arXiv subjects
Publications and source records attributed to J. M. van Ruitenbeek.
The formation of gold nanowires in vacuum at room temperature reveals a periodic spectrum of exceptionally stable diameters. This is identified as shell structure similar to that which was recently discovered for alkali metals at low temperatures. The gold nanowires present two competing `magic' series of stable diameters, one governed by electronic structure and the other by the atomic packing.
A conducting bridge of a single hydrogen molecule between Pt electrodes is formed in a break junction experiment. It has a conductance near the quantum unit, G_0 = 2e^2/h, carried by a single channel. Using point contact spectroscopy three vibration modes are observed and their variation upon stretching and isotope substitution is obtained. The interpretation of the experiment in terms of a Pt-H_2-Pt bridge is verified by Density Functional Theory calculations for the stability, vibrational modes, and conductance of the structure.
The oscillatory voltage dependence of the conductance of a quantum point contact in the presence of a single point-like defect has been analyzed theoretically. Such signals are detectable and may be exploited to obtain information on defect positions below a metal surface. Both tunnel junctions and ballistic contacts of adiabatic shape have been considered. The effect of quantum interference has been taking into account between the principal wave that is directly transmitted through the contact and the partial wave that is scattered by the contact and the defect. This effect leads to oscillations of the conductance as a function of applied voltage. We obtain the dependence of the period and amplitude of the conductance oscillations on the position of the defect inside the metal.
Experimental conductance histograms for Na nanowires are analyzed in detail and compared to recent theoretical results on the stability of cylindrical and elliptical nanowires, using the free-electron model. We find a one-to-one correspondence between the peaks in the histograms and the most stable nanowire geometries, indicating that several of the commonly observed nanowires have elliptical cross sections.
We supplement our previous observations of the shell effect in alkali-metal nanowires (Li, Na, K) with data extended to the heavy alkalis Rb and Cs. Our observations include: i) a non-monotonous dependence of conductance-histogram peak heights on atomic weight, ii) a rapid transition to an atomic shell structure at elevated temperatures, and iii) a ''reverse'' atomic-electronic shell transition, caused by the closeness to the liquid state.
For the metals Au, Pt and Ir it is possible to form freely suspended monatomic chains between bulk electrodes. The atomic chains sustain very large current densities, but finally fail at high bias. We investigate the breaking mechanism, that involves current-induced heating of the atomic wires and electromigration forces. We find good agreement of the observations for Au based on models due to Todorov and coworkers. The high-bias breaking of atomic chains for Pt can also be described by the models, although here the parameters have not been obtained independently. In the limit of long chains the breaking voltage decreases inversely proportional to the length.
Using a scanning tunnel microscope or mechanically controlled break junctions, atomic contacts of Au, Pt and Ir are pulled to form chains of atoms. We have recorded traces of conductance during the pulling process and averaged these for a large amount of contacts. An oscillatory evolution of conductance is observed during the formation of the monoatomic chain suggesting a dependence on even or odd numbers of atoms forming the chain. This behaviour is not only present in the monovalent metal Au, as it has been previously predicted, but is also found in the other metals which form chains suggesting it to be a universal feature of atomic wires.
Using the mechanically controlled break junction technique at low temperatures and under cryogenic vacuum conditions we have studied atomic contacts of several magnetic (Fe, Co and Ni) and non-magnetic (Pt) metals, which recently were claimed to show fractional conductance quantization. In the case of pure metals we see no quantization of the conductance nor half-quantization, even when high magnetic fields are applied. On the other hand, features in the conductance similar to (fractional) quantization are observed when the contact is exposed to gas molecules. Furthermore, the absence of fractional quantization when the contact is bridged by H_2 indicates the current is never fully polarized for the metals studied here. Our results are in agreement with recent model calculations.
The conductance of a single-atom contact is sensitive to the coupling of this contact atom to the atoms in the leads. Notably for the transition metals this gives rise to a considerable spread in the observed conductance values. The mean conductance value and spread can be obtained from the first peak in conductance histograms recorded from a large set of contact-breaking cycles. In contrast to the monovalent metals, this mean value for Pt depends strongly on the applied voltage bias and other experimental conditions, ranging from about 1 to 2.5 times 2e^2/h. We propose that the different results in part can be explained by the inclusion of hydrogen in the contacts. The bias dependence of the conductance is on the other hand due to the electron current that destabilizes monatomic Pt chains at high bias.
Recent years have shown steady progress in research towards molecular electronics [1,2], where molecules have been investigated as switches [3-5], diodes [6], and electronic mixers [7]. In much of the previous work a Scanning Tunnelling Microscope was employed to address an individual molecule. As this arrangement does not provide long-term stability, more recently metal-molecule-metal links have been made using break junction devices [8-10]. However, it has been difficult to establish unambiguously that a single molecule forms the contact [11]. Here, we show that a single H2 molecule can form a stable bridge between Pt electrodes. In contrast to results for other organic molecules, the bridge has a nearly perfect conductance of one quantum unit, carried by a single channel. The H2-bridge provides a simple test system and a fundamental step towards understanding transport properties of single-molecule devices.
We present a systematic study of the effect of the disorder in copper point contacts. We show that peaks in the conductance histogram of copper point contacts shift upon addition of nickel impurities. The shift increases initially linerarly with the nickel concentration, thus confirming that it is due to disorder in the nanowire, in accordance with predictions. In general, this shift is modelled as a resistance R_s which is placed in series with the contact resistance R_c. However, we obtain different R_s values for the two peaks in the histogram, R_s being larger for the peak at higher conductance.
During the fracture of nanocontacts gold spontaneously forms freely suspended chains of atoms, which is not observed for the iso-electronic noble metals Ag and Cu. Au also differs from Ag and Cu in forming reconstructions at its low-index surfaces. Using mechanically controllable break junctions we show that all the 5d metals that show similar reconstructions (Ir, Pt and Au) also form chains of atoms, while both properties are absent in the 4d neighbor elements (Rh, Pd, Ag), indicating a common origin for these two phenomena. A competition between s and d bonding is proposed as an explanation.
After making a cold weld by pressing two clean metal surfaces together, upon gradually separating the two pieces a metallic nanowire is formed, which progressively thins down to a single atom before contact is lost. In previous experiments [1,2] we have observed that the stability of such nanowires is influenced by electronic shell filling effects, in analogy to shell effects in metal clusters [3]. For sodium and potassium at larger diameters there is a crossover to crystalline wires with shell-closings corresponding to the completion of additional atomic layers. This observation completes the analogy between shell effects observed for clusters and nanowires.
Point-contact spectroscopy is applied to study the energy dependence of paramagnetic impurities in noble metals. The samples are in the form of the so-called "mechanically controllable break-junctions" where the investigated piece of alloy makes a nanowire connecting two bulk electrodes.The lateral dimensions of the bridge are of the order of a few nm and can be continuously changed. Three qualitative dependences manifest the size effect while decreasing the contact diameter: 1) Intensity of Kondo peak due to Kondo scattering in point-contact spectra decreases slower than the nonlinearities due to phonon scatterings, 2) The width of the Kondo peak becomes broder, and 3) Due to the Zeeman energy, the splitting of Kondo peak in external and internal (for a spin glass) fields, is suppressed. Explanation of the phenomena is given in terms of the theory of Zarand and Udvardi where the local density of states (LDOS) of conduction electron fluctuates strongly inside a nanowire due to interference of electronic states. Since Kondo effect is a local probe of LDOS, the impurities located close to the maxima of LDOS show the increase of the Kondo temperature and give the primary contribution to the contact resistance.
Nanowires are formed by indenting and subsequently retracting two pieces of sodium metal. Their cross-section gradually reduces upon retraction and the diameters can be obtained from the conductance. In previous work we have demonstrated that when one constructs a histogram of diameters from large numbers of indentation-retraction cycles, such histograms show a periodic pattern of stable nanowire diameters due to shell structure in the conductance modes. Here, we report the observation of a modulation of this periodic pattern, in agreement with predictions of a supershell structure.
The electrical transport properties of atomic-scale conductors are reviewed, with an emphasis on the relations of this problem with studies on quantum size effects in metallic clusters. A brief introduction is given of the natural formalism for discussing electron transport in ballistic conductors: the Landauer theory. After introducing the experimental techniques, which are used for studying ballistic point contacts in metals, the experimental observations for the conductance of atomic-scale contacts are presented. In order to obtain a full description in terms of the quantum modes for conductance, several recently developed techniques are reviewed, which go beyond straightforward measurement of the conductance. A brief discussion is given of an unusual atomic geometry for gold contacts, which evolve into a chain of freely suspended atoms. Then shell filling effects in sodium nanowires are discussed in the context of the influence of the conductance modes on the total energy of the system. The chapter ends with an outlook on promising new developments.
Single atom junctions between superconducting niobium leads are produced using the Mechanically Controllable Break Junction technique. The current-voltage characteristics of these junctions are analysed using an exact formulation for a superconducting quantum point contact. For tunnelling between two single atoms with a sufficiently large vacuum barrier, it is found that a single channel dominates the current, and that the current-voltage characteristic is described by the theory, without adjustable parameters. For a contact of a single Nb atom it is shown that five conductance channels contribute to the conductance, in agreement with the number expected based on the number of valence orbitals for this d-metal. For each of the channels the transmission probability is obtained from the fits and the limits of accuracy for these numbers are discussed.
The quantum states of a system of particles in a finite spatial domain in general consist of a set of discrete energy eigenvalues; these are usually grouped into bunches of degenerate or close-lying levels, called shells. In fermionic systems, this gives rise to a local minimum in the total energy when all the states of a given shell are occupied. In particular, the closed-shell electronic configuration of the noble gases produces their exceptional stability. Shell effects have previously been observed for protons and neutrons in nuclei and for clusters of metal atoms. Here we report the observation of shell effects in an open system - a sodium metal nanowire connecting two bulk sodium metal electrodes, which are progressively pulled apart. We measure oscillations in the statistical distribution of conductance values, for contact cross-sections containing up to a hundred atoms or more. The period follows the law expected from shell-closure effects, similar to the abundance peaks at `magic numbers' of atoms in metal clusters.