ChemPhysChem

Cover image for Vol. 15 Issue 12

August 25, 2014

Volume 15, Issue 12

Pages 2401–2633

  1. Cover Pictures

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. You have free access to this content
      Cover Picture: Multistimuli-Responsive Supramolecular Gels: Design Rationale, Recent Advances, and Perspectives (ChemPhysChem 12/2014) (page 2401)

      Zhifang Sun, Dr. Qiyu Huang, Ting He, Zhengyuan Li, Prof. Yi Zhang and Dr. Lunzhao Yi

      Article first published online: 13 AUG 2014 | DOI: 10.1002/cphc.201490057

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      Y. Zhang, L. Yi et al. present on p. 2421 a minireview of recent advances in multistimuli-responsive supramolecular gels (MRSGs). In particular, a new strategy for preparing MRSGs through a hierarchical self-assembly pathway is introduced.

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      Inside Cover: Continuous Re-hyperpolarization of Nuclear Spins Using Parahydrogen: Theory and Experiment (ChemPhysChem 12/2014) (page 2402)

      Dr. Jan-Bernd Hövener , Stephan Knecht, M.Sc. Niels Schwaderlapp, Prof. Dr. Jürgen Hennig and Dr. Dominik von Elverfeldt

      Article first published online: 13 AUG 2014 | DOI: 10.1002/cphc.201490058

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      Continuous hyperpolarization and the fate of singlet order strongly depend on the magnetic field and interaction time and exhibit distinct maxima, which coincide with experimental data as reported on p. 2451 by J.-B. Hövener et al.

    3. You have free access to this content
      Back Cover: Fluorescence Microscopy with 6 nm Resolution on DNA Origami (ChemPhysChem 12/2014) (page 2636)

      Mario Raab, Jürgen J. Schmied, Ija Jusuk, Dr. Carsten Forthmann and Prof. Dr. Philip Tinnefeld

      Article first published online: 13 AUG 2014 | DOI: 10.1002/cphc.201490061

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      To demonstrate resolution down to 6 nm with the superresolution technique DNA PAINT, binding sites for fluorescent dyes are placed at different distances on top of DNA origami nanostructures, analogous to a macroscopic vision test. P. Tinnefeld et al. show on p. 2431 that distances down to 6 nm can be resolved with DNA PAINT. DNA origami can be used to prove this resolution as many identical structures allow statistical evaluation.

  2. Graphical Abstract

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. Graphical Abstract: ChemPhysChem 12/2014 (pages 2403–2412)

      Article first published online: 13 AUG 2014 | DOI: 10.1002/cphc.201490059

  3. News

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. Editors' Selection: ChemPhysChem 12/2014 (page 2413)

      Article first published online: 13 AUG 2014 | DOI: 10.1002/cphc.201490060

  4. Minireview

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. Multistimuli-Responsive Supramolecular Gels: Design Rationale, Recent Advances, and Perspectives (pages 2421–2430)

      Zhifang Sun, Dr. Qiyu Huang, Ting He, Zhengyuan Li, Prof. Yi Zhang and Dr. Lunzhao Yi

      Article first published online: 20 JUN 2014 | DOI: 10.1002/cphc.201402187

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      Multitalented gels: Multistimuli-responsive supramolecular gels (MRSG) are regarded as ideal templates for industrial and biological processes. However, MRSGs are rare because it is a tough challenge to design and fabricate soft materials with multistimuli responsiveness. The authors highlight the design rationale, recent advances, and future perspectives of MRSGs.

  5. Communications

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. Fluorescence Microscopy with 6 nm Resolution on DNA Origami (pages 2431–2435)

      Mario Raab, Jürgen J. Schmied, Ija Jusuk, Dr. Carsten Forthmann and Prof. Dr. Philip Tinnefeld

      Article first published online: 4 JUN 2014 | DOI: 10.1002/cphc.201402179

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      Resolution down to 6 nm is demonstrated by using the superresolution technique DNA PAINT (point accumulation for imaging in nanoscale topography). Distances of 18, 12, and 6 nm between DNA docking sites are designed on DNA origami nanostructures and imaged as clearly separable double spots (see picture).

    2. Two-Photon Probes for Metal Ions Based on Phenylaza[18]crown-6 Ethers and 1,2,3-Triazoles as π-Linkers (pages 2436–2439)

      Dr. Thomas Schwarze, Dr. Andreas Garz, Dr. Klaus Teuchner, Prof. Dr. Ralf Menzel and Prof. Dr. Hans-Jürgen Holdt

      Article first published online: 28 MAY 2014 | DOI: 10.1002/cphc.201402232

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      Selective response: Two new cation-responsive two-photon absorption (2PA) dyes containing phenylaza[18]crown-6 moieties and 1,2,3-triazole units as π-linkers are described. One of the dyes (see picture) without cations exhibits a 2PA cross-section of 190 GM. Through binding of cations, the 2PA cross-section is reduced or enhanced.

    3. Super-Elastic Air/Water Interfacial Films Self-Assembled from Soluble Surfactants (pages 2440–2444)

      Dr. Artem Kovalenko, Dr. Prasad Polavarapu, Dr. Jean-Louis Gallani, Dr. Geneviève Pourroy, Dr. Gilles Waton and Dr. Marie Pierre Krafft

      Article first published online: 20 JUN 2014 | DOI: 10.1002/cphc.201402248

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      Second skin: In spite of being water-soluble, monosodic salts of (perfluoroalkyl)alkyl phosphates self-assemble at the surface of water into Gibbs films that display exceptional elasticity (∼900 mN m−1) in their condensed phases.

    4. An Interwoven Network of MnO2 Nanowires and Carbon Nanotubes as the Anode for Bendable Lithium-Ion Batteries (pages 2445–2449)

      Shu Jing Ee, Dr. Hongchang Pang, Dr. Ulaganathan Mani, Assoc. Prof. Qingyu Yan, Siong Luong Ting and Assoc. Prof. Peng Chen

      Article first published online: 28 MAY 2014 | DOI: 10.1002/cphc.201402010

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      Bending the rules: An anode comprising interwoven ultralong MnO2 nanowires and multi-walled carbon nanotubes (MWCNTs) is made. By taking advantage of the synergy between these materials, and their strength and flexibility, a low-cost, bendable lithium-ion battery is constructed, demonstrating high capacity and cycling stability.

  6. Articles

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Minireview
    6. Communications
    7. Articles
    1. Continuous Re-hyperpolarization of Nuclear Spins Using Parahydrogen: Theory and Experiment (pages 2451–2457)

      Dr. Jan-Bernd Hövener , Stephan Knecht, M.Sc. Niels Schwaderlapp, Prof. Dr. Jürgen Hennig and Dr. Dominik von Elverfeldt

      Article first published online: 30 JUL 2014 | DOI: 10.1002/cphc.201402177

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      Polar opposites: The continuous re-hyperpolarization of nuclear spins offers intriguing perspectives for both nuclear magnetic resonance spectroscopy and magnetic resonance imaging. In this contribution, we provide a theoretical description of the effect. We simulate the polarization transfer and spin-order loss as functions of magnetic field and time-at-catalyst and compare the results to the experimental data (Mes=2,4,6-trimethylphenyl, py=pyridine).

    2. Stacking of Benzene with Metal Chelates: Calculated CCSD(T)/CBS Interaction Energies and Potential-Energy Curves (pages 2458–2461)

      Dušan P. Malenov, Dragan B. Ninković, Dr. Dušan N. Sredojević and Prof.Dr. Snežana D. Zarić

      Article first published online: 30 JUN 2014 | DOI: 10.1002/cphc.201402114

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      Stacks of energy: Energies of stacking interactions between benzene and metal chelates are calculated at the CCSD(T)/CBS level of theory. A copper chelate is found to stack more favorably with benzene than a nickel chelate. The energies of these interactions are significantly higher than that of benzene–benzene stacking. These results might be important for tuning the magnetic and electrical properties of organic–inorganic materials.

    3. High-Potential Perfluorinated Phthalocyanine–Fullerene Dyads for Generation of High-Energy Charge-Separated States: Formation and Photoinduced Electron-Transfer Studies (pages 2462–2472)

      Dr. Sushanta K. Das, Andrew Mahler, Prof. Angela K. Wilson and Prof. Dr. Francis D'Souza

      Article first published online: 21 MAY 2014 | DOI: 10.1002/cphc.201402118

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      Reach your potential! Electron donor–acceptor dyads composed of perfluorinated zinc phthalocyanine bound to fullerene undergo ultrafast electron transfer, leading to the formation of high-energy radical ion pairs.

    4. Direct In Situ Nitridation of Nanostructured Metal Oxide Deposited Semiconductor Interfaces: Tuning the Response of Reversibly Interacting Sensor Sites (pages 2473–2484)

      William I. Laminack and Prof. James L. Gole

      Article first published online: 26 MAY 2014 | DOI: 10.1002/cphc.201402108

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      Tune in! In situ nitridation of metal oxides deposited on porous silicon is studied by conductometric responses to analyte gases and X-ray photoelectron spectroscopy. These studies show the modification of the chemical structure and the band gap of the metals oxide particles, which thus changes the Lewis acidity of the metal. These results allow for the creation of tunable chemical interactions in sensors and microreactors.

    5. Effect of Protic Ionic Liquid and Surfactant Structure on Partitioning of Polyoxyethylene Non-ionic Surfactants (pages 2485–2489)

      Inga L. Topolnicki, Dr. Paul A. FitzGerald, Prof. Rob Atkin and Prof. Gregory G. Warr

      Article first published online: 23 MAY 2014 | DOI: 10.1002/cphc.201402087

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      Surfactants in ionic liquids: The dissolution and solvation of the hydrophilic and hydrophobic components of non-ionic surfactants in ionic liquids are affected by solvent nanostructure and hydrogen bonding. The polar domains of protic ionic liquids ethyl- and propylammonium nitrate are, thermodynamically speaking, remarkably water-like.

    6. Do Ni/Cu and Cu/Ni Alloys have Different Catalytic Performances towards Water-Gas Shift? A Density Functional Theory Investigation (pages 2490–2496)

      Yu Cheng Huang, Tao Zhou, Hai Liu, ChongYi Ling, SuFan Wang and Jin Yan Du

      Article first published online: 10 JUL 2014 | DOI: 10.1002/cphc.201402285

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      Shifting gear: First-principles calculations are employed to investigate the water-gas shift performance with Cu/Ni and Ni/Cu alloys.

    7. The Nature of One-Dimensional Carbon: Polyynic versus Cumulenic (pages 2497–2502)

      Dr. Christian Neiss, Egor Trushin and Prof. Dr. Andreas Görling

      Article first published online: 24 JUN 2014 | DOI: 10.1002/cphc.201402266

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      BLA or no BLA? The occurrence and magnitude of bond length alternation (BLA) in carbon chains and rings as a function of the chain or ring length is explained. Although in the limit of infinite length, carbon chains have a polyynic structure at the minimum of the potential energy surface, the authors show that zero-point vibrations lead to an effective equalization of all carbon–carbon bond lengths and thus to a cumulenic structure.

    8. Temperature Effects on the Capacitance of an Imidazolium-based Ionic Liquid on a Graphite Electrode: A Molecular Dynamics Simulation (pages 2503–2509)

      Xiaohong Liu, Yining Han and Prof. Dr. Tianying Yan

      Article first published online: 1 JUL 2014 | DOI: 10.1002/cphc.201402220

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      The heat is on: The effects of temperature on the electric double-layer structure and differential capacitance of the ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate (BMIM+/PF6) at a positively or negatively charged graphite electrode are studied by molecular dynamics simulations. BMIM+ is shown (see picture) as the polar head of the imidazolium ring with methyl as + with a butyl tail and PF6 as −.

    9. Effect of Electrical Contact on the Performance of Bi2S3 Single Nanowire Photodetectors (pages 2510–2516)

      Renxiong Li, Juehan Yang, Nengjie Huo, Chao Fan, Fangyuan Lu, Tengfei Yan, Dr. Zhongming Wei and Prof. Jingbo Li

      Article first published online: 6 AUG 2014 | DOI: 10.1002/cphc.201402201

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      Based on high-quality Bi2S3 single nanowires, two kinds of photodetectors with different electrical contacts (ohmic contact and non-ohmic contact) are fabricated and investigated in detail (see figure).

    10. Enhanced Phosphorescence Emission by Incorporating Aromatic Halides into an Entangled Coordination Framework Based on Naphthalenediimide (pages 2517–2521)

      Dr. Virginia Martínez-Martínez, Rebeca Sola Llano, Dr. Shuhei Furukawa, Dr. Yohei Takashima, Prof. Iñigo López Arbeloa and Prof. Susumu Kitagawa

      Article first published online: 20 JUN 2014 | DOI: 10.1002/cphc.201402188

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      Turning on phosphorescence: When halogenated guests are incorporated into the pores of an entangled porous coordination polymer (PCP) with naphthalenediimide (NDI) as chromophore, phosphorescence emission is seen at room temperature. The phosphorescent efficiency is increased on the incorporation of aromatic halides guests, as a result of an extra population process of the triplet state through charge transfer (CT) complex formation.

    11. The Local Kinetic Energy Profile of an Inverted Carbon[BOND]Carbon Bond Reveals and Refines its Charge-Shift Character (pages 2522–2529)

      Dr. Heiko Jacobsen

      Article first published online: 5 JUN 2014 | DOI: 10.1002/cphc.201402184

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      Not either-or anymore: Bond descriptors based on the local kinetic energy not only confirm the essence of charge-shift bonding, but also articulate this concept with nuances.

    12. Speed Dependence of Thermochemical Nanolithography for Gray-Scale Patterning (pages 2530–2535)

      Dr. Keith M. Carroll, Maitri Desai, Dr. Anthony J. Giordano, Prof. Jan Scrimgeour, Prof. William P. King, Prof. Elisa Riedo and Prof. Jennifer E. Curtis

      Article first published online: 26 MAY 2014 | DOI: 10.1002/cphc.201402168

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      Speed control: Thermochemical nanolithography is a versatile, high-speed patterning technique capable of gray-scale chemical patterning with nanoscale resolution. Localized chemical reactions driven by a thermal cantilever enable controlled submicron variations in a diverse set of materials. Here, the technique is extended by providing a quantitative description of how the cantilever speed alters the reaction rate and controls the extent of product formation at a surface.

    13. Exciton Coupling of Surface Complexes on a Nanocrystal Surface (pages 2536–2541)

      Dr. Xiangxing Xu, Jianwei Ji, Guan Wang and Prof. Xiaozeng You

      Article first published online: 23 MAY 2014 | DOI: 10.1002/cphc.201402156

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      Intra-nanocrystal exciton coupling of the surface complexes formed by coordination of 8-hydroxyquinoline (Q) to ZnS nanocrystals (NCs) tunes the photoluminescence (PL) color from blue to green (see picture), broadens the absorption and PL excitation windows of the NCs, and thus is a potential strategy for improving the light-harvesting efficiency of NC solar cells and photocatalysts.

    14. Rules of Boron–Nitrogen Doping in Defect Graphene Sheets: A First-Principles Investigation of Band-Gap Tuning and Oxygen Reduction Reaction Catalysis Capabilities (pages 2542–2549)

      Dipayan Sen, Ranjit Thapa and Prof. Kalyan Kumar Chattopadhyay

      Article first published online: 6 JUN 2014 | DOI: 10.1002/cphc.201402147

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      Who needs to be replaced? Various boron and nitrogen doping/codoping schemes on double-vacancy defect graphene sheets are systematically explored by the means of first-principles calculations. The oxygen reduction reaction capabilities of such structures are investigated in detail (see picture).

    15. Probing Protonation Sites of Isolated Flavins Using IR Spectroscopy: From Lumichrome to the Cofactor Flavin Mononucleotide (pages 2550–2562)

      Dr. Judith Langer, Alan Günther, Sophie Seidenbecher, Dr. Giel Berden, Prof. Dr. Jos Oomens and Prof. Dr. Otto Dopfer

      Article first published online: 4 JUN 2014 | DOI: 10.1002/cphc.201402146

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      It adds to the flavin: The preferred protonation site of the isolated flavins lumichrome, lumiflavin, riboflavin (vitamin B2), and the cofactor flavin mononucleotide, as determined by infrared multiphoton dissociation (IRMPD) spectroscopy and quantum chemical calculations, strongly depends on the substituent of the isoalloxazine chromophore.

    16. Cohesive-Energy-Resolved Bandgap of Nanoscale Graphene Derivatives (pages 2563–2568)

      Prof. Zi Wen, Jinsong Luo, Prof. Yongfu Zhu and Prof. Qing Jiang

      Article first published online: 23 MAY 2014 | DOI: 10.1002/cphc.201402125

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      On the edge: Using thermodynamics, a unified formula is established to investigate the bandgap variation in quantum dots and nanoribbons of graphene derivatives. The bandgaps, which depend on the physicochemical nature of the nanostructure edges, increase substantially as the size of the material decreases. This variation is attributed to the change in cohesive energy of edge carbon atoms.

    17. Sensitive Detection of Trypsin using Liquid-Crystal Droplet Patterns Modulated by Interactions between Poly-L-Lysine and a Phospholipid Monolayer (pages 2569–2574)

      Minmin Zhang and Prof. Chang-Hyun Jang

      Article first published online: 21 MAY 2014 | DOI: 10.1002/cphc.201402120

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      Counting crosses: Liquid crystals (LCs) of 4-cyano-4′-pentylbiphenyl form a bright fan shape (planar orientation at the water–LC interface) when in contact with a mixture of 1,2-dioleoyl-sn-glycero-3-phospho-rac-(1-glycerol) (DOPG) and poly-L-lysine (PLL). The LCs take on a dark cross appearance (homeotropic orientation) in a DOPG–PLL mixture preincubated with the protease trypsin. This optical response can be used to measure trypsin activity. OTS=octyltrichlorosilane.

    18. Experimental and Theoretical Investigation of the First-Order Hyperpolarizability of Octupolar Merocyanine Dyes (pages 2575–2581)

      Dr. Frédéric Castet, Dr. Mireille Blanchard-Desce, Frédéric Adamietz, Yevgen M. Poronik, Prof. Dr. Daniel T. Gryko and Prof. Dr. Vincent Rodriguez

      Article first published online: 20 JUN 2014 | DOI: 10.1002/cphc.201402083

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      Poles apart: Hyper-Rayleigh scattering (HRS) experiments and quantum chemical calculations are combined to investigate the second-order nonlinear optical responses of a series of three-arm merocyanine derivatives. The figure shows the structure and normalized HRS intensity of one of the four investigated octupolar merocyanines.

    19. Discrete Dipole Approximation Analysis of Plasmonic Core/Alloy Nanoparticles (pages 2582–2587)

      Wenjie Wu and Prof. Mathew M. Maye

      Article first published online: 30 MAY 2014 | DOI: 10.1002/cphc.201402082

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      To the core: The surface plasmon resonance (SPR) of Au/AuxAg1−x core/alloy nanoparticles (NPs) has been studied by discrete dipole approximation (DDA; see figure). The SPRs were tunable by both alloy shell composition x and thickness tS. Through simulations of a series of core/alloy model NPs with x=0.2–0.8 and shell thickness to core radius ratio 0.05–1.0, the SPR features were compared with experimental measurements.

    20. Orbital Effect-Induced Anomalous Anion–π Interactions between Electron-Rich Aromatic Hydrocarbons and Fluoride (pages 2588–2594)

      Dr. Guosheng Shi, Jinrong Yang, Prof. Yihong Ding and Prof. Haiping Fang

      Article first published online: 30 MAY 2014 | DOI: 10.1002/cphc.201402075

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      Orbital attraction: An orbital effect-induced anomalous anion–π interaction between electron-rich π systems (aromatic hydrocarbons) and fluoride is reported. The anion–π interactions between fluoride and electron-rich π rings increase markedly with increasing number of π electrons and increasing size of the π rings.

    21. You have free access to this content
      Enhancement of the Photovoltaic Performance of CH3NH3PbI3 Perovskite Solar Cells through a Dichlorobenzene-Functionalized Hole-Transporting Material (pages 2595–2603)

      Jin-Wook Lee, Sungmin Park, Dr. Min Jae Ko, Dr. Hae Jung Son and Prof. Nam-Gyu Park

      Article first published online: 23 MAY 2014 | DOI: 10.1002/cphc.201402033

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      Made to interact: A functionalized hole-transporting material (HTM) for improved interactions between a halide perovskite and HTM is reported (see picture). A dichlorobenzene-functionalized HTM improves the power conversion efficiency of a CH3NH3PbI3 perovskite solar cell by 18.5 %.

    22. Ion Pairing in Protic Ionic Liquids Probed by Far-Infrared Spectroscopy: Effects of Solvent Polarity and Temperature (pages 2604–2609)

      Dr. Koichi Fumino, Verlaine Fossog, Peter Stange, Kai Wittler, Wigbert Polet, Prof. Dr. Rolf Hempelmann and Prof. Dr. Ralf Ludwig

      Article first published online: 12 JUN 2014 | DOI: 10.1002/cphc.201402205

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      Solvent-separated ion pairs: The balance between contact and solvent-separated ion pairs in protic ionic liquids can be tuned by altering the temperature or concentration and polarity of the solvent. Equilibrium constants, free energies, enthalpies, and entropies for ion pair formation in protic ionic liquids are determined by a combination of far-infrared spectroscopy and density functional theory calculations.

    23. Band-Gap Manipulations of Monolayer Graphene by Phenyl Radical Adsorptions: A Density Functional Theory Study (pages 2610–2617)

      Lin Huang, Mahasin Alam Sk, Prof. Peng Chen and Prof. Kok Hwa Lim

      Article first published online: 12 JUN 2014 | DOI: 10.1002/cphc.201402133

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      A radical manipulation: Density functional theory (DFT) reveals that the orthoortho or orthopara adsorption pairings of phenyl radicals on graphene can manipulate graphene′s band gap.

    24. Ab Initio Study on the Stability of NgnBe2N2, NgnBe3N2 and NgBeSiN2 Clusters (pages 2618–2625)

      Sudip Pan, Diego Moreno, Dr. José Luis Cabellos, Prof. Gabriel Merino and Prof. Pratim K. Chattaraj

      Article first published online: 30 MAY 2014 | DOI: 10.1002/cphc.201402101

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      Noble bonds: An ab initio study shows that the positively charged Be centers in experimentally accessible Be2N2, Be3N2, and BeSiN2 clusters can bind noble gas (Ng) atoms.

    25. Organic Nonlinear Optical Materials: The Mechanism of Intermolecular Covalent Bonding Interactions of Kekulé Hydrocarbons with Significant Singlet Biradical Character (pages 2626–2633)

      Jing Liu, Jiarui Xia, Prof. Peng Song, Prof. Yong Ding, Yanling Cui, Xuemei Liu, Prof. Yumei Dai and Prof. Fengcai Ma

      Article first published online: 30 MAY 2014 | DOI: 10.1002/cphc.201402026

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      Splitting the distance: The π–π covalent bond lengths in the title materials are shorter than the van der Waals distance between carbon atoms. Increasing the linker length and/or number of molecules involved in the 1D stack decreases the HOMO–LUMO energy gap and increases the wavelength of the systems.

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