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A reproducible procedure for creating STM tips with nanometrically defined apices out of 0.25mm iron wire is presented.

We present a recipe based on field-directed Ar ion etching of iron tips that results in probes suitable for stable spin-polarized scanning tunneling spectroscopy. This is illustrated by a measurement of the spectroscopic mapping of the magnetization of Co islands on Cu(111)., Comment: 6 figures, 5 pages

Motivated by experimental reports on chirality induced spin selectivity, we investigate a minimal model that allows us to calculate the charge and spin conductances through helical molecules analytically. The spin-orbit interaction is assumed to be non-vanishing on the molecule and negligible in the reservoirs (leads). The band-structure of the molecule features four helical modes with spin-momentum locking that are analogous of edge-currents in the quantum spin Hall effect. While charge is conserved and therefore the charge current is independent of where it is measured, - reservoirs or molecule, - our detailed calculations reveal that the spin currents in the left and right lead are equal in magnitudes but with opposite signs (in linear response). We predict that transport currents flowing through helical molecules are accompanied by a spin accumulation in the contact region with the same magnetization direction for source and drain. Further, we predict that the spin-conductance can be extracted directly from measuring the (quasi-static) spin accumulation - rather than the spin current itself, which is very challenging to obtain experimentally.

Chirality-induced spin selectivity has been reported in many experiments, but a generally accepted theoretical explanation has not yet been proposed. Here, we introduce a simple model system of a straight cylindrical free-electron wire, containing a helical string of atomic scattering centers, with spin-orbit interaction. The advantage of this simple model is that it allows deriving analytical expressions for the spin scattering rates, such that the origin of the effect can be easily followed. We find that spin-selective scattering can be viewed as resulting from constructive interference of partial waves scattered by the spin-orbit terms. We demonstrate that forward scattering rates are independent of spin, while back scattering is spin dependent over wide windows of energy. Although the model does not represent the full details of electron transmission through chiral molecules, it clearly reveals a mechanism that could operate in chiral systems., Comment: 7 pages, 4 figures

We provide a critical overview of the theory of the chirality-induced spin selectivity (CISS) effect, i.e., phenomena in which the chirality of molecular species imparts significant spin selectivity to various electron processes. Based on discussions in a recently held workshop, and further work published since, we review the status of CISS effects - in electron transmission, electron transport, and chemical reactions. For each, we provide a detailed discussion of the state-of-the-art in theoretical understanding and identify remaining challenges and research opportunities.

One-dimensional diffusion of Co ad-atoms on graphene nanoribbons has been induced and investigated by means of scanning tunnelling microscopy (STM). To this end, the nanoribbons and the Co ad-atoms have been imaged before and after injecting current pulses into the nanoribbons, with the STM tip in direct contact with the ribbon. We observe current-induced motion of the Co atoms along the nanoribbons, which is approximately described by a distribution expected for a thermally activated one-dimensional random walk. This indicates that the nanoribbons reach temperatures far beyond 100 K, which is well above the temperature of the underlying Au substrate. This model system can be developed further for the study of electromigration at the single-atom level., Comment: 11 pages, 4 figures

Under the challenge of growing a single bilayer of Bi oriented in the (111) crystallographic direction over amorphous substrates, we have studied different thicknesses of Bi thermally evaporated onto silicon oxide in order to shed light on the dominant atomic structures and their oxidation. We have employed atomic force microscope, X-ray diffraction, and scanning electron microscope approaches to demonstrate that Bi is crystalline and oriented in the (111) direction for thicknesses over 20 nm. Surprisingly, Raman spectroscopy indicates that the rhombohedral structure is preserved even for ultra-thin layers of Bi, down to $\sim 5$ nm. Moreover, the signals also reveal that bismuth films exposed to ambient conditions do not suffer major surface oxidation., Comment: 6 pages,4 figures

The idea that preformed Cooper pairs could exist in a superconductor above its zero-resistance state has been explored for unconventional, interface, and disordered superconductors, yet direct experimental evidence is lacking. Here, we use scanning tunneling noise spectroscopy to unambiguously show that preformed Cooper pairs exist up to temperatures much higher than the zero-resistance critical temperature $T_{C}$ in the disordered superconductor titanium nitride, by observing a clear enhancement in the shot noise that is equivalent to a change of the effective charge from 1 to 2 electron charges. We further show that spectroscopic gap fills up rather than closes when increasing temperature. Our results thus demonstrate the existence of a novel state above $T_{C}$ that, much like an ordinary metal, has no (pseudo)gap, but carries charge via paired electrons.

Electronic transport properties for single-molecule junctions have been widely measured by several techniques, including mechanically controllable break junctions, electromigration break junctions or by means of scanning tunneling microscopes. In parallel, many theoretical tools have been developed and refined for describing such transport properties and for obtaining numerical predictions. Most prominent among these theoretical tools are those based upon density functional theory. In this review, theory and experiment are critically compared and this confrontation leads to several important conclusions. The theoretically predicted trends nowadays reproduce the experimental findings quite well for series of molecules with a single well-defined control parameter, such as the length of the molecules. The quantitative agreement between theory and experiment usually is less convincing, however. Many reasons for quantitative discrepancies can be identified, from which one may decide that qualitative agreement is the best one may expect with present modeling tools. For further progress, benchmark systems are required that are sufficiently well-defined by experiment to allow quantitative testing of the approximation schemes underlying the theoretical modeling. Several key experiments can be identified suggesting that the present description may even be qualitatively incomplete in some cases. Such key experimental observations and their current models are also discussed here, leading to several suggestions for extensions of the models towards including dynamic image charges, electron correlations, and polaron formation., Comment: Review paper 71 pages, 35 figures, 541 references

Ionic liquid gating has become a popular tool for tuning the charge carrier densities of complex oxides. Among these the band insulator SrTiO$_3$ is one of the most extensively studied materials. While experiments have succeeded in inducing (super)conductivity, the process by which ionic liquid gating turns this insulator into a conductor is still under scrutiny. Recent experiments have suggested an electrochemical rather than electrostatic origin of the induced charge carriers. Here, we report experiments probing the time evolution of conduction of SrTiO$_3$ near the glass transition temperature of the ionic liquid. By cooling down to temperatures near the glass transition of the ionic liquid the process develops slowly and can be seen to evolve in time. The experiments reveal a process characterized by waiting times that can be as long as several minutes preceding a sudden appearance of conduction. For the conditions applied in our experiments we find a consistent interpretation in terms of an electrostatic mechanism for the formation of a conducting path at the surface of SrTiO$_3$. The mechanism by which the conducting surface channel develops relies on a nearly homogeneous lowering of the surface potential until the conduction band edge of SrTiO$_3$ reaches the Fermi level of the electrodes., Comment: 22 pages, 7 figures

Shot noise measurements on atomic and molecular junctions provide rich information about the quantum transport properties of the junctions and on the inelastic scattering events taking place in the process. Dissipation at the nanoscale, a problem of central interest in nano-electronics, can be studied in its most explicit and simplified form. Here, we describe a measurement technique that permits extending previous noise measurements to a much higher frequency range, and to much higher bias voltage range, while maintaining a high accuracy in noise and conductance. We also demonstrate the advantages of having access to the spectral information for diagnostics., Comment: 8 figures

Scanning tunneling microscopes (STM) are used extensively for studying and manipulating matter at the atomic scale. In spite of the critical role of the STM tip, the control of the atomic-scale shape of STM tips remains a poorly solved problem. Here, we present a method for preparing tips {\it in-situ} and for ensuring the crystalline structure and reproducibly preparing tip structure up to the second atomic layer. We demonstrate a controlled evolution of such tips starting from undefined tip shapes., Comment: 12 pages preprint-style; 5 figures

One dimensional systems strongly enhance the quantum character of electron transport. Such systems can be realized in 5d transition metals Au, Pt and Ir, in the form of suspended monatomic chains between bulk leads. Atomic chains between ferromagnetic leads would open up many perspectives in the context of spin-dependent transport and spintronics, but the evidence suggests that for pure metals only the mentioned three 5d metals are susceptible to chain formation. It has been argued that the stability of atomic chains made up from ferromagnetic metals is compromised by the same exchange interaction that produces the local moments. Here we demonstrate that magnetic atomic chains can be induced to form in break junctions under the influence of light molecules. Explicitly, we find deuterium assisted chain formation in the 3d ferromagnetic transition metals Fe and Ni. Chain lengths up to eight atoms are formed upon stretching the ferromagnetic atomic contact in deuterium atmosphere at cryogenic temperatures. From differential conductance spectra vibronic states of D$_2$ can be identified, confirming the presence of deuterium in the atomic chains., Comment: 15 pages, 4 figures and Supplementary information(3 pages and 3 figures)

Pt is known to show spontaneous formation of monatomic chains upon breaking a metallic contact. From model calculations, these chains are expected to be spin polarized. However, direct experimental evidence for or against magnetism is lacking. Here, we investigate shot noise as a potential source of information on the magnetic state of Pt atomic chains. We observe a remarkable structure in the distribution of measured shot-noise levels, where the data appear to be confined to the region of nonmagnetic states. While this suggests a nonmagnetic ground state for the Pt atomic chains, from calculations we find that the magnetism in Pt chains is due to 'actor' electron channels, which contribute very little to ballistic conductance and noise. On the other hand, there are weakly polarized 'spectator' channels, which carry most of the current and are only slightly modified by the magnetic state., Comment: The paper gives a new interpretation of the experiments presented in arXiv:1101.3939

Porphyrin molecules can form stable single molecule junctions without anchoring groups. Adding thiol end groups and pyridine axial groups yields more stable junctions with an increased spread in low-bias conductance. This is a result of different bridging geometries during breaking, the stability of which is demonstrated in time-dependent conductance measurements. This is in strong contrast with rod like molecules which show one preferential binding geometry., Comment: 8 pages, 4 figures

We have investigated charge transport in ZnTPPdT-Pyr molecular junctions using the lithographic MCBJ technique at room temperature and cryogenic temperature (6K). We combined low-bias statistical measurements with spectroscopy of the molecular levels using I(V) characteristics. This combination allows us to characterize the transport in a molecular junction in detail. This complex molecule can form different junction configurations, which is observed in trace histograms and in current-voltage (I(V)) measurements. Both methods show that multiple stable single-molecule junction configurations can be obtained by modulating the inter-electrode distance. In addition we demonstrate that different ZnTPPdT-Pyr junction configurations can lead to completely different spectroscopic features with the same conductance values. We show that statistical low-bias conductance measurements should be interpreted with care, and that the combination with I(V) spectroscopy represents an essential tool for a more detailed characterization of the charge transport in a single molecule., Comment: 10 pages, 3 figures

Pt is known to show spontaneous formation of chains of metal atoms upon breaking a metallic contact. From model calculations these have been predicted to be spin polarized, which is reasonable in view of the Stoner enhanced susceptibility of bulk Pt and the increased density of states due to the reduced dimensionality. Here, we demonstrate that shot noise reveals information on the magnetic state of Pt atomic chains. Against all predictions, we find clear evidence for a non-magnetic ground state for the conductance channels of Pt atomic chains., Comment: 10 pages and 8 figures Included supplementary information

We present a quantitative analysis of the steady state electronic transport in a resistive switching device. The device is composed of a thin film of Ag$_{2}$S (solid electrolyte) contacted by a Pt nano-contact acting as ion-blocking electrode, and a large area Ag reference electrode. When applying a bias voltage both ionic and electronic transport occurs, and depending on the polarity it causes an accumulation of ions around the nano-contact. At small applied voltages (pre-switching) we observed this as a strongly nonlinear current-voltage curve, which have been modeled using the Hebb-Wagner treatment for polarization of a mixed conductor. This model correctly describes the transport of the electrons within the polarized solid electrolyte in the steady state up until the resistance switching, covering the entire range of non-stoichiometries, and including the supersaturation range just before the deposition of elemental silver. In this way, it is a step towards a quantitative understanding of the processes that lead to resistance switching., Comment: 21 pages, 6 figures.

We have measured conductance histograms of atomic point contacts made from the noble-transition metal alloys CuNi, AgPd, and AuPt for a concentration ratio of 1:1. For all alloys these histograms at low bias voltage (below 300 mV) resemble those of the noble metals whereas at high bias (above 300 mV) they resemble those of the transition metals. We interpret this effect as a change in the composition of the point contact with bias voltage. We discuss possible explanations in terms of electromigration and differential diffusion induced by current heating., Comment: 5 pages, 6 figures

Using remarkably simple experimental techniques it is possible to gently break a metallic contact and thus form conducting nanowires. During the last stages of the pulling a neck-shaped wire connects the two electrodes, the diameter of which is reduced to single atom upon further stretching. For some metals it is even possible to form a chain of individual atoms in this fashion. Although the atomic structure of contacts can be quite complicated, as soon as the weakest point is reduced to just a single atom the complexity is removed. The properties of the contact are then dominantly determined by the nature of this atom. This has allowed for quantitative comparison of theory and experiment for many properties, and atomic contacts have proven to form a rich test-bed for concepts from mesoscopic physics. Properties investigated include multiple Andreev reflection, shot noise, conductance quantization, conductance fluctuations, and dynamical Coulomb blockade. In addition, pronounced quantum effects show up in the mechanical properties of the contacts, as seen in the force and cohesion energy of the nanowires. We review this reseach, which has been performed mainly during the past decade, and we discuss the results in the context of related developments., Comment: Review, 120 pages, 98 figures. In view of the file size figures have been compressed. A higher-resolution version can be found at: http://lions1.leidenuniv.nl/wwwhome/ruitenbe/review/QPASC-hr-ps-v2.zip (5.6MB zip PostScript)