Advanced Materials

Cover image for Vol. 25 Issue 39

October 18, 2013

Volume 25, Issue 39

Pages 5521–5672

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      Imaging: Conjugated Polymer/Photochromophore Binary Nanococktails: Bistable Photoswitching of Near-Infrared Fluorescence for In Vivo Imaging (Adv. Mater. 39/2013) (page 5521)

      Keunsoo Jeong, Solji Park, Yong-Deok Lee, Chang-Keun Lim, Jungahn Kim, Bong Hyun Chung, Ick Chan Kwon, Chong Rae Park and Sehoon Kim

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370244

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      Fluorescence photoswitching in autofluorescencerich in vivo environments is demonstrated by Sehoon Kim, Chong Rae Park, and co-workers on page 5574. Nanoscopic dense integration between solid-state emission and photochromism provides nanococktails capable of photoswitching of bright NIR fluorescence with high on/off contrast, bistability, and improved signal identification. These nanoprobes represent great progress in the field of fluorescence bioimaging.

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      Hydrogels: In Situ Self-Folding Assembly of a Multi-Walled Hydrogel Tube for Uniaxial Sustained Molecular Release (Adv. Mater. 39/2013) (page 5522)

      Kwanghyun Baek, Jae Hyun Jeong, Artem Shkumatov, Rashid Bashir and Hyunjoon Kong

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370245

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      Multiwalled poly(ethylene glycol) diacrylate (PEGDA) hydrogel tubes are assembled via in situ self-folding of a bilayered hydrogel patch with different expansion ratios and rigidity between the two layers, as described by Hyunjoon Kong and co-workers on page 5568. The resulting gel tubes exhibit unidirectional, sustained release of proangiogenic growth factors and significantly stimulated vascularization around the gel implant.

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      Camouflage Coatings: Reconfigurable Infrared Camouflage Coatings from a Cephalopod Protein (Adv. Mater. 39/2013) (page 5676)

      Long Phan, Ward G. Walkup IV, David D. Ordinario, Emil Karshalev, Jonah-Micah Jocson, Anthony M. Burke and Alon A. Gorodetsky

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370246

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      Graphene-templated, camouflage coatings that possess several important advantages are demonstrated by Alon A. Gorodetsky and co-workers on page 5621. These coatings are inspired by the unique dynamic camouflage mechanisms or cephalopods. A squid's ability to control transmission and reflection of light can be applied to a substrate and made controllable. Such substrates are shown to be a home window that reflects long wave light (IR) and transmits short wave light. The thin film fabrication strategy is inexpensive, robust, and compatible with a wide range of substrates of arbitrary form factor.

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    1. Masthead: (Adv. Mater. 39/2013)

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370247

  5. Contents

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  6. Reviews

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    1. 25th Anniversary Article: Reversible and Adaptive Functional Supramolecular Materials: “Noncovalent Interaction” Matters (pages 5530–5548)

      Kai Liu, Yuetong Kang, Zhiqiang Wang and Xi Zhang

      Article first published online: 4 SEP 2013 | DOI: 10.1002/adma201302015

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      This review article aims to highlight the very recent and important progress in the area of functional supramolecular materials, focusing on their extraordinary functions arising from the reversible and adaptive noncovalent interactions. It mainly includes adaptive mechanical materials, smart sensors with enhanced selectivity, soft luminescent and electronic nanomaterials, and biomimetic and biomedical materials with tailored structures and functions.

  7. Communications

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    1. High-Performance Nanowire Oxide Photo-Thin Film Transistor (pages 5549–5554)

      Seung-Eon Ahn, Sanghun Jeon, Youg Woo Jeon, Changjung Kim, Myoung-Jae Lee, Chang-Won Lee, Jongbong Park, Ihun Song, Arokia Nathan, Sungsik Lee and U-In Chung

      Article first published online: 27 AUG 2013 | DOI: 10.1002/adma201301102

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      A gate-modulated nanowire oxide photosensor is fabricated by electron-beam lithography and conventional dry etch processing.. The device characteristics are good, including endurance of up to 106 test cycles, and gate-pulse excitation is used to remove persistent photoconductivity. The viability of nanowire oxide phototransistors for high speed and high resolution applications is demonstrated, thus potentially expanding the scope of exploitation of touch-free interactive displays.

    2. Low-Voltage Switching of Crease Patterns on Hydrogel Surfaces (pages 5555–5559)

      Bin Xu and Ryan C. Hayward

      Article first published online: 22 JUL 2013 | DOI: 10.1002/adma.201300968

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      We report electrically driven creasing of polyelectrolye hydrogel surfaces with low switching voltages (2–4 V). Deep creases (up to 70% of the swelled film thickness) can be reversibly formed and eliminated on time-scales of a few seconds, with control of crease locations by micro-patterning of underlying electrodes.

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      Phase Transitions, Phase Coexistence, and Piezoelectric Switching Behavior in Highly Strained BiFeO3 Films (Adv. Mater. 39/2013) (page 5560)

      C. Beekman, W. Siemons, T. Z. Ward, M. Chi, J. Howe, M. D. Biegalski, N. Balke, P. Maksymovych, A. K. Farrar, J. B. Romero, P. Gao, X. Q. Pan, D. A. Tenne and H. M. Christen

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370249

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      A complex phase coexistence forms in epitaxial films of BiFeO3 due to the effects of epitaxial strain and temperature-induced stresses. The work by H. M. Christen and co-workers on page 5561 shows that the stripe patterns that form upon cooling of these atomically flat layers are a prerequisite for piezoelectric switching, i.e., the phase coexistence enables the functionality of the material.

  9. Communications

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    1. Phase Transitions, Phase Coexistence, and Piezoelectric Switching Behavior in Highly Strained BiFeO3 Films (pages 5561–5567)

      C. Beekman, W. Siemons, T. Z. Ward, M. Chi, J. Howe, M. D. Biegalski, N. Balke, P. Maksymovych, A. K. Farrar, J. B. Romero, P. Gao, X. Q. Pan, D. A. Tenne and H. M. Christen

      Article first published online: 12 JUL 2013 | DOI: 10.1002/adma.201302066

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      Highly strained BiFeO3 films transition into a true tetragonal state at 430 °C but remain polar to much higher temperatures (∼800 °C). Piezoelectric switching is only possible up to 300 °C, i.e., at temperatures for which strain stabilizes the stripe-like coexistence of multiple polymorphs.

    2. In Situ Self-Folding Assembly of a Multi-Walled Hydrogel Tube for Uniaxial Sustained Molecular Release (pages 5568–5573)

      Kwanghyun Baek, Jae Hyun Jeong, Artem Shkumatov, Rashid Bashir and Hyunjoon Kong

      Article first published online: 17 JUL 2013 | DOI: 10.1002/adma.201300951

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      This study presents a multi-walled poly(ethylene glycol) diacrylate hydrogel tube formed by the simple self-folding of a bi-layered hydrogel patch. The gel tube has the capability to release encapsulated molecules through designated pathways in a sustained manner. Therefore, the gel tube encapsulating the vascular endothelial growth factor significantly increases the vascular densities and vessel diameters at an implantation site.

    3. Conjugated Polymer/Photochromophore Binary Nanococktails: Bistable Photoswitching of Near-Infrared Fluorescence for In Vivo Imaging (pages 5574–5580)

      Keunsoo Jeong, Solji Park, Yong-Deok Lee, Chang-Keun Lim, Jungahn Kim, Bong Hyun Chung, Ick Chan Kwon, Chong Rae Park and Sehoon Kim

      Article first published online: 12 JUL 2013 | DOI: 10.1002/adma.201301901

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      Nanoscopic dense integration between solid-state emission and photochromism provides nanoprobes capable of photoswitching of bright NIR fluorescence with high on/off contrast, bistability and improved signal identification, being suitable for imaging applications in autofluorescence-rich in vivo environments.

    4. Electric-Field-Dependent Spin Polarization in GdN Spin Filter Tunnel Junctions (pages 5581–5585)

      Avradeep Pal, K. Senapati, Z. H. Barber and M. G. Blamire

      Article first published online: 29 JUL 2013 | DOI: 10.1002/adma.201300636

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      Tunnel junctions incorporating GdN ferromagnetic semiconductor barriers show a spin polarization exceeding 90% and a high conductance. These devices show an unusual low-bias conductance peak arising from a strong bias-dependence of the spin polarization. This originates from a strong magneto-electric coupling within a double Schottky barrier formed with the NbN electrodes.

    5. Doping Control Via Molecularly Engineered Surface Ligand Coordination (pages 5586–5592)

      Mingjian Yuan, David Zhitomirsky, Valerio Adinolfi, Oleksandr Voznyy, Kyle W. Kemp, Zhijun Ning, Xinzheng Lan, Jixian Xu, Jin Young Kim, Haopeng Dong and Edward H. Sargent

      Article first published online: 5 AUG 2013 | DOI: 10.1002/adma201302802

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      A means to control the net doping of a CQD solid is identified via the design of the bidentate ligand crosslinking the material. The strategy does not rely on implementing different atmospheres at different steps in device processing, but instead is a robust strategy implemented in a single processing ambient. We achieve an order of magnitude difference in doping that allows us to build a graded photovoltaic device and maintain high current and voltage at maximum power-point conditions.

    6. Tunable Electroluminescence in Planar Graphene/SiO2 Memristors (pages 5593–5598)

      Congli He, Jiafang Li, Xing Wu, Peng Chen, Jing Zhao, Kuibo Yin, Meng Cheng, Wei Yang, Guibai Xie, Duoming Wang, Donghua Liu, Rong Yang, Dongxia Shi, Zhiyuan Li, Litao Sun and Guangyu Zhang

      Article first published online: 6 AUG 2013 | DOI: 10.1002/adma.201302447

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      Electroluminescence and resistive switching are first realized simultaneously in graphene/SiO2 memristor devices. The electroluminescence peaks can be tuned between 550 nm and 770 nm reliably via setting the device to different resistance states by applying different voltages. The combination of resistive switching and electroluminescence may bring new functionalities for these memristor devices which are fully compatible with silicon-based electronics.

    7. Wet-Chemical Preparation of Copper Foam Monoliths with Tunable Densities and Complex Macroscopic Shapes (pages 5599–5604)

      Niklaus Kränzlin and Markus Niederberger

      Article first published online: 6 AUG 2013 | DOI: 10.1002/adma.201301749

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      Macroscopic monoliths of copper foams have been prepared by a template-assisted wet-chemical process. The method offers subtle control over the pore size and size distribution, density and macroscopic size and shape of the metal foam. Uniaxial compression tests revealed different deformation behavior depending on the relative density. Non-vacuum-based and low-temperature routes are attractive for the cost-effective production of metal foams.

    8. Fractional Diffusion in Silicon (pages 5605–5608)

      Eeuwe S. Zijlstra, Alan Kalitsov, Tobias Zier and Martin E. Garcia

      Article first published online: 7 AUG 2013 | DOI: 10.1002/adma201302559

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      Microscopic processes leading to ultrafast laser-induced melting of silicon are investigated by large-scale ab initio molecular dynamics simulations. Before becoming a liquid, the atoms are shown to be fractionally diffusive, which is a property that has so far been observed in crowded fluids consisting of large molecules. Here, it is found to occur in an elemental semiconductor.

    9. Polyphosphoester-Based Cationic Nanoparticles Serendipitously Release Integral Biologically-Active Components to Serve as Novel Degradable Inducible Nitric Oxide Synthase Inhibitors (pages 5609–5614)

      Yuefei Shen, Shiyi Zhang, Fuwu Zhang, Alexander Loftis, Adriana Pavía-Sanders, Jiong Zou, Jingwei Fan, John-Stephen A. Taylor and Karen L. Wooley

      Article first published online: 3 SEP 2013 | DOI: 10.1002/adma.201302842

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      A degradable polyphosphoester (PPE)-based cationic nanoparticle (cSCK), which is integrated constructed as a novel degradable drug device, demonstrates surprisingly efficient inhibition of inducible nitric oxide synthase (iNOS) transcription, and eventually inhibits nitric oxide (NO) over-production, without loading of any specific therapeutic drugs. This system may serve as a promising anti-inflammatory agent toward the treatment of acute lung injury.

  10. Frontispiece

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      Nanoparticles: Detection of Single Nanoparticles and Lentiviruses Using Microcavity Resonance Broadening (Adv. Mater. 39/2013) (page 5615)

      Linbo Shao, Xue-Feng Jiang, Xiao-Chong Yu, Bei-Bei Li, William R. Clements, Frank Vollmer, Wei Wang, Yun-Feng Xiao and Qihuang Gong

      Article first published online: 20 OCT 2013 | DOI: 10.1002/adma.201370250

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      A new label-free optical sensing mechanism is demonstrated experimentally by Qihuang Gong, Yun-Feng Xiao, and co-workers on page 5616, by monitoring the mode broadening in whispering gallery microcavities. This new sensing is not only immune to both noise from the probe laser and environmental disturbances, but is also able to remove the strict requirement for ultra-high-Q microcavities for sensitive nanoparticle detection.

  11. Communications

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    1. Detection of Single Nanoparticles and Lentiviruses Using Microcavity Resonance Broadening (pages 5616–5620)

      Linbo Shao, Xue-Feng Jiang, Xiao-Chong Yu, Bei-Bei Li, William R. Clements, Frank Vollmer, Wei Wang, Yun-Feng Xiao and Qihuang Gong

      Article first published online: 12 AUG 2013 | DOI: 10.1002/adma201302572

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      A new label-free sensing mechanism is demonstrated experimentally by monitoring the whispering-gallery mode broadening in microcavities. It is immune to both noise from the probe laser and environmental disturbances, and is able to remove the strict requirement for ultra-high-Q mode cavities for sensitive nanoparticle detection. This ability to sense nanoscale objects and biological analytes is particularly crucial for wide applications.

      Corrected by:

      Correction: Detection of Single Nanoparticles and Lentiviruses Using Microcavity Resonance Broadening

      Vol. 26, Issue 7, 991, Article first published online: 18 FEB 2014

    2. Reconfigurable Infrared Camouflage Coatings from a Cephalopod Protein (pages 5621–5625)

      Long Phan, Ward G. Walkup IV, David D. Ordinario, Emil Karshalev, Jonah-Micah Jocson, Anthony M. Burke and Alon A. Gorodetsky

      Article first published online: 30 JUL 2013 | DOI: 10.1002/adma.201301472

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      In nature, cephalopods employ unique dynamic camouflage mechanisms. Herein, we draw inspiration from self-assembled structures found in cephalopods to fabricate tunable biomimetic camouflage coatings. The reflectance of these coatings is dynamically modulated between the visible and infrared regions of the electromagnetic spectrum in situ. Our studies represent a crucial step towards reconfigurable and disposable infrared camouflage for stealth applications.

    3. Sticker-Type Alq3-Based OLEDs Based on Printable Ultrathin Substrates in Periodically Anchored and Suspended Configurations (pages 5626–5631)

      Su Ok Yun, Youngkyu Hwang, Jeongpil Park, Yunkyung Jeong, Suk Ho Kim, Byeong Il Noh, Hoon Sun Jung, Hun Soo Jang, Yujun Hyun, Sung-Hoon Choa and Heung Cho Ko

      Article first published online: 12 AUG 2013 | DOI: 10.1002/adma201302503

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      Introducing two-dimensional post arrays and a water-soluble sacrificial layer between an ultrathin substrate and a handling substrate provides controllability of the interfacial adhesion in a stable manner. The periodically anchored and suspended configuration after the chemical etching process facilitates the development of, for example, printable Alq3-based OLEDs that can be attached to unconventional surfaces.

    4. Fluorinated Graphene Oxide; a New Multimodal Material for Biological Applications (pages 5632–5637)

      Rebeca Romero-Aburto, Tharangattu. N. Narayanan, Yutaka Nagaoka, Takashi Hasumura, Trevor M. Mitcham, Takahiro Fukuda, Paris J. Cox, Richard R. Bouchard, Toru Maekawa, D. Sakthi Kumar, Suzy V. Torti, Sendurai A. Mani and Pulickel M. Ajayan

      Article first published online: 27 AUG 2013 | DOI: 10.1002/adma201301804

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      Fluorinated graphene oxide (FGO) is reported for the first time as a magnetically responsive drug carrier that can serve both as a magnetic resonance imaging (MRI) and photoacoustic contrast agent, under preclinical settings, and as a type of photothermal therapy. Its hydrophilic nature facilitates biocompatibility. FGO as a broad wavelength absorber, with high charge transfer and strong non-linear scattering is optimal for NIR laser-induced hyperthermia.

    5. Plasma Break-Down and Re-Build: Same Functional Vertical Graphenes from Diverse Natural Precursors (pages 5638–5642)

      Dong Han Seo, Amanda Evelyn Rider, Zhao Jun Han, Shailesh Kumar and Kostya (Ken) Ostrikov

      Article first published online: 4 SEP 2013 | DOI: 10.1002/adma201301510

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      Plasmas, the 4th state of matter, uniformly transform natural precursors with different chemical composition in solid, liquid, and gas states into the same functional vertical graphenes in a single-step process within a few minutes. Functional vertical graphenes show reliable biosensing properties, strong binding with proteins, and improved adhesion to substrates.

    6. Flexoelectric Effect in the Reversal of Self-Polarization and Associated Changes in the Electronic Functional Properties of BiFeO3 Thin Films (pages 5643–5649)

      Byung Chul Jeon, Daesu Lee, Myang Hwan Lee, Sang Mo Yang, Seung Chul Chae, Tae Kwon Song, Sang Don Bu, Jin-Seok Chung, Jong-Gul Yoon and Tae Won Noh

      Article first published online: 30 JUL 2013 | DOI: 10.1002/adma.201301601

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      Flexoelectricity can play an important role in the reversal of the self-polarization direction in epitaxial BiFeO3 thin films. The flexoelectric and interfacial effects compete with each other to determine the self-polarization state. In Region I, the self-polarization is downward because the interfacial effect is more dominant than the flexoelectric effect. In Region II, the self-polarization is upward, because the flexoelectric effect becomes more dominant than the interfacial effect.

    7. SWCNT/Graphite Nanoplatelet Hybrid Thin Films for Self-Temperature-Compensated, Highly Sensitive, and Extensible Piezoresistive Sensors (pages 5650–5657)

      Sida Luo and Tao Liu

      Article first published online: 13 AUG 2013 | DOI: 10.1002/adma.201301796

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      Highly sensitive single-wall carbon nanotube/graphite nanoplatelet (SWCNT/GNP) hybrid thin-film sensors are developed, which possess the unique capability for self-temperature compensation. This unique property in combination with their high gauge sensitivity and large reversible extensibility promises the SWCNT/GNP hybrid thin film piezoresistive sensors for a wide range applications, such as in man-machine interaction and body monitoring.

    8. Mechanically Flexible and Multifunctional Polymer-Based Graphene Foams for Elastic Conductors and Oil-Water Separators (pages 5658–5662)

      Chao Wu, Xingyi Huang, Xinfeng Wu, Rong Qian and Pingkai Jiang

      Article first published online: 2 AUG 2013 | DOI: 10.1002/adma.201302406

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      We present a novel strategy for the fabrication of ordered and flexible polymer-based graphene foams by self-assembly of graphene sheets on a 3D polymer skeleton. The obtained graphene foams show excellent mechanical, electrical, and hydrophobic properties, thus holding great potential as elastic conductors and oil-water separators.

    9. Field-Induced Transition from Room-Temperature Ferromagnetism to Diamagnetism in Proton-Irradiated Fullerene (pages 5663–5667)

      Kyu Won Lee, Hyocheon Kweon and Cheol Eui Lee

      Article first published online: 15 AUG 2013 | DOI: 10.1002/adma201301635

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      Room-temperature ferromagnetism in proton-irradiated C60 fullerene is demonstrated. The ferromagnetism turns into diamagnetism intrinsic to the fullerene as the magnetic field increases above a critical field.

    10. Ordered Hierarchical Mesoporous/Macroporous Carbon: A High-Performance Catalyst for Rechargeable Li–O2 Batteries (pages 5668–5672)

      Ziyang Guo, Dandan Zhou, XiaoLi Dong, Zijie Qiu, Yonggang Wang and Yongyao Xia

      Article first published online: 2 AUG 2013 | DOI: 10.1002/adma.201302459

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      Three-dimensional ordered mesoporous/macroporous carbon sphere arrays (MMCSAs) are synthesized and then used as a catalyst for Li−O2 batteries. The hierarchical porous structure of the MMCSAs not only facilitates electrolyte immersion and Li+ diffusion but also provides an effective space for O2 diffusion and O2/Li2O2 conversion, and thus efficiently improves the performance of Li–O2 batteries.

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