Formation and properties of metal-oxygen atomic chains

Suspended chains consisting of single noble metal and oxygen atoms have been formed. We provide evidence that oxygen can react with and be incorporated into metallic one-dimensional atomic chains. Oxygen incorporation reinforces the linear bonds in the chain, which facilitates the creation of longer atomic chains. The mechanical and electrical properties of these diatomic chains have been investigated by determining local vibration modes of the chain and by measuring the dependence of the average chain-conductance on the length of the chain. Additionally, we have performed calculations that give insight in the physical mechanism of the oxygen-induced strengthening of the linear bonds and the conductance of the metal-oxygen chains.Comment: 10 pages, 9 fig

Interference enhanced thermoelectricity in quinoid type structures

Quantum interference (QI) effects in molecular junctions may be used to obtain large thermoelectric responses. We study the electrical conductance G and the thermoelec- tric response of a series of molecules featuring a quinoid core using density functional theory (DFT), as well as a semi-empirical interacting model Hamiltonian describing the {\pi}-system of the molecule which we treat in the GW approximation. Molecules with a quinoid type structure are shown to have two distinct destructive QI features close to the frontier orbital energies. These manifest themselves as two dips in the transmission, that remain separated, even when either electron donating or withdraw- ing side groups are added. We find that the position of the dips in the transmission and the frontier molecular levels can be chemically controlled by varying the electron donating or withdrawing character of the side groups as well as the conjugation length inside the molecule. This feature results in a very high thermoelectric power factor S^2G and figure of merit ZT, where S is the Seebeck coefficient, making quinoid type molecules potential candidates for efficient thermoelectric devices.Comment: 22 pages, 11 figure

Electric-field control of interfering transport pathways in a single-molecule anthraquinone transistor

It is understood that molecular conjugation plays an important role in charge transport through single-molecule junctions. Here, we investigate electron transport through an anthraquinone based single-molecule three-terminal device. With the use of an electric-field induced by a gate electrode, the molecule is reduced resulting into a ten-fold increase in the off-resonant differential conductance. Theoretical calculations link the change in differential conductance to a reduction-induced change in conjugation, thereby lifting destructive interference of transport pathways.Comment: Nano Letters (2015

Three Phases in the 3D Abelian Higgs Model with Nonlocal Gauge Interactions

We study the phase structure of the 3D nonlocal compact U(1) lattice gauge theory coupled with a Higgs field by means of Monte-Carlo simulations. The nonlocal interactions among gauge variables are along the temporal direction and mimic the effect of local coupling to massless particles. We found that in contrast to the 3D local abelian Higgs model which has only one phase, the present model exhibits the confinement, Higgs, and Coulomb phases separated by three second-order transition lines emanating from a triple point. This result is quite important for studies on electron fractionalization phenomena in strongly-correlated electron systems. Implications to them are discussed

Opportunities and limitations of transition voltage spectroscopy: a theoretical analysis

In molecular charge transport, transition voltage spectroscopy (TVS) holds the promise that molecular energy levels can be explored at bias voltages lower than required for resonant tunneling. We investigate the theoretical basis of this novel tool, using a generic model. In particular, we study the length dependence of the conducting frontier orbital and of the 'transition voltage' as a function of length. We show that this dependence is influenced by the amount of screening of the electrons in the molecule, which determines the voltage drop to be located at the contacts or across the entire molecule. We observe that the transition voltage depends significantly on the length, but that the ratio between the transition voltage and the conducting frontier orbital is approximately constant only in strongly screening (conjugated) molecules. Uncertainty about the screening within a molecule thus limits the predictive power of TVS. We furthermore argue that the relative length independence of the transition voltage for non-conjugated chains is due to strong localization of the frontier orbitals on the end groups ensuring binding of the rods to the metallic contacts. Finally, we investigate the characteristics of TVS in asymmetric molecular junctions. If a single level dominates the transport properties, TVS can provide a good estimate for both the level position and the degree of junction asymmetry. If more levels are involved the applicability of TVS becomes limited.Comment: 8 pages, 12 figure

Oxygen enhanced atomic chain formation

We report experimental evidence for atomic chain formation during stretching of atomic-sized contacts for gold and silver, that is strongly enhanced due to oxygen incorporation. While gold has been known for its tendency to form atomic chains, for silver this is only observed in the presence of oxygen. With oxygen the silver chains are as long as those for gold, but the conductance drops with chain length to about 0.1 conductance quantum. A relation is suggested with previous work on surface reconstructions for silver (110) surfaces after chemisorption of oxygen.Comment: 4 pages, 4 figure

Quantum Monte Carlo study of a magnetic-field-driven 2D superconductor-insulator transition

We numerically study the superconductor-insulator phase transition in a model disordered 2D superconductor as a function of applied magnetic field. The calculation involves quantum Monte Carlo calculations of the (2+1)D XY model in the presence of both disorder and magnetic field. The XY coupling is assumed to have the form -J\cos(\theta_i-\theta_j-A_{ij}), where A_{ij} has a mean of zero and a standard deviation \Delta A_{ij}. In a real system, such a model would be approximately realized by a 2D array of small Josephson-coupled grains with slight spatial disorder and a uniform applied magnetic field. The different values \Delta A_{ij} then corresponds to an applied field such that the average number of flux quanta per plaquette has various integer values N: larger N corresponds to larger \Delta A_{ij}. For any value of \Delta A_{ij}, there appears to be a critical coupling constant K_c(\Delta A_{ij})=\sqrt{[J/(2U)]_c}, where U is the charging energy, above which the system is a Mott insulator; there is also a corresponding critical conductivity \sigma^*(\Delta A_{ij}) at the transition. For \Delta A_{ij}=\infty, the order parameter of the transition is a renormalized coupling constant g. Using a numerical technique appropriate for disordered systems, we show that the transition at this value of \Delta A_{ij} takes place from an insulating (I) phase to a Bose glass (BG) phase, and that the dynamical critical exponent characterizing this transition is z \sim 1.3. By contrast, z=1 for this model at \Delta A_{ij}=0. We suggest that the superconductor to insulator transition is actually of this I to BG class at all nonzero \Delta A_{ij}'s, and we support this interpretation by both numerical evidence and an analytical argument based on the Harris criterion.Comment: 17 pages, 23 figures, accepted for publication in Phys. Rev.

Image effects in transport at metal-molecule interfaces

We present a method for incorporating image-charge effects into the description of charge transport through molecular devices. A simple model allows us to calculate the adjustment of the transport levels, due to the polarization of the electrodes as charge is added to and removed from the molecule. For this, we use the charge distributions of the molecule between two metal electrodes in several charge states, rather than in gas phase, as obtained from a density-functional theory-based transport code. This enables us to efficiently model level shifts and gap renormalization caused by image-charge effects, which are essential for understanding molecular transport experiments. We apply the method to benzene di-amine molecules and compare our results with the standard approach based on gas phase charges. Finally, we give a detailed account of the application of our approach to porphyrin-derivative devices recently studied experimentally by Perrin et al. [Nat. Nanotechnol. 8, 282 (2013)], which demonstrates the importance of accounting for image-charge effects when modeling transport through molecular junctions