Advanced Materials

Cover image for Vol. 28 Issue 20

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

  1. Communications

    1. Chemical Dealloying Derived 3D Porous Current Collector for Li Metal Anodes

      Qinbai Yun, Yan-Bing He, Wei Lv, Yan Zhao, Baohua Li, Feiyu Kang and Quan-Hong Yang

      Version of Record online: 24 MAY 2016 | DOI: 10.1002/adma.201601409

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      A 3D porous Cu current collector is fabricated through chemical dealloying from a commerial Cu-Zn alloy tape. The interlinked porous framework naturally integrated can accommodate Li deposition, suppressing dendrite growth and alleviating the huge volume change during cycling. The Li metal anode combined with such a porous Cu collector demonstrates excellent performance and commerial potentials in Li-based secondary batteries.

    2. A Surface-Confined Proton-Driven DNA Pump Using a Dynamic 3D DNA Scaffold

      Dan Zhu, Hao Pei, Guangbao Yao, Lihua Wang, Shao Su, Jie Chao, Lianhui Wang, Ali Aldalbahi, Shiping Song, Jiye Shi, Jun Hu, Chunhai Fan and Xiaolei Zuo

      Version of Record online: 24 MAY 2016 | DOI: 10.1002/adma.201506407

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      Here, a proton-driven molecular pump is devised using a surface-confined dynamic 3D DNA scaffold. A dynamic DNA tetrahedral nanostructure is designed by incorporating a pH-sensitive i-motif sequence in one edge, which serves as the scaffold to ensure highly ordered orientation and spatial isolation of this nanomachine on the macroscopic gold surface. It is found that the switching ability of this dynamic tetrahedron is fully maintained on the surface. Importantly, this proton-driven nanomachine can reversibly pump water and ferricynide in response to pH variation in solution.

    3. Full-Polarization 3D Metasurface Cloak with Preserved Amplitude and Phase

      Yihao Yang, Liqiao Jing, Bin Zheng, Ran Hao, Wenyan Yin, Erping Li, Costas M. Soukoulis and Hongsheng Chen

      Version of Record online: 24 MAY 2016 | DOI: 10.1002/adma.201600625

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      A full-polarization arbitrary-shaped 3D metasurface cloak with preserved amplitude and phase in microwave frequencies is experimentally demonstrated. By taking the unique feature of metasurfaces, it is shown that the cloak can completely restore the polarization, amplitude, and phase of light for full polarization as if light was incident on a flat mirror.

    4. Ultrafast Response p-Si/n-ZnO Heterojunction Ultraviolet Detector Based on Pyro-Phototronic Effect

      Zhaona Wang, Ruomeng Yu, Xingfu Wang, Wenzhuo Wu and Zhong Lin Wang

      Version of Record online: 24 MAY 2016 | DOI: 10.1002/adma.201600884

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      Here, light-self-induced pyro-phototronic effect in wurtzite ZnO nanowires has been proposed as an effective approach to achieve ultrafast response ultraviolet sensing in p-Si/n-ZnO heterostructures. The relatively long response/recovery time of zinc oxide-based ultraviolet sensors in air/vacuum has long been an obstacle to developing such detectors for practical applications. The response/recovery time and photoresponsivity are greatly improved by the pyro-phototronic effect.

    5. 3D Freeze-Casting of Cellular Graphene Films for Ultrahigh-Power-Density Supercapacitors

      Yuanlong Shao, Maher F. El-Kady, Cheng-Wei Lin, Guanzhou Zhu, Kristofer L. Marsh, Jee Youn Hwang, Qinghong Zhang, Yaogang Li, Hongzhi Wang and Richard B. Kaner

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201506157

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      3D cellular graphene films with open porosity, high electrical conductivity, and good tensile strength, can be synthesized by a method combining freeze-casting and filtration. The resulting supercapacitors based on 3D porous reduced graphene oxide (RGO) film exhibit extremely high specific power densities and high energy densities. The fabrication process provides an effective means for controlling the pore size, electronic conductivity, and loading mass of the electrode materials, toward devices with high energy-storage performance.

  2. Progress Reports

    1. Synthetic Two-Dimensional Materials: A New Paradigm of Membranes for Ultimate Separation

      Zhikun Zheng, Ronny Grünker and Xinliang Feng

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201506237

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      2D materials with a thickness of one to a few atoms, or monomer units, minimize transport resistance and maximize permeate flux, offering membranes for ultimate separation. Recent advances in the synthesis and fabrication of 2D materials, including functional graphene oxide, 2D transition-metal dichalcogenides, 2D polymers, 2D metal–organic frameworks and carbon nanomembranes are discussed, holding great potential for gas and ion separation, and water desalination.

  3. Communications

    1. Photoresponsive Cyanostilbene Bent-Core Liquid Crystals as New Materials with Light-Driven Modulated Polarization

      Marta Martínez-Abadía, Beatriz Robles-Hernández, María Rosario de la Fuente, Raquel Giménez and Maria Blanca Ros

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201600311

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      Two isomeric cyanostilbene photoswitchable bent-core mesogens with polar liquid crystal phases in which macroscopic polarization and luminescence can be light-modulated are claimed. Z/E isomerization or [2+2] cycloaddition photochemical processes occur depending on the chemical structure, which make the compounds very innovative multifunctional advanced materials.

    2. Giant Resistive Switching via Control of Ferroelectric Charged Domain Walls

      Linze Li, Jason Britson, Jacob R. Jokisaari, Yi Zhang, Carolina Adamo, Alexander Melville, Darrell G. Schlom, Long-Qing Chen and Xiaoqing Pan

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201600160

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      Controlled switching of resistivity in ferroelectric thin films is demonstrated by writing and erasing stable, nanoscale, strongly charged domain walls using an in situ transmission electron microscopy technique. The resistance can be read nondestructively and presents the largest off/on ratio (≈105) ever reported in room temperature ferroelectric devices, opening new avenues for engineering ferroelectric thin film devices.

    3. Blocking Oxidation Failures of Carbon Nanotubes through Selective Protection of Defects

      Chuan-Fu Sun, Bryan J. Glaz, Morihiro Okada, Edward Baker III, Xi-Yuan Cheng, Shashi P. Karna and YuHuang Wang

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201601027

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      The selective growth of Al2O3 islands over defect sites on carbon nanotube surface significantly increases oxidation breakdown thresholds to 6.8 W cm−2, more than double than that of unprotected films. The elevated input power enables thermoacoustic emissions at loud audible sound pressure levels of 90.1 dB that are inaccessible with the unprotected films.

  4. Reviews

    1. Perovskite Materials for Light-Emitting Diodes and Lasers

      Sjoerd A. Veldhuis, Pablo P. Boix, Natalia Yantara, Mingjie Li, Tze Chien Sum, Nripan Mathews and Subodh G. Mhaisalkar

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201600669

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      Perovskites have sparked a revolution in photovoltaics, and their excellent optoelectronic properties hold the potential to trigger a similar advance in the field of light emission. Here, the versatility of organic–inorganic hybrid perovskites as emitters and gain media is explored, device performance/architectures, processing conditions, and working mechanisms are analyzed, and the main barriers toward market viability are addressed.

  5. Communications

    1. Dynamic Triboelectrification-Induced Electroluminescence and its Use in Visualized Sensing

      Xiao Yan Wei, Xiandi Wang, Shuang Yang Kuang, Li Su, Hua Yang Li, Ying Wang, Caofeng Pan, Zhong Lin Wang and Guang Zhu

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201600604

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      Triboelectrification-induced electroluminescence converts dynamic motion into light emission. Tribocharges resulting from the relative mechanical interactions between two dissimilar materials can abruptly and significantly alter the surrounding electric potential, exciting the electroluminescence of phosphor along the motion trajectory. The position, trajectory, and contour profile of a moving object can be visualized in high resolution, demonstrating applications in sensing.

    2. Structured Liquids with pH-Triggered Reconfigurability

      Caili Huang, Zhiwei Sun, Mengmeng Cui, Feng Liu, Brett A. Helms and Thomas P. Russell

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201600691

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      Through pH-tuning of electrostatic interactions between polymer ligands and nanoparticles at structured-liquid interfaces, liquid droplets can be directed between a jammed nonequilibrium state and a dynamic reconfigurable state. The nanoparticle-surfactant dynamics highly depends on the pH, so that the liquids can be structured using an external field and under variation of pH, or alternatively being realized by remote photo-triggering.

    3. Dithienylthienothiophenebisimide, a Versatile Electron-Deficient Unit for Semiconducting Polymers

      Masahiko Saito, Itaru Osaka, Yosuke Suda, Hiroyuki Yoshida and Kazuo Takimiya

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201601373

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      A novel electron-deficient building unit, dithienylthienothiophenebisimide, and its polymers (PTBIs) are reported. Organic photovoltaic (OPV) cells based on PTBIs as p-type material exhibit 8.0% efficiencies with open-circuit voltages higher than 1 V. Interestingly, PTBIs also function as n-type material in OPVs depending on the molecular structure. These polymers also exhibit p-channel, n-channel, and ambipolar behaviors in field-effect transistors.

    4. A Supramolecular Shear-Thinning Anti-Inflammatory Steroid Hydrogel

      Qian Liu, Changyou Zhan, Aoune Barhoumi, Weiping Wang, Claudia Santamaria, James Brian McAlvin and Daniel S. Kohane

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201601147

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      Shear-thinning and self-healing steroid-drug-based hydrogels are presented, which exhibit rapid and complete recovery of their mechanical properties within seconds following stress-induced flow. The hydrogels release steroid drug in vivo with no visible residue when release is complete.

    5. Evaluation of Small Molecules as Front Cell Donor Materials for High-Efficiency Tandem Solar Cells

      Qian Zhang, Xiangjian Wan, Feng Liu, Bin Kan, Miaomiao Li, Huanran Feng, Hongtao Zhang, Thomas P. Russell and Yongsheng Chen

      Version of Record online: 23 MAY 2016 | DOI: 10.1002/adma.201601435

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      Three small molecules as front cell donors for tandem cells are thoroughly evaluated and a high power conversion efficiency of 11.47% is achieved, which demonstrates that the oligomer-like small molecules offer a good choice for high-performance tandem solar cells.

    6. Recyclable Crosslinked Polymer Networks via One-Step Controlled Radical Polymerization

      Kailong Jin, Lingqiao Li and John M. Torkelson

      Version of Record online: 20 MAY 2016 | DOI: 10.1002/adma.201600871

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      A nitroxide-mediated polymerization strategy allows one-step synthesis of recyclable crosslinked polymeric materials from any monomers or polymers that contain carbon–carbon double bonds amenable to radical polymerization. The resulting materials with dynamic covalent bonds can show full property recovery after multiple melt-reprocessing recycles. This one-step strategy provides for both robust, relatively sustainable recyclability of crosslinked polymers and design of networks for advanced technologies.

    7. High-Performance 2D Rhenium Disulfide (ReS2) Transistors and Photodetectors by Oxygen Plasma Treatment

      Jaewoo Shim, Aely Oh, Dong-Ho Kang, Seyong Oh, Sung Kyu Jang, Jaeho Jeon, Min Hwan Jeon, Minwoo Kim, Changhwan Choi, Jaehyeong Lee, Sungjoo Lee, Geun Young Yeom, Young Jae Song and Jin-Hong Park

      Version of Record online: 20 MAY 2016 | DOI: 10.1002/adma.201601002

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      A high-performance ReS2-based thin-film transistor and photodetector with high on/off-current ratio (104), high mobility (7.6 cm2 V−1 s−1), high photoresponsivity (2.5 × 107 A W−1), and fast temporal response (rising and decaying time of 670 ms and 5.6 s, respectively) through O2 plasma treatment are reported.

    8. Superhard Monoborides: Hardness Enhancement through Alloying in W1−xTaxB

      Michael T. Yeung, Jialin Lei, Reza Mohammadi, Christopher L. Turner, Yue Wang, Sarah H. Tolbert and Richard B. Kaner

      Version of Record online: 20 MAY 2016 | DOI: 10.1002/adma.201601187

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      In tungsten monoboride (WB), the boron atoms are linked in parallel serpentine arrays, with tungsten atoms in between. This lattice is metallic, unlike conventional covalent superhard materials such as diamond or cubic boron nitride. By selectively substituting tungsten atoms with tantalum, the Vickers hardness can be increased to 42.8 GPa, creating a new superhard metal.

    9. Implementing Metal-to-Ligand Charge Transfer in Organic Semiconductor for Improved Visible-Near-Infrared Photocatalysis

      Yanrui Li, Zhaowu Wang, Tong Xia, Huanxin Ju, Ke Zhang, Ran Long, Qian Xu, Chengming Wang, Li Song, Junfa Zhu, Jun Jiang and Yujie Xiong

      Version of Record online: 20 MAY 2016 | DOI: 10.1002/adma.201601960

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      The coordination of organic semiconductor with metal cations can induce metal-to-ligand charge transfer which broadens light absorption to cover visible-near-infrared (vis–NIR) spectrum. As a proof-of-concept demonstration, the g-C3N4–based complex exhibits dramatically enhanced photocatalytic H2 production with excellent durability under vis–NIR irradiation.

    10. Flexible Rechargeable Zinc-Air Batteries through Morphological Emulation of Human Hair Array

      Jing Fu, Fathy Mohamed Hassan, Jingde Li, Dong Un Lee, Abdul Rahman Ghannoum, Gregory Lui, Md. Ariful Hoque and Zhongwei Chen

      Version of Record online: 19 MAY 2016 | DOI: 10.1002/adma.201600762

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      An electrically rechargeable, nanoarchitectured air electrode that morphologically emulates human hair array is demonstrated on a zinc-air battery. The hair-like array of mesoporous cobalt oxide nanopetals in nitrogen-doped carbon nanotubes is grown directly on a stainless-steel mesh. This electrode produces both flexibility and improved battery performance, and thus fully manifests the advantages of flexible rechargeable zinc-air batteries in practical applications.

    11. Nanoscale Electrodes for Flexible Electronics by Swelling Controlled Cracking

      Qiang Zhao, Wenjun Wang, Jinyou Shao, Xiangming Li, Hongmiao Tian, Lu Liu, Xuesong Mei, Yucheng Ding and Bingheng Lu

      Version of Record online: 19 MAY 2016 | DOI: 10.1002/adma.201601007

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      Nanogap electrodes are realized using pre-patterned electrodes and a swelling controlled cracking method. Parallel fabrication of nanogap electrodes on flexible substrate can be achieved using this method. This swelling controlled cracking method is promising for fabricating high-performance flexible electronics. UV photodetector with ZnO nanoparticle-bridged nanogap electrodes exhibit high responsivity and external quantum efficiency.

    12. Anisotropic Slippery Surfaces: Electric-Driven Smart Control of a Drop's Slide

      Tianqi Guo, Pengda Che, Liping Heng, Lizhen Fan and Lei Jiang

      Version of Record online: 19 MAY 2016 | DOI: 10.1002/adma.201601239

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      Anisotropic slippery surfaces composed of directional, porous, conductive poly(3-hexylthiophene) (P3HT) fibers, and silicone oil exhibit excellent anisotropic sliding properties for several liquid droplets and the reversible control of conductive liquid droplets sliding on these surfaces under the application of voltage.

    13. A Centrosymmetric Hexagonal Magnet with Superstable Biskyrmion Magnetic Nanodomains in a Wide Temperature Range of 100–340 K

      Wenhong Wang, Ying Zhang, Guizhou Xu, Licong Peng, Bei Ding, Yue Wang, Zhipeng Hou, Xiaoming Zhang, Xiyang Li, Enke Liu, Shouguo Wang, Jianwang Cai, Fangwei Wang, Jianqi Li, Fengxia Hu, Guangheng Wu, Baogen Shen and Xi-Xiang Zhang

      Version of Record online: 18 MAY 2016 | DOI: 10.1002/adma.201600889

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      Superstable biskyrmion magnetic nanodomains are experimentally observed for the first time in a hexagonal MnNiGa, a common and easily produced centrosymmetric material. The biskyrmion states in MnNiGa thin plates, as determined by the combination of in situ Lorentz transmission electron microscopy images, magnetoresistivity, and topological Hall effect measurements, are surprisingly stable over a broad temperature range of 100–340 K.

    14. Organolead Halide Perovskites for Low Operating Voltage Multilevel Resistive Switching

      Jaeho Choi, Sunghak Park, Joohee Lee, Kootak Hong, Do-Hong Kim, Cheon Woo Moon, Gyeong Do Park, Junmin Suh, Jinyeon Hwang, Soo Young Kim, Hyun Suk Jung, Nam-Gyu Park, Seungwu Han, Ki Tae Nam and Ho Won Jang

      Version of Record online: 18 MAY 2016 | DOI: 10.1002/adma.201600859

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      Organolead halide perovskites have been used for low operating voltage multilevel resistive switching. Ag/CH3NH3PbI3/Pt cells exhibit electroforming-free resistive switching at an electric field of 3.25 × 103 V cm–1 for four distinguishable ON-state resistance levels. The migration of iodine interstitials and vacancies with low activation energies is responsible for the low electric field resistive switching via filament formation and annihilation.

    15. Synthesis of Organized Layered Carbon by Self-Templating of Dithiooxamide

      Jingsan Xu, Jixin Zhu, Xiaofei Yang, Shaowen Cao, Jiaguo Yu, Menny Shalom and Markus Antonietti

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600707

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      An unusual, small-molecule dithiooxamide is used to produce nanostructured carbon via direct pyrolysis. The carbon shows a unique 2D-layer assembled structure and is in situ dual-heteroatom (N and S) doped, meanwhile having relatively high surface area. The carbon materials can be further decorated with inorganic parts via a precomplexing approach. The functionalized carbon and the hybrid nanomaterials demonstrate remarkable performance for lithium-ion storage.

    16. Persistent State-of-Charge Heterogeneity in Relaxed, Partially Charged Li1−xNi1/3Co1/3Mn1/3O2 Secondary Particles

      William E. Gent, Yiyang Li, Sungjin Ahn, Jongwoo Lim, Yijin Liu, Anna M. Wise, Chirranjeevi Balaji Gopal, David N. Mueller, Ryan Davis, Johanna Nelson Weker, Jin-Hwan Park, Seok-Kwang Doo and William C. Chueh

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201601273

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      Ex situ transmission X-ray microscopy reveals micron-scale state-of-charge heterogeneity in solid-solution Li1−xNi1/3Co1/3Mn1/3O2 secondary particles even after extensive relaxation. The heterogeneity generates overcharged domains at the cutoff voltage that may accelerate capacity fade and increase impedance with extended cycling. It is proposed that optimized secondary structures can minimize the state-of-charge heterogeneity by mitigating the buildup of nonuniform internal stresses associated with volume changes during charge.

    17. Spontaneous Patterning of High-Resolution Electronics via Parallel Vacuum Ultraviolet

      Xuying Liu, Masayuki Kanehara, Chuan Liu, Kenji Sakamoto, Takeshi Yasuda, Jun Takeya and Takeo Minari

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201506151

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      Spontaneous patterning technique via parallel vacuum ultraviolet is developed for fabricating large-scale, complex electronic circuits with 1 μm resolution. The prepared organic thin-film transistors exhibit low contact resistance of 1.5 kΩ cm, high mobility of 0.3 and 1.5 cm2 V−1 s−1 in the devices with the channel lengths of 1 and 5 μm, respectively.

    18. Engineering Bandgaps of Monolayer MoS2 and WS2 on Fluoropolymer Substrates by Electrostatically Tuned Many-Body Effects

      Bo Liu, Weijie Zhao, Zijing Ding, Ivan Verzhbitskiy, Linjun Li, Junpeng Lu, Jianyi Chen, Goki Eda and Kian Ping Loh

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201504876

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      Intrinsic electrical and excitonic properties of monolayer transition-metal dichalcogenides can be revealed on CYTOP fluoropolymer substrates with greatly suppressed unintentional doping and dielectric screening. Ambipolar transport behavior is observed in monolayer WS2 by applying solid-state back gates. The excitonic properties of monolayer MoS2 and WS2 are determined by intricate interplays between the bandgap renormalization, Pauli blocking, and carrier screening against carrier doping.

  6. Reviews

    1. Physical, Chemical, and Biological Structures based on ROS-Sensitive Moieties that are Able to Respond to Oxidative Microenvironments

      Christos Tapeinos and Abhay Pandit

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201505376

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      Reactive oxygen species (ROS)-sensitive structures with different architectures and properties, able to respond to oxidative microenvironments, are widely used as drug carriers, imaging probes, prodrugs, and prochelators. These structures exploit the increased levels of ROS found in damaged and/or hypoxic tissues and alter their properties (morphology, release profile, fluorescence intensity, etc.) accordingly. The properties of these structures, as well as their applications are described.

  7. Communications

    1. Ultrastiff and Strong Graphene Fibers via Full-Scale Synergetic Defect Engineering

      Zhen Xu, Yingjun Liu, Xiaoli Zhao, Li Peng, Haiyan Sun, Yang Xu, Xibiao Ren, Chuanhong Jin, Peng Xu, Miao Wang and Chao Gao

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201506426

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      Kilometer-scale continuous graphene fibers (GFs) with outstanding mechanical properties and excellent electrical conductivity are produced by high-throughput wet-spinning of graphene oxide liquid crystals followed by graphitization through a full-scale synergetic defect-engineering strategy. GFs with superior performances promise wide applications in functional textiles, lightweight motors, microelectronic devices, and so on.

    2. Deep Photoacoustic/Luminescence/Magnetic Resonance Multimodal Imaging in Living Subjects Using High-Efficiency Upconversion Nanocomposites

      Yu Liu, Ning Kang, Jing Lv, Zijian Zhou, Qingliang Zhao, Lingceng Ma, Zhong Chen, Lei Ren and Liming Nie

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201506460

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      A gadolinium-doped multi-shell upconversion nanoparticle under 800 nm excitation is synthesized with a 10-fold fluorescence-intensity enhancement over that under 980 nm. The nanoformulations exhibit excellent photoacoustic/luminescence/magnetic resonance tri-modal imaging capabilities, enabling visualization of tumor morphology and microvessel distribution at new imaging depth.

    3. A Perovskite Electrocatalyst for Efficient Hydrogen Evolution Reaction

      Xiaomin Xu, Yubo Chen, Wei Zhou, Zhonghua Zhu, Chao Su, Meilin Liu and Zongping Shao

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600005

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      Perovskite oxides are demonstrated for the first time as efficient electrocatalysts for the hydrogen evolution reaction (HER) in alkaline solutions. A-site praseodymium-doped Pr0.5(Ba0.5Sr0.5)0.5Co0.8Fe0.2O3– δ (Pr0.5BSCF) exhibits dramatically enhanced HER activity and stability compared to Ba0.5Sr0.5Co0.8Fe0.2O3– δ (BSCF), superior to many well-developed bulk/nanosized nonprecious electroctatlysts. The improved HER performance originates from the modified surface electronic structures and properties of Pr0.5BSCF induced by the Pr-doping.

    4. Intrinsic Charge Transport across Phase Transitions in Hybrid Organo-Inorganic Perovskites

      Hee Taek Yi, Xiaoxi Wu, Xiaoyang Zhu and Vitaly Podzorov

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600011

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      Hall effect measurements in CH3NH3PbBr3 single crystals reveal that the charge carrier mobility follows an inverse-temperature power law dependence, μTγ, with the power exponent γ = 1.4 ± 0.1 in the cubic phase, indicating an acoustic phonon dominated carrier scattering, and γ = 0.5 ± 0.1 in the tetragonal phase, suggesting another dominant mechanism, such as a piezoelectric or space-charge scattering.

    5. A Palladium-Binding Deltarhodopsin for Light-Activated Conversion of Protonic to Electronic Currents

      Jessica Soto-Rodríguez, Zahra Hemmatian, Erik E. Josberger, Marco Rolandi and François Baneyx

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600222

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      Fusion of a palladium-binding peptide to an archaeal rhodopsin promotes intimate integration of the lipid-embedded membrane protein with a palladium hydride protonic contact. Devices fabricated with the palladium-binding deltarhodopsin enable light-activated conversion of protonic currents to electronic currents with on/off responses complete in seconds and a nearly tenfold increase in electrical signal relative to those made with the wild-type protein.

  8. Reviews

    1. Nanometals for Solar-to-Chemical Energy Conversion: From Semiconductor-Based Photocatalysis to Plasmon-Mediated Photocatalysis and Photo-Thermocatalysis

      Xianguang Meng, Lequan Liu, Shuxin Ouyang, Hua Xu, Defa Wang, Naiqin Zhao and Jinhua Ye

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600305

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      Nanometal materials play very important roles in solar-to-chemical energy conversion due to their unique catalytic and optical characteristics. Recent research achievements of nanometals regarding applications in semiconductor photocatalysis, plasmonic photocatalysis, and plasmonic photo-thermocatalysis are presented. Instructive information on how to take the advantage of nanometals in these catalytic processes for efficient artificial photosynthesis is provided.

  9. Communications

    1. A Novel Slicing Method for Thin Supercapacitors

      Hao Sun, Xuemei Fu, Songlin Xie, Yishu Jiang, Guozhen Guan, Bingjie Wang, Houpu Li and Huisheng Peng

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600506

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      Thin and flexible supercapacitors with low cost and individual variation are fabricated by a new and efficient slicing method. Tunable output voltage and energy can be realized with a high specific capacitance of 248.8 F g−1 or 150.8 F cm−3, which is well maintained before and after bending.

    2. Highly Sensitive Built-In Strain Sensors for Polymer Composites: Fluorescence Turn-On Response through Mechanochemical Activation

      Zhong'an Li, Ryan Toivola, Feizhi Ding, Jeffrey Yang, Po-Ni Lai, Tucker Howie, Gary Georgeson, Sei-Hum Jang, Xiaosong Li, Brian D. Flinn and Alex K.-Y. Jen

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600589

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      A new class of rationally designed mechanophores is developed for highly sensitive built-in strain sensors in polymer composites. These mechanophores are designed to regenerate the π-conjugation pathway between the electron donor and electron acceptor by force-induced cleavage of the covalent bond to form a fluorescent dipolar dye.

    3. High Efficiency Pb–In Binary Metal Perovskite Solar Cells

      Zhao-Kui Wang, Meng Li, Ying-Guo Yang, Yun Hu, Heng Ma, Xing-Yu Gao and Liang-Sheng Liao

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600626

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      Mixed Pb–In perovskite solar cells are fabricated by using lead(II) chloride and indium(III) chloride with methylammonium iodide. A maximum power conversion efficiency as high as 17.55% is achieved owing to the high quality of perovskites with multiple ordered crystal orientations.

    4. Strong, Twist-Stable Carbon Nanotube Yarns and Muscles by Tension Annealing at Extreme Temperatures

      Jiangtao Di, Shaoli Fang, Francisco A. Moura, Douglas S. Galvão, Julia Bykova, Ali Aliev, Mônica Jung de Andrade, Xavier Lepró, Na Li, Carter Haines, Raquel Ovalle-Robles, Dong Qian and Ray H. Baughman

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600628

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      A high-speed incandescent tension annealing process (ITAP) is used to increase the modulus and strength of twist-spun carbon nanotube yarns by up to 12-fold and 2.6-fold, respectively, provide remarkable resistance to oxidation and powerful protonating acids, and freeze yarn untwist. This twist stability enables torsional artificial muscles motors having improved performance and minimizes problematic untwist during weaving nanotube yarns.

    5. Light-Modulation of the Charge Injection in a Polymer Thin-Film Transistor by Functionalizing the Electrodes with Bistable Photochromic Self-Assembled Monolayers

      Thomas Mosciatti, Maria G. del Rosso, Martin Herder, Johannes Frisch, Norbert Koch, Stefan Hecht, Emanuele Orgiu and Paolo Samorì

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600651

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      High fatigue resistance, bistability, and drastic property changes among isomers allow efficient modulation of the current output of organic thin-film transistors (OTFTs) to be obtained by a photogating of the charge-injection mechanism.

    6. Harnessing Buckling to Design Architected Materials that Exhibit Effective Negative Swelling

      Jia Liu, Tianyu Gu, Sicong Shan, Sung H. Kang, James C. Weaver and Katia Bertoldi

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600812

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      Inspired by the need to develop materials capable of targeted and extreme volume changes during operation, numerical simulations and experiments are combined to design a new class of soft architected materials that achieve a reduction of projected surface area coverage during swelling.

    7. Near Room-Temperature Memory Devices Based on Hybrid Spin-Crossover@SiO2 Nanoparticles Coupled to Single-Layer Graphene Nanoelectrodes

      Anastasia Holovchenko, Julien Dugay, Mónica Giménez-Marqués, Ramón Torres-Cavanillas, Eugenio Coronado and Herre S. J. van der Zant

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600890

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      The charge transport properties of SCO [Fe(Htrz)2(trz)](BF4) NPs covered with a silica shell placed in between single-layer graphene electrodes are reported. A reproducible thermal hysteresis loop in the conductance above room-temperature is evidenced. This bistability combined with the versatility of graphene represents a promising scenario for a variety of technological applications but also for future sophisticated fundamental studies.

    8. Hierarchical Assemblies of Carbon Nanotubes for Ultraflexible Li-Ion Batteries

      Shahab Ahmad, Davor Copic, Chandramohan George and Michael De Volder

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600914

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      The flexible batteries that are needed to power flexible circuits and displays remain challenging, despite considerable progress in the fabrication of such devices. Here, it is shown that flexible batteries can be fabricated using arrays of carbon nanotube microstructures, which decouple stress from the energy-storage material. It is found that this battery architecture imparts exceptional flexibility (radius ≈ 300 μm), high rate (20 A g−1), and excellent cycling stability.

    9. From ScOOH to Sc2O3: Phase Control, Luminescent Properties, and Applications

      Baozhou Zhao, Xiaoji Xie, Shuilin Xu, Yue Pan, Bingxiao Yang, Shaohong Guo, Tian Wei, Haiquan Su, Haibo Wang, Xinqi Chen, Vinayak P. Dravid, Ling Huang and Wei Huang

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600960

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      In the controlled synthesis of ScOOH nanomaterials, the surfactant molecule Na3Cit not only helps to manipulate the crystallographic structures, but also to initiate the transfer from α-ScOOH to γ-ScOOH. Further annealing of ScOOH generates cubic Sc2O3 with morphologies inherited from respective origins. When doped with lanthanide ions, both ScOOH and Sc2O3 can be utilized for high-temperature probing and light-emitting-diode lighting.

    10. Thin Insulating Tunneling Contacts for Efficient and Water-Resistant Perovskite Solar Cells

      Qi Wang, Qingfeng Dong, Tao Li, Alexei Gruverman and Jinsong Huang

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201600969

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      Tunneling contacts made of any insulating polymers, a champion technology in silicon solar cells, has been shown to increase the stabilized efficiency of perovskite solar cells (PSCs) to 20.3%. The tunneling layers spatially separate photo-generated electrons and holes at the perovskite-cathode interface and reduce charge recombination. The tunneling layers made of hydrophobic polymers also significantly enhance the resistance of PSCs to water-caused damage.

    11. You have full text access to this OnlineOpen article
      Double-Network Hydrogels Strongly Bondable to Bones by Spontaneous Osteogenesis Penetration

      Takayuki Nonoyama, Susumu Wada, Ryuji Kiyama, Nobuto Kitamura, Md.Tariful Islam Mredha, Xi Zhang, Takayuki Kurokawa, Tasuku Nakajima, Yasuaki Takagi, Kazunori Yasuda and Jian Ping Gong

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201601030

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      Implanting hydroxyapatite-mineralized tough hydrogel into osteochondral defects of rabbits, osteogenesis spontaneously penetrates into the gel matrix owing to the semi-permeablility of the hydrogel. The gradient layer (around 40 μm thick) contributes quite strong bonding of the gel to bone. This is the first success in realizing the robust osteointegration of tough hydrogels, and the method is simple and feasible for practical use.

    12. Near-Infrared Upconversion Chemodosimeter for In Vivo Detection of Cu2+ in Wilson Disease

      Yi Liu, Qianqian Su, Min Chen, Yi Dong, Yibing Shi, Wei Feng, Zhi-Ying Wu and Fuyou Li

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201601140

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      Near-infrared upconversion chemodosimetry is a promising detection method by virtue of the frequency upconversion technique, which shows very high sensitivity and selectivity for the detection of Cu2+ ions in vitro and in vivo. This method offers a new opportunity for noninvasive diagnosis of Wilson disease associated with Cu2+ detection in clinical medicine.

    13. Design of Mixed-Metal Silver Decamolybdate Nanostructures for High Specific Energies at High Power Density

      Vipin Kumar, Sebastian Matz, Dirk Hoogestraat, Venkateswarlu Bhavanasi, Kaushik Parida, Katharina Al-Shamery and Pooi See Lee

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201601158

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      Mixed-metal molybdates are interesting host materials for ion-insertion electrodes due to their versatile crystal chemistry, which confers a highway for the conduction of electrons as well as ions. Silver decamolybdate in triclinic crystal structure (T-Ag6Mo10O33) consists of layers of MoO6 octahedra separated by arrays of silver ions that are able to store a high amount of charges.

    14. Simple Spinning of Heterogeneous Hollow Microfibers on Chip

      Yue Yu, Wenbo Wei, Yaqing Wang, Cong Xu, Yaqiong Guo and Jianhua Qin

      Version of Record online: 17 MAY 2016 | DOI: 10.1002/adma.201601504

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      A novel and simple chip-based microfluidic strategy is proposed for continuously controlled spinning of desirable hollow microfibers. These fabricated fiber-shaped materials exhibit extraordinary morphological and structural complexity, as well as a heterogeneous composition. The resulting specific hollow microfibers have potential applications in numerous chemical and biomedical fields.

  10. Progress Reports

    1. Halide Perovskites: Poor Man's High-Performance Semiconductors

      Constantinos C. Stoumpos and Mercouri G. Kanatzidis

      Version of Record online: 13 MAY 2016 | DOI: 10.1002/adma.201600265

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      Halide perovskites are a promising new class of semiconductors that deliver clean energy from inexpensive inorganic materials. Perovskite materials compete in conversion efficiency with classical inorganic semiconductors and promise a bright future toward exploitation of cheap, clean energy resources. Understanding how these materials actually work poses the main challenge in contemporary materials science research.

  11. Communications

    1. A Flexible UV–Vis–NIR Photodetector based on a Perovskite/Conjugated-Polymer Composite

      Shan Chen, Changjiu Teng, Miao Zhang, Yingru Li, Dan Xie and Gaoquan Shi

      Version of Record online: 13 MAY 2016 | DOI: 10.1002/adma.201600468

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      A lateral photodetector based on the bilayer composite film of a perovskite and a conjugated polymer is reported. It exhibits significantly enhanced responsivity in the UV–vis region and sensitive photoresponse in the near-IR (NIR) region at a low applied voltage. This broadband photodetector also shows excellent mechanical flexibility and improved environmental stability.

    2. Flexible Transparent Molybdenum Trioxide Nanopaper for Energy Storage

      Bin Yao, Liang Huang, Jing Zhang, Xiang Gao, Jiabin Wu, Yongliang Cheng, Xu Xiao, Bo Wang, Yat Li and Jun Zhou

      Version of Record online: 13 MAY 2016 | DOI: 10.1002/adma.201600529

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      A flexible transparent molybdenum trioxide nanopaper, assembled via ultralong molybdenum trioxide nanobelts, displays an excellent average transmittance of ≈90% in the visible region. The free-standing nanopaper electrode delivers an outstanding specific capacitance of 1198 F g−1 and shows an excellent long-term stability performance over 20 000 cycles with a retention rate of 99.1%.

    3. High Pressure Chemical Vapor Deposition of Hydrogenated Amorphous Silicon Films and Solar Cells

      Rongrui He, Todd D. Day, Justin R. Sparks, Nichole F. Sullivan and John V. Badding

      Version of Record online: 13 MAY 2016 | DOI: 10.1002/adma.201600415

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      Thin films of hydrogenated amorphous silicon can be produced at MPa pressures from silane without the use of plasma at temperatures as low as 345 °C. High pressure chemical vapor deposition may open a new way to low cost deposition of amorphous silicon solar cells and other thin film structures over very large areas in very compact, simple reactors.

    4. Bandgap Restructuring of the Layered Semiconductor Gallium Telluride in Air

      Jose J. Fonseca, Sefaattin Tongay, Mehmet Topsakal, Annabel R. Chew, Alan J. Lin, Changhyun Ko, Alexander V. Luce, Alberto Salleo, Junqiao Wu and Oscar D. Dubon

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201601151

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      A giant bandgap reduction in layered GaTe is demonstrated. Chemisorption of oxygen to the Te-terminated surfaces produces significant restructuring of the conduction band resulting in a bandgap below 0.8 eV, compared to 1.65 eV for pristine GaTe. Localized partial recovery of the pristine gap is achieved by thermal annealing demonstrating that reversible band engineering in layered semiconductors is accessible through their surfaces.

    5. Co3O4 Hexagonal Platelets with Controllable Facets Enabling Highly Efficient Visible-Light Photocatalytic Reduction of CO2

      Chao Gao, Qiangqiang Meng, Kun Zhao, Huajie Yin, Dawei Wang, Jun Guo, Shenlong Zhao, Lin Chang, Meng He, Qunxiang Li, Huijun Zhao, Xingjiu Huang, Yan Gao and Zhiyong Tang

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201601387

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      A heterogeneous catalyst made of well-defined Co3O4 hexagonal platelets with varied exposed facets is coupled with [Ru(bpy)3]Cl2 photosensitizers to effectively and efficiently reduce CO2 under visible-light irradiation. Systematic investigation based on both experiment and theory discloses that the exposed {112} facets are crucial for activating CO2 molecules, giving rise to significant enhancement of photocatalytic CO2 reduction efficiency.

    6. Increasing Polymer Solar Cell Fill Factor by Trap-Filling with F4-TCNQ at Parts Per Thousand Concentration

      Han Yan, Joseph G. Manion, Mingjian Yuan, F. Pelayo García de Arquer, George R. McKeown, Serge Beaupré, Mario Leclerc, Edward H. Sargent and Dwight S. Seferos

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201601553

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      Intrinsic traps in organic semiconductors can be eliminated by trap-filling with F4-TCNQ. Photovoltaic tests show that devices with F4-TCNQ at parts per thousand concentration outperform control devices due to an improved fill factor. Further studies confirm the trap-filling pathway and demonstrate the general nature of this finding.

    7. High Conductivity in Molecularly p-Doped Diketopyrrolopyrrole-Based Polymer: The Impact of a High Dopant Strength and Good Structural Order

      Yevhen Karpov, Tim Erdmann, Ivan Raguzin, Mahmoud Al-Hussein, Marcus Binner, Uwe Lappan, Manfred Stamm, Kirill L. Gerasimov, Tetyana Beryozkina, Vasiliy Bakulev, Denis V. Anokhin, Dimitri A. Ivanov, Florian Günther, Sibylle Gemming, Gotthard Seifert, Brigitte Voit, Riccardo Di Pietro and Anton Kiriy

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201506295

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      [3]-Radialene-based dopant CN6-CP studied herein, with its reduction potential of +0.8 versus Fc/Fc+ and the lowest unoccupied molecular orbital level of −5.87 eV, is the strongest molecular p-dopant reported in the open literature, so far. The efficient p-doping of the donor–acceptor dithienyl-diketopyrrolopyrrole-based copolymer having the highest unoccupied molecular orbital level of −5.49 eV is achieved. The doped films exhibit electrical conductivities up to 70 S cm−1.

    8. Novel Emitting System Based on a Multifunctional Bipolar Phosphor: An Effective Approach for Highly Efficient Warm-White Light-Emitting Devices with High Color-Rendering Index at High Luminance

      Mingxu Du, Yansong Feng, Dongxia Zhu, Tai Peng, Yu Liu, Yue Wang and Martin R. Bryce

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201600451

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      A three-color warm-white organic light-emitting diode employing an efficient phosphor–phosphor type host–guest emitting system achieves efficiencies of 27.3% for external quantum efficiency and 74.5 lm W–1 for power efficiency at a luminance of 1000 cd m–2, which maintained the high levels of 24.3% and 45.8 lm W−1 at 10 000 cd m−2, with a stable color-rendering index of 86–87.

    9. Acceptor End-Capped Oligomeric Conjugated Molecules with Broadened Absorption and Enhanced Extinction Coefficients for High-Efficiency Organic Solar Cells

      Liu Yuan, Kun Lu, Benzheng Xia, Jianqi Zhang, Zhen Wang, Zaiyu Wang, Dan Deng, Jin Fang, Lingyun Zhu and Zhixiang Wei

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201600512

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      Acceptor end-capping of oligomeric conjugated molecules is found to be an effective strategy for simultaneous spectra broadening, extinction coefficient enhancement, and energy level optimization, resulting in profoundly enhanced power conversion efficiencies (of 9.25% and 8.91%) compared to the original oligomers. This strategy is effective in overcoming the absorption disadvantage of oligomers and small molecules due to conjugation limitation.

    10. Modulation of Exciton Generation in Organic Active Planar pn Heterojunction: Toward Low Driving Voltage and High-Efficiency OLEDs Employing Conventional and Thermally Activated Delayed Fluorescent Emitters

      Dongcheng Chen, Kunkun Liu, Lin Gan, Ming Liu, Kuo Gao, Gaozhan Xie, Yuguang Ma, Yong Cao and Shi-Jian Su

      Version of Record online: 12 MAY 2016 | DOI: 10.1002/adma.201600612

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      OLEDs combining low driving voltage and high efficiency are designed by employing conventional and thermally activated delayed fluorescence emitters through modulation of excitons generated at the planar pn heterojunction region. To date, this approach enables the highest power efficiency for yellow-green emitting fluorescent OLEDs with a simplified structure.

    11. PDMS-Based Elastomer Tuned Soft, Stretchable, and Sticky for Epidermal Electronics

      Seung Hee Jeong, Shuo Zhang, Klas Hjort, Jöns Hilborn and Zhigang Wu

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201505372

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      A highly soft, stretchable, and sticky polydimethylsiloxane-based elastomer is achieved by adding small fractions of an amine-based polymer. The modified elastomer is tuned with a simple mixing step and shows good processability for microstructure fabrication. The modified elastomer shows excellent compatibility with an epidermal strain sensor on the human skin.

    12. Enhancing Crystalline Structural Orders of Polymer Semiconductors for Efficient Charge Transport via Polymer-Matrix-Mediated Molecular Self-Assembly

      Yanlian Lei, Ping Deng, Ming Lin, Xuelin Zheng, Furong Zhu and Beng S. Ong

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600580

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      A facile polymer-matrix-mediated molecular self-assembly of polymer semiconductors into highly crystalline orders for efficient charge transport in organic thin-film transistors is demonstrated. Phenomenal enhancements in field-effect mobility of about one order of magnitude and current on/off ratio of two to three orders of magnitude have been realized with polyacrylonitrile-incorporated polymer semiconductor compositions via solution deposition.

    13. Enhanced Efficiency and Stability of Inverted Perovskite Solar Cells Using Highly Crystalline SnO2 Nanocrystals as the Robust Electron-Transporting Layer

      Zonglong Zhu, Yang Bai, Xiao Liu, Chu-Chen Chueh, Shihe Yang and Alex K.-Y. Jen

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600619

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      Highly crystalline SnO2 is demonstrated in this study to serve as a stable and robust electron-transporting layer for high-performance perovskite solar cells. Benefiting from its high crystallinity, the relatively thick SnO2 electron-transporting layer (≈120 nm) provides respectable electron-transporting property to yield a promising power conversion efficiency (PCE, 18.8%) and over 90% of the initial PCE can retain after 30 d storage in ambient with ≈70% relative humidity.

    14. Oxidative Chemical Vapor Deposition of Neutral Hole Transporting Polymer for Enhanced Solar Cell Efficiency and Lifetime

      Won Jun Jo, Justin T. Nelson, Sehoon Chang, Vladimir Bulović, Silvija Gradečak, Michael S. Strano and Karen K. Gleason

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601221

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      The concept of a neutral hole transporting polymer is realized for the first time, by integrating patterned Cl doped poly(3,4-dimethoxythiophene) thin films into organic solar cells through a vacuum-based polymer vapor printing technique. Due to this novel polymer's neutrality, high transparency, good conductivity, and appropriate energy levels, the solar cell efficiency and lifetime are significantly enhanced.

    15. Topological Defects in Metal-Free Nanocarbon for Oxygen Electrocatalysis

      Cheng Tang, Hao-Fan Wang, Xiang Chen, Bo-Quan Li, Ting-Zheng Hou, Bingsen Zhang, Qiang Zhang, Maria-Magdalena Titirici and Fei Wei

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601406

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      A bifunctional graphene catalyst with abundant topological defects is achieved via the carbonization of natural gelatinized sticky rice to probe the underlying oxygen electrocatalytic mechanism. A nitrogen-free configuration with adjacent pentagon and heptagon carbon rings is revealed to exhibit the lowest overpotential for both oxygen reduction and evolution catalysis. The versatile synthetic strategy and novel insights on the activity origin facilitate the development of advanced metal-free carbocatalysts for a wide range of electrocatalytic applications.

    16. Colloidal Gold Nanocups with Orientation-Dependent Plasmonic Properties

      Ruibin Jiang, Feng Qin, Yejing Liu, Xing Yi Ling, Jun Guo, Minghua Tang, Si Cheng and Jianfang Wang

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601442

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      Colloidal gold nanocups are synthesized through single-vertex-initiated gold deposition on PbS nanooctahedrons and subsequent selective dissolution of the PbS component. They possess strong magnetic plasmon resonance and exhibit remarkable orientation-dependent plasmonic properties when deposited on flat substrates. They can also effectively couple s-polarized light into the interfacial region between the nanocup and substrate.

    17. Stable Hematite Nanosheet Photoanodes for Enhanced Photoelectrochemical Water Splitting

      Piangjai Peerakiatkhajohn, Jung-Ho Yun, Hongjun Chen, Miaoqiang Lyu, Teera Butburee and Lianzhou Wang

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601525

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      A vertically grown hematite nanosheet film modified with Ag nanoparticles (NPs) and Co-Pi cocatalyst exhibits a remarkably high photocurrent density of 4.68 mA cm−2 at 1.23 V versus RHE. The Ag NPs leads to significantly improved light harvesting and better charge transfer, while the Co-Pi facilitates highly stable oxygen evolution process. This photoelectrode design provides more efficient photoelectrochemical systems for solar energy conversion.

    18. Carbonized Silk Fabric for Ultrastretchable, Highly Sensitive, and Wearable Strain Sensors

      Chunya Wang, Xiang Li, Enlai Gao, Muqiang Jian, Kailun Xia, Qi Wang, Zhiping Xu, Tianling Ren and Yingying Zhang

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601572

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      A carbonized plain-weave silk fabric is fabricated into wearable and robust strain sensors, which can be stretched up to 500% and show high sensitivity in a wide strain range. This sensor can be assembled into wearable devices for detection of both large and subtle human activities, showing great potential for monitoring human motions and personal health.

    19. Selective Breaking of Hydrogen Bonds of Layered Carbon Nitride for Visible Light Photocatalysis

      Yuyang Kang, Yongqiang Yang, Li-Chang Yin, Xiangdong Kang, Lianzhou Wang, Gang Liu and Hui-Ming Cheng

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601567

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      Selective breaking hydrogen bonds of graphitic carbon nitride can introduce a couple of favorable features including increased band tails close to the band edges and created abundant pores. These features can simultaneously improve the three basic processes of photocatalysis. As a consequence, the photocatalytic hydrogen generation activity of carbon nitride under visible light is drastically increased by tens of times.

    20. Polymer Acceptor Based on Double B[LEFTWARDS ARROW]N Bridged Bipyridine (BNBP) Unit for High-Efficiency All-Polymer Solar Cells

      Xiaojing Long, Zicheng Ding, Chuandong Dou, Jidong Zhang, Jun Liu and Lixiang Wang

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601205

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      A novel polymer acceptor based on the double B[LEFTWARDS ARROW]N bridged bipyridine building block is reported. All-polymer solar cells based on the new polymer acceptor show a power conversion efficiency of as high as 6.26% at a photon energy loss of only 0.51 eV.

    21. Metal-Organic Framework-Derived Honeycomb-Like Open Porous Nanostructures as Precious-Metal-Free Catalysts for Highly Efficient Oxygen Electroreduction

      Qi-Long Zhu, Wei Xia, Tomoki Akita, Ruqiang Zou and Qiang Xu

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600979

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      Honeycomb-like porous carbon nanostructures are rationally constructed from a metal-organic framework composite. The unique architecture with uniformly distributed high-density active sites significantly enhances the electrocatalytic performance by increasing the accessible active sites and enhancing mass transport of the gas and electrolyte, rendering the resulting catalyst adequate in reaching the desired catalytic performance afforded by Pt for oxygen reduction reaction.

    22. Traceable Nanoparticle Delivery of Small Interfering RNA and Retinoic Acid with Temporally Release Ability to Control Neural Stem Cell Differentiation for Alzheimer's Disease Therapy

      Ran Zhang, Yan Li, Bingbing Hu, Zhiguo Lu, Jinchao Zhang and Xin Zhang

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600554

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      Nanoparticles that can efficiently control the differentiation of neural stem cells (NSCs) into neurons are developed for Alzheimer's disease (AD) therapy. The treatment with these nanoparticles results in an attenuation of neuronal loss and rescues the memory deficiencies in mice. The system can also be used to monitor the transplantation site, as well as the migration of NSCs in real time. Therefore, the system is proposed to open up new avenues for AD treatment.

    23. Infiltrated Porous Polymer Sheets as Free-Standing Flexible Lithium-Sulfur Battery Electrodes

      Feixiang Wu, Enbo Zhao, Daniel Gordon, Yiran Xiao, Chenchen Hu and Gleb Yushin

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600757

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      Free-standing high capacity Li2S electrodes with capacity loadings in the range from 1.5 to 3.8 mAh cm−2 have been produced by using infiltration of active materials into porous carbonized biomass sheets. The proposed electrode design can be effectively utilized for the low-cost fabrication of flexible lithium batteries with high specific energy.

    24. Stretchable E-Skin Apexcardiogram Sensor

      Insang You, Bongsoo Kim, Jaeyoon Park, Kunsuk Koh, Sangbaie Shin, Sungjune Jung and Unyong Jeong

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600720

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      A new strategy to measure the apex cardiogram with electronic skin technology is presented. An electronic skin apexcardiogram sensor, which can compensate the conventional electrocardiogram for cardiac diagnosis, is demonstrated through highly sensitive and stretchable strain sensor with gold nanoparticle composites.

    25. High-Performance Phototransistor of Epitaxial PbS Nanoplate-Graphene Heterostructure with Edge Contact

      Qisheng Wang, Yao Wen, Peng He, Lei Yin, Zhenxing Wang, Feng Wang, Kai Xu, Yun Huang, Fengmei Wang, Chao Jiang and Jun He

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601071

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      Fast infrared response (rising time = 24 ms) and ultrahigh photoconductive gain (108) are obtained in epitaxial PbS nanoplate-graphene heterostructures. Combining density functional theory with experiments, this study finds single-crystalline PbS nanoplates are covalently bound to grapheme edge with strong chemical hybridization, which offers a fast carriers transmission path.

    26. Thickness Dependence of the Quantum Anomalous Hall Effect in Magnetic Topological Insulator Films

      Xiao Feng, Yang Feng, Jing Wang, Yunbo Ou, Zhenqi Hao, Chang Liu, Zuocheng Zhang, Liguo Zhang, Chaojing Lin, Jian Liao, Yongqing Li, Li-Li Wang, Shuai-Hua Ji, Xi Chen, Xucun Ma, Shou-Cheng Zhang, Yayu Wang, Ke He and Qi-Kun Xue

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600919

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      The evolution of the quantum anomalous Hall effect with the thickness of Cr-doped (Bi,Sb)2Te3 magnetic topological insulator films is studied, which reveals how the effect is caused by the interplay of the surface states, band-bending and ferromagnetic exchange energy. Homogeneity in ferromagnetism is found to be the key to high temperature quantum anomalous Hall material.

    27. Organometal Halide Perovskite Artificial Synapses

      Wentao Xu, Himchan Cho, Young-Hoon Kim, Young-Tae Kim, Christoph Wolf, Chan-Gyung Park and Tae-Woo Lee

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201506363

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      Organometal halide perovskite synaptic devices are fabricated; they emulate important working principles of a biological synapse, including excitatory postsynaptic current, paired-pulse facilitation, short-term plasticity, long-term plasticity, and spike-timing dependent plasticity. These properties originate from possible ion migration in the ion-rich perovskite matrix. This work has extensive applicability and practical significance in neuromorphic electronics.

    28. A Furan–Thiophene-Based Quinoidal Compound: A New Class of Solution-Processable High-Performance n-Type Organic Semiconductor

      Yu Xiong, Jingwei Tao, Ruihao Wang, Xiaolan Qiao, Xiaodi Yang, Deliang Wang, Hongzhuo Wu and Hongxiang Li

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600120

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      The furan–thiophene-based quinoidal organic semiconductor, TFT-CN, is designed and synthesized. TFT-CN displays a high electron mobility of 7.7 cm2 V−1 s−1, two orders of magnitude higher than the corresponding thiophene-based derivative.

  12. Progress Reports

    1. Modulation of Immune Responses by Particulate Materials

      Filipa Lebre, Claire H. Hearnden and Ed C. Lavelle

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201505395

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      Particulate materials are increasingly used for biomedical applications. Thus, understanding of how they modulate the immune system is critical for designing systems with improved efficacy. This report describes recent progress in the immunomodulatory effects of particulate materials with a focus on underlying mechanisms.

    2. Adding Functions to Biomaterial Surfaces through Protein Incorporation

      Małgorzata A. Wronska, Iain B. O'Connor, Maura A. Tilbury, Akshay Srivastava and J. Gerard Wall

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201504310

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      Functionalization of material surfaces with biomolecules is critical to evade immunorecognition, interact with surrounding tissues and avoid bacterial colonization. The use of antibody molecules, growth factors, extracellular matrix proteins and peptides to promote endothelialization, mediate osteogeneration, impart cell-binding or prevent biofilm formation on materials is described. Recombinant protein production and chemical strategies approaches are also discussed.

  13. Reviews

    1. Amyloid Fibrils as Building Blocks for Natural and Artificial Functional Materials

      Tuomas P. J. Knowles and Raffaele Mezzenga

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201505961

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      Amyloid materials have recently been discovered at the origin of biological functionality and attention is increasingly turning towards their use in artificial materials. These roles contrast markedly with their original picture as pathological materials. A unified view of this class of functional materials, both in their natural roles and as synthetic materials, is given here, and how function emerges directly from the hierarchical protein self-assembly process is illustrated.

  14. Communications

    1. Protein-Nanoreactor-Assisted Synthesis of Semiconductor Nanocrystals for Efficient Cancer Theranostics

      Tao Yang, Yong Wang, Hengte Ke, Qiaoli Wang, Xiaoyan Lv, Hong Wu, Yongan Tang, Xiangliang Yang, Chunying Chen, Yuliang Zhao and Huabing Chen

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201506119

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      Transition metal sulfide nanocrystals are developed as a theranostic platform through the protein-nanoreactor approach with facile functionalization for multimodal NIRF/PA/SPECT/CT imaging and photothermal tumor ablation.

    2. Self-Assembled Organic Single Crystalline Nanosheet for Solution Processed High-Performance n-Channel Field-Effect Transistors

      Jin Hong Kim, Sang Kyu Park, Jong H. Kim, Dong Ryeol Whang, Won Sik Yoon and Soo Young Park

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201506387

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      Submillimeter sized n-channel organic single crystalline nanosheet based on dicyanodistyrylbenzene derivative, (2E,2′E)-3,3′-(2,5-dimethoxy-1,4-pheny­lene)bis(2-(5-(4-(trifluoromethyl)phenyl)thiophen-2-yl)acrylonitrile) (Me-4-TFPTA), is developed. Strong π–π interaction, hydrogen bonding interactions derived from cyano group ([BOND]CN) as well as solvent inclusion along the lateral direction play a key role in forming nanosheet morphology. Me-4-TFPTA nanosheets exhibit excellent field-effect electron mobility of up to 7.81 cm2 v−1 s−1.

    3. Architected Materials with Ultra-Low Porosity for Vibration Control

      Farhad Javid, Pai Wang, Ali Shanian and Katia Bertoldi

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600052

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      Periodic structures with extremely low porosities capable of forming large band gaps—frequency ranges with strong wave attenuation—are designed by patterning an elastic sheet with an array of alternating crack-like pores separated by small ligaments. The results indicate that the presence and size of the band gaps are controlled by the smallest geometric ­feature in the system (which can be easily controlled by tuning the aspect ratio of the pores), providing an important guideline for the design of systems with the ­desired response.

    4. Deepening Insights of Charge Transfer and Photophysics in a Novel Donor–Acceptor Cocrystal for Waveguide Couplers and Photonic Logic Computation

      Weigang Zhu, Lingyun Zhu, Ye Zou, Yishi Wu, Yonggang Zhen, Huanli Dong, Hongbing Fu, Zhixiang Wei, Qiang Shi and Wenping Hu

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600280

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      The charge transfer and photophysics in a new light-emitting cocrystal with ribbon-like morphology are revealed in-depth. These cocrystals can serve as an efficient 1D optical waveguide, and the cocrystal waveguide couplers fabricated by a probe-assisted crystal-moving technique exhibit interfacial white emission and can function as basic photonic logic gates, showing potential for future integrated photonics.

  15. Progress Reports

    1. Rational Co-Design of Polymer Dielectrics for Energy Storage

      Arun Mannodi-Kanakkithodi, Gregory M. Treich, Tran Doan Huan, Rui Ma, Mattewos Tefferi, Yang Cao, Gregory A. Sotzing and Rampi Ramprasad

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600377

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      A rational co-design approach in materials science involves synergistic use of computations and experiments aimed at faster and more efficient design. Recent progress in using such an approach towards the design of advanced polymer dielectrics for energy-storage applications is reviewed. A number of new, promising dielectric materials in known and novel polymer classes that have been discovered are discussed in detail.

  16. Communications

    1. Balanced Dual Emissions from Tridentate Phosphine-Coordinate Copper(I) Complexes toward Highly Efficient Yellow OLEDs

      Jing Zhang, Chunbo Duan, Chunmiao Han, He Yang, Ying Wei and Hui Xu

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600487

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      Dual emissive copper(I) halide complexes TTPPCuX (X = Cl, Br, I) with a triphosphine ligand and stable tetrahedral geometries are constructed, in which TTPPCuI successfully achieves the balanced dual thermally activated delayed fluorescence and phosphorescence (PH) emissions with PH fraction of 39% at ambient temperature, supporting the equal triplet exciton reallocation for the state-of-the-art device performance.

    2. A Nanocapsule-Based Approach Toward Physical Thermolatent Catalysis

      Ann-Christin Bijlard, Anne Hansen, Ingo Lieberwirth, Katharina Landfester and Andreas Taden

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600830

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      Performance under pressure is utilized as a key concept for colloidal control of reaction kinetics. Barrier nanocapsules containing a catalyst and a low-boiling-point release agent enable a highly desired, adjustable, and distinct non-Arrhenius behavior for thermoset curing.

    3. You have full text access to this OnlineOpen article
      Decoupling Charge Transport and Electroluminescence in a High Mobility Polymer Semiconductor

      David J. Harkin, Katharina Broch, Maximilian Schreck, Harald Ceymann, Andreas Stoy, Chaw-Keong Yong, Mark Nikolka, Iain McCulloch, Natalie Stingelin, Christoph Lambert and Henning Sirringhaus

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201600851

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      Fluorescence enhancement of a high mobility polymer semiconductor is achieved via energy transfer to a higher fluorescence quantum yield squaraine dye molecule on 50 ps timescales. In organic light emitting diodes an order of magnitude enhancement of the external quantum efficiency is observed without reduction in the charge carrier mobility resulting in radiances of up to 5 W str−1 m−2 at 800 nm.

    4. Broad Detection Range Rhenium Diselenide Photodetector Enhanced by (3-Aminopropyl)Triethoxysilane and Triphenylphosphine Treatment

      Seo-Hyeon Jo, Hyung-Youl Park, Dong-Ho Kang, Jaewoo Shim, Jaeho Jeon, Seunghyuk Choi, Minwoo Kim, Yongkook Park, Jaehyeong Lee, Young Jae Song, Sungjoo Lee and Jin-Hong Park

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601248

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      The effects of triphenylphosphine and (3-aminopropyl)triethoxysilane on a rhenium diselenide (ReSe2) photodetector are systematically studied by comparing with conventional MoS2 device. This study demonstrates a very high performance ReSe2 photodetector with high photoresponsivity (1.18 × 106 A W−1), fast photoswitching speed (rising/decaying time: 58/263 ms), and broad photodetection range (possible above 1064 nm).

    5. Harnessing Topological Band Effects in Bismuth Telluride Selenide for Large Enhancements in Thermoelectric Properties through Isovalent Doping

      Devender, Pascal Gehring, Andrew Gaul, Alexander Hoyer, Kristina Vaklinova, Rutvik J. Mehta, Marko Burghard, Theodorian Borca-Tasciuc, David J. Singh, Klaus Kern and Ganpati Ramanath

      Version of Record online: 11 MAY 2016 | DOI: 10.1002/adma.201601256

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      Dilute isovalent sulfur doping simultaneously increases electrical conductivity and Seebeck coefficient in Bi2Te2Se nanoplates, and bulk pellets made from them. This unusual trend at high electron concentrations is underpinned by multifold increases in electron effective mass attributable to sulfur-induced band topology effects, providing a new way for accessing high thermoelectric figure-of-merit in topological insulator-based nanomaterials through doping.

    6. Propeller-Like Nanorod-Upconversion Nanoparticle Assemblies with Intense Chiroptical Activity and Luminescence Enhancement in Aqueous Phase

      Xiaoling Wu, Liguang Xu, Wei Ma, Liqiang Liu, Hua Kuang, Nicholas A. Kotov and Chuanlai Xu

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201601261

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      Propeller-like nanoscale assemblies with exceptionally intense chiroptical activity and strong luminescence are prepared using gold nanorods and upconversion nanoparticles. The circular dichroism intensity of the tetramer reached 80.9 mdeg, with g-factor value of 2.1 × 10–2. The enhancement factor of upconversion luminescence is as high as 21.3 in aqueous phase. Attomolar bioanalysis of cancer biomarker with two model is also achieved, showing potential for early disease diagnosis and environmental monitoring.

    7. Metal-Organic Framework Templated Synthesis of Copper Azide as the Primary Explosive with Low Electrostatic Sensitivity and Excellent Initiation Ability

      Qianyou Wang, Xiao Feng, Shan Wang, Naimeng Song, Yifa Chen, Wenchao Tong, Yuzhen Han, Li Yang and Bo Wang

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201601371

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      A powerful yet safe primary explosive, embedded in a conductive carbon scaffold, is prepared by using a metal-organic framework as precursor. It simultaneously possesses low electrostatic sensitivity, good flame sensitivity, and excellent initiation ability. This method is simple, scalable, and provides a new platform for the development of energetic materials especially those employed in miniaturized explosive systems.

    8. A Water-Based Silver-Nanowire Screen-Print Ink for the Fabrication of Stretchable Conductors and Wearable Thin-Film Transistors

      Jiajie Liang, Kwing Tong and Qibing Pei

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201600772

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      A water-based silver-nanowire (AgNW) ink is formulated for screen printing. Screen-printed AgNW patterns have uniform sharp edges, ≈50 μm resolution, and electrical conductivity as high as 4.67 × 104 S cm−1. The screen-printed AgNW patterns are used to fabricate a stretchable composite conductor, and a fully printed and intrinsically stretchable thin-film transistor array is also realized.

    9. Flexible Metal Oxide/Graphene Oxide Hybrid Neuromorphic Transistors on Flexible Conducting Graphene Substrates

      Chang Jin Wan, Yang Hui Liu, Ping Feng, Wei Wang, Li Qiang Zhu, Zhao Ping Liu, Yi Shi and Qing Wan

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201600820

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      Flexible metal oxide/graphene oxide hybrid multi-gate neuromorphic transistors are fabricated on flexible conducting graphene substrates. Dendritic integrations in both spatial and temporal modes are emulated, and spatiotemporal correlated logics are obtained. A proof-of-principle visual system model for emulating Lobula Giant Motion Detector neuron is also investigated. The results are of great significance for flexible sensors and neuromorphic cognitive systems.

    10. Molecular Dynamics of Flexible Polar Cations in a Variable Confined Space: Toward Exceptional Two-Step Nonlinear Optical Switches

      Wei-Jian Xu, Chun-Ting He, Cheng-Min Ji, Shao-Li Chen, Rui-Kang Huang, Rui-Biao Lin, Wei Xue, Jun-Hua Luo, Wei-Xiong Zhang and Xiao-Ming Chen

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201600895

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      The changeable molecular dynamics of flexible polar cations in the variable confined space between inorganic chains brings about a new type of two-step nonlinear optical (NLO) switch with genuine “off–on–off” second harmonic generation (SHG) conversion between one NLO-active state and two NLO-inactive states.

    11. High-Performance TiO2-Based Electron-Selective Contacts for Crystalline Silicon Solar Cells

      Xinbo Yang, Qunyu Bi, Haider Ali, Kristopher Davis, Winston V. Schoenfeld and Klaus Weber

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201600926

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      Thin TiO2 films are demonstrated to be an excellent electron-selective contact for crystalline silicon solar cells. An efficiency of 21.6% is achieved for crystalline silicon solar cells featuring a full-area TiO2-based electron-selective contact.

    12. Superfluorinated PEI Derivative Coupled with 99mTc for ASGPR Targeted 19F MRI/SPECT/PA Tri-Modality Imaging

      Zhide Guo, Mengna Gao, Manli Song, Yesen Li, Deliang Zhang, Duo Xu, Linyi You, Liangliang Wang, Rongqiang Zhuang, Xinhui Su, Ting Liu, Jin Du and Xianzhong Zhang

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201601064

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      Fluorinated polyethylenimine derivative labeled with radionuclide 99mTc is developed as a 19F MRI/SPECT/PA multifunctional imaging agent with good asialoglycoprotein receptors (ASGPR)-targeting ability. This multifunctional agent is safe and suitable for 19F MRI/SPECT/PA imaging and has the potential to detect hepatic diseases and to assess liver function, which provide powerful support for the development of personalized and precision medicine.

    13. Freestanding, Hydrophilic Nitrogen-Doped Carbon Foams for Highly Compressible All Solid-State Supercapacitors

      Kang Xiao, Liang-Xin Ding, Guoxue Liu, Hongbin Chen, Suqing Wang and Haihui Wang

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201601125

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      Freestanding and highly compressible nitrogen-doped carbon foam (NCF) with excellent hydrophilicity and good electrochemical properties is prepared. Based on NCF electrodes, a high-performance all solid-state symmetric supercapacitor device is fabricated with native, full compressibility, and excellent mechanical stability, addressing two major problems in the current technology.

    14. A Robust Polyionized Hydrogel with an Unprecedented Underwater Anti-Crude-Oil-Adhesion Property

      Shoujian Gao, Jichao Sun, Pingping Liu, Feng Zhang, Wenbin Zhang, Shiling Yuan, Jingye Li and Jian Jin

      Version of Record online: 9 MAY 2016 | DOI: 10.1002/adma.201600417

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      A polyionized hydrogel polymer (sodium polyacrylate-grafted poly(vinylidene fluoride) (PAAS-g-PVDF)) is fabricated via an alkaline-induced phase-inversion process. PAAS-g-PVDF coatings exhibit unprecedented anti-adhesion and self-cleaning properties to crude oils under an aqueous environment. A PAAS-g-PVDF-coated copper mesh can effectively separate a crude oil/water mixture with extremely high flux and high oil rejection driven by gravity, and is oil-fouling-free for long-term use.

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