ChemPhysChem

Cover image for Vol. 11 Issue 7

Special Issue: Interface Phenomena

May 17, 2010

Volume 11, Issue 7

Pages 1325–1583

  1. Cover Picture

    1. Top of page
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    3. Inside Cover
    4. Graphical Abstract
    5. Editorials
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    1. Cover Picture: Entropy Effects in Atom Distribution and Electrochemical Properties of AuxPt1−x/Pt(111) Surface Alloys / Substrate Registry in Disordered Layers of Large Molecules / Tuning Adsorption via Strain and Vertical Ligand Effects (ChemPhysChem 7/2010) (page 1325)

      Andreas Bergbreiter, Otávio B. Alves, Harry E. Hoster, Thomas Waldmann, Robert Reichert and Marc T. M. Koper

      Article first published online: 3 MAY 2010 | DOI: 10.1002/cphc.201090030

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      The cover picture reflects the interdisciplinarity of modern interface research, with special focus on the close cooperation of theory and experiment in the fields of surface science and electrochemistry. The round icons on the right-hand side show, from top to bottom, a surface alloy (H. E. Hoster et al., p. 1505), an ordered oligopyridine adlayer (H. E. Hoster et al., p. 1513), a model of a bimetallic cluster, an electrode nanostructured with lithography methods, and a Ru(0001) surface covered by Pt islands (H. E. Hoster et al., p. 1518). The lower left corner of the picture is filled by a set of thermal desorption spectra recorded for oligopyridines on graphite.

  2. Inside Cover

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    4. Graphical Abstract
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    8. Minireviews
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    1. Inside Cover: Surface Patterning of Silver using an Electron- or Photon-Assisted Oxidation Reaction (ChemPhysChem 7/2010) (page 1326)

      Sebastian Günther, Sebastian Böcklein, Robert Reichelt, Joost Wintterlin, Alexej Barinov, Tefvik O. Menteş, Miguel Á. Niño and Andrea Locatelli

      Article first published online: 3 MAY 2010 | DOI: 10.1002/cphc.201090031

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      The inside cover picture illustrates the patterning of a silver foil by applying an electron-beam-assisted oxidation reaction using NO2 as oxidizing agent. On p. 1525, S. Günther et al. present details on the growth process and confirm that photon-assisted surface patterning is possible as well.

  3. Graphical Abstract

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    1. Graphical Abstract: ChemPhysChem 7/2010 (pages 1327–1338)

      Article first published online: 3 MAY 2010 | DOI: 10.1002/cphc.201090032

  4. Editorials

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  5. News

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  6. Review

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    1. Model Studies on CO Oxidation Catalyst Systems: Titania and Gold Nanoparticles (pages 1344–1363)

      Klaus Christmann, Sebastian Schwede, Susanne Schubert and Wilhelmine Kudernatsch

      Article first published online: 22 FEB 2010 | DOI: 10.1002/cphc.200900769

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      Pocket rockets: Recent data concerning preparation and structural characterisation of planar catalyst model systems consisting of single-crystalline titania (see picture) and/or gold nanoparticles deposited thereon is presented and reviewed.

  7. Minireviews

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    1. Studying Surface Chemistry beyond the Diffraction Limit: 10 Years of TERS (pages 1365–1373)

      Katrin F. Domke and Bruno Pettinger

      Article first published online: 14 APR 2010 | DOI: 10.1002/cphc.200900975

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      What does the interface look like? What is its chemical composition? Tip-enhanced Raman spectrocopy (TERS) allows the correlation of topographic (left) and chemical information on the nanoscale by providing the unique spectroscopic fingerprint (right) characteristic for the sample. TER spectra reveal highly local details about the surface chemistry, for example, about adsorbate–substrate interactions, molecular orientation or surface tension.

    2. Ab Initio Molecular Dynamics Simulations of the Adsorption of H2 on Palladium Surfaces (pages 1374–1381)

      Axel Groß

      Article first published online: 22 JAN 2010 | DOI: 10.1002/cphc.200900818

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      The cover counts: Recent ab initio molecular dynamics studies of the dissociative adsorption of H2 on clean and precovered Pd(100) are reviewed (see picture). These results illustrate that AIMD simulations are well-suited for unraveling details of reaction dynamics at complex surface structures that are not accessible to experiment.

    3. Elimination of Biological Contaminations from Surfaces by Plasma Discharges: Chemical Sputtering (pages 1382–1389)

      Hubert Rauscher, Ondřej Kylián, Jan Benedikt, Achim von Keudell and François Rossi

      Article first published online: 4 DEC 2009 | DOI: 10.1002/cphc.200900757

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      Squeaky clean: Removal of proteins, polypeptides, bacteria and their spores from surfaces by low pressure plasma depends strongly on the gas mixture, but only weakly on the type of contamination (see graph for protein etching). This, and the finding that the Ar/O2 mixture has the highest removal rate, indicates that chemical sputtering is the most important removal mechanism.

  8. Communication

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    1. Breaking the C[BOND]C Bond in the Ethanol Oxidation Reaction on Platinum Electrodes: Effect of Steps and Ruthenium Adatoms (pages 1391–1394)

      Janaina Souza-Garcia, Enrique Herrero and Juan M. Feliu

      Article first published online: 1 APR 2010 | DOI: 10.1002/cphc.201000139

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      Until platinum do us part: The most important step in ethanol oxidation is breaking the C[BOND]C bond. This process is studied by FTIR using platinum single-crystal stepped surfaces, which have a high catalytic activity (see picture). The active sites can be also modified by Ru, which allows determining the role of the adatom in the oxidation mechanism.

  9. Articles

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    1. Self-Diffusion on Au(100): A Density Functional Theory Study (pages 1395–1404)

      Kay Pötting, Wolfgang Schmickler and Timo Jacob

      Article first published online: 22 DEC 2009 | DOI: 10.1002/cphc.200900807

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      Self-diffusion on Au(100) has been studied on perfect and imperfect surfaces using density functional theory (see picture). Various Au migration pathways in the presence of surface defects and along step edges are reported and their energetics are explained in terms of chemical bonding as well as providing rate constants for each process which can be implemented into large-scale simulations.

    2. Oscillatory behaviour in Galvanostatic Formaldehyde Oxidation on Nanostructured Pt/Glassy Carbon Model Electrodes (pages 1405–1415)

      Yvonne E. Seidel, Zenonas Jusys, Rakel W. Lindström, Marie Stenfeldt, Bengt Kasemo and Katharina Krischer

      Article first published online: 20 APR 2010 | DOI: 10.1002/cphc.200901029

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      Collective behavior of individual oscillators: The electrocatalytic oxidation of formaldehyde is investigated. The picture shows time-resolved electrode potential/CO2 current efficiency oscillatory maps during galvanostatic formaldehyde oxidation at different applied current densities over a Pt nanostructure array fabricated onto a planar glassy carbon substrate.

    3. Heat Effects upon Electrochemical Copper Deposition on Polycrystalline Gold (pages 1416–1424)

      Kai D. Etzel, Katrin R. Bickel and Rolf Schuster

      Article first published online: 9 MAR 2010 | DOI: 10.1002/cphc.200900981

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      The heat is on: Heat effects upon different electrochemical Cu deposition processes from sulphuric acid electrolytes on polycrystalline Au surfaces are calorimetrically measured (see picture). Cu underpotential deposition (UPD), Cu deposition onto a Cu UPD layer and bulk Cu deposition all yielded different molar heat effects, pointing to distinct differences in the deposition mechanisms.

    4. In Situ Characterization of Thermo-Responsive Poly(N-Isopropylacrylamide) Films with Sum-Frequency Generation Spectroscopy (pages 1425–1429)

      Volker Kurz, Michael Grunze and Patrick Koelsch

      Article first published online: 9 MAR 2010 | DOI: 10.1002/cphc.200900978

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      Macroscopic features elucidated on a molecular scale: The thermo-responsive behaviour of poly(N-isopropylacrylamide) [pNIPAM] films on gold is probed by in situ sum-frequency generation (SFG) spectroscopy (see figure). At the lower critical solution temperature an instant reorientation of the outermost CH3 groups towards the water phase was detected analogous to previously observed sharp changes in wettability.

    5. Planar Au/TiO2 Model Catalysts: Fabrication, Characterization and Catalytic Activity (pages 1430–1437)

      Menhild Eyrich, Stefan Kielbassa, Thomas Diemant, Johannes Biskupek, Ute Kaiser, Ulf Wiedwald, Paul Ziemann and Joachim Bansmann

      Article first published online: 8 APR 2010 | DOI: 10.1002/cphc.200900942

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      A sketch of the CO oxidation reaction on planar Au/TiO2(110) model catalysts is presented in the figure. The Au nanoparticles on the substrate are created by thermal evaporation of Au under ultrahigh-vacuum conditions. Both CO and O2 first adsorb on the planar model catalyst and then react to CO2, already at temperatures below 100 °C.

    6. In Situ Video-STM Studies of Adsorbate Dynamics at Electrochemical Interfaces (pages 1438–1445)

      Tunay Tansel, Andriy Taranovskyy and Olaf M. Magnussen

      Article first published online: 18 MAR 2010 | DOI: 10.1002/cphc.200900939

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      Viewing atomic interactions: The motion of sulfur atoms, adsorbed on Cu(100) electrodes in HCl solution, has been followed by in situ video-rate STM (see picture). These measurements provide direct data on the adsorbate-adsorbate and adsorbate-substrate interactions of species at electrochemical interfaces.

    7. Supramolecular Organization and Chiral Resolution of p-Terphenyl-m-Dicarbonitrile on the Ag(111) Surface (pages 1446–1451)

      Matthias Marschall, Joachim Reichert, Knud Seufert, Willi Auwärter, Florian Klappenberger, Alexander Weber-Bargioni, Svetlana Klyatskaya, Giorgio Zoppellaro, Alexei Nefedov, Thomas Strunskus, Christof Wöll, Mario Ruben and Johannes V. Barth

      Article first published online: 22 FEB 2010 | DOI: 10.1002/cphc.200900938

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      The supramolecular organization and layer formation of a non-linear, prochiral molecule adsorbed on the Ag(111) surface is investigated. Upon 2D confinement the molecules are deconvoluted in three stereoisomers. The ordering within the expressed supramolecular arrays reflects a substrate templating effect, steric constraints and the operation of weak lateral interactions (see picture).

    8. The Electrochemical Promotion of Ethylene Oxidation at a Pt/YSZ Catalyst (pages 1452–1459)

      Arafat Toghan, Liz M. Rösken and Ronald Imbihl

      Article first published online: 22 FEB 2010 | DOI: 10.1002/cphc.200900936

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      The electrochemical promotion of the C2H4+O2 reaction to form CO2 and H2O is studied with a Pt catalyst interfaced as working electrode to yttrium-stabilized zirconia (YSZ), as shown in the graphic. The large non-Faradayicity reported in the literature for this reaction system is explained as an ignition effect caused by the partial removal of the inhibiting carbonaceaous layer.

    9. SERS of β-Thioglucose Adsorbed on Nanostructured Silver Electrodes (pages 1460–1467)

      Mansoor Vezvaie, Christa L. Brosseau, John D. Goddard and Jacek Lipkowski

      Article first published online: 22 APR 2010 | DOI: 10.1002/cphc.200900930

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      Experimental and theoretical methods were used to investigate the adsorption and potential-driven reorientation of β-D-thioglucose on a nanocavity-patterned silver electrode (see picture). In the presence of water, thioglucose anomerizes to a mixture of α- and β-anomers. The SERS data indicate that the lactol ring of adsorbed thioglucose molecules rotates with the potential applied to the electrode.

    10. Structural, Compositional and Electrochemical Characterization of Pt–Co Oxygen-Reduction Catalysts (pages 1468–1475)

      S. Axnanda, K. D. Cummins, T. He, D. W. Goodman and M. P. Soriaga

      Article first published online: 14 APR 2010 | DOI: 10.1002/cphc.200900924

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      Not exclusive: When a dual-layer deposit of Pt and Co is annealed at high temperatures, the outermost layer becomes single-crystalline and forms a Pt-rich alloy. The preferential surface segregation of Pt, however, is not sufficient to generate a platinum-only overlayer (see picture). Invariably, Co co-exists with Pt, independent of the substrate [Mo(110) or Ru(0001)] employed.

    11. Classification of a Novel Surface Phase Transition: The Knight-Move Phase (pages 1476–1481)

      Alison Andrews, Matthew Novenstern and Lyle D. Roelofs

      Article first published online: 9 FEB 2010 | DOI: 10.1002/cphc.200900840

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      Atomic chess: The knight move or equation image phase (see picture) occurs on some surfaces relevant for growth of high-Tc superconducting films. The nature of the disordering transition of this phase has not been determined. Simulations demonstrate that this disordering transition is first-order (discontinuous), a result with important implications for preparation of these surfaces.

    12. Coadsorption of Hydrogen and CO on Hydrogen Pre-Covered PtRu/Ru(0001) Surface Alloys (pages 1482–1490)

      Thomas Diemant, Joachim Bansmann and Hubert Rauscher

      Article first published online: 30 DEC 2009 | DOI: 10.1002/cphc.200900839

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      Coadsorption on bimetallic surfaces: The modification of the adsorption properties of CO on hydrogen pre-covered PtRu/Ru(0001) surface alloys and the influence of coadsorption on pre-adsorbed Had is addressed (see picture). CO adsorption remains possible on Had-saturated surfaces and the initial sticking coefficient and maximal CO uptake increase with growing Pt content of the surface alloy. Hydrogen adsorption is destabilized upon coadsorption.

    13. Hydrogen Evolution on Single-Crystal Copper and Silver: A Theoretical Study (pages 1491–1495)

      Elizabeth Santos, Kay Pötting, Angelica Lundin, Paola Quaino and Wolfgang Schmickler

      Article first published online: 25 JAN 2010 | DOI: 10.1002/cphc.200900808

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      Speedy surface: Hydrogen evolution on single-crystal copper and silver (see picture) is investigated by a combination of theoretical methods. At short times, the reaction rate is determined by the transfer of the first proton to the electrode surface. In accord with experiment, it is found for both metals that this reaction proceeds faster on the (111) surfaces than on the (100) ones.

    14. Microscopic Insights into Methane Activation and Related Processes on Pt/Ceria Model Catalysts (pages 1496–1504)

      Yaroslava Lykhach, Thorsten Staudt, Michael Peter Andreas Lorenz, Regine Streber, Andreas Bayer, Hans-Peter Steinrück and Jörg Libuda

      Article first published online: 27 JAN 2010 | DOI: 10.1002/cphc.200900673

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      Supporting role: Ceria-supported noble-metal catalysts release oxygen, which may help to reduce the formation of carbonaceous residues during hydrocarbon reforming. The microscopic origins of these effects are examined using single-crystal-based supported model catalysts. The systems involve Pt nanoparticles on well-defined CeO2(111) films studied by molecular beam experiments, XPS, and STM (see picture).

    15. Entropy Effects in Atom Distribution and Electrochemical Properties of AuxPt1−x/Pt(111) Surface Alloys (pages 1505–1512)

      Andreas Bergbreiter, Otávio B. Alves and Harry E. Hoster

      Article first published online: 14 APR 2010 | DOI: 10.1002/cphc.201000105

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      Mix them up: Annealing of Au-covered Pt(111) yields AuxPt1−x/Pt(111) surface alloys. upd-Had and OHad related features in cyclic voltammograms shrink with increasing Au content. Au immobilizes Had (see picture), which shifts the upd-Had region to lower potentials.

    16. Substrate Registry in Disordered Layers of Large Molecules (pages 1513–1517)

      Thomas Waldmann, Robert Reichert and Harry E. Hoster

      Article first published online: 15 APR 2010 | DOI: 10.1002/cphc.200901028

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      Getting to the bottom: Localized nitrogen-metal attraction determines optimized azimuth orientations of oligopyridines flat-adsorbed on Ag(111) and Au(111), see picture. These orientations occur preferentially and exclusively in disordered and ordered adlayers, respectively.

    17. Tuning Adsorption via Strain and Vertical Ligand Effects (pages 1518–1524)

      Harry E. Hoster, Otávio B. Alves and Marc T. M. Koper

      Article first published online: 22 DEC 2009 | DOI: 10.1002/cphc.200900500

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      The electrochemical properties of Pt thin films on Ru(0001) are very similar to those of Pt(111). Shifts of voltammetric features indicate that the Ru substrate destabilizes the adsorption of Had and OHad on Pt. This effect is stronger for thinner Pt films. Based on STM imaging in combination with density functional theory calculations, the upd-Had region of the cyclic voltammograms is simulated (see picture).

    18. Surface Patterning of Silver using an Electron- or Photon-Assisted Oxidation Reaction (pages 1525–1532)

      Sebastian Günther, Sebastian Böcklein, Robert Reichelt, Joost Wintterlin, Alexej Barinov, Tefvik O. Menteş, Miguel Á. Niño and Andrea Locatelli

      Article first published online: 2 DEC 2009 | DOI: 10.1002/cphc.200900740

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      Silver surfaces can be patterned in a one-step process applying an electron- or photon-assisted oxidation reaction using NO2 as oxidizing agent. When adsorbing NO2 under a laterally confined irradiating beam, local Ag2O patches can be grown on a metallic Ag surface (see figure). Details on the process and the formation of intermediate phases during the growth process are discussed.

    19. Enhanced Reactivity for Hydrogen Reactions at Pt Nanoislands on Au(111) (pages 1533–1541)

      Holger Wolfschmidt, Daniel Weingarth and Ulrich Stimming

      Article first published online: 15 APR 2010 | DOI: 10.1002/cphc.201000148

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      High exchange current densities exceeding 1 A cm−2 at Pt nanostructures on Au(111) for hydrogen-related reactions are reported (see graph). The reactivity obtained on Pt nanostructured Au(111) is confirmed by single-particle reactivity measurements. Aspects such as an involvement of the substrate, highly reactive defect sites and enhanced mass transport are discussed.

    20. Redox Activity and Structural Transition of Heptyl Viologen Adlayers on Cu(100) (pages 1542–1549)

      Min Jiang, Emilia Sak, Knud Gentz, Aleksander Krupski and Klaus Wandelt

      Article first published online: 16 MAR 2010 | DOI: 10.1002/cphc.200900964

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      Wave after wave: The redox behaviour of adsorbed heptyl viologen and its phase transition processes is described. The process is divided into the first electron-transfer step, the reorientation of the radical cation phase on the c(2×2)-Cl adlayer and on the bare Cu(100) surface, the chloride desorption/adsorption process and the second one-electron transfer step (numbered 1–5 in the picture).

    21. Stability of TiO2 Polymorphs: Exploring the Extreme Frontier of the Nanoscale (pages 1550–1557)

      Andrea Vittadini, Francesco Sedona, Stefano Agnoli, Luca Artiglia, Maurizio Casarin, Gian Andrea Rizzi, Mauro Sambi and Gaetano Granozzi

      Article first published online: 22 JAN 2010 | DOI: 10.1002/cphc.200900872

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      Titania at the nanoscale: what′s at the bottom? Because of the weak titania/Pt interaction, the Pt substrate behaves as a simple nanolab bench where titania nanostructures self-assemble on the basis of their intrinsic stability. It is proposed that the stability sequence of the TiO2 polymorphs at the bottom of the nanoscale is rutile[RIGHTWARDS ARROW]brookite[RIGHTWARDS ARROW]anatase[RIGHTWARDS ARROW]TiO2(B)[RIGHTWARDS ARROW]lepidocrocite (see picture).

    22. Coverage-Dependent Self-Assembly of Rubrene Molecules on Noble Metal Surfaces Observed by Scanning Tunneling Microscopy (pages 1558–1569)

      Marina Pivetta, Marie-Christine Blüm , François Patthey and Wolf-Dieter Schneider

      Article first published online: 20 APR 2010 | DOI: 10.1002/cphc.200900846

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      Evolution of self-assembly of rubrene molecules on gold(111) is a complex coverage-dependent process that, with increasing surface coverage, involves formation of small homochiral structures, honeycomb islets, chains of pentagonal supermolecules, and close-packed islands (see picture; ML=monolayer). A different behavior is observed for molecular organization on silver surfaces.

    23. Size-Dependent Binding Energies of Methane to Small Gold Clusters (pages 1570–1577)

      Sandra M. Lang, Thorsten M. Bernhardt, Robert N. Barnett and Uzi Landman

      Article first published online: 8 APR 2010 | DOI: 10.1002/cphc.200900844

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      Approaching the bulk: The interaction of methane with a series of small gold cluster cations Aux+ (x=2–6) is investigated via gas-phase reaction kinetics experiments and first-principles calculations. The results obtained employing a “loose” transition state model (blue) are in good agreement with the calculated binding energies (red) and decrease with increasing cluster size slowly approaching the binding energy of CH4 to an extended Au(111) surface (black line).

  10. Preview

    1. Top of page
    2. Cover Picture
    3. Inside Cover
    4. Graphical Abstract
    5. Editorials
    6. News
    7. Review
    8. Minireviews
    9. Communication
    10. Articles
    11. Preview
    1. Preview: ChemPhysChem 8/2010 (page 1583)

      Article first published online: 3 MAY 2010 | DOI: 10.1002/cphc.201090034

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