Advanced Materials

Cover image for Vol. 27 Issue 32

Early View (Online Version of Record published before inclusion in an issue)


  1. 1 - 100
  2. 101 - 164
  1. Reviews

    1. Revealing Optical Properties of Reduced-Dimensionality Materials at Relevant Length Scales

      D. Frank Ogletree, P. James Schuck, Alexander F. Weber-Bargioni, Nicholas J. Borys, Shaul Aloni, Wei Bao, Sara Barja, Jiye Lee, Mauro Melli, Keiko Munechika, Stephan Whitelam and Sebastian Wickenburg

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201500930

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      Nano-optical characterization of 2D transition-metal dichalcogenides, 1D semiconductor nanowires, and energy-transfer in 0D quantum-dot systems is reviewed. Understanding and optimizing material properties requires characterization at the relevant length scale, which is often below the diffraction limit. Recent advances in hyperspectral and tip-scattering near-field scanning optical microscopy (NSOM), along with ultrafast NSOM and cathodoluminescence are given close attention. Advances in STM, transport, and in situ studies are highlighted.

  2. Communications

    1. Tailorable Zero-Phase Delay of Subwavelength Particles toward Miniaturized Wave Manipulation Devices

      Qian Zhao, Zongqi Xiao, Fuli Zhang, Junming Ma, Ming Qiao, Yonggang Meng, Chuwen Lan, Bo Li, Ji Zhou, Peng Zhang, Nian-Hai Shen, Thomas Koschny and Costas M. Soukoulis

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201502298

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      Adjustable zero-phase delay and equiphase control are demonstrated in single and multilayer dielectric particle arrays with high index and low loss. The polarization-independent near-zero permeability is the origin of the wave control near the first Mie magnetic resonance. The proposed design paves the way for subwavelength devices and opens up new avenues for the miniaturization and integration of THz and optical components.

    2. High-Rate Oxygen Evolution Reaction on Al-Doped LiNiO2

      Asha Gupta, William D. Chemelewski, C. Buddie Mullins and John B. Goodenough

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201502256

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      LiNi0.8Al0.2O2 with a higher Ni3+/Li+ ordering, synthesized by the solution-combustion method, gives oxygen-evolution-reaction (OER) activity in alkaline solution that is comparable to that of IrO2. This confirms that the octahedral-site NiIV/NiIII couple in an oxide is an active redox center for the OER with ­redox energy pinned at the top of the O-2p bands.

    3. Control of Mesh Size and Modulus by Kinetically Dependent Cross-Linking in Hydrogels

      Zachary K. Zander, Geng Hua, Clinton G. Wiener, Bryan D. Vogt and Matthew L. Becker

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201501822

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      Kinetically controlled cross-linking processes produce mechanically distinguishable hydrogels using identical precursor chemistry. The oxime ligation demonstrates tunable reaction kinetics with pH and buffer strength, which induce changes in the structural features of hydrogels and determine their mechanical properties. Small-angle neutron scattering and swelling studies provide an insight into how structural properties correlate with mechanical properties for this hydrogel system.

    4. A Unified Approach for Patterning via Frontal Photopolymerization

      Alessandra Vitale, Matthew G. Hennessy, Omar K. Matar and João T. Cabral

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201502607

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      A unified patterning strategy via frontal photopolymerization (FPP) that is robust to a wide range of radical photopolymerizing systems, including thiol–ene and acrylic monomers is reported. The factors governing the spatiotemporal solidification process, including front position, profile shape, and thermal effects, are investigated and modeled theoretically, resulting in the predictive FPP patterning of polymer networks with prescribed dimensions.

    5. Enhancing Quantum Dots for Bioimaging using Advanced Surface Chemistry and Advanced Optical Microscopy: Application to Silicon Quantum Dots (SiQDs)

      Xiaoyu Cheng, Elizabeth Hinde, Dylan M. Owen, Stuart B. Lowe, Peter J. Reece, Katharina Gaus and J. Justin Gooding

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201503223

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      Fluorescence lifetime imaging microscopy is successfully demonstrated in both one- and two-photon cases with surface modified, nanocrystalline silicon quantum dots in the context of bioimaging. The technique is further demonstrated in combination with Förster resonance energy transfer studies where the color of the nanoparticles is tuned by using organic dye acceptors directly conjugated onto the nanoparticle surface.

    6. Resistive Switching Behavior in Organic–Inorganic Hybrid CH3NH3PbI3−xClx Perovskite for Resistive Random Access Memory Devices

      Eun Ji Yoo, Miaoqiang Lyu, Jung-Ho Yun, Chi Jung Kang, Young Jin Choi and Lianzhou Wang

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201502889

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      The CH3NH3PbI3−xClx organic–inorganic hybrid perovskite material demonstrates remarkable resistive switching behavior, which can be applicable in resistive random access memory devices. The simply designed Au/CH3NH3PbI3−xClx/FTO structure is fabricated by a low-temperature, solution-processable method, which exhibits remarkable bipolar resistive switching and nonvolatile properties.

    7. Polymer/Perovskite Amplifying Waveguides for Active Hybrid Silicon Photonics

      Isaac Suárez, Emilio J. Juárez-Pérez, Juan Bisquert, Iván Mora-Seró and Juan P. Martínez-Pastor

      Article first published online: 31 AUG 2015 | DOI: 10.1002/adma.201503245

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      The emission properties of hybrid halide perovskites are exploited to implement a stable and very low power operation waveguide optical amplifier integrated in a silicon platform. By optimizing its design with a poly(methyl methacrylate) (PMMA) encapsulation, this novel photonic device presents a net gain of around 10 dB cm−1 and 3–4 nm linewidth with an energy threshold as low as 2 nJ pulse−1 and exhibiting no degradation after one year.

    8. You have full text access to this OnlineOpen article
      Hyperbolic Polaritonic Crystals Based on Nanostructured Nanorod Metamaterials

      Wayne Dickson, Stephen Beckett, Christina McClatchey, Antony Murphy, Daniel O'Connor, Gregory A. Wurtz, Robert Pollard and Anatoly V. Zayats

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201501325

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      Surface plasmon polaritons usually exist on a few suitable plasmonic materials; however, nanostructured plasmonic metamaterials allow a much broader range of optical properties to be designed. Here, bottom-up and top-down nanostructuring are combined, creating hyperbolic metamaterial-based photonic crystals termed hyperbolic polaritonic crystals, allowing free-space access to the high spatial frequency modes supported by these metamaterials.

    9. Monodisperse Magnesium Hydride Nanoparticles Uniformly Self-Assembled on Graphene

      Guanglin Xia, Yingbin Tan, Xiaowei Chen, Dalin Sun, Zaiping Guo, Huakun Liu, Liuzhang Ouyang, Min Zhu and Xuebin Yu

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502005

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      Monodisperse MgH2 nanoparticles with homogeneous distribution and a high loading percent are developed through hydrogenation-induced self-assembly under the structure-directing role of graphene. Graphene acts not only as a structural support, but also as a space barrier to prevent the growth of MgH2 nanoparticles and as a thermally conductive pathway, leading to outstanding performance.

    10. Electrolyte-Gated Graphene Schottky Barrier Transistors

      Beom Joon Kim, Euyheon Hwang, Moon Sung Kang and Jeong Ho Cho

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502020

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      A new device architecture for flexible vertical Schottky barrier (SB) transistors and logic gates based on graphene–organic-semiconductor–metal heterostructures and ion gel gate dielectrics are demonstrated. The devices show well-behaved p- and n-type characteristics under low-voltage operation (<1 V), yielding high current densities (>100 mA cm−2) and on/off current ratios (>103).

    11. Highly Compressible and All-Solid-State Supercapacitors Based on Nanostructured Composite Sponge

      Zhiqiang Niu, Weiya Zhou, Xiaodong Chen, Jun Chen and Sishen Xie

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502263

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      Based on polyaniline–single-walled carbon nanotubes –sponge electrodes, highly compressible all-solid-state supercapacitors are prepared with an integrated configuration using poly(vinyl alcohol) (PVA)/H2SO4 gel as the electrolyte. The unique configuration enables the resultant supercapacitors to be compressed as an integrated unit arbitrarily during 60% compressible strain. Furthermore, the performance of the resultant supercapacitors is nearly unchanged even under 60% compressible strain.

    12. Engineering the Electronic State of a Perovskite Electrocatalyst for Synergistically Enhanced Oxygen Evolution Reaction

      Yuqiao Guo, Yun Tong, Pengzuo Chen, Kun Xu, Jiyin Zhao, Yue Lin, Wangsheng Chu, Zhenmeng Peng, Changzheng Wu and Yi Xie

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502024

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      A surface hydrogen effect to modulate the pure electronic-state transition in perovskite Ca0.9Yb0.1MnO3 synergistically generates a more suitable eg electron filling status and better conductivity. This achieves 100 times higher catalytic activity compared to that of a pristine sample.

    13. Hybrid Electrolytes with Controlled Network Structures for Lithium Metal Batteries

      Qiwei Pan, Derrick M. Smith, Hao Qi, Shijun Wang and Christopher Y. Li

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502059

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      Solid polymer electrolytes (SPEs) with tunable network structures are prepared by a facile one-pot reaction of polyhedral oligomeric silsesquioxane and poly(ethylene glycol). These SPEs, with high conductivity and high modulus, exhibit superior resistance to lithium dendrite growth even at high current densities. Measurements of lithium metal batteries with a LiFePO4 cathode show excellent cycling stability and rate capability.

    14. Multilevel Conductance Switching of a Memory Device Induced by Enhanced Intermolecular Charge Transfer

      Qian-Feng Gu, Jing-Hui He, Dong-Yun Chen, Hui-Long Dong, You-Yong Li, Hua Li, Qing-Feng Xu and Jian-Mei Lu

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502274

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      The modification of the terminal electron-donating groups induces a critical change in molecular aggregation and the intermolecular charge-transfer effect of the symmetric D–A1–A2–A1–D molecules that correlate with an addressable variation of memory performance from binary to ternary.

    15. A Nitrogen and Sulfur Dual-Doped Carbon Derived from Polyrhodanine@Cellulose for Advanced Lithium–Sulfur Batteries

      Quan Pang, Juntao Tang, He Huang, Xiao Liang, Connor Hart, Kam C Tam and Linda F. Nazar

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502467

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      A sulfur electrode exhibiting strong polysulfide chemisorption using a porous N, S dual-doped carbon is reported. The synergistic functionalization from the N and S heteroatoms dramatically modifies the electron density distribution and leads to much stronger polysulfide binding. X-ray photoelectron spectroscopy studies combined with ab initio calculations reveal strong Li+–N and Sn2−–S interactions. The sulfur electrodes exhibit an ultralow capacity fading of 0.052% per cycle over 1100 cycles.

    16. Assessing Structural Correlations and Heterogeneity Length Scales in Functional Porous Polymers from Physical Reconstructions

      Tibor Müllner, Armin Zankel, Yongqin Lv, Frantisek Svec, Alexandra Höltzel and Ulrich Tallarek

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502332

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      A general, model-free, quantitative approach to the key morphological properties of a porous polymer monolith is presented. After 3D reconstruction, image-based analysis delivers detailed spatial and spatially correlated information on the structural heterogeneities in the void space and the polymer skeleton. Identified heterogeneities, which limit the monolith's performance in targeted applications, are traced back to the preparation process.

    17. Snapping Mechanical Metamaterials under Tension

      Ahmad Rafsanjani, Abdolhamid Akbarzadeh and Damiano Pasini

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502809

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      A snapping mechanical metamaterial is designed, which exhibits a sequential snap-through behavior under tension. The tensile response of this mechanical metamaterial can be altered by tuning the architecture of the snapping segments to achieve a range of nonlinear mechanical responses, including monotonic, S-shaped, plateau, and non-monotonic snap-through behavior.

    18. Ultra-Low Voltage and Ultra-Low Power Consumption Nonvolatile Operation of a Three-Terminal Atomic Switch

      Qi Wang, Yaomi Itoh, Tohru Tsuruoka, Masakazu Aono and Tsuyoshi Hasegawa

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502678

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      Nonvolatile three-terminal operation, with a very small range of bias sweeping (−80 to 250 mV), a high on/off ratio of up to six orders of magnitude, and a very small gate leakage current (<1 pA) is demonstrated using an Ag (gate)/Ta2O5 (ionic transfer layer)/Pt (source), Pt (drain) three-terminal atomic switch structure.

    19. Single Cell Nanobiosensors for Dynamic Gene Expression Profiling in Native Tissue Microenvironments

      Shue Wang, Reza Riahi, Na Li, Donna D. Zhang and Pak Kin Wong

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502814

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      A gold nanorod-locked nucleic acid nano­biosensor for dynamic single cell gene expression analysis in living cells and tissues is developed. The nanoparticle facilitates endocytic delivery and dynamic monitoring of the gene expression in human umbilical cord endothelial cells, mouse skin tissues, mouse retina tissues, and mouse cornea tissues at the single cell level.

    20. An Optical Nanoruler Based on a Conjugated Polymer−Silver Nanoprism Pair for Label-Free Protein Detection

      Xiaoyu Wang, Shengliang Li, Pengbo Zhang, Fengting Lv, Libing Liu, Lidong Li and Shu Wang

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201502880

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      An optical nanoruler system based on a conjugated polyelectrolyte−silver nanoprism pair is developed for label-free protein detection by taking advantage of the metal-enhanced fluorescence effect of silver nanostructures. The antibody–antigen interactions induce the change in metal–fluorophore distance, followed by the response of a fluorescent signal of conjugated polyelectrolyte. The system is used to detect target antigens sensitively and selectively.

    21. Manipulating Aggregation and Molecular Orientation in All-Polymer Photovoltaic Cells

      Long Ye, Xuechen Jiao, Meng Zhou, Shaoqing Zhang, Huifeng Yao, Wenchao Zhao, Andong Xia, Harald Ade and Jianhui Hou

      Article first published online: 28 AUG 2015 | DOI: 10.1002/adma.201503218

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      Manipulating molecular orientation at the donor/acceptor interface is the key to boosting charge separation properties and efficiencies of anisotropic materials-based organic photovoltaics (OPVs). By replacing the polymeric donor PBDTBDD with its 2D-conjugated polymer PBDTBDD-T, the power conversion efficiency of OPV featuring the anisotropic polymer acceptor PNDI is drastically boosted from 2.4% up to 5.8%.

    22. Highly Robust Transparent and Conductive Gas Diffusion Barriers Based on Tin Oxide

      Andreas Behrendt, Christian Friedenberger, Tobias Gahlmann, Sara Trost, Tim Becker, Kirill Zilberberg, Andreas Polywka, Patrick Görrn and Thomas Riedl

      Article first published online: 27 AUG 2015 | DOI: 10.1002/adma.201502973

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      Transparent and electrically conductive gas diffusion barriers are reported. Tin oxide (SnOx) thin films grown by atomic layer deposition afford extremely low water vapor transmission rates (WVTR) on the order of 10−6 g (m2 day)−1, six orders of magnitude better than that established with ITO layers. The electrical conductivity of SnOx remains high under damp heat conditions (85 °C/85% relative humidity (RH)), while that of ZnO quickly degrades by more than five orders of magnitude.

    23. Graphene/Sulfur Hybrid Nanosheets from a Space-Confined “Sauna” Reaction for High-Performance Lithium–Sulfur Batteries

      Linfeng Fei, Xiaogang Li, Wentuan Bi, Zhiwen Zhuo, Wenfei Wei, Li Sun, Wei Lu, Xiaojun Wu, Keyu Xie, Changzheng Wu, Helen L. W. Chan and Yu Wang

      Article first published online: 27 AUG 2015 | DOI: 10.1002/adma.201502668

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      A space-confined “sauna” reaction system is introduced for the simultaneous reduction and functionalization of graphene oxide to unique graphene–sulfur hybrid nanosheets, in which thin layers of amorphous sulfur are tightly anchored on graphene sheet via strong chemical bonding. Upon being used as the cathode material in lithium–sulfur batteries, the as-synthesized composite shows an excellent electrochemical performance.

    24. Optical Anisotropy and Strong H-Aggregation of Poly(3-Alkylthiophene) in a Surface Monolayer

      Fanji Wang, Kazuhito Hashimoto and Keisuke Tajima

      Article first published online: 27 AUG 2015 | DOI: 10.1002/adma.201502339

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      Slab optical waveguide absorption spectra reveal that surface segregated monolayers of a vertically oriented poly(3-buthylthiophene) derivative have large optical anisotropy, and confinement of the polymer chains in the isolated monolayer causes strong H-aggregation.

    25. Interface Engineering for Ternary Blend Polymer Solar Cells with a Heterostructured Near-IR Dye

      Huajun Xu, Hideo Ohkita, Yasunari Tamai, Hiroaki Benten and Shinzaburo Ito

      Article first published online: 27 AUG 2015 | DOI: 10.1002/adma.201502773

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      Ternary blend polymer solar cells can be effectively improved by incorporating a heterostructured near-IR dye, which has a hexyl group compatible with the polymer and a benzyl group compatible with the fullerene. Because of the compatibility with both materials, the heterostructured dye can be loaded up to 15 wt% and hence can boost the photocurrent generation by 30%.

    26. Multichannel-Improved Charge-Carrier Dynamics in Well-Designed Hetero-nanostructural Plasmonic Photocatalysts toward Highly Efficient Solar-to-Fuels Conversion

      Zhenyi Zhang, Yingzhou Huang, Kuichao Liu, Lijiao Guo, Qing Yuan and Bin Dong

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201502203

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      The charge-carrier dynamics process in well-designed hetero-nanostructural plasmonic photocatalysts is greatly improved through a multichannel sensitization effect, which therefore results in a significant enhancement of the efficiencies of solar-to-fuels conversion.

    27. Design Strategy for 25% External Quantum Efficiency in Green and Blue Thermally Activated Delayed Fluorescent Devices

      Dong Ryun Lee, Mounggon Kim, Sang Kyu Jeon, Seok-Ho Hwang, Chil Won Lee and Jun Yeob Lee

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201502053

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      Carbazole- and triazine-derived thermally activated delayed fluorescent (TADF) emitters, with three donor units and an even distribution of the highest occupied molecular orbital, achieve high external quantum efficiencies of above 25% in blue and green TADF devices.

    28. Dye Monolayers Used as the Hole Transporting Medium in Dye-Sensitized Solar Cells

      Davide Moia, Tomas Leijtens, Nakita Noel, Henry J. Snaith, Jenny Nelson and Piers R. F. Barnes

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201501919

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      Dye-sensitized TiO2 can be used as the active layer of solar cell devices without an additional hole transporting material. In this architecture holes are transported through the dye monolayer.

    29. Green Processing of Metal Oxide Core–Shell Nanoparticles as Low-Temperature Dielectrics in Organic Thin-Film Transistors

      Luis Portilla, Sebastian H. Etschel, Rik R. Tykwinski and Marcus Halik

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201502792

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      TiO2, Fe3O4, AlOx, ITO (indium tin oxide), and CeO2 nanoparticles are tailored to exhibit excellent dispersability in deionized water and alcohols. The latter provides an ecofriendly solution for processing metal oxide nanoparticles at a neutral pH. Water processed dielectrics from the metal oxide nanoparticles are incorporated into organic thin-film transistors fabricated on rigid and flexible substrates.

    30. Single-Crystal-Conjugated Polymers with Extremely High Electron Sensitivity through Template-Assisted In Situ Polymerization

      Mianqi Xue, Yue Wang, Xiaowei Wang, Xiaochun Huang and Junhui Ji

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201502511

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      Single-crystal-conjugated polymer (SCCP) arrays are prepared successfully via a simple method, which is a combination of the contact thermochemical reaction and solvent-free in situ polymerization. The dramatic X-ray diffraction and selective-area electron diffraction results show the high crystallinity of the SCCP arrays. These SCCP arrays display unique physical properties and show great potential in flexible electronics.

    31. Disposable Plasmonics: Plastic Templated Plasmonic Metamaterials with Tunable Chirality

      Affar S. Karimullah, Calum Jack, Ryan Tullius, Vincent M. Rotello, Graeme Cooke, Nikolaj Gadegaard, Laurence D. Barron and Malcolm Kadodwala

      Article first published online: 26 AUG 2015 | DOI: 10.1002/adma.201501816

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      Development of low-cost disposable plasmonic substrates is vital for the applicability of plasmonic sensing. Such devices can be made using injection-molded templates to create plasmonic films. The elements of these plasmonic films are hybrid nanostructures composed of inverse and solid structures. Tuning the modal coupling between the two allows optimization of the optical properties for nanophotonic applications.

  3. Reviews

    1. Structural Design Elements in Biological Materials: Application to Bioinspiration

      Steven E. Naleway, Michael M. Porter, Joanna McKittrick and Marc A. Meyers

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502403

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      A new paradigm in the field of biological materials science is proposed. Eight structural design elements are identified that serve as a toolbox for the rationalization of the complex mechanical behavior of structural biological materials and for systematizing the development of bioinspired designs for structural applications. These structures are: fibrous, helical, gradient, layered, tubular, cellular, suture, and overlapping.

  4. Communications

    1. Site-Selective Trimetallic Heterogeneous Nanostructures for Enhanced Electrocatalytic Performance

      Xiaobin Xie, Guanhui Gao, Shendong Kang, Tamaki Shibayama, Yanhua Lei, Duyang Gao and Lintao Cai

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201501133

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      Trimetallic Au/Ag/Pt hetero-nanostructures (AAPHNs) with distinctive, designed morphology are synthesized by galvanic replacement reaction and a site-selective strategy. The three metals present on the surface are shown to act synergistically to enhance the electro-catalytic performance and durability for methanol oxidation. The described structural modification of the nanocomposites increases the range of potential applications to include both the oxygen reduction reaction in fuel cells and photocatalysis of the hydrogen evolution reaction.

    2. Enzyme-Responsive Nanoparticles for Targeted Accumulation and Prolonged Retention in Heart Tissue after Myocardial Infarction

      Mary M. Nguyen, Andrea S. Carlini, Miao-Ping Chien, Sonya Sonnenberg, Colin Luo, Rebecca L. Braden, Kent G. Osborn, Yiwen Li, Nathan C. Gianneschi and Karen L. Christman

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502003

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      A method for targeting to and retaining intravenously injected nanoparticles at the site of acute myocardial infarction in a rat model is described. Enzyme-responsive peptide–polymer amphiphiles are assembled as spherical micellar nanoparticles, and undergo a morphological transition from spherical-shaped, discrete materials to network-like assemblies when acted upon by matrix metalloproteinases (MMP-2 and MMP-9), which are up-regulated in heart tissue post-myocardial infarction.

    3. Layer-by-Layer-Assembled Healable Antifouling Films

      Dongdong Chen, Mingda Wu, Bochao Li, Kefeng Ren, Zhongkai Cheng, Jian Ji, Yang Li and Junqi Sun

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201501726

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      Healable antifouling films are fabricated by the exponential layer-by-layer assembly of PEGylated branched poly(ethylenimine) and hyaluronic acid followed by post crosslinking. The antifouling function originates from the grafted PEG and the extremely soft nature of the films. The rapid and multiple healing of damaged antifouling functions caused by cuts and scratches can be readily achieved by immersing the films in normal saline solution.

    4. Enhancing the Thermal Stability of Solution-Processed Small-Molecule Semiconductor Thin Films Using a Flexible Linker Approach

      Andrea Gasperini, Xavier A. Jeanbourquin, Aiman Rahmanudin, Xiaoyun Yu and Kevin Sivula

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201501826

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      Using flexible aliphatic chains to link conjugated molecular semiconductors affords a polymeric material that possesses defined conjugated segments but extended covalent connectivity that enhances crystallinity and thermal stability in field-effect transistors and bulk heterojunction solar-cell devices when used as an additive.

    5. A Hierarchical Particle–Shell Architecture for Long-Term Cycle Stability of Li2S Cathodes

      Feixiang Wu, Jung Tae Lee, Feifei Fan, Naoki Nitta, Hyea Kim, Ting Zhu and Gleb Yushin

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502289

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      A hierarchical particle–shell architecture for long-term cycle stability of Li2S cathodes is described. Multiscale and multilevel protection prevents mechanical degradation and polysulfide dissolution in lithium–sulfur battery chemistries.

    6. Hierarchical Carbon Framework Wrapped Na3V2(PO4)3 as a Superior High-Rate and Extended Lifespan Cathode for Sodium-Ion Batteries

      Yongjin Fang, Lifen Xiao, Xinping Ai, Yuliang Cao and Hanxi Yang

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502018

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      Hierarchical carbon framework wrapped Na3V2(PO4)3 (HCF-NVP) is successfully synthesized through chemical vapor deposition on pure Na3V2(PO4)3 particles. Electrochemical experiments show that the HCF-NVP electrode can deliver a large reversible capacity (115 mA h g−1 at 0.2 C), superior high-rate rate capability (38 mA h g−1 at 500 C), and ultra-long cycling stability (54% capacity retention after 20 000 cycles).

    7. A New Tubular Graphene Form of a Tetrahedrally Connected Cellular Structure

      Hui Bi, I-Wei Chen, Tianquan Lin and Fuqiang Huang

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502682

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      3D architectures constructed from a tubular graphene network can withstand repeated >95% compression cycling without damage. Aided by intertubular covalent bonding, this material takes full advantage of the graphene tube's unique attributes, including complete pre- and post-buckling elasticity, outstanding electrical conductivity, and extraordinary physicochemical stability. A highly connected tubular graphene will thus be the ultimate, structurally robust, ultrastrong, ultralight material.

    8. Microscopic Mechanism of Doping-Induced Kinetically Constrained Crystallization in Phase-Change Materials

      Tae Hoon Lee, Desmond Loke and Stephen R. Elliott

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502295

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      A comprehensive microscopic mechanism of doping-induced kinetically constrained crystallization in phase-change materials is provided by investigating structural and dynamical dopant characteristics via ab initio molecular dynamics simulations. The information gained from this study may provide a basis for a fast screening of dopant species for electronic memory devices, or for understanding the general physics involved in the crystallization of doped glasses.

    9. A Low Cost, High Energy Density, and Long Cycle Life Potassium–Sulfur Battery for Grid-Scale Energy Storage

      Xiaochuan Lu, Mark E. Bowden, Vincent L. Sprenkle and Jun Liu

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502343

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      A potassium–sulfur battery using K+-conducting beta-alumina as the electrolyte to separate a molten potassium metal anode and a sulfur cathode is presented. Results indicate that the battery can operate at as low as 150 °C with excellent performance. This study demonstrates a new type of high-performance metal-sulfur battery that is ideal for grid-scale energy storage applications.

    10. Atomically Flat Ultrathin Cobalt Ferrite Islands

      Laura Martín-García, Adrián Quesada, Carmen Munuera, Jose F. Fernández, Mar García-Hernández, Michael Foerster, Lucía Aballe and Juan de la Figuera

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502799

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      A route for fabricating structurally perfect cobalt ferrite magnetic nanostructures is demonstrated. Ultrathin islands of up to 100 μm2 with atomically flat surfaces and free from antiphase boundaries are developed. The extremely low defect concentration leads to a robust magnetic order, even for thicknesses below 1 nm, and exceptionally large magnetic domains. This approach allows the evaluation of the influence of specific extrinsic effects on domain wall pinning.

    11. Flexible High-Energy Polymer-Electrolyte-Based Rechargeable Zinc–Air Batteries

      Jing Fu, Dong Un Lee, Fathy Mohamed Hassan, Lin Yang, Zhengyu Bai, Moon Gyu Park and Zhongwei Chen

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502853

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      A thin-film, flexible, and rechargeable zinc–air battery having high energy density is reported particularly for emerging portable and wearable electronic applications. This freeform battery design is the first demonstrated by sandwiching a porous-gelled polymer electrolyte with a freestanding zinc film and a bifunctional catalytic electrode film. The flexibility of both the electrode films and polymer electrolyte membrane gives great freedom in tailoring the battery geometry and performance.

    12. Freestanding Artificial Synapses Based on Laterally Proton-Coupled Transistors on Chitosan Membranes

      Yang Hui Liu, Li Qiang Zhu, Ping Feng, Yi Shi and Qing Wan

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502719

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      Freestanding synaptic transistors are fabricated on solution-processed chitosan membranes. A short-term memory to long-term memory transition is observed due to proton-related electrochemical doping under repeated pulse stimulus. Moreover, freestanding artificial synaptic devices with multiple presynaptic inputs are investigated, and spiking logic operation and logic modulation are realized.

    13. A Highly Photoreflective and Heat-Insulating Alumina Film Composed of Stacked Mesoporous Layers in Hierarchical Structure

      Tetsuya Kodaira, Yo-hei Suzuki, Naofumi Nagai, Gozo Matsuda and Fujio Mizukami

      Article first published online: 25 AUG 2015 | DOI: 10.1002/adma.201502064

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      An alumina film with highly photoreflective and heat-insulating properties can be simply synthesized using a sol of fibrous boehmite with an additive. The entangled fibers bring about mesopores among them and form stacked 2D nonwoven-like nanosheets. The porosity and the layered structure of alumina accompanying the heat resistivity provide the upper properties that are usually difficult to realize simultaneously.

    14. Facile Synthesis of Single Crystal Vanadium Disulfide Nanosheets by Chemical Vapor Deposition for Efficient Hydrogen Evolution Reaction

      Jiangtan Yuan, Jingjie Wu, Will J. Hardy, Philip Loya, Minhan Lou, Yingchao Yang, Sina Najmaei, Menglei Jiang, Fan Qin, Kunttal Keyshar, Heng Ji, Weilu Gao, Jiming Bao, Junichiro Kono, Douglas Natelson, Pulickel M. Ajayan and Jun Lou

      Article first published online: 21 AUG 2015 | DOI: 10.1002/adma.201502075

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      A facile chemical vapor deposition method to prepare single crystalline VS2 nanosheets for hydrogen evolution reaction is reported. The electrocatalytic hydrogen evolution reaction (HER) activities of VS2 show an extremely low overpotential of −68 mV at 10 mA cm−2, small Tafel slopes of ≈34 mV decade−1, as well as high stability, demonstrating its potential as a candidate non-noble metal catalyst for HER.

    15. A Van Der Waals Homojunction: Ideal p–n Diode Behavior in MoSe2

      Youngjo Jin, Dong Hoon Keum, Sung-Jin An, Joonggyu Kim, Hyun Seok Lee and Young Hee Lee

      Article first published online: 21 AUG 2015 | DOI: 10.1002/adma.201502278

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      A MoSe2 p–n diode with a van der Waals homojunction is demonstrated by stacking undoped (n-type) and Nb-doped (p-type) semiconducting MoSe2 synthesized by chemical vapor transport for Nb substitutional doping. The p–n diode reveals an ideality factor of ≈1.0 and a high external quantum efficiency (≈52%), which increases in response to light intensity due to the negligible recombination rate at the clean homojunction interface.

    16. Self-Protection of Electrochemical Storage Devices via a Thermal Reversible Sol–Gel Transition

      Hui Yang, Zhiyuan Liu, Bevita K. Chandran, Jiyang Deng, Jiancan Yu, Dianpeng Qi, Wenlong Li, Yuxin Tang, Chenguang Zhang and Xiaodong Chen

      Article first published online: 21 AUG 2015 | DOI: 10.1002/adma.201502484

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      Thermal self-protected intelligent electrochemical storage devices are fabricated using a reversible sol–gel transition of the electrolyte, which can decrease the specific capacitance and increase and enable temperature-dependent charging and discharging rates in the device. This work represents proof of a simple and useful concept, which shows tremendous promise for the safe and controlled power delivery in electrochemical devices.

  5. Reviews

    1. Graphene-Based Materials for Lithium-Ion Hybrid Supercapacitors

      Yanfeng Ma, Huicong Chang, Miao Zhang and Yongsheng Chen

      Article first published online: 21 AUG 2015 | DOI: 10.1002/adma.201501622

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      Lithium-ion hybrid supercapacitors (LIHSs) attract much attention due to the combination of the rapid charge–discharge and long cycle life of supercapacitors and the high energy-storage capacity of lithium-ion batteries. The latest advances in electrode materials based on graphene (including 3D graphene) for LIHSs applications are summarized, and an outlook to highlight some future directions is presented.

  6. Communications

    1. Topology Optimized Architectures with Programmable Poisson's Ratio over Large Deformations

      Anders Clausen, Fengwen Wang, Jakob S. Jensen, Ole Sigmund and Jennifer A. Lewis

      Article first published online: 20 AUG 2015 | DOI: 10.1002/adma.201502485

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      Topology optimized architectures are designed and printed with programmable Poisson's ratios ranging from −0.8 to 0.8 over large deformations of 20% or more.

    2. Control of Skin Potential by Triboelectrification with Ferroelectric Polymers

      Ju-Hyuck Lee, Ronan Hinchet, Tae Yun Kim, Hanjun Ryu, Wanchul Seung, Hong-Joon Yoon and Sang-Woo Kim

      Article first published online: 20 AUG 2015 | DOI: 10.1002/adma.201502463

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      Negatively polarized ferroelectric polymer β-P(VDF-TrFE) shows higher positive triboelectric properties than skin, which could lead to new medical applications. Kelvin force microscope measurements and triboelectric nanogenerator characterizations are performed to demonstrate this new property. In addition, how many negative charges are exchanged by contact electrification between the negatively polarized β-P(VDF-TrFE) and the skin is estimated.

    3. Suspended Wavy Graphene Microribbons for Highly Stretchable Microsupercapacitors

      Dianpeng Qi, Zhiyuan Liu, Yan Liu, Wan Ru Leow, Bowen Zhu, Hui Yang, Jiancan Yu, Wei Wang, Hua Wang, Shengyan Yin and Xiaodong Chen

      Article first published online: 20 AUG 2015 | DOI: 10.1002/adma.201502549

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      Highly stretchable microsupercapacitors with stable electrochemical performance are fabricated. Their excellent stretchable and electrochemical performance relies on the suspended wavy structures of graphene microribbons. This avoids the detachment and cracks of the electrode materials. In addition, it ensures the electrode fingers keep a relatively constant distance so the stability of the microsupercapacitors can be enhanced.

  7. Reviews

    1. Tungsten Oxides for Photocatalysis, Electrochemistry, and Phototherapy

      Zhen-Feng Huang, Jiajia Song, Lun Pan, Xiangwen Zhang, Li Wang and Ji-Jun Zou

      Article first published online: 19 AUG 2015 | DOI: 10.1002/adma.201501217

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      Recent breakthroughs on structure control and modification of the WOx≤3 family for energy-related applications are summarized, including for solar-light-driven water splitting, CO2 reduction, pollutant removal, electrochromism, supercapacitors, lithium batteries, solar and fuel cells, non-volatile memory devices, gas sensors, and cancer therapy, from the aspects of function-oriented structure design and control.

  8. Communications

    1. A New Type of Low Density Material: Shellular

      Seung Chul Han, Jeong Woo Lee and Kiju Kang

      Article first published online: 19 AUG 2015 | DOI: 10.1002/adma.201501546

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      A new type of cellular material named Shellular, in which cells are composed of a continuous, smooth-curved shell according to the minimal surface theory, is proposed. Shellular specimens are fabricated using 3D lithography with negative templates and hard coating, and exhibit superb strength and stiffness at densities lower than 10−2 Mg m−3, incorporating benefits from hierarchical structures and constituent materials with nanosized grains.

    2. A New Cubic Phase for a NaYF4 Host Matrix Offering High Upconversion Luminescence Efficiency

      Limin Wang, Xiyu Li, Zhengquan Li, Wangsheng Chu, Renfu Li, Ke Lin, Haisheng Qian, Yao Wang, Changfeng Wu, Jiong Li, Datao Tu, Qun Zhang, Li Song, Jun Jiang, Xueyuan Chen, Yi Luo, Yi Xie and Yujie Xiong

      Article first published online: 19 AUG 2015 | DOI: 10.1002/adma.201502748

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      A NaYF4 host matrix with a new cubic phase is fabricated to offer high upconversion luminescence efficiency. The new cubic phase is formed through a hexagonal-to-cubic phase transition by shining intense near-infrared light on lanthanide-doped hexagonal NaYF4 materials.

    3. High Charge-Carrier Mobility of 2.5 cm2 V−1 s−1 from a Water-Borne Colloid of a Polymeric Semiconductor via Smart Surfactant Engineering

      Jangwhan Cho, Kwang Hee Cheon, Hyungju Ahn, Kwang Hun Park, Soon-Ki Kwon, Yun-Hi Kim and Dae Sung Chung

      Article first published online: 19 AUG 2015 | DOI: 10.1002/adma.201503122

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      Semiconducting polymer nanoparticles dispersed in water are synthesized by a novel method utilizing non-ionic surfactants. By developing a smart surfactant engineering technique involving a selective post-removal process of surfactants, an unprecedentedly high mobility of 2.51 cm2 V−1 s−1 from a water-borne colloid is demonstrated for the first time.

    4. Rapid 3D Extrusion of Synthetic Tumor Microenvironments

      Joshua M. Grolman, Douglas Zhang, Andrew M. Smith, Jeffrey S. Moore and Kristopher A. Kilian

      Article first published online: 18 AUG 2015 | DOI: 10.1002/adma.201501729

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      The spatial positioning of 3D tumor-mimetic microenvironments, containing multiple cell types, is controlled with a simple concentric flow device in a single step. A range of geometric architectures are demonstrated, and the migration of segregated tumor cells and macrophages is explored using drugs that inhibit heterotypic interactions.

  9. Research News

    1. Fabrication of Nanocarbon Composites Using In Situ Chemical Vapor Deposition and Their Applications

      Chunnian He, Naiqin Zhao, Chunsheng Shi, Enzuo Liu and Jiajun Li

      Article first published online: 18 AUG 2015 | DOI: 10.1002/adma.201501493

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      The in situ chemical vapor deposition (CVD) strategy is a well-known, versatile and powerful tool for directly preparing advanced nanocarbon composites with controllable morphologies, dispersion, and interfaces. The recent progress regarding in situ CVD to construct nano­carbon composites, specifically, carbon-nanotube (CNT)-reinforced bulk structural composites, as well as CNT, graphene (GN), and CNT/GN functional composites, together with their practical and potential applications, are discussed.

  10. Communications

    1. High-Pressure Synthesis of Boron-Doped Ultrasmall Diamonds from an Organic Compound

      Evgeny A. Ekimov, Oleg S. Kudryavtsev, Andrey A. Khomich, Oleg I. Lebedev, Tatiana A. Dolenko and Igor I. Vlasov

      Article first published online: 18 AUG 2015 | DOI: 10.1002/adma.201502672

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      The first application of the high pressure–high temperature (HPHT) technique for direct production of doped ultrasmall diamonds starting from a one-component organic precursor is reported. Heavily boron-doped diamond nanoparticles with a size below 10 nm are produced by HPHT treatment of 9-borabicyclo [3,3,1]nonane dimer molecules.

  11. Reviews

    1. Recent Advances and Prospects of Cathode Materials for Sodium-Ion Batteries

      Xingde Xiang, Kai Zhang and Jun Chen

      Article first published online: 14 AUG 2015 | DOI: 10.1002/adma.201501527

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      Various inorganic and organic compounds are being studied as cathode materials of sodium-ion batteries (SIBs), which mainly cover transition-metal oxides, polyanionic compounds, metal hexacyanometalates, aromatic carbonyl compounds, pteridine derivatives, and functional polymers. Currently, layered transition-metal oxides are most promising for application in SIBs owing to their high specific energies and the large space of promoting cycling life and rate capability.

  12. Progress Reports

    1. Peptide-Modulated Self-Assembly of Chromophores toward Biomimetic Light-Harvesting Nanoarchitectonics

      Qianli Zou, Kai Liu, Manzar Abbas and Xuehai Yan

      Article first published online: 14 AUG 2015 | DOI: 10.1002/adma.201502454

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      Self-assembling nanoarchitectonics of synthetic peptides and chromophores show great promise in mimicking natural light-harvesting complexes. Recent advances in the construction and application of artificial light-harvesting systems based on peptide-modulated self-assembly of chromophores are highlighted, especially the systems comprising small peptides.

    2. Advanced Graphene-Based Binder-Free Electrodes for High-Performance Energy Storage

      Junyi Ji, Yang Li, Wenchao Peng, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201501115

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      Advanced graphene-based binder-free electrodes with high energy-storage performance are reviewed with regard to recent progress in their research and development, providing a fundamental outline of the design and preparation of binder-free electrodes. Guidance for the design of next-generation energy-storage electrodes is provided. The challenges and perspectives of the field of graphene-based binder-free electrodes are also discussed.

  13. Research News

    1. Construction and Functions of Cyclodextrin-Based 1D Supramolecular Strands and their Secondary Assemblies

      Yong Chen and Yu Liu

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201501216

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      The construction and functions of 1D supramolecular strands from cyclic oligo­saccharides, namely cyclodextrins, as building blocks and other organic/inorganic/polymeric molecules as templates are summarized. Significantly, their properties can be further improved through secondary assembly.

  14. Progress Reports

    1. Nanostructured Ion-Exchange Membranes for Fuel Cells: Recent Advances and Perspectives

      Guangwei He, Zhen Li, Jing Zhao, Shaofei Wang, Hong Wu, Michael D. Guiver and Zhongyi Jiang

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201501406

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      Polymer-based materials with tunable ion nanochannels hold great promise as next-generation ion-exchange membranes (IEMs) for acid or alkaline fuel cells. Using the physical and chemical micro­environments of ion nanochannels as the central pivots, an overview of nano­structured IEMs is presented, targeting at elucidating the relationships between nanostructures, microenvironments, and ion-transport properties.

  15. Communications

    1. Nanotheranostics: Congo Red/Rutin-MNPs with Enhanced Magnetic Resonance Imaging and H2O2-Responsive Therapy of Alzheimer's Disease in APPswe/PS1dE9 Transgenic Mice

      Bingbing Hu, Fengying Dai, Zhanming Fan, Guanghui Ma, Qunwei Tang and Xin Zhang

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201502227

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      As nanotheranostics , Congo red/Rutin-MNPs combine the abilities of diagnosis and treatment of Alzheimer's disease (AD). The biocompatible nanotheranostics system based on iron oxide magnetic nanoparticles, with ultrasmall size and excellent magnetic properties, can specifically detect amyloid plaques by magnetic resonance imaging, realize targeted delivery of AD therapeutic agents, achieve drug controlled release by H2O2 response, and prevent oxidative stress.

  16. Research News

    1. Flexible Metal–Organic Frameworks: Recent Advances and Potential Applications

      Ze Chang, Dong-Hui Yang, Jian Xu, Tong-Liang Hu and Xian-He Bu

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201501523

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      Flexible metal–organic frameworks are widely investigated as functional materials based on their remarkable properties, and potential applications of these materials are found in many fields. The most recent advances in the discovery, understanding and property investigations are reviewed, and new trends for their applications are highlighted.

  17. Communications

    1. Bioinspired Hybrid White Light-Emitting Diodes

      Michael D. Weber, Lukas Niklaus, Marlene Pröschel, Pedro B. Coto, Uwe Sonnewald and Rubén D. Costa

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201502349

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      The first bioinspired hybrid white light-emitting diodes (bio-HLEDs) featuring protein cascade coatings are presented. For easy fabrication a new strategy to stabilize proteins in rubber-like material was developed. The synergy between the excellent features of fluorescent proteins and the easily processed rubber produces bio-HLEDs with less than 10% loss in luminous efficiency over 100 hours.

    2. Black Phosphorus Terahertz Photodetectors

      Leonardo Viti, Jin Hu, Dominique Coquillat, Wojciech Knap, Alessandro Tredicucci, Antonio Politano and Miriam Serena Vitiello

      Article first published online: 13 AUG 2015 | DOI: 10.1002/adma.201502052

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      The first room-temperature terahertz (THz)-frequency nanodetector exploiting a 10 nm thick flake of exfoliated crystalline black phosphorus as an active channel of a field-effect transistor, is devised. By engineering and embedding planar THz antennas for efficient light harvesting, the authors provide the first technological demonstration of a phosphorus-based active THz device.

  18. Reviews

    1. Mechanistic Understanding of the Plasmonic Enhancement for Solar Water Splitting

      Peng Zhang, Tuo Wang and Jinlong Gong

      Article first published online: 12 AUG 2015 | DOI: 10.1002/adma.201500888

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      The plasmonic enhancement for solar water splitting and the enhancement mechanisms are reviewed in three aspects including: i) light absorption and scattering; ii) hot-electron injection, and iii) plasmon-induced resonance energy transfer (PIRET). Perspectives are also proposed to trigger further innovative thinking on plasmonic-enhanced solar water splitting.

  19. Communications

    1. Artificial Protection Film on Lithium Metal Anode toward Long-Cycle-Life Lithium–Oxygen Batteries

      Qing-Chao Liu, Ji-Jing Xu, Shuang Yuan, Zhi-Wen Chang, Dan Xu, Yan-Bin Yin, Lin Li, Hai-Xia Zhong, Yin-Shan Jiang, Jun-Min Yan and Xin-Bo Zhang

      Article first published online: 12 AUG 2015 | DOI: 10.1002/adma.201501490

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      An artificial while very stable solid electrolyte interphase film is formed on the lithium metal using an electrochemical strategy. When this protected Li anode is first used in a Li–O2 battery, the film formed on the anode can effectively suppress the parasitic reactions on the Li anode/electrolyte interface and significantly enhance the cycling stability of Li–O2 battery.

  20. Research News

    1. Emergent Functionality and Controllability in Few-Layer Metasurfaces

      Hua Cheng, Zhaocheng Liu, Shuqi Chen and Jianguo Tian

      Article first published online: 12 AUG 2015 | DOI: 10.1002/adma.201501506

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      Few-layer metasurfaces are attracting increasing attention due to their novel functionality, high controllability, and low losses compared with traditional metasurfaces and metamaterials in light manipulation. Recent progress in the design new-type few-layer metasurfaces is presented, whereby improvements in function and efficiency, control of phase and amplitude, and manipulation of polarization and propagation are achieved.

  21. Communications

    1. You have full text access to this OnlineOpen article
      Nanoparticle-Loaded Protein–Polymer Nanodroplets for Improved Stability and Conversion Efficiency in Ultrasound Imaging and Drug Delivery

      Jeong Yu Lee, Dario Carugo, Calum Crake, Joshua Owen, Marie de Saint Victor, Anjali Seth, Constantin Coussios and Eleanor Stride

      Article first published online: 11 AUG 2015 | DOI: 10.1002/adma.201502022

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      A new formulation of volatile nanodroplets stabilized by a protein and polymer coating and loaded with magnetic nanoparticles is developed. The droplets show enhanced stability and phase conversion efficiency upon ultrasound exposure compared with existing formulations. Magnetic targeting, encapsulation, and release of an anticancer drug are demonstrated in vitro with a 40% improvement in cytotoxicity compared with free drug.

    2. Mechanism and Kinetics of Li2S Precipitation in Lithium–Sulfur Batteries

      Frank Y. Fan, W. Craig Carter and Yet-Ming Chiang

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201501559

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      The kinetics of Li2S electrodeposition onto carbon in lithium–sulfur batteries are characterized. Electrodeposition is found to be dominated by a 2D nucleation and growth process with rate constants that depend strongly on the electrolyte solvent. Nucleation is found to require a greater overpotential than growth, which results in a morphology that is dependent on the discharge rate.

    3. Low-Temperature Synthesis of Large-Scale Molybdenum Disulfide Thin Films Directly on a Plastic Substrate Using Plasma-Enhanced Chemical Vapor Deposition

      Chisung Ahn, Jinhwan Lee, Hyeong-U Kim, Hunyoung Bark, Minhwan Jeon, Gyeong Hee Ryu, Zonghoon Lee, Geun Young Yeom, Kwangsu Kim, Jaehyuck Jung, Youngseok Kim, Changgu Lee and Taesung Kim

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201501678

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      By plasma-enhanced chemical vapor deposition, a molybdenum disulfide (MoS2) thin film is synthesized directly on a wafer-scale plastic substrate at below 300 °C. The carrier mobility of the films is 3.74 cm2 V−1 s−1. Also, humidity is successfully detected with MoS2-based sensors fabricated on the flexible substrate, which reveals its potential for flexible sensing devices.

    4. Graphene Quantum Dots Doping of MoS2 Monolayers

      Ziwei Li, Ruquan Ye, Rui Feng, Yimin Kang, Xing Zhu, James M. Tour and Zheyu Fang

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201501888

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      Graphene quantum dots (GQDs) interacting with MoS2 monolayers induce an effective photoexcited charge transfer at the interface. Both the photoluminescence (PL) and valley polarization of this GQDs/MoS2 heterostructure can be modulated under various doping charge densities. The photon–exciton interaction is used to explain and calculate the heterostructure PL control, and is further applied to the valley-polarization tuning.

    5. Droplet-Array (DA) Sandwich Chip: A Versatile Platform for High-Throughput Cell Screening Based on Superhydrophobic–Superhydrophilic Micropatterning

      Anna A. Popova, Sebastian M. Schillo, Konstantin Demir, Erica Ueda, A. Nesterov-Mueller and Pavel A. Levkin

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201502115

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      A droplet-array (DA) sandwich chip is a miniaturized platform for cell-based high-throughput screening. It is based on sandwiching of a glass slide with a preprinted library and a superhydrophobic–superhydrophilic pattern, which consists of thousands of simultaneously formed microdroplets containing cells. The DA sandwich chip allows for one-step cell seeding, simultaneous initiation of screening, and 1000 times less reagent consumption than a regular 96-well plate.

    6. High-Performance Monolayer WS2 Field-Effect Transistors on High-κ Dielectrics

      Yang Cui, Run Xin, Zhihao Yu, Yiming Pan, Zhun-Yong Ong, Xiaoxu Wei, Junzhuan Wang, Haiyan Nan, Zhenhua Ni, Yun Wu, Tangsheng Chen, Yi Shi, Baigeng Wang, Gang Zhang, Yong-Wei Zhang and Xinran Wang

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201502222

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      The combination of high-quality Al2O3 dielectric and thiol chemistry passivation can effectively reduce the density of interface traps and Coulomb impurities, leading to a significant improvement of the mobility and a transition of the charge transport from the insulating to the metallic regime. A record high mobility of 83 cm2 V−1 s−1 (337 cm2 V−1 s−1) is reached at room temperature (low temperature) for monolayer WS2. A theoretical model for electron transport is also developed.

    7. Roll-to-Roll Green Transfer of CVD Graphene onto Plastic for a Transparent and Flexible Triboelectric Nanogenerator

      Bananakere Nanjegowda Chandrashekar, Bing Deng, Ankanahalli Shankaregowda Smitha, Yubin Chen, Congwei Tan, Haixia Zhang, Hailin Peng and Zhongfan Liu

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201502560

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      A novel roll-to-roll, etching-free, clean transfer of CVD-grown graphene from copper to plastic using surface-energy-assisted delamination in hot deionized water is reported. The delamination process is realized by water penetration between the hydrophobic graphene and a hydrophilic native oxide layer on a copper foil.The transferred graphene on plastic is used as a high-output flexible and transparent triboelectric nanogenerator.

    8. Soft Poly(dimethylsiloxane) Elastomers from Architecture-Driven Entanglement Free Design

      Li-Heng Cai, Thomas E. Kodger, Rodrigo E. Guerra, Adrian F. Pegoraro, Michael Rubinstein and David A. Weitz

      Article first published online: 10 AUG 2015 | DOI: 10.1002/adma.201502771

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      Soft, solvent-free poly(dimethylsiloxane) elastomers are fabricated by a one-step process via crosslinking bottlebrush polymers. The bottlebrush architecture prevents the formation of entanglements, resulting in elastomers with precisely controllable low moduli from 1 to 100 kPa, below the lower limit of traditional elastomers; moreover, the solvent-free nature enables their negligible adhesiveness compared to commercially available silicone products of similar stiffness.

  22. Reviews

    1. Graphene-Based Fibers: A Review

      Fancheng Meng, Weibang Lu, Qingwen Li, Joon-Hyung Byun, Youngseok Oh and Tsu-Wei Chou

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201501126

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      Graphene-based fibers (GBFs) integrate the superb mechanical and electrical properties of individual graphene into macroscopic 1D assemblies, and attract significant research interest. The current progress regarding fabrication, characterization, and multifunctional applications of GBFs in the fields of conducting wires, energy-related devices, actuators, etc. is summarized, and their challenges and opportunities for the future are also proposed.

  23. Communications

    1. Biomimetic Approach for Ion Channels Based on Surfactant Encapsulated Spherical Porous Metal-Oxide Capsules

      Eugene Mahon, Somenath Garai, Achim Müller and Mihail Barboiu

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201501255

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      Distinguished hybrid clusters with hydrophilic and hydrophobic interiors embedded within cationic surfactant shells are spontaneously inserted into lipid bilayers, showing well-defined ionic conductance behaviors. The transport via the narrow pore gates acting as selectivity filters is controlled by the dehydration energy of the cations.

    2. Crosslinking Graphene Oxide into Robust 3D Porous N-Doped Graphene

      Yong Qin, Jie Yuan, Juan Li, Dongchang Chen, Yong Kong, Fuqiang Chu, Yongxin Tao and Meilin Liu

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201501735

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      3D N-doped graphene crosslinked by covalent bonds is fabricated through thermal treatment of graphene oxide with a nitrogen-contained resin. The material possesses a hierarchical porous architecture, robust mechanical stability, and abundant N-doped properties. As an electrode material for supercapacitors, this multifunctional material exhibits an unprecedented specific capacitance, high rate capability, and excellent long-term cycle stability.

    3. Diketopyrrolopyrrole-Based Semiconducting Polymer Nanoparticles for In Vivo Photoacoustic Imaging

      Kanyi Pu, Jianguo Mei, Jesse V. Jokerst, Guosong Hong, Alexander L. Antaris, Niladri Chattopadhyay, Adam J. Shuhendler, Tadanori Kurosawa, Yan Zhou, Sanjiv S. Gambhir, Zhenan Bao and Jianghong Rao

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201502285

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      Diketopyrrolopyrrole-based semiconducting polymer nanoparticles with high photostability and strong photoacoustic brightness are designed and synthesized, which results in 5.3-fold photoacoustic signal enhancement in tumor xenografts after systemic administration.

    4. Two-Inch-Sized Perovskite CH3NH3PbX3 (X = Cl, Br, I) Crystals: Growth and Characterization

      Yucheng Liu, Zhou Yang, Dong Cui, Xiaodong Ren, Jiankun Sun, Xiaojing Liu, Jingru Zhang, Qingbo Wei, Haibo Fan, Fengyang Yu, Xu Zhang, Changming Zhao and Shengzhong (Frank) Liu

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201502597

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      Two-inch-sized perovskite crystals, CH3NH3PbX3 (X=I, Br, Cl) with high crystalline quality are prepared by a solution-grown strategy. The availability of large perovskite crystals is expected to tranform its broad applications in photovoltaics, optoelectronics, lasers, photodetectors, LEDs, etc., just as crystalline silicon has done in revolutionizing the modern electronics and photovoltaic industries.

    5. Single-Layer Light-Emitting Diodes Using Organometal Halide Perovskite/Poly(ethylene oxide) Composite Thin Films

      Junqiang Li, Sri Ganesh R. Bade, Xin Shan and Zhibin Yu

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201502490

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      Organometal halide perovskite and poly(ethylene oxide) composite thin films are studied. Single-layer light-emitting diodes using the composite thin film sandwiched between indium tin oxide and indium-gallium eutectic alloy exhibit a low turn-on voltage and high brightness because of the ionic conductivity of the composite film and the formation of a p-i-n homojunction.

    6. Perovskite Sr-Doped LaCrO3 as a New p-Type Transparent Conducting Oxide

      Kelvin H. L. Zhang, Yingge Du, Alexandra Papadogianni, Oliver Bierwagen, Shawn Sallis, Louis F. J. Piper, Mark E. Bowden, Vaithiyalingam Shutthanandan, Peter V. Sushko and Scott A. Chambers

      Article first published online: 6 AUG 2015 | DOI: 10.1002/adma.201501959

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      Epitaxial La1−xSrxCrO3 deposited on SrTiO3(001) is shown to be a p-type transparent conducting oxide with competitive figures of merit and a cubic perovskite structure, facilitating integration into oxide electronics. Holes in the Cr 3d t2g bands play a critical role in enhancing p-type conductivity, while transparency to visible light is maintained because low-lying d–d transitions arising from hole doping are dipole forbidden.

    7. Organic-Catholyte-Containing Flexible Rechargeable Lithium Batteries

      Minjoon Park, Dong-Seon Shin, Jaechan Ryu, Min Choi, Noejung Park, Sung You Hong and Jaephil Cho

      Article first published online: 3 AUG 2015 | DOI: 10.1002/adma.201502329

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      Organic-catholyte-containing flexible rechargeable lithium batteries are developed using fused cyclic quinone derivatives. The structural dependence of the quinone isomers in the liquid catholyte is studied using a combined experimental and theoretical approach. Stable electrochemical performances even under severe bending/stretching deformations are successfully demonstrated by prototype batteries containing liquid catholytes.

    8. Multifunctional Thrombin-Activatable Polymer Capsules for Specific Targeting to Activated Platelets

      Sylvia T. Gunawan, Kristian Kempe, Thomas Bonnard, Jiwei Cui, Karen Alt, Lok S. Law, Xiaowei Wang, Erik Westein, Georgina K. Such, Karlheinz Peter, Christoph E. Hagemeyer and Frank Caruso

      Article first published online: 3 AUG 2015 | DOI: 10.1002/adma.201502243

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      Smart poly(2-oxazoline) (POx)-based multifunctional polymer capsules that specifically target glycoprotein (GP) IIb/IIIa on the surface of activated platelets are degraded by the serine protease thrombin and release the urokinase plasminogen activator loaded into the polymer capsules, only in the area of acute thrombosis.

  24. Essays

    1. Hybrid Organic–Inorganic Perovskites (HOIPs): Opportunities and Challenges

      Joseph Berry, Tonio Buonassisi, David A. Egger, Gary Hodes, Leeor Kronik, Yueh-Lin Loo, Igor Lubomirsky, Seth R. Marder, Yitzhak Mastai, Joel S. Miller, David B. Mitzi, Yaron Paz, Andrew M. Rappe, Ilan Riess, Boris Rybtchinski, Oscar Stafsudd, Vladan Stevanovic, Michael F. Toney, David Zitoun, Antoine Kahn, David Ginley and David Cahen

      Article first published online: 30 JUL 2015 | DOI: 10.1002/adma.201502294

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      The conclusions reached by a diverse group of scientists who attended an intense 2-day workshop on hybrid organic–inorganic perovskites are presented, including their thoughts on the most burning fundamental and practical questions regarding this unique class of materials, and their suggestions on various approaches to resolve these issues.

  25. Communications

    1. Engineering Melanin Nanoparticles as an Efficient Drug–Delivery System for Imaging-Guided Chemotherapy

      Ruiping Zhang, Quli Fan, Min Yang, Kai Cheng, Xiaomei Lu, Lei Zhang, Wei Huang and Zhen Cheng

      Article first published online: 29 JUL 2015 | DOI: 10.1002/adma.201502201

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      In order to promote imaging-guided chemotherapy for preclinical and clinical applications, endogenous nanosystems with both contrast and drug-delivery properties are highly desired. Here, the simple use of melanin is first reported, and this biopolymer with good biocompatibility and biodegradability, binding ability to drugs and ions, and intrinsic photoacoustic properties, can serve as an efficient endogenous nanosystem for imaging-guided tumor chemotherapy in living mice.

    2. High Performance Polymer Nanowire Field-Effect Transistors with Distinct Molecular Orientations

      Chengyi Xiao, Guangyao Zhao, Andong Zhang, Wei Jiang, René A. J. Janssen, Weiwei Li, Wenping Hu and Zhaohui Wang

      Article first published online: 28 JUL 2015 | DOI: 10.1002/adma.201502617

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      Polymer nanowires based on two diketopyrrolopyrrole conjugated polymers with similar chemical structures are shown to have distinct “edge-on” and “face-on” configurations in addition to high well-balanced hole and electron mobilities of 5.47 and 5.33 cm2 V–1 s–1 in field-effect transistors.

  26. Research News

    1. Freestanding Ultrathin Metallic Nanosheets: Materials, Synthesis, and Applications

      Tao Ling, Jing-Jing Wang, Hao Zhang, Shu-Tao Song, Yu-Zhu Zhou, Jiong Zhao and Xi-Wen Du

      Article first published online: 27 JUL 2015 | DOI: 10.1002/adma.201501403

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      Free-standing ultrathin metallic nano­sheets with atomic thickness are the subject of considerable attention. Many kinds of metallic nanosheets with several atomic layers can be successfully synthesized through well-controlled anisotropic growth. These ultrathin metallic nanosheets display unique physical and chemical properties, and show great potential in biochemical sensing and imaging, industrial catalysis, and magnetic recording devices.

  27. Communications

    1. Large-Scale Precise Printing of Ultrathin Sol–Gel Oxide Dielectrics for Directly Patterned Solution-Processed Metal Oxide Transistor Arrays

      Won-June Lee, Won-Tae Park, Sungjun Park, Sujin Sung, Yong-Young Noh and Myung-Han Yoon

      Article first published online: 26 JUL 2015 | DOI: 10.1002/adma.201502239

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      Ultrathin and dense metal oxide gate di­electric layers are reported by a simple printing of AlOx and HfOx sol–gel precursors. Large-area printed indium gallium zinc oxide (IGZO) thin-film transistor arrays, which exhibit mobilities >5 cm2 V−1 s−1 and gate leakage current of 10−9 A cm−2 at a very low operation voltage of 2 V, are demonstrated by continuous simple bar-coated processes.

  28. Research News

    1. Two-Dimensional Porous Carbon: Synthesis and Ion-Transport Properties

      Xiaoyu Zheng, Jiayan Luo, Wei Lv, Da-Wei Wang and Quan-Hong Yang

      Article first published online: 24 JUL 2015 | DOI: 10.1002/adma.201501452

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      Two-dimensional (2D) porous carbon sheets, which can be synthesized by templating approaches, biomass carbonization, biomass carbonization–activation, in situ activation, etc, are good candidates for supercapacitors due to their advantages in their short ion-transport length and high aspect ratio for electrode packing and electron transport.

  29. Communications

    1. Controlled Assembly of Biocompatible Metallic Nanoaggregates Using a Small Molecule Crosslinker

      Desiree Van Haute, Julia M. Longmate and Jacob M. Berlin

      Article first published online: 24 JUL 2015 | DOI: 10.1002/adma.201501602

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      By introducing a capping step and controlling reaction parameters, the assembly of metallic nanoparticle aggregates can be achieved using a small molecule crosslinker. Aggregates can be assembled from particles of varied size and composition and the size of the aggregates can be systematically adjusted. Following cell uptake of 60 nm aggregates, the aggregates are stable and nontoxic to macrophage cells up to 55 × 10−3m Au.

    2. Measurement of the Charge Carrier Mobility Distribution in Bulk Heterojunction Solar Cells

      Jason Seifter, Yanming Sun, Hyosung Choi, Byoung Hoon Lee, Thanh Luan Nguyen, Han Young Woo and Alan J. Heeger

      Article first published online: 22 JUL 2015 | DOI: 10.1002/adma.201500416

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      Charge carrier transport through organic solar cells is fundamentally dispersive due to the disordered structure and complex film morphology within the photoactive layer. A novel application of transient photocurrent and short circuit variable time-delayed collection field measurements is used to reconstruct the complete charge carrier mobility distribution for the photogenerated carriers in optimized organic solar cells.

    3. Glass and Plastics Platforms for Foldable Electronics and Displays

      Moon Jong Han and Dahl-Young Khang

      Article first published online: 21 JUL 2015 | DOI: 10.1002/adma.201501060

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      Reversibly, repeatedly foldable electronics and displays have been enabled by employing engineered glass or plastics substrates, where folding deformation has been localized in thinned parts only. This design concept can further be extended to dual folding, leading to size reduction down to 1/4. Notably, the foldable electronics and displays can be implemented with no need to introduce any novel materials.

    4. Nanocarrier-Integrated Microspheres: Nanogel Tectonic Engineering for Advanced Drug-Delivery Systems

      Yoshiro Tahara, Sada-atsu Mukai, Shin-ichi Sawada, Yoshihiro Sasaki and Kazunari Akiyoshi

      Article first published online: 21 JUL 2015 | DOI: 10.1002/adma.201501557

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      A nanocarrier-integrated bottom-up method is a promising strategy for advanced drug-release systems. Self-assembled nanogels, which are one of the most beneficial nanocarriers for drug-delivery systems, are tectonically integrated to prepare nanogel-crosslinked (NanoClik) microspheres. NanoClik microspheres consisting of nanogel-derived structures (observed by STED microscopy) release “drug-loaded nanogels” after hydrolysis, resulting in successful sustained drug delivery in vivo.

    5. Mapping Local Cytosolic Enzymatic Activity in Human Esophageal Mucosa with Porous Silicon Nanoneedles

      Ciro Chiappini, Paola Campagnolo, Carina S. Almeida, Nima Abbassi-Ghadi, Lesley W. Chow, George B. Hanna and Molly M. Stevens

      Article first published online: 21 JUL 2015 | DOI: 10.1002/adma.201501304

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      Porous silicon nanoneedles can map Cathepsin B activity across normal and tumor human esophageal mucosa. Assembling a peptide-based Cathepsin B cleavable sensor over a large array of nano­needles allows the discrimination of cancer cells from healthy ones in mixed culture. The same sensor applied to tissue can map Cathepsin B activity with high resolution across the tumor margin area of esophageal adenocarcinoma.


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