Advanced Materials

Cover image for Vol. 26 Issue 27

July 16, 2014

Volume 26, Issue 27

Pages 4597–4747

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      Bioassays: A Bubble-Mediated Intelligent Microscale Electrochemical Device for Single-Step Quantitative Bioassays (Adv. Mater. 27/2014) (page 4597)

      Fan Yang, Xiaolei Zuo, Zhenhua Li, Wangping Deng, Jiye Shi, Guojun Zhang, Qing Huang, Shiping Song and Chunhai Fan

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470181

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      C. Fan and co-workers demonstrate on page 4671 an intelligent microscale electrochemical device with a “plugin-cartridge” for one-step, quantitative, and multiplexed electrochemical detection of biomarkers for infectious diseases and tumors.

  2. Inside Front Cover

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      Photoconversion: Photocatalytic Conversion of CO2 into Renewable Hydrocarbon Fuels: State-of-the-Art Accomplishment, Challenges, and Prospects (Adv. Mater. 27/2014) (page 4598)

      Wenguang Tu, Yong Zhou and Zhigang Zou

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470182

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      Photocatalytic reduction of CO2 into hydrocarbon fuels, an artificial photosynthesis, is a challenging, yet promising avenue for achieving a sustainable alternative to conventional fossil fuels. Accordingly, many scientists worldwide develop new and effective materials for CO2 fixation and reduction. On page 4607, Z. Zou, Y. Zhou, and W. Tu review recent state-of-the-art accomplishments in this area.

  3. Inside Back Cover

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      Ferromagnets: Intercalation-Driven Reversible Control of Magnetism in Bulk Ferromagnets (Adv. Mater. 27/2014) (page 4751)

      Subho Dasgupta, Bijoy Das, Michael Knapp, Richard. A. Brand, Helmut Ehrenberg, Robert Kruk and Horst Hahn

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470186

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      A new concept of controlling magnetism in bulk ferromagnets via reversible lithium chemistry is illustrated. The approach bridges electrochemistry with magnetism and is pertinent to any volume of an intercalation-friendly ferromagnetic material. An iron oxide (maghemite) nanoparticle ensemble, chosen as a representative system, shows a fully reversible and large variation of saturation magnetization upon a controlled intercalation/de-intercalation process of Li+ ions. A detailed description of the phenomenon can be found in the article by S. Dasgupta and co-workers on page 4639.

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      Transistors: Inkjet Printing Short-Channel Polymer Transistors with High-Performance and Ultrahigh Photoresponsivity (Adv. Mater. 27/2014) (page 4752)

      Hanlin Wang, Cheng Cheng, Lei Zhang, Hongtao Liu, Yan Zhao, Yunlong Guo, Wenping Hu, Gui Yu and Yunqi Liu

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470187

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      Y. Q. Liu, W. P. Hu, and co-workers demonstrate on page 4683 that the channel lengths of inkjet-printed transistors can be reduced to a sub-micrometer scale via a simple and direct method, without any sophisticated substrate-treatments with photolithography and organosilanes. By inkjet printing solvents on ultrathin poly(methyl methacrylate) (PMMA), channel regions with high resolution are welldefined. With an inkjet-printed polymeric semiconductor, this technique provides a short-cut to low-cost, massfabrication of photodetectors with ultrahigh responsivity.

  5. Masthead

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    1. Masthead: (Adv. Mater. 27/2014)

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470184

  6. Contents

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  7. Correction

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      Solution-Processed, Molecular Photovoltaics that Exploit Hole Transfer from Non Fullerene, n-Type Materials (page 4606)

      Jessica D. Douglas, Mark S. Chen, Jeremy R. Niskala, Olivia P. Lee, Alan T. Yiu, Eric P. Young and Jean M. J. Fréchet

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201402481

      This article corrects:

      Solution-Processed, Molecular Photovoltaics that Exploit Hole Transfer from Non-Fullerene, n-Type Materials

      Vol. 26, Issue 25, 4313–4319, Article first published online: 12 MAY 2014

  8. Reviews

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    1. Photocatalytic Conversion of CO2 into Renewable Hydrocarbon Fuels: State-of-the-Art Accomplishment, Challenges, and Prospects (pages 4607–4626)

      Wenguang Tu, Yong Zhou and Zhigang Zou

      Article first published online: 26 MAY 2014 | DOI: 10.1002/adma.201400087

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      Recent state-of-the-art accomplishments of overcoming the drawback of low photo­conversion efficiency and selectivity through the design of highly active photo­catalysts, from the point of view of adsorption of reactants, charge separation and transport, light harvesting, and CO2 activation are reviewed.

  9. Communications

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    1. Stem Cells Loaded with Nanoparticles as a Drug Carrier for In Vivo Breast Cancer Therapy (pages 4627–4631)

      Binrui Cao, Mingying Yang, Ye Zhu, Xuewei Qu and Chuanbin Mao

      Article first published online: 30 MAY 2014 | DOI: 10.1002/adma.201401550

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      A novel anti-cancer drug carrier, mesenchymal stem cells (MSCs) encapsulating drug-loaded hollow silica nanoparticles, is used to carry a photosensitizer drug and deliver it to breast tumors, due to the natural high tumor affinity of the MSCs, and inhibit tumor growth by photo dynamic therapy. This new strategy for delivering a photo sensitizer to tumors by using tumor-affinitive MSCs addresses the challenge of the accumulation of photosensitizer drugs in tumors in photodynamic therapy.

  10. Frontispiece

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      Monolayers: Quick, Large-Area Assembly of a Single-Crystal Monolayer of Spherical Particles by Unidirectional Rubbing (Adv. Mater. 27/2014) (page 4632)

      ChooJin Park, Taeil Lee, Younan Xia, Tae Joo Shin, Jaemin Myoung and Unyong Jeong

      Article first published online: 14 JUL 2014 | DOI: 10.1002/adma.201470185

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      Unidirectional rubbing of a dry powder between two flat rubbery substrates enables quick large-area single-crystal monolayer assembly of microparticles. The rubbing process is applicable to curved surfaces, as shown here in this frontispiece. Various parameters for the rubbing conditions, such as pressure, rubbing speed, and adhesion energy of substrate, are discussed in detail by U. Jeong, J. Myoung, and co-workers on page 4633.

  11. Communications

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    1. Quick, Large-Area Assembly of a Single-Crystal Monolayer of Spherical Particles by Unidirectional Rubbing (pages 4633–4638)

      ChooJin Park, Taeil Lee, Younan Xia, Tae Joo Shin, Jaemin Myoung and Unyong Jeong

      Article first published online: 7 APR 2014 | DOI: 10.1002/adma.201305875

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      Rubbing a dry powder of particles in one direction between two rubbery substrates is found to be a quick and highly reproducible, yet inexpensive fabrication technique for assembling particle monolayers with perfect spatial registry on flat or curved surfaces. The optimum rubbing conditions – pressure and speed – for a single-crystal monolayer are shown to depend on particle size. Potential applications are in biosensors, photovoltaics, and light manipulators.

    2. Intercalation-Driven Reversible Control of Magnetism in Bulk Ferromagnets (pages 4639–4644)

      Subho Dasgupta, Bijoy Das, Michael Knapp, Richard. A. Brand, Helmut Ehrenberg, Robert Kruk and Horst Hahn

      Article first published online: 3 MAR 2014 | DOI: 10.1002/adma.201305932

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      An extension in magnetoelectric effects is proposed to include reversible chemistry-controlled magnetization variations. This ion-intercalation-driven magnetic control can be fully reversible and pertinent to bulk material volumes. The concept is demonstrated for ferromagnetic iron oxide where the intercalated lithium ions cause valence change and partial redistribution of Fe3+ cations yielding a large and fully reversible change in magnetization at room temperature.

    3. Multiferroic Iron Oxide Thin Films at Room Temperature (pages 4645–4652)

      Martí Gich, Ignasi Fina, Alessio Morelli, Florencio Sánchez, Marin Alexe, Jaume Gàzquez, Josep Fontcuberta and Anna Roig

      Article first published online: 15 MAY 2014 | DOI: 10.1002/adma.201400990

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      Multiferroic behaviour at room temperature is demonstrated in ε-Fe2O3. The simple composition of this new ferromagnetic ferroelectric oxide and the discovery of a robust path for its thin film growth by using suitable seed layers may boost the exploitation of ε-Fe2O3 in novel devices.

    4. Unique Properties of Halide Perovskites as Possible Origins of the Superior Solar Cell Performance (pages 4653–4658)

      Wan-Jian Yin, Tingting Shi and Yanfa Yan

      Article first published online: 15 MAY 2014 | DOI: 10.1002/adma.201306281

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      Halide perovskites solar cells have the potential to exhibit higher energy conversion efficiencies with ultrathin films than conventional thin-film solar cells based on CdTe, CuInSe2, and Cu2ZnSnSe4. The superior solar-cell performance of halide perovskites may originate from its high optical absorption, comparable electron and hole effective mass, and electrically clean defect properties, including point defects and grain boundaries.

    5. Li-O2 Battery Based on Highly Efficient Sb-Doped Tin Oxide Supported Ru Nanoparticles (pages 4659–4664)

      Fujun Li, Dai-Ming Tang, Zelang Jian, Dequan Liu, Dmitri Golberg, Atsuo Yamada and Haoshen Zhou

      Article first published online: 26 MAY 2014 | DOI: 10.1002/adma.201400162

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      Novel cathodes based on Sb-doped tin oxide (STO)-supported Ru particles enable Li–O2 batteries to be operated below 4.0 V, which is of crucial importance for the realization of rechargeable Li–O2 batteries, and to deliver a high specific capacity of 750 mA h g−1 even after 50 discharge–charge cycles at 0.1 mA cm−2.

    6. Wrinkle-Directed Self-Assembly of Block Copolymers for Aligning of Nanowire Arrays (pages 4665–4670)

      Bong Hoon Kim, Yemuk Choi, Ju Young Kim, Hyunjae Shin, Sungyong Kim, Seung-Woo Son, Sang Ouk Kim and Pilnam Kim

      Article first published online: 22 MAY 2014 | DOI: 10.1002/adma.201400804

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      Highly aligned metal nanowire arrays with feature sizes approaching 10 nm are fabricated. This is made possible by the self-assembly of block copolymers (BCPs) on graphene-wrinkle arrays. Thickness-modulated BCP films confined on the wrinkled reduced graphene oxide (rGO) surface promote the strict alignment of the self-assembled BCP lamellae in the direction of the film thickness gradient.

    7. A Bubble-Mediated Intelligent Microscale Electrochemical Device for Single-Step Quantitative Bioassays (pages 4671–4676)

      Fan Yang, Xiaolei Zuo, Zhenhua Li, Wangping Deng, Jiye Shi, Guojun Zhang, Qing Huang, Shiping Song and Chunhai Fan

      Article first published online: 14 APR 2014 | DOI: 10.1002/adma.201400451

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      An intelligent microscale electrochemical device (iMED) for one-step, quantitative and multiplexed electrochemical detection of biomarkers for infectious diseases and tumors is developed. A “plug-in-cartridge” technology is introduced and adapted for use in screen-printed electrodes (SPEs) in electrochemical devices. Using this iMED, biomarkers for two types of tumors and one infectious disease are detected at sub-ng/mL levels in less than 30 min.

    8. Inkjet Printing of Conductive Inks with High Lateral Resolution on Omniphobic “RF Paper” for Paper-Based Electronics and MEMS (pages 4677–4682)

      Joshua Lessing, Ana C. Glavan, S. Brett Walker, Christoph Keplinger, Jennifer A. Lewis and George M. Whitesides

      Article first published online: 30 MAY 2014 | DOI: 10.1002/adma.201401053

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      The use of omniphobic “fluoroalkylated paper” as a substrate for inkjet printing of aqueous inks that are the precursors of electrically conductive patterns is described. By controlling the surface chemistry of the paper, it is possible to print high resolution, conductive patterns that remain conductive after folding and exposure to common solvents.

    9. Inkjet Printing Short-Channel Polymer Transistors with High-Performance and Ultrahigh Photoresponsivity (pages 4683–4689)

      Hanlin Wang, Cheng Cheng, Lei Zhang, Hongtao Liu, Yan Zhao, Yunlong Guo, Wenping Hu, Gui Yu and Yunqi Liu

      Article first published online: 6 APR 2014 | DOI: 10.1002/adma.201400697

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      Inkjet-printed short-channel polymer transistors exhibit a high performance (μavg = 1.20 cm2 V−1 s−1). With a 50 μm orifice nozzle, polymer transistors with a sub-micrometer (700 nm) channel length are mass-fabricated with good uniformity and reproducibility. In addition, owing to the device geometry, an ultrahigh photoresponsivity up to 106 A W−1 is achieved, which realizes economical, lithography-free photodetectors.

    10. Harvesting Water Drop Energy by a Sequential Contact-Electrification and Electrostatic-Induction Process (pages 4690–4696)

      Zong-Hong Lin, Gang Cheng, Sangmin Lee, Ken C. Pradel and Zhong Lin Wang

      Article first published online: 15 MAY 2014 | DOI: 10.1002/adma.201400373

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      A new prototype triboelectric nanogenerator with superhydrophobic and self-cleaning features is invented to harvest water drop energy based on a sequential contact electrification and electrostatic induction process. Because of the easy-fabrication, cost-effectiveness, and robust properties, the developed triboelectric nanogenerator expands the potential applications to harvesting energy from household wastewater and raindrops.

    11. Electronic Properties of Conjugated Polyelectrolyte/Single-Walled Carbon Nanotube Composites (pages 4697–4703)

      Yao Li, Cheng-Kang Mai, Hung Phan, Xiaofeng Liu, Thuc-Quyen Nguyen, Guillermo C. Bazan and Mary B. Chan-Park

      Article first published online: 19 MAY 2014 | DOI: 10.1002/adma.201400612

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      Two narrow-bandgap conjugated polyelectrolytes (CPEs) of identical backbone structure but different pendant charges are used to disperse single-walled carbon nanotubes (SWNTs) in MeOH. Films of the resulting CPE:SWNT composites have electrical conductivity dependent on the SWNT loading, which can be increased with acid vapor treatment. The anionic CPE gives higher electrical conductivity for the composite immediately after deposition, whereas a more-significant increase is observed for the cationic counterpart after acid treatment.

    12. Atomic Layer Deposited Gallium Oxide Buffer Layer Enables 1.2 V Open-Circuit Voltage in Cuprous Oxide Solar Cells (pages 4704–4710)

      Yun Seog Lee, Danny Chua, Riley E. Brandt, Sin Cheng Siah, Jian V. Li, Jonathan P. Mailoa, Sang Woon Lee, Roy G. Gordon and Tonio Buonassisi

      Article first published online: 23 MAY 2014 | DOI: 10.1002/adma.201401054

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      The power conversion efficiency of solar cells based on copper (I) oxide (Cu2O) is enhanced by atomic layer deposition of a thin gallium oxide (Ga2O3) layer. By improving band-alignment and passivating interface defects, the device exhibits an open-circuit voltage of 1.20 V and an efficiency of 3.97%, showing potential of over 7% efficiency.

    13. Defect-Driven Interfacial Electronic Structures at an Organic/Metal-Oxide Semiconductor Heterojunction (pages 4711–4716)

      Paul Winget, Laura K. Schirra, David Cornil, Hong Li, Veaceslav Coropceanu, Paul F. Ndione, Ajaya K. Sigdel, David S. Ginley, Joseph J. Berry, Jaewon Shim, Hyungchui Kim, Bernard Kippelen, Jean-Luc Brédas and Oliver L. A. Monti

      Article first published online: 15 MAY 2014 | DOI: 10.1002/adma.201305351

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      The electronic structure of the hybrid interface between ZnO and the prototypical organic semiconductor PTCDI is investigated via a combination of ultraviolet and X-ray photoelectron spectroscopy (UPS/XPS) and density functional theory (DFT) calculations. The interfacial electronic interactions lead to a large interface dipole due to substantial charge transfer from ZnO to 3,4,9,10-perylenetetracarboxylicdiimide (PTCDI), which can be properly described only when accounting for surface defects that confer ZnO its n-type properties.

    14. Effect of Solvent Environment on Colloidal-Quantum-Dot Solar-Cell Manufacturability and Performance (pages 4717–4723)

      Ahmad R. Kirmani, Graham H. Carey, Maged Abdelsamie, Buyi Yan, Dongkyu Cha, Lisa R. Rollny, Xiaoyu Cui, Edward H. Sargent and Aram Amassian

      Article first published online: 4 JUN 2014 | DOI: 10.1002/adma.201400577

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      The absorbing layer in state-of-the-art colloidal quantum-dot solar cells is fabricated using a tedious layer-by-layer process repeated ten times. It is now shown that methanol, a common exchange solvent, is the main culprit, as extended exposure leaches off the surface halide passivant, creating carrier trap states. Use of a high-dipole-moment aprotic solvent eliminates this problem and is shown to produce state-of-the-art devices in far fewer steps.

    15. Water Surface Assisted Synthesis of Large-Scale Carbon Nanotube Film for High-Performance and Stretchable Supercapacitors (pages 4724–4729)

      Minghao Yu, Yangfan Zhang, Yinxiang Zeng, Muhammad-Sadeeq Balogun, Kancheng Mai, Zishou Zhang, Xihong Lu and Yexiang Tong

      Article first published online: 19 MAY 2014 | DOI: 10.1002/adma.201401196

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      A kind of multiwalled carbon-nanotube (MWCNT)/polydimethylsiloxane (PDMS) film with excellent conductivity and mechanical properties is developed using a facile and large-scale water surface assisted synthesis method. The film can act as a conductive support for electrochemically active PANI nano fibers. A device based on these PANI/MWCNT/PDMS electrodes shows good and stable capacitive behavior, even under static and dynamic stretching conditions.

    16. Blue Phosphorescent Organic Light-Emitting Diodes Using an Exciplex Forming Co-host with the External Quantum Efficiency of Theoretical Limit (pages 4730–4734)

      Hyun Shin, Sunghun Lee, Kwon-Hyeon Kim, Chang-Ki Moon, Seung-Jun Yoo, Jeong-Hwan Lee and Jang-Joo Kim

      Article first published online: 19 MAY 2014 | DOI: 10.1002/adma.201400955

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      A high-efficiency blue-emitting organic light-emitting diode (OLED) approaching theoretical efficiency using an exciplex-forming co-host composed of N,N′-dicarbazolyl-3,5-benzene (mCP) and bis-4,6-(3,5-di-3-pyridylphenyl)- 2-methylpyrimidine (B3PYMPM) is fabricated. Iridium(III)bis[(4,6-difluorophenyl)- pyridinato-N,C2′]picolinate (FIrpic) is used as the emitter, which turns out to have a preferred horizontal dipole orientation in the emitting layer. The OLED shows a maximum external quantum efficiency of 29.5% (a maximum current efficiency of 62.2 cd A−1), which is in perfect agreement with the theoretical prediction.

    17. Transparent, Low-Power Pressure Sensor Matrix Based on Coplanar-Gate Graphene Transistors (pages 4735–4740)

      Qijun Sun, Do Hwan Kim, Sang Sik Park, Nae Yoon Lee, Yu Zhang, Jung Heon Lee, Kilwon Cho and Jeong Ho Cho

      Article first published online: 20 MAY 2014 | DOI: 10.1002/adma.201400918

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      A novel device architecture for preparing a transparent and low-voltage graphene pressure-sensor matrix on plastic and rubber substrates is demonstrated. The coplanar gate configuration of the graphene transistor enables a simplified procedure. The resulting devices exhibit excellent device performance, including a high transparency of ca. 80% in the visible range, a low operating voltage less than 2 V, a high pressure sensitivity of 0.12 kPa−1, and excellent mechanical durability over 2500 cycles.

    18. Remote Trap Passivation in Colloidal Quantum Dot Bulk Nano-heterojunctions and Its Effect in Solution-Processed Solar Cells (pages 4741–4747)

      Arup. K. Rath, F. Pelayo Garcia de Arquer, Alexandros Stavrinadis, Tania Lasanta, Maria Bernechea, Silke L. Diedenhofen and Gerasimos Konstantatos

      Article first published online: 4 JUN 2014 | DOI: 10.1002/adma.201400297

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      More-efficient charge collection and suppressed trap recombination in colloidal quantum dot (CQD) solar cells is achieved by means of a bulk nano-heterojunction (BNH) structure, in which p-type and n-type materials are blended on the nanometer scale. The improved performance of the BNH devices, compared with that of bilayer devices, is displayed in higher photocurrents and higher open-circuit voltages (resulting from a trap passivation mechanism).

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