Advanced Functional Materials

Cover image for Vol. 24 Issue 6

February 12, 2014

Volume 24, Issue 6

Pages 721–872

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      Plasmonics: Rational Assembly of Optoplasmonic Hetero-nanoparticle Arrays with Tunable Photonic–Plasmonic Resonances (Adv. Funct. Mater. 6/2014) (page 721)

      Yan Hong, Yue Qiu, Tianhong Chen and Björn M. Reinhard

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470032

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      Template-guided self-assembly facilitates the fabrication of optoplasmonic hetero-nanoparticle arrays that contain metallic and dielectric nanoparticles or nanoparticle clusters at pre-defined lattice sites. On page 739, the integration of nanoparticles with different compositions at programmable positions into an array by B. M. Reinhard and co-workers generates hybrid electromagnetic materials with new degrees of freedom for tailoring near- and far-field optical responses as well as enhancing light–matter interactions through synergistic electromagnetic interactions between the building blocks.

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      Collagen Scaffolds: Iron Oxide-Labeled Collagen Scaffolds for Non-Invasive MR Imaging in Tissue Engineering (Adv. Funct. Mater. 6/2014) (page 722)

      Marianne E. Mertens, Alina Hermann, Anne Bühren, Leon Olde-Damink, Diana Möckel, Felix Gremse, Josef Ehling, Fabian Kiessling and Twan Lammers

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470033

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      The physical or chemical integration of ultrasmall superparamagnetic iron oxide nanoparticles into the 3D collagen-based scaffold matrix of tissue-engineered implants by T. Lammers and co-workers on page 754 allows highly sensitive visualization and monitoring using MRI, and enables the longitudinal assessment of implant localization, function, remodeling, and resorption. Labeled scaffolds are shown to be highly biocompatible and suitable for tissue engineering applications.

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      Luminescent Materials: Cation–Anion Interaction-Directed Molecular Design Strategy for Mechanochromic Luminescence (Adv. Funct. Mater. 6/2014) (page 876)

      Gaocan Li, Feijie Song, Di Wu, Jingbo Lan, Xingyan Liu, Jie Wu, Shuaijun Yang, Dan Xiao and Jingsong You

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470038

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      A series of common N-heteroaromatic onium fluorophores with striking reversible mechanochromic luminescence are designed and synthesized on page 747 based on a cation–anion interactiondirected molecular design strategy, which has great potential for a wide variety of applications such as sensors, memory devices, motion systems, security systems, rewritable optical media, etc. The image by J. You and co-workers illustrates how color printing could be realized without ink through the adoption of their mechanochromic materials.

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      Masthead: (Adv. Funct. Mater. 6/2014)

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470037

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      Phototunable Underwater Oil Adhesion of Micro/Nanoscale Hierarchical-Structured ZnO Mesh Films with Switchable Contact Mode (page 729)

      Dongliang Tian, Zhenyan Guo, Yiliang Wang, Wenxian Li, Xiaofang Zhang, Jin Zhai and Lei Jiang

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201304123

      This article corrects:
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      Hierarchical Structures: Large Scale Graphene/Hexagonal Boron Nitride Heterostructure for Tunable Plasmonics (Adv. Funct. Mater. 6/2014) (page 730)

      Kai Zhang, Fung Ling Yap, Kun Li, Chang Tai Ng, Lin Jun Li and Kian Ping Loh

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470035

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      K. P. Loh and co-workers develop a method to synthesize wafer scale, high-quality, fewlayer, hexagonal boron nitride (h-BN) films. On page 731, they use a remotely discharged plasma beam source in high vacuum. Lithographic patterning of layer-by-layer stacked h-BN and graphene films enables the fabrication of a (h-BN-G)n disk array, which can exhibit tunable plasmonic resonances in the infrared region depending on the height of the disk. Plasmonic resonance upshifts of up to 240 cm−1 are demonstrated.

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    1. Large Scale Graphene/Hexagonal Boron Nitride Heterostructure for Tunable Plasmonics (pages 731–738)

      Kai Zhang, Fung Ling Yap, Kun Li, Chang Tai Ng, Lin Jun Li and Kian Ping Loh

      Version of Record online: 1 SEP 2013 | DOI: 10.1002/adfm.201302009

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      An array of graphene/h-BN vertically stacked micrometer-sized disks is fabricated by lithography and transfer techniques, and infrared spectroscopy is used to observe the modes of tunable graphene plasmonic absorption as a function of the repeating (G/h-BN)n units in the vertical stack.

    2. Rational Assembly of Optoplasmonic Hetero-nanoparticle Arrays with Tunable Photonic–Plasmonic Resonances (pages 739–746)

      Yan Hong, Yue Qiu, Tianhong Chen and Björn M. Reinhard

      Version of Record online: 19 AUG 2013 | DOI: 10.1002/adfm.201301837

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      Photonic–plasmonic mode coupling in self-assembled optoplasmonic arrays. A template-guided self-assembly strategy for integrating metallic and dielectric nanoparticles into morphologically defined hybrid arrays is introduced. Control over the nanoparticle composition at pre-defined lattice sites provides electromagnetic materials with new functionalities and allows for a rational tuning of near- and far-field responses.

    3. Cation–Anion Interaction-Directed Molecular Design Strategy for Mechanochromic Luminescence (pages 747–753)

      Gaocan Li, Feijie Song, Di Wu, Jingbo Lan, Xingyan Liu, Jie Wu, Shuaijun Yang, Dan Xiao and Jingsong You

      Version of Record online: 3 SEP 2013 | DOI: 10.1002/adfm.201302086

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      Molecular Design: A cation–anion interaction-directed molecular design strategy for mechanochromic luminescence is proposed. On the basis of this strategy, a series of common N-heteroaromatic onium fluorophores such as imidazolium, 1,2,4-triazolium, triazolopyridinium, benzoimidazolium, γ-carbolinium, and pyridinium salts are designed and prove to have striking reversible mechanofluorochromic behaviors.

    4. Iron Oxide-Labeled Collagen Scaffolds for Non-Invasive MR Imaging in Tissue Engineering (pages 754–762)

      Marianne E. Mertens, Alina Hermann, Anne Bühren, Leon Olde-Damink, Diana Möckel, Felix Gremse, Josef Ehling, Fabian Kiessling and Twan Lammers

      Version of Record online: 28 AUG 2013 | DOI: 10.1002/adfm.201301275

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      Three-dimensional collagen-based scaffold materials are labeled with ultrasmall superparamagentic iron oxide (USPIO) nanoparticles, enabling their visualization and monitoring using magnetic resonance imaging. USPIO nanoparticles possessing different surface functionalities are incorporated either physically or chemically into the scaffolds. Labeled scaffolds are shown to be highly biocompatible and suitable for tissue engineering applications.

    5. Spider Silk Capsules as Protective Reaction Containers for Enzymes (pages 763–768)

      Claudia Blüm, Alfons Nichtl and Thomas Scheibel

      Version of Record online: 3 SEP 2013 | DOI: 10.1002/adfm.201302100

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      Capsules made of recombinant spider silk proteins are suitable as reaction containers for various encapsulates including enzymes. Since low molecular weight substances can freely diffuse through the silk membrane while high molecular weight substances are retained, a specific triggering of reactions is possible. The capsules further protect encapsulates from proteolysis.

    6. Maintaining Cytocompatibility of Biopolymers Through a Graphene Layer for Electrical Stimulation of Nerve Cells (pages 769–776)

      Peter C. Sherrell, Brianna C. Thompson, Jonathan K. Wassei, Amy A. Gelmi, Michael J. Higgins, Richard B. Kaner and Gordon G. Wallace

      Version of Record online: 8 OCT 2013 | DOI: 10.1002/adfm.201301760

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      Bilayer graphene, transferred as a layer onto biopolymers, is used as a flexible biological interface material for electrical cell stimulation. Bilayer graphene provides a conductive layer without changing the cytocompatibility of the underlying layer, allowing electrical stimulation of cells on substrates of chosen composition. The production of flexible, biocompatible electrodes is described and the differentiation of neural cells is demonstrated for the first time from a graphene-based electrode.

    7. CdS Quantum Dots Encapsulated in Chiral Nematic Mesoporous Silica: New Iridescent and Luminescent Materials (pages 777–783)

      Thanh-Dinh Nguyen, Wadood Y. Hamad and Mark J. MacLachlan

      Version of Record online: 24 OCT 2013 | DOI: 10.1002/adfm.201302521

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      Liquid crystal-templated self-assembly of water-soluble, stabilized CdS quantum dots into a lyotropic alkoxysilane/cellulose nanocrystal dispersion produced chiral nematic CdS/silica/cellulose composites. Subsequent removal of the cellulose template and other additives by controlled calcination generated freestanding iridescent, luminescent chiral nematic mesoporous silica-encapsulated CdS films. This one-pot alternative route to fabricate these new semiconducting photonic materials may prove useful in the design of sensors and optical devices.

    8. Understanding Local and Macroscopic Electron Mobilities in the Fullerene Network of Conjugated Polymer-based Solar Cells: Time-Resolved Microwave Conductivity and Theory (pages 784–792)

      Jordan C. Aguirre, Christopher Arntsen, Samuel Hernandez, Rachel Huber, Alexandre M. Nardes, Merissa Halim, Daniel Kilbride, Yves Rubin, Sarah H. Tolbert, Nikos Kopidakis, Benjamin J. Schwartz and Daniel Neuhauser

      Version of Record online: 23 SEP 2013 | DOI: 10.1002/adfm.201301757

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      The roles of local and macroscopic electron mobility in conjugated polymer/fullerene BHJ photovoltaics are examined via a combination of density functional theory, flash-photolysis time-resolved microwave conductivity, and space-charge-limit current (SCLC) mobility estimates. The local mobility of different fullerene derivatives (‘shuttlecock’ molecules) is similar, so differences in solar cell efficiency and SCLC mobilities result directly from the different propensities of these molecules to self-assemble on macroscopic length scales.

    9. Atomic-Scale Visualization of Polarization Pinning and Relaxation at Coherent BiFeO3/LaAlO3 Interfaces (pages 793–799)

      Rong Huang, Hang-Chen Ding, Wen-I Liang, Yong-Chao Gao, Xiao-Dong Tang, Qing He, Chun-Gang Duan, Ziqiang Zhu, Junhao Chu, Craig A. J. Fisher, Tsukasa Hirayama, Yuichi Ikuhara and Ying-Hao Chu

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adfm.201301470

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      Changes in lattice strain and symmetry in BiFeO3 (BFO) crystals at coherent T-BFO/LaAlO3 (LAO) and rhombohedral-BFO/LAO interfaces are imaged with atomic resolution using annular bright-field scanning transmission electron microscopy and first-principles calculations. A common pinned BFO layer and polarization relaxation at the interfaces are identified, providing insight into the ferroelectric behavior of thin films and the complex oxide heterointerfaces between them.

    10. Accelerated Iron Oxide Nanoparticle Degradation Mediated by Polyester Encapsulation within Cellular Spheroids (pages 800–807)

      Brandon Mattix, Timothy R. Olsen, Thomas Moore, Megan Casco, Dan Simionescu, Richard P. Visconti and Frank Alexis

      Version of Record online: 18 SEP 2013 | DOI: 10.1002/adfm.201301736

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      Methods to accelerate the degradation of nanomaterials within biological systems reduce their interaction and therefore limit potential adverse effects. It is shown that the degradation of iron oxide nanoparticles is accelerated by polymeric byproducts. Polymeric magnetic nanoparticles (PolyMNPs) can be safely incorporated within cellular spheroids to assemble fused tissues using magnetic force assembly.

  9. Frontispiece

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      Oleophobicity: Filefish-Inspired Surface Design for Anisotropic Underwater Oleophobicity (Adv. Funct. Mater. 6/2014) (page 808)

      Yue Cai, Ling Lin, Zhongxin Xue, Mingjie Liu, Shutao Wang and Lei Jiang

      Version of Record online: 8 FEB 2014 | DOI: 10.1002/adfm.201470036

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      Natural systems inspire the design of smart antifouling surfaces. S. T. Wang, L. Jiang, and co-workers noticed the direction-dependent underwater oleophobicity of the skin of the fish Navodon septentrionalis, resulting from its unique hook-like surface structure. On page 809, by mimicking these oriented microtextures, surfaces with remarkable anisotropic underwater oleophobicity are achieved. The anisotropy can be controlled by adjusting the hydrophilicity and oriented microtexture of the surface.

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    1. Filefish-Inspired Surface Design for Anisotropic Underwater Oleophobicity (pages 809–816)

      Yue Cai, Ling Lin, Zhongxin Xue, Mingjie Liu, Shutao Wang and Lei Jiang

      Version of Record online: 13 SEP 2013 | DOI: 10.1002/adfm.201302034

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      Unique anisotropic underwater oleopho­bicity of the skin of filefish Navodon septentrionalis is revealed, which results from its oriented hook-like spines. Inspired by this, an anisotropic underwater oleophobic surface is fabricated on an oxygen plasma-treated PDMS layer. Anisotropic microfeatures on the surfaces and hydrophilicity are proposed as two main factors in achieving anisotropic underwater oleophobicity.

    2. Polymerization-Induced Colloidal Assembly and Photonic Crystal Multilayer for Coding and Decoding (pages 817–825)

      Dongpeng Yang, Yuhang Qin, Siyun Ye and Jianping Ge

      Version of Record online: 19 AUG 2013 | DOI: 10.1002/adfm.201301590

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      Polymerization-induced colloidal assembly is developed to prepare photonic crystal films with an ultra-narrow bandgap and tunable thickness and size. As the liquid monomer becomes solid polymer, the highly concentrated particles are driven to precipitate into colloidal microcrystals. Based on this synthesis, a coding–decoding system is developed in which the film's composition and stacking sequence can be identified by its distinctive reflection spectrum.

    3. Near-Infrared Light-Encoded Orthogonally Triggered and Logical Intracellular Release Using Gold Nanocage@Smart Polymer Shell (pages 826–834)

      Peng Shi, Enguo Ju, Jinsong Ren and Xiaogang Qu

      Version of Record online: 3 SEP 2013 | DOI: 10.1002/adfm.201302145

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      An NIR light-encoded orthogonally triggered logic gate for intracellular release is presented based on a gold nanocage (AuNC)@smart polymer shell. By using defined logic operations and the tunable LSPR properties of AuNCs, a sophisticated release system can be realized. This system could provide new insights into developing NIR light-encoded, logically controlled, intracellular release systems

    4. Direct Growth of Nanocrystalline Graphene/Graphite Transparent Electrodes on Si/SiO2 for Metal-Free Schottky Junction Photodetectors (pages 835–840)

      Zengxing Zhang, Yunxian Guo, Xiaojuan Wang, Dong Li, Fengli Wang and Sishen Xie

      Version of Record online: 1 SEP 2013 | DOI: 10.1002/adfm.201301924

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      A simple low-cost approach to directly produce nanographene/graphite transparent electrodes on Si/SiO2 for Schottky junction photoelectronics is developed. The approach is based on conventional photolithography and silicon techniques with high-temperature heating to transform photoresist into nanographene/graphite hybrids. The obtained devices exhibit excellent photodetection properties.

    5. Generation of Monodisperse, Shape-Controlled Single and Hybrid Core–Shell Nanoparticles via a Simple One-Step Process (pages 841–847)

      Jong-Seon Kim, Hwan-Jin Jeon, Hae-Wook Yoo, Youn-Kyoung Baek, Kyoung Hwan Kim, Dae Woo Kim and Hee-Tae Jung

      Version of Record online: 27 AUG 2013 | DOI: 10.1002/adfm.201302494

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      A method for fabricating highly monodisperse 3D hybrid nanoparticles uses a unique top-down method based on secondary sputtering lithography. Nanostructures formed on a PEDOT sacrificial layer are transferred to an aqueous solution in a process that could successfully disperse a variety of nanoparticle shapes and hybrid nanoparticles. By this method, a fluorescent dye could be encapsulated within the fabricated hybrid nanoparticles for use in bio-sensing and drug delivery.

    6. Nitridation and Layered Assembly of Hollow TiO2 Shells for Electrochemical Energy Storage (pages 848–856)

      Geon Dae Moon, Ji Bong Joo, Michael Dahl, Heejung Jung and Yadong Yin

      Version of Record online: 19 SEP 2013 | DOI: 10.1002/adfm.201301718

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      Hollow shells of TiO2 are nitridated by annealing in NH3, assembled into a mono­layer film on water surface, and stacked layer-by-layer into electrodes for electrochemical energy storage. This approach facilitates supercapacitor cell design by simplifying the electrode structure and avoiding the use of any organic binder or carbon-based conducting materials. The increased electrical conductivity due to the formation of TiN greatly enhances the electrochemical performance.

    7. Facile Generation of L10-FePt Nanodot Arrays from a Nanopatterned Metallopolymer Blend of Iron and Platinum Homopolymers (pages 857–862)

      Qingchen Dong, Guijun Li, Cheuk-Lam Ho, Chi-Wah Leung, Philip Wing-Tat Pong, Ian Manners and Wai-Yeung Wong

      Version of Record online: 17 SEP 2013 | DOI: 10.1002/adfm.201301143

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      Rapid single-step fabrication of large-area nanodot arrays of L10-FePt nanoparticles (NPs) are achieved by employing a metallopolymer blend of individual Fe- and Pt-containing homopolymers as the precursor through nanoimprint lithography. Imaging of the nanodot pattern indicates that the patterned NPs exhibit a decent magnetic response, which suggests potential to be utilized directly in the fabrication of bit-patterned media for the next generation of magnetic recording technology.

    8. Gyroid-Structured 3D ZnO Networks Made by Atomic Layer Deposition (pages 863–872)

      Ellie Kim, Yana Vaynzof, Alessandro Sepe, Stefan Guldin, Maik Scherer, Pedro Cunha, Stephan V. Roth and Ullrich Steiner

      Version of Record online: 3 SEP 2013 | DOI: 10.1002/adfm.201302238

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      3D continuous ZnO morphologies with characteristic feature sizes on the 10 nm length scale are replicated into crystalline ZnO by atomic layer deposition (ALD). Gyroid-structured and random worm-like polymer morphologies are voided and filled by ALD to generate continuous networks of polycrystalline ZnO. A photovoltaic device based on this material shows promising performance.

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