ChemPhysChem

Cover image for Vol. 11 Issue 3

February 22, 2010

Volume 11, Issue 3

Pages 529–739

  1. Cover Picture

    1. Top of page
    2. Cover Picture
    3. Inside Cover
    4. Graphical Abstract
    5. News
    6. Minireview
    7. Highlight
    8. Communications
    9. Articles
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    1. Cover Picture: Electrochemical Machining of Gold Microstructures in LiCl/Dimethyl Sulfoxide (ChemPhysChem 3/2010) (page 529)

      Xinzhou Ma, Andreas Bán and Rolf Schuster

      Version of Record online: 15 FEB 2010 | DOI: 10.1002/cphc.201090010

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      The application of short voltage pulses between a tool electrode and a workpiece electrode in electrolyte solution allows localization of electrochemical reactions to the vicinity of the tool with unprecedented precision. This can be used for three- dimensional microstructuring of electrochemically active materials. The cover picture shows SEM images of structures machined into a gold sheet with a sub-micron sized carbon-fiber tool. Upon application of a pulse train of 20 ns, 4 V pulses the carbon tip is fed into the Au sheet like the tool in a milling machine. The experimental setup is sketched on the right-hand side of the cover. As discussed by R. Schuster et al. on p. 616, the machining precision is determined by the time constant of double layer charging and varies linearly with the pulse length (lower panel). Non-aqueous electrolytes like LiCl in dimethyl sulfoxide are shown to be particularly useful for achieving high machining precision, because of their low specific electrolyte conductivity compared to typical aqueous electrolytes.

  2. Inside Cover

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    3. Inside Cover
    4. Graphical Abstract
    5. News
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    1. Inside Cover: Graphene on Au(111): A Highly Conductive Material with Excellent Adsorption Properties for High-Resolution Bio/Nanodetection and Identification (ChemPhysChem 3/2010) (page 530)

      Bo Song, Di Li, Wenpeng Qi, Marcus Elstner, Chunhai Fan and Haiping Fang

      Version of Record online: 15 FEB 2010 | DOI: 10.1002/cphc.201090011

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      Material composed of graphene on a Au(111) surface that can stably adsorb carbon-based rings in biomolecules and has excellent conductivity is proposed and demonstrated by C. Fan, H. Fang et al. on p. 585. By using this material as the substrate, the signal-to-noise ratio is greatly enhanced, so that different nucleobases can be clearly distinguishable.

  3. Graphical Abstract

    1. Top of page
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    3. Inside Cover
    4. Graphical Abstract
    5. News
    6. Minireview
    7. Highlight
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  4. News

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    4. Graphical Abstract
    5. News
    6. Minireview
    7. Highlight
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  5. Minireview

    1. Top of page
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    1. Analytical Expressions for Quantitative Scanning Electrochemical Microscopy (SECM) (pages 547–556)

      Christine Lefrou and Renaud Cornut

      Version of Record online: 7 JAN 2010 | DOI: 10.1002/cphc.200900600

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      Valid expressions: Analytical expressions available in the scanning electrochemical microscopy (SECM) literature in steady-state feedback experiments are reviewed (see figure). Some of them are claimed as general expressions, other are presented as approximate. Their validity is discussed in the light of the current understanding and computer facilities.

  6. Highlight

    1. Top of page
    2. Cover Picture
    3. Inside Cover
    4. Graphical Abstract
    5. News
    6. Minireview
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    1. Coulomb Physics in Spin Ice: From Magnetic Monopoles to Magnetic Currents (pages 557–559)

      Claudio Castelnovo

      Version of Record online: 10 DEC 2009 | DOI: 10.1002/cphc.200900873

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      The route to magnetricity: It was proposed that spin ice, a class of rare earth titanates, hosts magnetic monopoles as elementary excitations (see picture). Recently, Bramwell and co-workers measured the Wien effect in Dy2Ti2O7, directly probing the nature of these monopoles and making dysprosium titanate the first example of a magnetolyte.

  7. Communications

    1. Top of page
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    3. Inside Cover
    4. Graphical Abstract
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    1. Very Low Energy Electrons Transform the Cyclobutane-Pyrimidine Dimer into a Highly Reactive Intermediate (pages 561–564)

      Achim Edtbauer, Stephan Denifl, Violaine Vizcaino, Lukas An der Lan, Katherine Russell, Jörg Taubitz, Uta Wille, Linda Feketeova, Richard A. J. O'Hair, Tilmann D. Märk, Eugen Illenberger and Paul Scheier

      Version of Record online: 23 DEC 2009 | DOI: 10.1002/cphc.200900912

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      Explosive reactions: The response of cytotoxic cyclobutane-pyrimidine dimer (CPD), a cross-linked pyrimidine base, to the attachment of a low-energy electron is remarkably similar to explosives like trinitrotoluene. The dominant unimolecular reaction is the splitting into two thymine like units, which is the essential molecular step in the photolyase of CPD (see picture).

    2. Fibrinogen Nanofibril Growth and Self-Assembly on Au (1,1,1) Surface in the Absence of Thrombin (pages 565–568)

      Guojun Chen, Nanting Ni, Binghe Wang and Bingqian Xu

      Version of Record online: 16 DEC 2009 | DOI: 10.1002/cphc.200900916

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      Gold self-assembly: Understanding protein adsorption on gold surface bears increasing importance because of surface-induced changes in conformation and bioactivity. Nanofibril structures of protein fibrinogen (fg) molecules, playing paramount role in blood coagulation, are found self-assembled on a Au(1,1,1) surface without any addition of thrombin, growing in two orientations (longitude and transverse, see figure).

    3. A Self-assembly Route for Double Bilayer Lipid Membrane Formation (pages 569–574)

      Xiaojun Han, Ammathnadu S. Achalkumar, Matthew R. Cheetham, Simon D. A. Connell, Benjamin R. G. Johnson, Richard J. Bushby and Stephen D. Evans

      Version of Record online: 5 JAN 2010 | DOI: 10.1002/cphc.200900798

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      Biomembranes: A new method of forming double bilayer lipid membranes uses NHS/EDC chemistry to link adjacent bilayers, both of which remain fluid. This approach provides a novel platform for the study of biomembranes, in which the components of the upper membrane are shielded from the solid substrate by a second membrane (see figure); and for studying more complex membrane protein systems which span double lipid bilayers.

    4. On the Reversible Photoisomerization of Spiropyran-Modified Zeolite L Single Crystals (pages 575–578)

      R. Q. Albuquerque, J. Kühni, P. Belser and L. De Cola

      Version of Record online: 4 JAN 2010 | DOI: 10.1002/cphc.200900860

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      Having it both ways: The reversible photoisomerization of a derivative of spiropyran at the level of a single crystal by using zeolite L is demonstrated. The synthesized spiropyran exhibits rare negative photochromism when dissolved in a 1:1 mixture of H2O and EtOH The spiropyran is functionalized predominantly at the channel entrances in the case of 4 μm long crystals (see picture).

    5. Angle-Independent Structural Color in Colloidal Amorphous Arrays (pages 579–583)

      Mohammad Harun-Ur-Rashid, Abu Bin Imran, Takahiro Seki, Masahiko Ishii, Hiroshi Nakamura and Yukikazu Takeoka

      Version of Record online: 30 DEC 2009 | DOI: 10.1002/cphc.200900869

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      3-D colloidal amorphous arrays prepared from two different submicron-sized silica particles, exhibit a specific structural color that remains unchanged during the alternation of viewing angle (see figure). The refractive index in amorphous photonic material changes identically in all directions. This isotropic feature of the dielectric distribution leads to wavelength-selective light scattering.

  8. Articles

    1. Top of page
    2. Cover Picture
    3. Inside Cover
    4. Graphical Abstract
    5. News
    6. Minireview
    7. Highlight
    8. Communications
    9. Articles
    10. Preview
    1. Graphene on Au(111): A Highly Conductive Material with Excellent Adsorption Properties for High-Resolution Bio/Nanodetection and Identification (pages 585–589)

      Bo Song, Di Li, Wenpeng Qi, Marcus Elstner, Chunhai Fan and Haiping Fang

      Version of Record online: 7 JAN 2010 | DOI: 10.1002/cphc.200900743

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      Attached to gold: A material composed of graphene on Au(111) (see picture) exhibits a very good adsorption to carbon-based rings in biomolecules as well as an excellent conductivity. The composite material can be used in a range of bio/nano-applications including DNA-based biodevices and biosensors.

    2. Deuteration of Water Enables Self-Organization of Phospholipid-Based Reverse Micelles (pages 590–598)

      Jeannine Milhaud, Nadia Bouchemal, Tomasz Rog and Edith Hantz

      Version of Record online: 1 FEB 2010 | DOI: 10.1002/cphc.200900668

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      Stable water bridges: Upon heating, branches of micelles shrink and branching points (which slide along the branches) swell. This sliding is slowed down when water is deuterated because the H(D)-bonded water bridges joining the phospholipid molecules are more stable. Thus, swollen branching points remain in contact and can fuse (see picture).

    3. Can Copper(II) Mediate Hoogsteen Base-Pairing in a Left-Handed DNA Duplex? A Pulse EPR Study (pages 599–606)

      Maria Grazia Santangelo, Philipp M. Antoni, Bernhard Spingler and Gunnar Jeschke

      Version of Record online: 22 DEC 2009 | DOI: 10.1002/cphc.200900672

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      Bending over for copper: Electron paramagnetic resonance spectroscopy reveals two copper(II) coordination sites in poly(dG-dC)⋅poly(dG-dC). Analysis of the proton hyperfine couplings suggests that in one of these sites a syn to anti conformational change of guanosine enables the copper to bind to two nucleobases (see figure).

    4. Orientational Analysis of Dodecanethiol and p-Nitrothiophenol SAMs on Metals with Polarisation-Dependent SFG Spectroscopy (pages 607–615)

      Francesca Cecchet, Dan Lis, Julien Guthmuller, Benoît Champagne, Yves Caudano, Christophe Silien, Alaa Addin Mani , Paul A. Thiry and André Peremans

      Version of Record online: 27 JAN 2010 | DOI: 10.1002/cphc.200900733

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      Combining polarisations: Polarisation-dependent sum frequency generation (SFG) spectroscopy is used to investigate the orientation of molecules on metallic surfaces. For the first time, by simply combining ppp and ssp polarisations, both the tilt and rotation angles of methyl groups in dodecanethiol SAMs are determined (see picture).

    5. Electrochemical Machining of Gold Microstructures in LiCl/Dimethyl Sulfoxide (pages 616–621)

      Xinzhou Ma, Andreas Bán and Rolf Schuster

      Version of Record online: 16 DEC 2009 | DOI: 10.1002/cphc.200900713

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      Miniature art: LiCl/dimethyl sulfoxide electrolytes are applied for the electrochemical micromachining of Au. Upon the application of short potential pulses in the nanosecond range to a small carbon-fiber electrode, three-dimensional microstructures with high aspect ratios are fabricated (see picture).

    6. The Protonated Guanine–Cytosine Base Pair (pages 622–629)

      Hongyan Wang, Jun D. Zhang and Henry F. Schaefer III

      Version of Record online: 28 DEC 2009 | DOI: 10.1002/cphc.200900687

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      Effects of protonation at different sites of the guanine–cytosine base pair (GC) are studied using density functional theory. Protonation of GC causes significant strengthening of the interstrand hydrogen bonds and a concomitant increase in the base dissociation energies. The picture shows the lowest-energy cation in the series, generated by addition of a proton (blue) to N7 of guanine.

    7. Concentration-Dependent Hydrogen-Bonding Effects on the Dimethyl Sulfoxide Vibrational Structure in the Presence of Water, Methanol, and Ethanol (pages 630–637)

      Kristina Noack, Johannes Kiefer and Alfred Leipertz

      Version of Record online: 18 DEC 2009 | DOI: 10.1002/cphc.200900691

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      Shifting the balance: Hydrogen bonds between dimethyl sulfoxide (DMSO) and water, methanol, and ethanol molecules are studied by Raman spectroscopy. Solvent-induced frequency changes in the CSC stretching modes of DMSO indicate the local structure in the binary mixtures under investigation (see figure).

    8. Behavior of Two Almost Identical Spins during the CPMG Pulse Sequence (pages 638–645)

      Zdeněk Tošner, Antonín Škoch and Jozef Kowalewski

      Version of Record online: 20 JAN 2010 | DOI: 10.1002/cphc.200900699

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      A relaxing time: The apparent transverse relaxation time T2 can be strongly influenced by the pulse repetition rate (see picture) in the Carr–Purcell–Meiboom–Gill experiment for a homonuclear pair assuming mutual dipole–dipole interaction.

    9. Inside a Superatom: The M7q (M=Cu, Ag, q=1+, 0, 1−) Case (pages 646–650)

      Alvaro Muñoz-Castro, Desmond Mac-Leod Carey and Ramiro Arratia-Pérez

      Version of Record online: 13 JAN 2010 | DOI: 10.1002/cphc.200900714

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      Relativistic DFT calculations are performed to obtain the molecular properties of the D5h Cu7q and Ag7q (q=1+, 0, 1−) clusters (see picture for pentagonal-bipyramidal structure). Scalar and spin–orbit relativistic effects are taken into account at two levels: the two-component ZORA Hamiltonian and fully relativistic four-component calculations via the Dirac equation.

    10. An Electrochemical and Photophysical Study of a Covalently Linked Inorganic–Organic Dyad (pages 651–658)

      Axel Kahnt, Leo-Philipp Heiniger, Shi-Xia Liu, Xiaoyan Tu, Zhiping Zheng, Andreas Hauser, Silvio Decurtins and Dirk M. Guldi

      Version of Record online: 5 JAN 2010 | DOI: 10.1002/cphc.200900728

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      A detailed study on the photophysical interaction between the inorganic rhenium cluster moiety and the fullerene moiety of the dyad (see picture) is described. Light-induced energy transfer from the rhenium cluster to the fullerene is clearly evidenced by time-resolved transient absorption spectroscopy based on femtosecond and nanosecond laser photolysis.

    11. Construction and Photophysical Properties of Organic–Inorganic Nanonetworks Based on Oligo(phenylenevinylene) and Functionalized Gold Nanoparticles (pages 659–664)

      Jien Yang, Xiaofeng Liu, Changshui Huang, Chunjie Zhou, Yuliang Li and Daoben Zhu

      Version of Record online: 18 JAN 2010 | DOI: 10.1002/cphc.200900734

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      Novel organic–inorganic nanonetworks of oligo(phenylenevinylene) and gold nanoparticles are synthesized by the amine-based epoxide ring-opening reaction (see figure). The as-prepared nanohybrids exhibit homogeneous and well-defined interfaces between the organic ligands and the inorganic nanoparticles, thereby promoting efficient electronic interfacial interaction between the two constituents.

    12. Controlled Interfacial Assembly and Transfer of Brushlike Copolymer Films (pages 665–669)

      Ronald V. Lerum and Harry Bermudez

      Version of Record online: 22 DEC 2009 | DOI: 10.1002/cphc.200900738

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      Interfacial transfer of highly compressed amphiphilic block copolymer films by a combination of Langmuir–Blodgett (LB) and Langmuir–Schaefer (LS) techniques results in brushlike monolayer and bilayer films (see picture). The bilayer films are resistant to protein adsorption while the monolayers present an attractive surface. This approach provides an opportunity for tunable biomaterial interfaces.

    13. Scanning Electron Microscopy Investigation of Molecular Transport and Reactivity within Polymer Brushes (pages 670–682)

      Tarik Matrab, Fanny Hauquier, Catherine Combellas and Frédéric Kanoufi

      Version of Record online: 15 JAN 2010 | DOI: 10.1002/cphc.200900766

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      A brush with probes: The transport of redox probes within polymer brushes grown by atom-transfer radical polymerization (ATRP) from surfaces (see picture, R=reducer) is investigated by scanning electrochemical microscopy. This allows depiction of the reactivity towards reduction of such macroinitiator surfaces and the patterning of channels into block-copolymer structures.

      Corrected by:

      Corrigendum: Corrigendum: Scanning Electron Microscopy Investigation of Molecular Transport and Reactivity within Polymer Brushes

      Vol. 11, Issue 9, 1804, Version of Record online: 14 JUN 2010

    14. Multi-Colour Electroluminescence of Dendronic Antennae Containing Pyrenes as Light Harvesters (pages 683–688)

      Umberto Giovanella, Wojciech Mróz, Paolo Foggi, Pierangelo Fabbrizzi, Stefano Cicchi and Chiara Botta

      Version of Record online: 29 DEC 2009 | DOI: 10.1002/cphc.200900771

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      Passing the flame: Dendrons containing pyrene moieties that act as light harvesters give multi-colour electroluminescence in spin-coatable single-layer light-emitting diodes through energy-transfer processes from a polyvinylcarbazole matrix (see picture).

    15. Exclusively Heteronuclear NMR Experiments to Obtain Structural and Dynamic Information on Proteins (pages 689–695)

      Wolfgang Bermel, Ivano Bertini , Isabella C. Felli , Riccardo Peruzzini and Roberta Pierattelli 

      Version of Record online: 14 JAN 2010 | DOI: 10.1002/cphc.200900772

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      Protonless NMR: Tools are reported for determining several NMR observables to obtain structural and dynamic information on proteins with atomic resolution (see picture). The new set of experiments is the further development of a strategy based on 13C direct-detection NMR spectroscopy to characterize biological macromolecules.

    16. Coupling Interactions between Sulfurous Acid and the Hydroperoxyl Radical (pages 696–705)

      Ping Li, Zhi-Ying Ma, Wei-Hua Wang, Zhi-Tao Shen, Si-Wei Bi, Hai-Tao Sun and Yu-Xiang Bu

      Version of Record online: 29 DEC 2009 | DOI: 10.1002/cphc.200900781

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      Stable radical–molecule complexes: The nature of the coupling interactions between sulfurous acid and hydroperoxyl radical is systematically investigated theoretical methods. Two stable complexes with strong double intermolecular H-bonds of partial covalence are described. The characteristics of their IR spectra are discussed to enable their possible experimental identification (see figure).

    17. Mesoscale Surface Patterning of a Laterally-Grafted Rod Amphiphile: Rings And Fibers (pages 706–712)

      Libin Liu, Jung-Keun Kim and Myongsoo Lee

      Version of Record online: 28 DEC 2009 | DOI: 10.1002/cphc.200900803

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      An aromatic amphiphilic molecule based on branched oligo(ethylene oxide) is synthesized (picture, center). The laterally-grafted rod amphiphile forms rings by droplet evaporation and the size of the rings can be controlled by the solvent evaporation rate (left). In the Langmuir–Blodgett films the molecule forms fine and long, straight fibers (right).

    18. Single-Electron Self-Exchange between Cage Hydrocarbons and Their Radical Cations in the Gas Phase (pages 713–721)

      Andrés Guerrero, Rebeca Herrero, Esther Quintanilla , Juan Z. Dávalos, José-Luis M. Abboud, Pedro B. Coto and Dieter Lenoir

      Version of Record online: 26 JAN 2010 | DOI: 10.1002/cphc.200900824

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      Stable radical cations are formed from adamantane (1 H), perdeuteroadamantane (1D) and adamantylideneadamantane (2H) in the gas phase. The rate constants for electron exchange in the dyads 1H.+/1H (see picture, distances in Å), 1D.+/1D and 2H.+2H are determined. Ab initio computations allow the mechanism of the process to be rationalized and give insights into the possible role of intermediate complexes in the reaction.

    19. Interfacial Molecular Assemblies of Metalloporphyrins with Two Trans or One Axial Ligands (pages 722–729)

      Pingping Yao, Yunfeng Qiu, Penglei Chen, Yanping Ma, Shenggui He, Jian-Yu Zheng and Minghua Liu

      Version of Record online: 15 JAN 2010 | DOI: 10.1002/cphc.200900831

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      Stable chiral nanofibrous structures exhibiting a bisignated Cotton effect (CE) in the circular dichroism (CD) spectrum are formed by interfacial assembly of metalloporphyrins with two trans axial ligands, while those with one axial ligand form achiral irregular nanoparticles without a CE (see picture). An interpretation of these results in terms of the effects of the axial ligands is proposed.

    20. Ion and pH Sensing with Colloidal Nanoparticles: Influence of Surface Charge on Sensing and Colloidal Properties (pages 730–735)

      Feng Zhang, Zulqurnain Ali, Faheem Amin, Anne Feltz, Martin Oheim and Wolfgang J. Parak

      Version of Record online: 4 FEB 2010 | DOI: 10.1002/cphc.200900849

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      Tuning pH sensitivity: The charged surface of nanoparticles in colloidal solutions, shifts the original pH sensitivity range or so-called pKa of the indicator molecule in a distance-dependant manner. By using different length spacers for the conjugation, the distance between indicators and the nanoparticle can be adjusted, thus tuning the indicator's pH sensitivity (see figure).

  9. Preview

    1. Top of page
    2. Cover Picture
    3. Inside Cover
    4. Graphical Abstract
    5. News
    6. Minireview
    7. Highlight
    8. Communications
    9. Articles
    10. Preview
    1. Preview: ChemPhysChem 4/2010 (page 739)

      Version of Record online: 15 FEB 2010 | DOI: 10.1002/cphc.201090014

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