highly efficient coherent tunneling in single-molecule wires of oligo-ferrocenes with one to three Fc units. The Fc units were directly coupled to the electrodes, i.e., without chemical anchoring groups between the Fc units and the terminal electrodes. We found that a single Fc unit readily interacts with the metal electrodes of an STM break junction (STM = scanning tunneling microscope) and that the zero-voltage bias conductance of an individual Fc molecular junction increased 5-fold, up to 80% of the conductance quantum G0 (77.4 μS), when the length of the molecular wire was increased from one to three connected Fc units. Our compendium of experimental evidence combined with nonequilibrium Green function calculations contemplate a plausible scenario to explain the exceedingly high measured conductance based on the electrode/molecule contact via multiple Fc units. The oligo-Fc backbone is initially connected through all Fc units, and, as one of the junction electrodes is pulled away, each Fc unit is sequentially disconnected from one of the junction terminals, resulting in several distinct conductance features proportional to the number of Fc units in the backbone. The conductance values are independent of the applied temperature (-10 to 85 °C), which indicates that the mechanism of charge transport is coherent tunneling for all measured configurations. These measurements show the direct Fc-electrode coupling provides highly efficient molecular conduits with very low barrier for electron tunneling and whose conductivity can be modulated near the ballistic regime through the number of Fc units able to bridge and the energy position of the frontier molecular orbital.

Thermoelectricity in B80-based single-molecule junctions: First-principles investigation

Thermoelectricity is a thermorelated property that is of great importance in single-molecule junctions. The electrical conductance (σ), electron-derived thermal conductance (κel) and Seebeck coefficient (S) of B80-based single-molecule junctions are investigated by using density functional theory in combination with non-equilibrium Green’s function. When the distance between the left/right electrodes is 11.4 A, the relationship between σ and κel obeys the Wiedemann–Franz law very well because of the strong hybridization between B80 molecular orbitals and the surface states of Au electrodes. Furthermore, the calculated Lorenz number is close to the famous value in metal or degenerate semiconductors. In addition, S is only −19.09 μV/K at 300 K, thus leading to the smaller electron’s thermoelectric figure of merit (ZelT = S2σT/κel). Interestingly, the strain and chemical potential can modulate B80-based single-molecule junctions from n-type to p-type when the compressive strain reaches −0.6 A or the chemical potential shifts to −0.16 eV. This might be attributed that S reflects the asymmetry in the electrical conductance with respect to the chemical potential and is proportional to the slopes of the transmission spectrum.

Proposal for Detecting Nodal-Line Semimetal Surface States with Resonant Spin-Flipped Reflection.

Topological nodal-line semimetals are predicted to exhibit unique drumheadlike surface states (DSSs). Yet, direct detection of such states remains a challenge. Here, we propose spin-resolved transport in a junction between a normal metal and a spin-orbit coupled nodal-line semimetal as the mechanism for their detection. Specifically, we find that in such an interface the DSSs induce resonant spin-flipped reflection. This effect can be probed by both vertical spin transport and lateral charge transport between antiparallel magnetic terminals. In the tunneling limit of the junction, both spin and charge conductances exhibit a resonant peak around zero energy, providing unique evidence of the DSSs. This signature is robust to both dispersive DSSs and interface disorder. Based on numerical calculations, we show that the scheme can be implemented in the topological semimetal HgCr_{2}Se_{4}.

Dopamine maintains network synchrony via direct modulation of gap junctions in the crustacean cardiac ganglion.

The Large Cell (LC) motor neurons of the crab cardiac ganglion have variable membrane conductance magnitudes even within the same individual, yet produce identical synchronized activity in the intact network. In a previous study we blocked a subset of K+ conductances across LCs, resulting in loss of synchronous activity (Lane et al., 2016). In this study, we hypothesized that this same variability of conductances makes LCs vulnerable to desynchronization during neuromodulation. We exposed the LCs to serotonin (5HT) and dopamine (DA) while recording simultaneously from multiple LCs. Both amines had distinct excitatory effects on LC output, but only 5HT caused desynchronized output. We further determined that DA rapidly increased gap junctional conductance. Co-application of both amines induced 5HT-like output, but waveforms remained synchronized. Furthermore, DA prevented desynchronization induced by the K+ channel blocker tetraethylammonium (TEA), suggesting that dopaminergic modulation of electrical coupling plays a protective role in maintaining network synchrony.

Topological quantum computation based on chiral Majorana fermions

The chiral Majorana fermion is a massless self-conjugate fermion which can arise as the edge state of certain 2D topological matters. It has been theoretically predicted and experimentally observed in a hybrid device of a quantum anomalous Hall insulator and a conventional superconductor. Its closely related cousin, the Majorana zero mode in the bulk of the corresponding topological matter, is known to be applicable in topological quantum computations. Here we show that the propagation of chiral Majorana fermions leads to the same unitary transformation as that in the braiding of Majorana zero modes and propose a platform to perform quantum computation with chiral Majorana fermions. A Corbino ring junction of the hybrid device can use quantum coherent chiral Majorana fermions to implement the Hadamard gate and the phase gate, and the junction conductance yields a natural readout for the qubit state.

Controlling the conductance of single-molecule junctions with high spin filtering efficiency by intramolecular proton transfer

Abstract The pursuit of miniaturization of magnetic electronic components spurs intensive theoretical and experimental researches on designing molecule-scale magnetic devices. Controlling the transport properties is one of the most vital focuses for magnetic molecular devices. In this work, magnetic devices constructed by a single epindolidione (Epi) molecule (5,11-dihydrodibenzo[b,g][1,5]naphthyridine-6,12-dione) bridging two zigzag graphene nanoribbon (zGNR) electrodes are theoretically designed. The Epi molecule can be converted between the keto and enol forms, which is confirmed by first principle molecular dynamics method. The influences of intramolecular proton transfer and the bridging manner between the core molecule and zGNR electrodes on the magnetic transport properties are investigated. Spin-resolved current-voltage (I-V) curves show that both the keto and enol devices display remarkable spin filtering effect. However, the effect of intramolecular proton transfer on the electron transport properties depends on the bridging manner between the Epi molecule and zGNR electrodes. When the Epi molecule is connected to zGNR electrodes with 4,7-sites (A bridging manner), the electron transport properties of molecular junctions are hardly affected by the intramolecular proton transfer. On the contrary, the conductance of the molecular junctions is significantly modulated by the intramolecular proton transfer when the Epi molecule is connected to zGNR electrodes with 4,4′-sites (B bridging manner). Further analysis reveals that the high spin filtering effect originates from stronger coupling between spin-up edge electronic states of zGNR electrodes and states of the core molecule. With B bridging manner, the conjugation characteristics of the Epi molecule as well as the transmission pathway of tunneling electrons can be largely modulated by the intramolecular proton transfer. Our work proposes a feasible way to control the conductance of single-molecule junctions by taking advantage of intramolecular proton transfer.

An Electromechanical Approach to Understanding Binding Configurations in Single-Molecule Devices.

The configuration of the molecule-electrode contact region plays an important role in determining the conductance of a single-molecule junction, and the variety of possible contact configurations have yielded multiple conductance values for a number of molecular families. In this report, we perform simultaneous conductance and electromechanical coupling parameter measurements on a series of oligophenylene-dithiol single-molecule junctions. These molecules show two distinct conductance values, and by examining the conductance changes, the electromechanical coupling, and the changes in the I- V characteristics coupled with a combination of analytical mechanical models and density functional theory (DFT) structure calculations, we are able to determine the most-probable binding configuration in each of the conductance states. We find that the lower-conductance state is likely due to the thiols binding to each electrode at a gold top site, and in the higher-conductance state, the phenylene π orbitals interact with electrodes, drastically modifying the transport behavior. This approach provides an expanded methodology for exploring the relationship between the molecule-electrode contact configuration and molecular conductance.

Molecules and the Eigenstate Thermalization Hypothesis.

We review a theory that predicts the onset of thermalization in a quantum mechanical coupled non-linear oscillator system, which models the vibrational degrees of freedom of a molecule. A system of N non-linear oscillators perturbed by cubic anharmonic interactions exhibits a many-body localization (MBL) transition in the vibrational state space (VSS) of the molecule. This transition can occur at rather high energy in a sizable molecule because the density of states coupled by cubic anharmonic terms scales as N3, in marked contrast to the total density of states, which scales as exp(aN), where a is a constant. The emergence of a MBL transition in the VSS is seen by analysis of a random matrix ensemble that captures the locality of coupling in the VSS, referred to as local random matrix theory (LRMT). Upon introducing higher order anharmonicity, the location of the MBL transition of even a sizable molecule, such as an organic molecule with tens of atoms, still lies at an energy that may exceed the energy to surmount a barrier to reaction, such as a barrier to conformational change. Illustrative calculations are provided, and some recent work on the influence of thermalization on thermal conduction in molecular junctions is also discussed.

Unconventional Single-Molecule Conductance Behavior for a New Heterocyclic Anchoring Group: Pyrazolyl.

Electrical conductance across a molecular junction is strongly determined by the anchoring group of the molecule. Here we highlight the unusual behavior of 1,4-bis(1H-pyrazol-4-ylethynyl)benzene that exhibits unconventional junction current versus junction-stretching distance curves, which are peak-shaped and feature two conducting states of 2.3 × 10-4 G0 and 3.4 × 10-4 G0. A combination of theory and experiments is used to understand the conductance of single-molecule junctions featuring this new anchoring group, i.e., pyrazolyl. These results demonstrate that the pyrazolyl moiety changes its protonation state and contact binding during junction evolution and that it also binds in either end-on or facial geometries with gold contacts. The pyrazolyl moiety holds general interest as a contacting group, because this linkage leads to a strong double anchoring of the molecule to the gold electrode, resulting in enhanced conductance values.

Differences in Functional Expression of Connexin43 and NaV1.5 by Pan- and Class-Selective Histone Deacetylase Inhibition in Heart.

Class-selective histone deacetylase (HDAC) inhibitors were designed to improve safety profiles and therapeutic effectiveness in the treatment of multiple cancers relative to pan-HDAC inhibitors. However, the underlying mechanisms for their therapeutic and cardiotoxic potentials remain poorly understood. Cardiac sodium currents (INa) and gap junction conductance (gj) were measured by whole cell patch clamp techniques on primary cultures of neonatal cardiomyocytes. Cardiac NaV1.5 sodium channel and connexin43 (Cx43) gap junction protein levels were assessed by Western blot analyses. Panobinostat produced concentration-dependent reductions in ventricular gj, peak INa density, and NaV1.5 protein expression levels. Membrane voltage (Vm)-dependent activation of INa was shifted by +3 to 6 mV with no effect on inactivation. Entinostat (1 μM) did not affect ventricular gj, peak INa density, or INa activation. However, the INa half-inactivation voltage (V½) was shifted by −3.5 mV. Ricolinostat had only minor effects on ventricular gj and INa properties, though INa activation was shifted by −4 mV. Cx43 and NaV1.5 protein expression levels were not altered by class-selective HDAC inhibitors. The lack of effects of class-selective HDAC inhibitors on ventricular gj and INa may help explain the improved cardiac safety profile of entinostat and ricolinostat.

Non-adiabatic corrections to electric current in molecular junctions due to nuclear motion at the molecule-electrode interfaces.

We present quantum electron transport theory that incorporates dynamical effects of motion of atoms on electrode-molecule interfaces in the calculations of the electric current. The theory is based on non-equilibrium Green's functions. We separate time scales in the Green's functions as fast relative time and slow central time. The derivative with respect to the central time serves as a small parameter in the theory. We solve the real-time Kadanoff-Baym equations for molecular Green's functions using Wigner representation and keep terms up to the second order with respect to the central time derivatives. Molecular Green's functions and consequently the electric current are expressed as functions of molecular junction coordinates as well as velocities and accelerations of molecule-electrode interface nuclei. We apply the theory to model a molecular system and study the effects of non-adiabatic nuclear motion on molecular junction conductivity.

Understanding and Engineering Phonon-Mediated Tunneling into Graphene on Metal Surfaces

Metal-intercalated graphene on Ir(111) exhibits phonon signatures in inelastic electron tunneling spectroscopy with strengths that depend on the intercalant. Extraordinarily strong graphene phonon signals are observed for Cs intercalation. Li intercalation 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 contact ranges. In contrast to Cs and Li, for Ni-intercalated graphene the phonon signals stay below the detection limit in all transport ranges. Going beyond the conventional two-terminal approach, transport calculations provide a comprehensive understanding of the subtle interplay between the graphene-electrode coupling and the observation of graphene phonon spectroscopic signatures.