Advanced Materials

Cover image for Vol. 25 Issue 14

April 11, 2013

Volume 25, Issue 14

Pages 1957–2100

  1. Cover Picture

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      Photopolymerization: Photopolymerization Reactions Using the Photoinitiated Copper (I)-Catalyzed Azide-Alkyne Cycloaddition (CuAAC) Reaction (Adv. Mater. 14/2013) (page 1957)

      Tao Gong, Brian J. Adzima, Noah H. Baker and Christopher N. Bowman

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370086

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      Christopher N. Bowman and co-workers report on page 2024 the development of a novel photopolymerization reaction using the copper (I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction to generate polymer networks with unique mechanical properties. The cover image illustrates the formation of a cross-linked network in the irradiated/light area while unreacted monomer molecules remain in the dark regions.

  2. Inside Front Cover

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      Sensors: Electrolyte-Gated Organic Field-Effect Transistor Sensors Based on Supported Biotinylated Phospholipid Bilayer (Adv. Mater. 14/2013) (page 1958)

      Maria Magliulo, Antonia Mallardi, Mohammad Yusuf Mulla, Serafina Cotrone, Bianca Rita Pistillo, Pietro Favia, Inger Vikholm-Lundin, Gerardo Palazzo and Luisa Torsi

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370087

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      An electrolyte gated organic field-effect transistor (EGOFET) endowed with a biological capturing layer can allow high performance electronic biodetection in a high ionic strength buffer solution as reported by Luisa Torsi, Gerardo Palazzo and co-workers on page 2090. The cover image illustrates flexible electronic circuits printed on a protein strand, imaginatively featuring the ultimate integration of the two systems. Image: Daniele Romeo.

  3. Back Cover

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      Solar Cells: Exciton Dissociation and Charge-Transport Enhancement in Organic Solar Cells with Quantum-Dot/N-doped CNT Hybrid Nanomaterials (Adv. Mater. 14/2013) (page 2104)

      Ju Min Lee, Byoung-Hwa Kwon, Hyung Il Park, Hoyeon Kim, Min Gyu Kim, Ji Sun Park, E Su Kim, Seunghyup Yoo, Duk Young Jeon and Sang Ouk Kim

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370088

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      QD/CNT hybrid nanomaterials enhance the exciton dissociation and electron transport in the bulk-heterojunction active layer of organic solar cells, as described by Sang Ouk Kim, Duk Young Jeon, and co-workers on page 2011. InP quantum dots (QDs) spontaneously bind at N-doped carbon nanotubes via electrostatic attraction. While the InP QDs encouraged the exciton dissociation, NCNTs enhanced the transport of the separated electrons. Such a synergistic effect successfully improved the PCE from 4.68% to 6.11%, which corresponds to 31% enhancement.

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    1. Masthead: (Adv. Mater. 14/2013)

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370089

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  6. Correction

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      Correction: Nd2Fe14B/FeCo Anisotropic Nanocomposite Films with a Large Maximum Energy Product (page 1966)

      Weibin Cui, Yukiko K. Takahashi and Kazuhiro Hono

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201390002

      This article corrects:

      Nd2Fe14B/FeCo Anisotropic Nanocomposite Films with a Large Maximum Energy Product

      Vol. 24, Issue 48, 6530–6535, Version of Record online: 26 OCT 2012

  7. Communication

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    1. Absence of Edge States in Covalently Bonded Zigzag Edges of Graphene on Ir(111) (pages 1967–1972)

      Yan Li, Dinesh Subramaniam, Nicolae Atodiresei, Predrag Lazić, Vasile Caciuc, Christian Pauly, Alexander Georgi, Carsten Busse, Marcus Liebmann, Stefan Blügel, Marco Pratzer, Markus Morgenstern and Riccardo Mazzarello

      Version of Record online: 5 FEB 2013 | DOI: 10.1002/adma.201204539

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      The zigzag edges of graphene on Ir(111) are studied by ab initio simulations and low-temperature scanning tunneling spectroscopy, providing information about their structural, electronic, and magnetic properties. No edge state is found to exist, which is explained in terms of the interplay between a strong geometrical relaxation at the edge and a hybridization of the d orbitals of Ir atoms with the graphene orbitals at the edge.

  8. Frontispiece

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      Single-Photon Sources: Non-Blinking Single-Photon Generation with Anisotropic Colloidal Nanocrystals: Towards Room-Temperature, Efficient, Colloidal Quantum Sources (Adv. Mater. 14/2013) (page 1973)

      Ferruccio Pisanello, Godefroy Leménager, Luigi Martiradonna, Luigi Carbone, Stefano Vezzoli, Pascal Desfonds, Pantaleo Davide Cozzoli, Jean-Pierre Hermier, Elisabeth Giacobino, Roberto Cingolani, Massimo De Vittorio and Alberto Bramati

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370091

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      High-quality core/shell CdSe/CdS colloidal nanocrystals are demonstrated to be efficient sources of non-classical light. As shown by Ferruccio Pisanello and co-workers on page 1974, the intrinsic anisotropy of these nanoparticles allows an independent tuning of shell length and thickness, resulting in a full control of photon statistics. This can be exploited to obtain non-blinking, room-temperature single-photon generation, thus bringing colloidal nanocrystals one step closer to non-classical light sources for quantum applications.

  9. Communications

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    1. Non-Blinking Single-Photon Generation with Anisotropic Colloidal Nanocrystals: Towards Room-Temperature, Efficient, Colloidal Quantum Sources (pages 1974–1980)

      Ferruccio Pisanello, Godefroy Leménager, Luigi Martiradonna, Luigi Carbone, Stefano Vezzoli, Pascal Desfonds, Pantaleo Davide Cozzoli, Jean-Pierre Hermier, Elisabeth Giacobino, Roberto Cingolani, Massimo De Vittorio and Alberto Bramati

      Version of Record online: 18 JAN 2013 | DOI: 10.1002/adma.201203171

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      Blinking and single-photon emission can be tailored in CdSe/CdS core/shell colloidal dot-in-rods. By increasing the shell thickness it is possible to obtain almost non-blinking nanocrystals, while the shell length can be used to control single-photon emission probability.

    2. Highly Discriminating Photorelease of Anticancer Drugs Based on Hypoxia Activatable Phototrigger Conjugated Chitosan Nanoparticles (pages 1981–1986)

      Qiuning Lin, Chunyan Bao, Yunlong Yang, Qiannan Liang, Dasheng Zhang, Shuiyu Cheng and Linyong Zhu

      Version of Record online: 7 FEB 2013 | DOI: 10.1002/adma.201204455

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      An ultimately selective photorelease system of chitosan-nanoparticles is constructed. Only under unique aspects of tumor-hypoxia physiological conditions, the preliminary locked phototrigger is unlocked by biological reduction to enable the release of the caged drug either by visible light or two-photon near-IR (NIR) excitation. This approach provides a highly discriminating photorelease of anticancer drug to hypoxic tumor cells, but not to healthy normal cells.

    3. Highly Improved Uniformity in the Resistive Switching Parameters of TiO2 Thin Films by Inserting Ru Nanodots (pages 1987–1992)

      Jung Ho Yoon, Jeong Hwan Han, Ji Sim Jung, Woojin Jeon, Gun Hwan Kim, Seul Ji Song, Jun Yeong Seok, Kyung Jean Yoon, Min Hwan Lee and Cheol Seong Hwang

      Version of Record online: 6 FEB 2013 | DOI: 10.1002/adma.201204572

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      Limiting the location where electron injection occurs at the cathode interface to a narrower region is the key factor for achieving a highly improved RS performance, which can be achieved by including Ru Nanodots. The development of a memory cell structure truly at the nanoscale with such a limiting factor for the electric-field distribution can solve the non-uniformity issue of future ReRAM.

    4. Microporous Carbon Nanoplates from Regenerated Silk Proteins for Supercapacitors (pages 1993–1998)

      Young Soo Yun, Se Youn Cho, Jinyong Shim, Byung Hoon Kim, Sung-Jin Chang, Seung Jae Baek, Yun Suk Huh, Yongsug Tak, Yung Woo Park, Sungjin Park and Hyoung-Joon Jin

      Version of Record online: 25 FEB 2013 | DOI: 10.1002/adma.201204692

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      Novel carbon-based microporous nanoplates containing numerous heteroatoms (H-CMNs) are fabricated from regenerated silk fibroin by the carbonization and activation of KOH. The H-CMNs exhibit superior electrochemical performance, displaying a specific capacitance of 264 F/g in aqueous electrolytes, a specific energy of 133 Wh/kg, a specific power of 217 kW/kg, and a stable cycle life over 10000 cycles.

    5. A Self-Organized Anisotropic Liquid-Crystal Plasmonic Metamaterial (pages 1999–2004)

      José Dintinger, Bai-Jia Tang, Xianbing Zeng, Feng Liu, Tobias Kienzler, Georg H. Mehl, Goran Ungar, Carsten Rockstuhl and Toralf Scharf

      Version of Record online: 7 FEB 2013 | DOI: 10.1002/adma.201203965

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      A composite material that leads to self organization of mesogen-coated gold nanospheres is synthesized and shows enhanced anisotropic optical properties due to synergistic effects of the mesogens intrinsic birefringence and its ability to drive the self-assembly process into highly anisotropic architectures with densely packed nanospheres. Such nanoengineered matter sustains a response beyond that achievable by its individual constituents, i.e., a metamaterial.

    6. Enzymatically Active Self-Standing Protein-Polymer Surfactant Films Prepared by Hierarchical Self-Assembly (pages 2005–2010)

      Kamendra P. Sharma, Andrew M. Collins, Adam W. Perriman and Stephen Mann

      Version of Record online: 5 FEB 2013 | DOI: 10.1002/adma.201204161

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      Cross-linked protein-polymer surfactant films consisting of enzymatically active hybrid nanoclusters are prepared using a novel approach based on electrostatically mediated hierarchical self-assembly. The free-standing films are structurally robust, highly hydrophilic, and exhibit sustained fluorescence or recyclable enzymatic phosphatase or oxido-reductase behavior.

    7. Exciton Dissociation and Charge-Transport Enhancement in Organic Solar Cells with Quantum-Dot/N-doped CNT Hybrid Nanomaterials (pages 2011–2017)

      Ju Min Lee, Byoung-Hwa Kwon, Hyung Il Park, Hoyeon Kim, Min Gyu Kim, Ji Sun Park, E Su Kim, Seunghyup Yoo, Duk Young Jeon and Sang Ouk Kim

      Version of Record online: 14 JAN 2013 | DOI: 10.1002/adma.201204454

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      The incorporation of InP quantum-dot/N-doped multiwalled carbon nanotube (QD:NCNT) nanohybrids in the active layer of poly(3-hexylthiophene)/indene−C60 bisadduct (P3HT/ICBA) bulk-heterojuction solar cells enhances VOC and JSC. The QDs encourage exciton dissociation by promoting electron transfer, while the NCNTs enhance the transport of the separated electrons and eventual charge collection. Such a synergistic effect successfully improves the power conversion efficiency (PCE) from 4.68% (reference cells) to 6.11%.

    8. Addressable Organic Structure by Anisotropic Wetting (pages 2018–2023)

      Wenchong Wang, Chuan Du, Liqiang Li, Hong Wang, Chenguang Wang, Yue Wang, Harald Fuchs and Lifeng Chi

      Version of Record online: 21 FEB 2013 | DOI: 10.1002/adma.201204475

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      The anisotropic wetting of functional organic molecules on a patterned surface and the development of a photolithography-compatible method to fabricate addressable organic structures is reported. For example, DtCDQA is grown on a SiO2 surface with a Au prepattern, achieving a high resolution cross-over organic structure.

    9. Photopolymerization Reactions Using the Photoinitiated Copper (I)-Catalyzed Azide-Alkyne Cycloaddition (CuAAC) Reaction (pages 2024–2028)

      Tao Gong, Brian J. Adzima, Noah H. Baker and Christopher N. Bowman

      Version of Record online: 11 FEB 2013 | DOI: 10.1002/adma.201203815

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      The first bulk photopolymerization of multifunctional alkyne and azide monomers using the CuAAC reaction is successfully carried out from low molecular weight, nonviscous monomer resins. Compared to other traditional step-growth bulk photopolymerization, this approach readily provides crosslinked, high glass transition temperature polymers that incorporate triazole linkages throughout the polymer structure with great temporal control.

    10. The Influence of Polymer Purification on Photovoltaic Device Performance of a Series of Indacenodithiophene Donor Polymers (pages 2029–2034)

      Raja Shahid Ashraf, Bob C. Schroeder, Hugo A. Bronstein, Zhenggang Huang, Stuart Thomas, R. Joseph Kline, Christoph J. Brabec, Patrice Rannou, Thomas D. Anthopoulos, James R. Durrant and Iain McCulloch

      Version of Record online: 18 FEB 2013 | DOI: 10.1002/adma.201300027

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      A series of low bandgap indacenodithiophene polymers is purified by recycling SEC in order to isolate narrow polydispersity fractions. This additional purification step is found to have a significant beneficial influence on the solar cell performance and the reasons for this performance increase are investigated.

    11. Enhanced Photocatalytic Oxygen Evolution by Crystal Cutting (pages 2035–2039)

      Min Sun, Shijie Xiong, Xinglong Wu, Chengyu He, Tinghui Li and Paul K. Chu

      Version of Record online: 20 JAN 2013 | DOI: 10.1002/adma.201203864

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      Uniformly cut In2O3 truncated octahedrons are fabricated on a large scale by a simple chemical vapor deposition (CVD) technique. This theoretical analysis predicts that the emergence of {100} facets on the In2O3 truncated octahedrons enhances oxygen evolution significantly in photocatalysis and experimental photoelectrochemical measurements are consistent.

    12. Complex Oxide–Noble Metal Conjugated Nanoparticles (pages 2040–2044)

      Jun-Ling Guo, Yao-De Chiou, Wen-I Liang, Heng-Jui Liu, Ying-Jiun Chen, Wei-Cheng Kuo, Chih-Ya Tsai, Kai-An Tsai, Ho-Hung Kuo, Wen-Feng Hsieh, Jenh-Yih Juang, Yung-Jung Hsu, Hong-Ji Lin, Chien-Te Chen, Xue-Pin Liao, Bi Shi and Ying-Hao Chu

      Version of Record online: 20 FEB 2013 | DOI: 10.1002/adma.201204582

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      Hybrid nanoparticles (NPs) composed of multiple components offer new opportunities for next-generation materials. In this study, a paradigm for the noble metal/ternary complex oxide hybrid NPs is reported by adopting pulsed laser ablation in liquids. As model hybrids, gold-spinel heterodimer (Au-CoFe2O4) and gold-pervoskite heterodimer (Au-SrTiO3) NPs are investigated. This work has demonstrated the diverse playgroup of NP conjugation enlarged by complex oxides.

    13. Oxidation-Resistant Silver Nanostructures for Ultrastable Plasmonic Applications (pages 2045–2050)

      R. Sachan, V. Ramos, A. Malasi, S. Yadavali, B. Bartley, H. Garcia, G. Duscher and R. Kalyanaraman

      Version of Record online: 18 FEB 2013 | DOI: 10.1002/adma.201204920

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      Reduced degradation (oxidation) of silver nanoparticles (NPs) is achieved by contacting Ag with immiscible Co NPs. The relative decay of the plasmon peak (plot) shows that pure Ag NPs (blue dashed curve) decay by 25% in ca 20 days, whereas AgCo NPs last about 10 times longer, requiring nearly five months for a similar decay (red solid curve). The TEM images for both Ag and AgCo were taken after 50 days of storage under ambient conditions.

    14. Low-Temperature Solution-Processed Hydrogen Molybdenum and Vanadium Bronzes for an Efficient Hole-Transport Layer in Organic Electronics (pages 2051–2055)

      Fengxian Xie, Wallace C. H. Choy, Chuandao Wang, Xinchen Li, Shaoqing Zhang and Jianhui Hou

      Version of Record online: 6 FEB 2013 | DOI: 10.1002/adma.201204425

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      A simple one-step method is reported to synthesize low-temperature solution-processed transition metal oxides (TMOs) of molybdenum oxide and vanadium oxide with oxygen vacancies for a good hole-transport layer (HTL). The oxygen vacancy plays an essential role for TMOs when they are employed as HTLs: TMO films with excess oxygen are highly undesirable for their application in organic electronics.

    15. Surface Enhanced Raman Scattering on Non-SERS Active Substrates and In Situ Electrochemical Study based on a Single Gold Microshell (pages 2056–2061)

      Solji Kim, Lilin Piao, Donghoon Han, Beom Jin Kim and Taek Dong Chung

      Version of Record online: 20 FEB 2013 | DOI: 10.1002/adma.201203187

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      A single gold microshell, which was elaborately fabricated to carry numerous hot spots on its own surface, enabled the acquisition of the SERS spectra from the molecules on non-SERS active substrates such as Si/SiO2, ITO, and glass. A self-assembled monolayer of 11-mercaptoundecanols on the gold microshell offered an easy and reliable way to electrically insulate from the underlying flat Pt electrode and accomplish in situ monitoring the electrochemical reaction with minimal interference.

    16. Millimeter-Size Single-Crystal Graphene by Suppressing Evaporative Loss of Cu During Low Pressure Chemical Vapor Deposition (pages 2062–2065)

      Shanshan Chen, Hengxing Ji, Harry Chou, Qiongyu Li, Hongyang Li, Ji Won Suk, Richard Piner, Lei Liao, Weiwei Cai and Rodney S. Ruoff

      Version of Record online: 6 FEB 2013 | DOI: 10.1002/adma.201204000

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      Millimeter-size single-crystal monolayer graphene is synthesized on polycrystalline Cu foil by a method that involves suppressing loss by evaporation of the Cu at high temperature under low pressure. This significantly diminishes the number of graphene domains, and large single crystal domains up to ∼2 mm in size are grown.

    17. Versatile Nanostructured Materials via Direct Reaction of Functionalized Catechols (pages 2066–2070)

      Javier Saiz-Poseu, Josep Sedó, Beatriz García, Cristina Benaiges, Teo Parella, Ramon Alibés, Jordi Hernando, Felix Busqué and Daniel Ruiz-Molina

      Version of Record online: 15 FEB 2013 | DOI: 10.1002/adma.201204383

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      A facile one-step polymerization strategy is explored to achieve novel catechol-based materials. Depending on the functionality of the catechol, the as-prepared product can be used to modify at will the surface tension of nano and bulk structures, from oleo-/hydrophobic to highly hydrophilic. A hydrophobic catechol prepared thus polymerized shows the ability to self-assemble as solid nanoparticles with sticky properties in polar solvent media. Such a versatile concept is ideal for the development of catechol-based multifunctional materials.

    18. Superhydrophobic and Superoleophilic PVDF Membranes for Effective Separation of Water-in-Oil Emulsions with High Flux (pages 2071–2076)

      Wenbin Zhang, Zhun Shi, Feng Zhang, Xia Liu, Jian Jin and Lei Jiang

      Version of Record online: 18 FEB 2013 | DOI: 10.1002/adma.201204520

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      A superhydrophobic-superoleophilic PVDF membrane is fabricated via an inert solvent-induced phase inversion for effective separation of both micrometer and nanometer-sized surfactant-free and surfactant-stabilized water-in-oil emulsions solely driven by gravity, with high separation efficiency (oil purity in filtrate after separation > 99.95 wt%) and high flux, which is several times higher than those of commercial filtration membranes and reported materials with similar permeation properties.

  10. Frontispiece

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    3. Inside Front Cover
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      Thin Films: Organic Vapor Passivation of Silicon at Room Temperature (Adv. Mater. 14/2013) (page 2077)

      Rong Yang, Tonio Buonassisi and Karen K. Gleason

      Version of Record online: 8 APR 2013 | DOI: 10.1002/adma.201370092

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      Initiated chemical vapor deposition is used to achieve air-stable organic passivation of silicon, as reported by Karen K. Gleason and co-workers on page 2078. This layer also functions as an anti-reflection coating. Resistively heated wires produce reactive gas phase species, including methyl radicals, while the silicon surface below remains near room temperature. Photoshop enhanced image by Felice C. Frankel.

  11. Communications

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    1. Organic Vapor Passivation of Silicon at Room Temperature (pages 2078–2083)

      Rong Yang, Tonio Buonassisi and Karen K. Gleason

      Version of Record online: 28 JAN 2013 | DOI: 10.1002/adma.201204382

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      A simple, inexpensive, efficient, and scalable method to create air-stable organic surface passivation layers on silicon using a vapor-phase treatment is demonstrated. A variant of initiated chemical vapor deposition is used to synthesize a thin film that acts as both a passivation layer and an antireflective coating. The lowest surface recombination velocity reported to date is achieved and maintained during prolonged exposure to air.

    2. Self-Assembled Organic Microfibers for Nonlinear Optics (pages 2084–2089)

      Jialiang Xu, Sergey Semin, Dorota Niedzialek, Paul H. J. Kouwer, Eduard Fron, Eduardo Coutino, Matteo Savoini, Yuliang Li, Johan Hofkens, Hiroshi Uji-I, David Beljonne, Theo Rasing and Alan E. Rowan

      Version of Record online: 21 FEB 2013 | DOI: 10.1002/adma.201204237

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      While highly desired in integrated optical circuits, multiresponsive and tunable nonlinear optical (NLO) active 1D (sub)wavelength scale superstructures from organic materials are rarely reported due to the strong tendency of organic molecules to self-assembly in centrosymmetric modes. Here a solution-processed assembly approach is reported to generate non-centrosymmetric single-crystalline organic microfibers with a cumulative dipole moment for anisotropic combined second- and third-order NLO.

    3. Electrolyte-Gated Organic Field-Effect Transistor Sensors Based on Supported Biotinylated Phospholipid Bilayer (pages 2090–2094)

      Maria Magliulo, Antonia Mallardi, Mohammad Yusuf Mulla, Serafina Cotrone, Bianca Rita Pistillo, Pietro Favia, Inger Vikholm-Lundin, Gerardo Palazzo and Luisa Torsi

      Version of Record online: 3 JAN 2013 | DOI: 10.1002/adma.201203587

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      Anchored, biotinylated phospholipids forming the capturing layers in an electrolyte-gated organic field-effect transistor (EGOFET) allow label-free electronic specific detection at a concentration level of 10 nM in a high ionic strength solution. The sensing mechanism is based on a clear capacitive effect across the PL layers involving the charges of the target molecules.

    4. Ultrathin PEGylated W18O49 Nanowires as a New 980 nm-Laser-Driven Photothermal Agent for Efficient Ablation of Cancer Cells In Vivo (pages 2095–2100)

      Zhigang Chen, Qian Wang, Huanli Wang, Lisha Zhang, Guosheng Song, Linlin Song, Junqing Hu, Hongzhi Wang, Jianshe Liu, Meifang Zhu and Dongyuan Zhao

      Version of Record online: 21 FEB 2013 | DOI: 10.1002/adma.201204616

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      A new photothermal coupling agent for photothermal ablation (PTA) therapy of tumors is developed based on ultrathin PEGylated W18O49 nanowires. After being injected with the nanowire solution, the in vivo tumors exhibit a rapid temperature rise to 50.0 ± 0.5 °C upon irradiation with NIR laser light at a safe, low intensity (0.72 W cm−2) for 2 min (left-hand mouse in the figure),), resulting in the efficient PTA of cancer cells in vivo in 10 min.

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