Atomic-scale Junctions Research Articles

Suppression of Andreev conductance in a topological insulator–superconductor nanostep junction**Project supported by the National Natural Science Foundation of China (Grant Nos. 11204065 and 11474085) and the Natural Science Foundation of Hebei Province, China (Grant Nos. A2013205168 and A2014205005).

When two three-dimensional topological insulators (TIs) are brought close to each other with their surfaces aligned, the surfaces form a line junction. Similarly, three TI surfaces, not lying in a single plane, can form an atomic-scale nanostep junction. In this paper, Andreev reflection in a TI–TI–superconductor nanostep junction is investigated theoretically. Because of the existence of edge states along each line junction, the conductance for a nanostep junction is suppressed. When the incident energy (ɛ) of an electron is larger than the superconductor gap (Δ), the Andreev conductance in a step junction is less than unity while for a plane junction it is unity. The Andreev conductance is found to depend on the height of the step junction. The Andreev conductance exhibits oscillatory behavior as a function of the junction height with the amplitude of the oscillations remaining unchanged when ɛ = 0, but decreasing for ɛ = Δ, which is different from the case of the plane junction. The height of the step is therefore an important parameter for Andreev reflection in nanostep junctions, and plays a role similar to that of the delta potential barrier in normal metal–superconductor plane junctions.

Symmetry-derived half-metallicity in atomic and molecular junctions.

Achieving highly spin-polarized electric currents in atomic-scale junctions is of great importance in the field of nanoelectronics and spintronics. Based on robust symmetry considerations, we propose a mechanism to block completely one of spin conduction channels for a broad class of atomic and molecular junctions bridging two ferromagnetic electrodes. This particular behavior is due to the wave function orthogonality between spin up s-like states in ferromagnetic electrode and available π channels in the junction. As a consequence, the system would ideally yield 100% spin-polarized current, with a junction acting thus as a "half-metallic" conductor. Using ab initio electron transport calculations, we demonstrate this principle on two examples: (i) a short carbon chain and (ii) a π-conjugated molecule (polythiophene) connected either to model semi-infinite Ni wires or to realistic Ni(111) electrodes. It is also predicted that such atomic-scale junctions should lead to very high (ideally, infinite) magneto-resistance ratios since the electric current gets fully blocked if two electrodes have antiparallel magnetic alignment.

Shot noise variation within ensembles of gold atomic break junctions at room temperature

Atomic-scale junctions are a powerful tool to study quantum transport, and are frequently examined through the mechanically controllable break junction technique. The junction-to-junction variation of atomic configurations often leads to a statistical approach, with ensemble-averaged properties providing access to the relevant physics. However, the full ensemble contains considerable additional information. We report a new analysis of shot noise over entire ensembles of junction configurations using scanning tunneling microscope-style gold break junctions at room temperature in ambient conditions, and compare these data with simulations based on molecular dynamics, a sophisticated tight-binding model, and nonequilibrium Green's functions. The experimental data show a suppression in the variation of the noise near conductances dominated by fully transmitting channels, and a surprising participation of multiple channels in the nominal tunneling regime. Comparison with the simulations, which agree well with published work at low temperatures and ultrahigh vacuum conditions, suggests that these effects likely result from surface contamination and disorder in the electrodes. We propose additional experiments that can distinguish the relative contributions of these factors.

Quantitative bond energetics in atomic-scale junctions.

A direct measurement of the potential energy surface that characterizes individual chemical bonds in complex materials has fundamental significance for many disciplines. Here, we demonstrate that the energy profile for metallic single-atom contacts and single-molecule junctions can be mapped by fitting ambient atomic force microscope measurements carried out in the near-equilibrium regime to a physical, but simple, functional form. We extract bond energies for junctions formed through metallic bonds as well as metal-molecule link bonds from atomic force microscope data and find that our results are in excellent quantitative agreement with density functional theory based calculations for exemplary junction structures. Furthermore, measurements from a large number of junctions can be collapsed to a single, universal force-extension curve, thus revealing a surprising degree of similarity in the overall shape of the potential surface that governs these chemical bonds. Compared to previous studies under ambient conditions where analysis was confined to trends in rupture force, our approach significantly expands the quantitative information extracted from these measurements, particularly allowing analysis of the trends in bond energy directly.

Proximity Effect between Two Superconductors Spatially Resolved by Scanning Tunneling Spectroscopy

How does a superconductor in contact with another through an atomic-scale junction influence the electronic properties in the latter? Investigating a submicron superconducting island of single-crystal Pb embedded in a pre-superconducting Pb crystalline monolayer, scientists reveal a giant region of induced superconductivity in the monolayer and also offer a theory for describing such proximity effects.

Potential-Dependent Restructuring and Chemical Noise at Au–Ag–Au Atomic Scale Junctions

The effect of electrochemical potential on the behavior of electrochemically deposited Au-Ag-Au bimetallic atomic scale junctions (ASJs) is addressed here. A common strategy for ASJ production begins with overgrown nanojunctions and uses electromigration to back-thin the junction. Here, these steps are carried out with the entire junction under electrochemical potential control, and the relationship between junction stability and applied potential is characterized. The control of electrochemical potential provides a reliable method of regulating the size of nanojunctions. In general, more anodic potentials decrease junction stability and increase the rate at which conductance decays. Conductance behavior under these labile conditions is principally determined by Ag oxidation potential, electrochemical potential-induced surface stress, and the nature of the adsorbate. Junctions fabricated at more cathodic potentials experience only slight changes in conductance, likely due to surface atom diffusion and stress-induced structural rearrangement. Electrochemical potential also plays a significant role in determining adsorption-desorption kinetics of surface pyridine at steady state at Au-Ag-Au ASJs, as revealed through fluctuation spectroscopy. Average cutoff frequencies increase at more anodic potentials, as does the width of the cutoff frequency distribution measured over 80 independent runs. Three reversible reactions--pyridine adsorption, Ag atom desorption, and Ag-pyridine complex dissolution--can occur on the surface, and the combination of the three can explain the observed results.

Electron–Vibration Interaction in Multichannel Single-Molecule Junctions

The effect of electron-vibration interaction in atomic-scale junctions with a single conduction channel was widely investigated both theoretically and experimentally. However, the more general case of junctions with several conduction channels has received very little attention. Here we study electron-vibration interaction in multichannel molecular junctions, formed by introduction of either benzene or carbon dioxide between platinum electrodes. By combining shot noise and differential conductance measurements, we analyze the effect of vibration activation on conductance in view of the distribution of conduction channels. Based on the shift of vibration energy while the junction is stretched, we identify vibration modes with transverse and longitudinal symmetry. The detection of different vibration modes is ascribed to efficient vibration coupling to different conduction channels according to symmetry considerations. While most of our observations can be explained in view of the theoretical models for a single conduction channel, the appearance of conductance enhancement, induced by electron-vibration interaction, at high conductance values indicates either unexpected high electron-vibration coupling or interchannel scattering.

Heat dissipation in atomic-scale junctions

Atomic and single-molecule junctions represent the ultimate limit to the miniaturization of electrical circuits. They are also ideal platforms for testing quantum transport theories that are required to describe charge and energy transfer in novel functional nanometre-scale devices. Recent work has successfully probed electric and thermoelectric phenomena in atomic-scale junctions. However, heat dissipation and transport in atomic-scale devices remain poorly characterized owing to experimental challenges. Here we use custom-fabricated scanning probes with integrated nanoscale thermocouples to investigate heat dissipation in the electrodes of single-molecule ('molecular') junctions. We find that if the junctions have transmission characteristics that are strongly energy dependent, this heat dissipation is asymmetric--that is, unequal between the electrodes--and also dependent on both the bias polarity and the identity of the majority charge carriers (electrons versus holes). In contrast, junctions consisting of only a few gold atoms ('atomic junctions') whose transmission characteristics show weak energy dependence do not exhibit appreciable asymmetry. Our results unambiguously relate the electronic transmission characteristics of atomic-scale junctions to their heat dissipation properties, establishing a framework for understanding heat dissipation in a range of mesoscopic systems where transport is elastic--that is, without exchange of energy in the contact region. We anticipate that the techniques established here will enable the study of Peltier effects at the atomic scale, a field that has been barely explored experimentally despite interesting theoretical predictions. Furthermore, the experimental advances described here are also expected to enable the study of heat transport in atomic and molecular junctions--an important and challenging scientific and technological goal that has remained elusive.

Nonequilibrium transport response from equilibrium transport theory

We propose a simple scheme that describes accurately essential non-equilibrium effects in nanoscale electronics devices using equilibrium transport theory. The scheme, which is based on the alignment and dealignment of the junction molecular orbitals with the shifted Fermi levels of the electrodes, simplifies drastically the calculation of current-voltage characteristics compared to typical non-equilibrium algorithms. We probe that the scheme captures a number of non-trivial transport phenomena such as the negative differential resistance and rectification effects. It applies to those atomic-scale junctions whose relevant states for transport are spatially placed on the contact atoms or near the electrodes.

Excess noise in STM-style break junctions at room temperature

Current noise in nanoscale systems provides additional information beyond the electronic conductance. We report measurements at room temperature of the nonequilibrium ``excess'' noise in ensembles of atomic-scale gold junctions repeatedly formed and broken between a tip and a film, as a function of bias conditions. We observe suppression of the noise near conductances associated with conductance quantization in such junctions, as expected from the finite temperature theory of shot noise in the limit of few quantum channels. In higher conductance junctions, the Fano factor of the noise approaches 1/3 the value seen in the low conductance tunneling limit, consistent with theoretical expectations for the approach to the diffusive regime. At conductance values where the shot noise is comparatively suppressed, there is a residual contribution to the noise that scales quadratically with the applied bias, likely due to a flicker noise/conductance fluctuation mechanism.

Counting statistics in nanoscale junctions

We present first-principles calculations for moments of the current up to the third order in atomic-scale junctions. The quantum correlations of the current are calculated using the current operator in terms of the wave functions obtained self-consistently within the static density-functional theory. We investigate the relationships of the conductance, the second, and the third moment of the current for carbon atom chains of various lengths bridging two metal electrodes in the linear and nonlinear regimes. The conductance, the second-, and the third-order Fano factors exhibit odd-even oscillation with the number of carbon atoms due to the full and half filled {\pi}* orbital near the Fermi levels. The third-order Fano factor and the conductance are positively correlated.

Shot Noise Suppression at Room Temperature in Atomic-Scale Au Junctions

Shot noise encodes additional information not directly inferable from simple electronic transport measurements. Previous measurements in atomic-scale metal junctions at cryogenic temperatures have shown suppression of the shot noise at particular conductance values. This suppression demonstrates that transport in these structures proceeds via discrete quantum channels. Using a high-frequency technique, we simultaneously acquire noise data and conductance histograms in Au junctions at room temperature and ambient conditions. We observe noise suppression at up to three conductance quanta, with possible indications of current-induced local heating and 1/f noise in the contact region at high biases. These measurements demonstrate the quantum character of transport at room temperature at the atomic scale. This technique provides an additional tool for studying dissipation and correlations in nanodevices.

Origin of negative differential resistance in molecular junctions of Rose Bengal

Negative differential resistance (NDR) is tuned at the junctions of electronically different dimers and trimers of Rose Bengal. Isolated molecule did not show any NDR. But it was induced to show double and triple NDRs with large peak to valley ratio (1.8–3.1) at 300K by varying number of neighbors and charging them by an electrical pulse. One could destroy or regenerate NDR by separating them or bringing together by a scanning tunneling microscope tip. NDR was also independent of polaronic nature. Bits 1 and 0 for cationic NDR (in dimer) and 0, 1, 2, and 3 for dianionic NDR (trimer) were written in an atomic scale junction. Importance of junction electronics and effective exposure is revealed.

Fabrication of atomic-scale gold junctions by electrochemical plating using a common medical liquid

Fabrication of nanometer-separated gold junctions has been performed using “iodine tincture,” a medical liquid known as a disinfectant, as an etching/deposition electrolyte. In the gold-dissolved iodine tincture, gold electrodes were grown or eroded slowly enough to form quantum point contacts in an atomic scale. The resistance evolution during the electrochemical deposition showed plateaus at integer multiples of the resistance quantum, (2e2∕h)−1, at room temperature (e: the elementary charge, h: the Planck constant). Iodine tincture is a commercially available common material, which makes the fabrication process to be simple and cost effective. Moreover, in contrast to the conventional electrochemical approaches, this method is free from highly toxic cyanide compounds or extraordinarily strong acids.

Gate-controlled atomic quantum switch.

An atomic-scale quantum conductance switch is demonstrated that allows us to open and close an electrical circuit by the controlled and reproducible reconfiguration of silver atoms within an atomic-scale junction. The only movable parts of the switch are the contacting atoms. The switch is entirely controlled by an external electrochemical voltage applied to an independent third gate electrode. Controlled switching was performed between a quantized, electrically conducting "on state" exhibiting a conductance of G(0)=2e(2)/h ( approximately 1/12.9 kOmega) or preselectable multiples of this value and an insulating "off state."

Density of states and magnetoconductance of disordered Au point contacts

We report low-temperature magnetotransport measurements on electrochemically fabricated atomic scale gold nanojunctions. As $\stackrel{\ensuremath{\rightarrow}}{T}0,$ the junctions exhibit nonperturbatively large zero bias anomalies (ZBA's) in their differential conductance. We consider several explanations and find that the ZBA's are consistent with a reduced local density of states in the disordered metal. We suggest that this is a result of Coulomb interactions in a granular metal with moderate intergrain coupling. Magnetoconductance of atomic scale junctions also differs significantly from that of less geometrically constrained devices, and supports this explanation.

Zero-bias anomalies in electrochemically fabricated nanojunctions

A streamlined technique for the electrochemical fabrication of metal nanojunctions (MNJs) between lithographically defined electrodes is presented. The first low-temperature transport measurements in such structures reveal suppression of the conductance near zero bias. The size of the zero-bias anomaly (ZBA) depends strongly on the fabrication electrochemistry and the dimensions of the resulting MNJ. We present evidence that the nonperturbative ZBA in atomic-scale junctions is due to a density of states suppression in the leads.

Tunnel-Coupled Quantum Dots: Atomistic Theory of Quantum Dot Molecules and Arrays

ABSTRACTAn understanding of how dots couple in quantum dot molecules and arrays is needed so that the possibilities for tailored nanooptics in these systems can be explored. The properties of tunnel-coupled dots will be determined by how the dots couple through atomic-scale junctions. We present an atomistic empirical tight-binding theory of coupled, CdS nanocrystal artificial-molecules, vertically and laterally coupled InAs/GaAs self-assembled dots, and arrays of InAs/GaAs self-assembled dots. Electron states follow the artificial molecule analogy. The coupling of hole states is much more complex. There are significant departures from the artificial molecule analogy because the interdot hole coupling is determined by the hole envelope functions, as for the electron states, and by the hole atomic state near interdot interfaces.

Tunable atomic-scale Josephson effect in dislocated high-Tc superconductors.

A scenario for a tunable dislocation-induced atomic-scale Josephson junction in intrinsically defected high-${\mathit{T}}_{\mathit{c}}$ single crystals is proposed which is based on a competition between different external forces acting upon a dislocation to stabilize its equilibrium position inside a crystal. A possible realization of the self-tuning Josephson effect in these materials is discussed as well.