44 research outputs found

    Structure transitions between copper-sulphate and copper-chloride UPD phases on Au(111)

    Get PDF
    Structure transitions between copper UPD adlayers on Au(111)-(1 × 1) in sulfuric acid and chloride containing electrolyte were investigated by in situ scanning tunnelling microscopy. We demonstrate that co-adsorbed sulphate ions in the (√3 × √3)R30° UPD adlayer are replaced by chloride ions and, depending on the halide coverage, a commensurate (2 × 2) or a slightly distorted (5 × 5)-like Cu-Cl UPD adlayer are formed. The stability ranges of these phases are controlled both by the electrode potential and the Cl− concentration. Phase transitions between the three UPD phases were monitored by time-resolved in situ STM. The observed structure details were attributed to mechanisms based on two-dimensional nucleation and growth processe

    Charge Transport in Single Au|Alkanedithiol|Au Junctions: Coordination Geometries and Conformational Degrees of Freedom

    Full text link
    Recent STM molecular break-junction experiments have revealed multiple series of peaks in the conductance histograms of alkanedithiols. To resolve a current controversy, we present here an in-depth study of charge transport properties of Au|alkanedithiol|Au junctions. Conductance histograms extracted from our STM measurements unambiguously confirm features showing more than one set of junction configurations. Based on quantum chemistry calculations, we propose that certain combinations of different sulfur-gold couplings and trans/gauche conformations act as the driving agents. The present study may have implications for experimental methodology: whenever conductances of different junction conformations are not statistically independent, the conductance histogram technique can exhibit a single series only, even though a much larger abundance of microscopic realizations exists.Comment: 19 pages, 9 figures, 1 table; published versio

    ATR-SEIRAS study of CO adsorption and oxidation on Rh modified Au(111-25 nm) film electrodes in 0.1 M H2SO4

    Get PDF
    Rh modified Au(111-25 nm) electrodes, prepared by electron beam evaporation and galvanostatic deposition, were employed to study adsorption and electro-oxidation of CO on Rh in 0.1 M sulfuric acid solution by in situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS). The results of ATR-SEIRAS experiments were compared with those obtained by infrared reflection absorption spectroscopy on three low-index Rh single crystal surfaces. The Rh film deposited on Au(111-25 nm) electrode consists of 3D clusters forming a highly stepped [n(111) × (111)]-like surface with narrow (111) terraces. When CO was dosed at the hydrogen adsorption potential region, CO adsorbed in both atop (COL) and bridge (COB) configurations, as well as coadsorbed water species, were detected on the Rh film electrode. A partial interconversion of spectroscopic bands due to the CO displacement from bridge to atop sites was found during the anodic potential scan, revealing that there is a potential-dependent preference of CO adsorption sites on Rh surfaces. Our data indicate that CO oxidation on Rh electrode surface in acidic media involves coadsorbed water and follows the nucleation and growth model of a Langmuir-Hinshelwood type reaction.The work was supported by the Research Center Jülich, the University of Bern, Swiss National Science Foundation (200020_144471, 200021-124643), the Spanish Ministerio de Economía y Competitividad (project CTQ2013-44083-P) and University of Alicante. QX acknowledges fellowships of the Research Center Jülich; IP acknowledges support by COST Action TD 1002; and AK acknowledges the financial support by CTI Swiss Competence Centers for Energy Research (SCCER Heat and Electricity Storage)

    Dynamic breaking of a single gold bond

    Get PDF
    AbstractWhile one might assume that the force to break a chemical bond gives a measure of the bond strength, this intuition is misleading. If the force is loaded slowly, thermal fluctuations may break the bond before it is maximally stretched, and the breaking force will be less than the bond can sustain. Conversely, if the force is loaded rapidly it is more likely that the maximum breaking force is measured. Paradoxically, no clear differences in breaking force were observed in experiments on gold nanowires, despite being conducted under very different conditions. Here we explore the breaking behaviour of a single Au–Au bond and show that the breaking force is dependent on the loading rate. We probe the temperature and structural dependencies of breaking and suggest that the paradox can be explained by fast breaking of atomic wires and slow breaking of point contacts giving very similar breaking forces.</jats:p

    A redox-active radical as an effective nanoelectronic component: stability and electrochemical tunnelling spectroscopy in ionic liquids

    Get PDF
    A redox-active persistent perchlorotriphenylmethyl (PTM) radical chemically linked to gold exhibits stable electrochemical activity in ionic liquids. Electrochemical tunnelling spectroscopy in this medium demonstrates that the PTM radical shows a highly effective redox-mediated current enhancement, demonstrating its applicability as an active nanometer-scale electronic component.We acknowledge the financial support from the EU projects ACMOL (FET Young Explorers, GA no. 618082), ERC StG 2012-306826 e-GAMES, ITN iSwitch (GA no. 642196), COST Action TD1002, the Swiss National Science Foundation (Grant No. 200020-144471), the Networking Research Center of Bioengineering, Biomaterials and Nanomedicine (CIBER-BBN), the DGI (Spain) with project BE-WELL CTQ2013-40480-R, the Generalitat de Catalunya with project 2014-SGR-17, and the Severo Ochoa program. N. C acknowledges the RyC program. C. F. is enrolled in the Materials Science PhD program of UAB. We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI). Editoria

    Electrochemical Scanning Tunneling Microscopy

    No full text
    corecore