Advanced Materials

Cover image for Vol. 29 Issue 4

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

  1. Communications

    1. Two-Photon Luminescence and Second-Harmonic Generation in Organic Nonlinear Surface Comprised of Self-Assembled Frustum Shaped Organic Microlasers

      Dasari Venkatakrishnarao, Yemineni S. L. V. Narayana, Mahamad A. Mohaiddon, Evgeniy A. Mamonov, Nikolai Mitetelo, Irina A. Kolmychek, Anton I. Maydykovskiy, Vladimir B. Novikov, Tatiana V. Murzina and Rajadurai Chandrasekar

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605260

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      An ultrathin nonlinear optical (NLO) organic surface comprised of numerous self-assembled frustum-shaped whispering-gallery mode resonators displays both two-photon luminescence and second-harmonic generation signals. A super-second-order increase of the NLO intensity with respect to pump power confirms the microlasing action and practical usefulness of the NLO organic surfaces.

  2. Reviews

    1. Amino Acids and Peptide-Based Supramolecular Hydrogels for Three-Dimensional Cell Culture

      Xiao-Qiu Dou and Chuan-Liang Feng

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201604062

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      Interest in amino acids and peptide-based supramolecular hydrogels for 3D cell culture is increasing. This review assesses current progress in the preparation of these hydrogels under external stimuli and in situ cell encapsulation into the hydrogels, with a focus on understanding the associations between their structures, properties, and functions during cell culture and the remaining challenges.

  3. Communications

    1. Patterning Multicolored Microdisk Laser Arrays of Cesium Lead Halide Perovskite

      Xianxiong He, Peng Liu, Haihua Zhang, Qing Liao, Jiannian Yao and Hongbing Fu

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201604510

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      A polydimethylsiloxane cylindrical-hole-template-confined solution-growth method is developed to fabricate densely packed CsPbCl3− x Br x microdisk laser arrays. Furthermore, a strategy to integrate multicolored microdisk laser (MDL) arrays is demonstrated that simultaneously lase in the deep blue, blue, cyan, and green by means of gas-phase replacement of Cl by Br from initial CsPbCl3 MDLs in HBr vapor.

  4. Reviews

    1. Multi-Scale Microstructural Thermoelectric Materials: Transport Behavior, Non-Equilibrium Preparation, and Applications

      Xianli Su, Ping Wei, Han Li, Wei Liu, Yonggao Yan, Peng Li, Chuqi Su, Changjun Xie, Wenyu Zhao, Pengcheng Zhai, Qingjie Zhang, Xinfeng Tang and Ctirad Uher

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201602013

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      Recent progress on optimization of thermoelectric performance via the engineering of structures with different dimensional aspects is reviewed here, spanning from the atomic and molecular scale, to nanometer sizes, and to mesoscale which can be achieved through non-equilibrium fast and controllable synthesis. Moreover, the design of two integrated thermoelectric power generating systems are described—a solar thermoelectric-photovoltaic hybrid system and a vehicle waste heat harvesting system.

  5. Communications

    1. Fully Solution-Processed n–i–p-Like Perovskite Solar Cells with Planar Junction: How the Charge Extracting Layer Determines the Open-Circuit Voltage

      Chen Tao, Jeroen Van Der Velden, Lydia Cabau, Nuria F. Montcada, Stefanie Neutzner, Ajay Ram Srimath Kandada, Sergio Marras, Luigi Brambilla, Matteo Tommasini, Weidong Xu, Roberto Sorrentino, Andrea Perinot, Mario Caironi, Chiara Bertarelli, Emilio Palomares and Annamaria Petrozza

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201604493

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      Fully solution-processed direct perovskite solar cells with planar junction are realized by incorporating a cross-linked [6,6]-phenyl-C61-butyric styryl dendron ester layer as an electron extracting layer. Power conversion efficiencies close to 19% and an open-circuit voltage exceeding 1.1 V with negligible hysteresis are delivered. A perovskite film with superb optoelectronic qualities is grown, which reduces carrier recombination losses and hence increases V oc.

    2. Biomimetic Engineering Using Cancer Cell Membranes for Designing Compartmentalized Nanoreactors with Organelle-Like Functions

      Vimalkumar Balasubramanian, Alexandra Correia, Hongbo Zhang, Flavia Fontana, Ermei Mäkilä, Jarno Salonen, Jouni Hirvonen and Hélder A. Santos

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605375

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      A new biomimetic nanoreactor design is presented based on cancer cell membrane material in combination with porous silicon nanoparticles. This cellular nanoreactor features a biocompartment enclosed by a cell membrane and readily integrated with cells and supplementing the cellular functions under oxidative stress. The study demonstrates the impact of the nanoreactors on improving cellular functions with a potential to serve as artificial organelles.

  6. Research News

    1. New Opportunities and Challenges of Smart Polymers in Post-Translational Modification Proteomics

      Guangyan Qing, Qi Lu, Yuting Xiong, Lei Zhang, Hongxi Wang, Xiuling Li, Xinmiao Liang and Taolei Sun

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201604670

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      Protein post-translational modifications (PTMs) greatly increase protein complexity and dynamics and regulate a series of biological processes. However, protein PTM studies are severely hampered by the lack of highly efficient enrichment materials capable of capturing trace amounts of PTM peptides from highly complex biosamples. Utilizing reversible conformational transition of polymer chains in response to the binding of PTM peptides, smart polymers provide novel solutions to tackle these enrichment challenges.

  7. Communications

    1. The Formation of Defect-Pairs for Highly Efficient Visible-Light Catalysts

      Qingbo Sun, David Cortie, Shaoyang Zhang, Terry J. Frankcombe, Guangwei She, Jie Gao, Leigh R. Sheppard, Wanbiao Hu, Hua Chen, Shangjun Zhuo, Dehong Chen, Ray L. Withers, Garry McIntyre, Dehong Yu, Wensheng Shi and Yun Liu

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605123

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      Highly efficient visible-light catalysts are achieved through forming defect-pairs in TiO2 nanocrystals. This study therefore proposes that fine-tuning the chemical scheme consisting of charge-compensated defect-pairs in balanced concentrations is a key missing step for realizing outstanding photocatalytic performance. This research benefits photocatalytic applications and also provides new insight into the significance of defect chemistry for functionalizing materials.

    2. Amplified Photodegradation of Cell-Laden Hydrogels via an Addition–Fragmentation Chain Transfer Reaction

      Tobin E. Brown, Ian A. Marozas and Kristi S. Anseth

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605001

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      Hydrogels crosslinked by allyl sulfide-containing molecules are presented. By exposure to light in the presence of a photoinitiator and a free monofunctional thiol, photodegradation is achieved. Both the gelation and degradation are cytocompatible and allow for cell encapsulation and subsequent release. The photodegradation kinetics and depths attainable are superior to those of traditional cell-laden photodegradable hydrogels.

  8. Reviews

    1. Carbon-Based Functional Materials Derived from Waste for Water Remediation and Energy Storage

      Qinglang Ma, Yifu Yu, Melinda Sindoro, Anthony G. Fane, Rong Wang and Hua Zhang

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605361

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      The conversion of waste into valuable carbon-based functional materials provides a low-cost and sustainable strategy for solving problems related to water scarcity and the energy crisis. The recent developments in waste-derived carbon-based functional materials are summarized for applications in water remediation and energy storage.

  9. Communications

    1. Highly Stable Sodium Batteries Enabled by Functional Ionic Polymer Membranes

      Shuya Wei, Snehashis Choudhury, Jun Xu, Pooja Nath, Zhengyuan Tu and Lynden A. Archer

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605512

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      A sodium metal anode protected by an ion-rich polymeric membrane exhibits enhanced stability and high-Columbic efficiency cycling. Formed in situ via electropolymerization of functional imidazolium-type ionic liquid monomers, the polymer membrane protects the metal against parasitic reactions with electrolyte and, for fundamental reasons, inhibits dendrite formation and growth. The effectiveness of the membrane is demonstrated using direct visualization of sodium electrodeposition.

    2. Fast-Response Photonic Device Based on Organic-Crystal Heterojunctions Assembled into a Vertical-Yet-Open Asymmetric Architecture

      Lei Zhang, Egon Pavlica, Xiaolan Zhong, Fabiola Liscio, Songlin Li, Gvido Bratina, Emanuele Orgiu and Paolo Samorì

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605760

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      Crystalline dioctyl-3,4,9,10-perylenedicarboximide nanowires and 6,13-bis(triisopropylsilylethynyl) pentacene microplates are integrated into a vertical-yet-open asymmetrical heterojunction for the realization of a high-performance organic photovoltaic detector, which shows fast photoresponse, ultrahigh signal-to-noise ratio, and high sensitivity to weak light.

    3. Improved Reversibility of Fe3+/Fe4+ Redox Couple in Sodium Super Ion Conductor Type Na3Fe2(PO4)3 for Sodium-Ion Batteries

      Ranjusha Rajagopalan, Bo Chen, Zhicheng Zhang, Xing-Long Wu, Yonghua Du, Ying Huang, Bing Li, Yun Zong, Jie Wang, Gwang-Hyeon Nam, Melinda Sindoro, Shi Xue Dou, Hua Kun Liu and Hua Zhang

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605694

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      The methodology employed here utilizes the sodium super ion conductor type sodium iron phosphate wrapped with conducting carbon network to generate a stable Fe3+/Fe4+ redox   couple, thereby exhibiting higher operating voltage and energy density of sodium-ion batteries. This new class of sodium iron phosphate wrapped by carbon also displays a cycling stability with >96% capacity retention after 200 cycles.

    4. High Speed Epitaxial Perovskite Memory on Flexible Substrates

      Saidur R. Bakaul, Claudy R. Serrao, Oukjae Lee, Zhongyuan Lu, Ajay Yadav, Carlo Carraro, Roya Maboudian, Ramamoorthy Ramesh and Sayeef Salahuddin

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605699

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      Single crystal perovskite ferroelectric material is integrated at room temperature on flexible substrate by layer transfer technique. Two terminal memory devices fabricated with these materials exhibit faster switching speed, lower operating voltage, and superior endurance than other existing flexible counterparts. The research provides an avenue towards combining the rich functionality of charge and spin states, offered by the general class of complex oxides, onto a flexible platform.

    5. A Defect-Free Principle for Advanced Graphene Cathode of Aluminum-Ion Battery

      Hao Chen, Fan Guo, Yingjun Liu, Tieqi Huang, Bingna Zheng, Nimrodh Ananth, Zhen Xu, Weiwei Gao and Chao Gao

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605958

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      A conceptually new defect-free principle is proposed for designing graphene cathode of aluminum-ion battery: the fewer the defects, the better the performances. Developed through scalable approach, defect-free graphene aerogel cathode affords high capacity of 100 mAh g−1 under an ultrahigh rate of 500 C, exceeding defective graphene and previous reports. This defect-free principle can guide us to fabricate better graphene-based electrodes.

    6. Large Area Synthesis of 1D-MoSe2 Using Molecular Beam Epitaxy

      Sock Mui Poh, Sherman J. R. Tan, Xiaoxu Zhao, Zhongxin Chen, Ibrahim Abdelwahab, Deyi Fu, Hai Xu, Yang Bao, Wu Zhou and Kian Ping Loh

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605641

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      Large area synthesis of 1D-MoSe2 nanoribbons on both insulating and conducting substrates via molecular beam epitaxy is presented. Dimensional controlled growth of 2D, 1D-MoSe2, and 1D-2D-MoSe2 hybrid heterostructure is achieved by tuning the growth temperature or Mo:Se precursor ratio.

    7. Dynamically Controlled Iridescence of Cholesteric Cellulose Nanocrystal Suspensions Using Electric Fields

      Bruno Frka-Petesic, Harisoa Radavidson, Bruno Jean and Laurent Heux

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201606208

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      Cellulose nanocrystal suspensions in apolar solvent spontaneously form iridescent liquid crystalline phases but the control of their macroscopic order is usually poor. The use of electric fields can provide control on the cholesteric orientation and its periodicity, allowing macroscopic sample homogeneity and dynamical tuning of their iridescent hues, and is demonstrated here.

    8. Soluble Polymers with Intrinsic Porosity for Flue Gas Purification and Natural Gas Upgrading

      Xinbo Wang, Yang Liu, Xiaohua Ma, Swapan K. Das, Mayur Ostwal, Ikhlas Gadwal, Kexin Yao, Xinglong Dong, Yu Han, Ingo Pinnau, Kuo-Wei Huang and Zhiping Lai

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201605826

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      A soluble polymer with intrinsic microporosity, 2,4-diamino-1,3,5-triazine-functionalized organic polymer, is used for the first time as a solid adsorbent which provides an easy solution to overcome the fouling issue. Promising adsorption performances including good CO2 adsorption capacity, excellent CO2/N2 and CO2/CH4 selectivities, high chemical and thermal stabilities, and easiness of preparation and regeneration are shown.

    9. van der Waals Metal-Organic Framework as an Excitonic Material for Advanced Photonics

      Valentin A. Milichko, Sergey V. Makarov, Alexey V. Yulin, Alexandr V. Vinogradov, Andrei A. Krasilin, Elena Ushakova, Vladimir P. Dzyuba, Evamarie Hey-Hawkins, Evgeny A. Pidko and Pavel A. Belov

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201606034

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      Synergistic combination of organic and inorganic nature in van der Waals metal-organic frameworks supports different types of robust excitons that can be effectively and independently manipulated by light at room temperature, and opens new concepts for all-optical data processing and storage.

    10. Controlled Encapsulation of Functional Organic Molecules within Metal–Organic Frameworks: In Situ Crystalline Structure Transformation

      Jinju Guan, Yu Hu, Yu Wang, Hongfeng Li, Zhiling Xu, Tao Zhang, Peng Wu, Suoying Zhang, Gengwu Xiao, Wenlan Ji, Linjie Li, Meixuan Zhang, Yun Fan, Lin Li, Bing Zheng, Weina Zhang, Wei Huang and Fengwei Huo

      Version of Record online: 23 JAN 2017 | DOI: 10.1002/adma.201606290

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      Functional organic molecules/metal–organic frameworks composites can be obtained by in situ crystalline structure transformation from ZIF-L to ZIF-8-L under double solvent conditions. Interestingly, the as-prepared molecules/ZIF-8-L composites with the leaf-like morphology exhibit good fluorescence properties and size selectivity in fluorescent quenchers due to the molecular sieving effect of the well-defined microporous ZIF-8-L.

    11. All-Vacuum-Deposited Stoichiometrically Balanced Inorganic Cesium Lead Halide Perovskite Solar Cells with Stabilized Efficiency Exceeding 11%

      Chien-Yu Chen, Hung-Yu Lin, Kai-Ming Chiang, Wei-Lun Tsai, Yu-Ching Huang, Cheng-Si Tsao and Hao-Wu Lin

      Version of Record online: 20 JAN 2017 | DOI: 10.1002/adma.201605290

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      Vacuum-sublimed inorganic cesium lead halide perovskite thin films are prepared and integrated in all-vacuum-deposited solar cells. Special care is taken to determine the stoichiometric balance of the sublimation precursors, which has great influence on the device performance. The mixed halide devices exhibit exceptional stabilized power conversion efficiency (11.8%) and promising thermal and long-term stabilities.

  10. Research News

    1. Metal–CO2 Batteries on the Road: CO2 from Contamination Gas to Energy Source

      Zhaojun Xie, Xin Zhang, Zhang Zhang and Zhen Zhou

      Version of Record online: 20 JAN 2017 | DOI: 10.1002/adma.201605891

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      Metal–CO2 batteries represent an alternative approach towards clean recycling and utilization of CO2 in energy storage systems. The development of metal–CO2 batteries is summarized, and the urgent challenges and future directions are also discussed.

  11. Communications

    1. Room-Temperature Formation of Highly Crystalline Multication Perovskites for Efficient, Low-Cost Solar Cells

      Taisuke Matsui, Ji-Youn Seo, Michael Saliba, Shaik M. Zakeeruddin and Michael Grätzel

      Version of Record online: 20 JAN 2017 | DOI: 10.1002/adma.201606258

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      A room-temperature perovskite material yielding a power conversion efficiency of 18.1% (stabilized at 17.7%) is demonstrated by judicious selection of cations. Both cesium and methylammonium are necessary for room-temperature formamidinium-based perovskite to obtain the photoactive crystalline perovskite phase and high-quality crystals. This room-temperature-made perovskite material shows great potential for low-cost, large-scale manufacturing such as roll-to-roll process.

  12. Reviews

    1. Porous One-Dimensional Nanomaterials: Design, Fabrication and Applications in Electrochemical Energy Storage

      Qiulong Wei, Fangyu Xiong, Shuangshuang Tan, Lei Huang, Esther H. Lan, Bruce Dunn and Liqiang Mai

      Version of Record online: 20 JAN 2017 | DOI: 10.1002/adma.201602300

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      Porous 1D nanomaterials utilize the advantages of both 1D nanoarchitecture and porous morphology to further enhance the performance of materials for energy storage applications. Here, the current status of porous 1D nanostructures, from methodologies for rational and controllable synthesis, to their successful application in lithium-ion batteries, sodium-ion batteries, lithium-sulfur batteries, lithium-oxygen batteries and supercapacitors is presented.

  13. Communications

    1. Roll-to-Roll Production of Metal-Organic Framework Coatings for Particulate Matter Removal

      Yifa Chen, Shenghan Zhang, Sijia Cao, Siqing Li, Fan Chen, Shuai Yuan, Cheng Xu, Junwen Zhou, Xiao Feng, Xiaojie Ma and Bo Wang

      Version of Record online: 19 JAN 2017 | DOI: 10.1002/adma.201606221

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      A powerful roll-to-roll hot-pressing strategy for mass production of metal-organic framework (MOF)-based filters (MOFilters) using various MOF systems with ranges of substrates is presented. Thus-obtained MOFilters show superior particulate matter removal efficiency under desired working temperatures. Such versatile MOFilters can be scaled up and purposely designed which endow MOFilters with great potentials in both residential and industrial pollution control.

    2. Postpatterned Electrodes for Flexible Node-Type Lithium-Ion Batteries

      Minjoon Park, Hyungyeon Cha, Yoonji Lee, Jaehyung Hong, Sung Youb Kim and Jaephil Cho

      Version of Record online: 19 JAN 2017 | DOI: 10.1002/adma.201605773

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      A flexible node-type lithium-ion battery (LIB) with novel postpatterned electrodes is developed via a simple, one-step process involving an imprinting step of a conventional electrode in the presence of a flattened mesh template. The node-type LIBs containing segmented parts for energy storage and mechanical deformation demonstrate a good cycle stability.

    3. Nickel Nanoparticles Encapsulated in Few-Layer Nitrogen-Doped Graphene Derived from Metal–Organic Frameworks as Efficient Bifunctional Electrocatalysts for Overall Water Splitting

      You Xu, Wenguang Tu, Bowei Zhang, Shengming Yin, Yizhong Huang, Markus Kraft and Rong Xu

      Version of Record online: 19 JAN 2017 | DOI: 10.1002/adma.201605957

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      Nickel nanoparticles encapsulated in few-layer nitrogen-doped graphene (Ni@NC) have been synthesized by using a Ni-based metal–organic framework as the precursor for high-temperature annealing treatment. The resulting Ni@NC materials exhibit highly efficient and ultrastable electrocatalytic activity toward hydrogen evolution reaction and oxygen evolution reaction as well as overall water splitting in alkaline environment.

    4. Realizing Small Energy Loss of 0.55 eV, High Open-Circuit Voltage >1 V and High Efficiency >10% in Fullerene-Free Polymer Solar Cells via Energy Driver

      Pei Cheng, Mingyu Zhang, Tsz-Ki Lau, Yao Wu, Boyu Jia, Jiayu Wang, Cenqi Yan, Meng Qin, Xinhui Lu and Xiaowei Zhan

      Version of Record online: 19 JAN 2017 | DOI: 10.1002/adma.201605216

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      A new, easy, and efficient approach is reported to enhance the driving force for charge transfer, break tradeoff between open-circuit voltage and short-circuit current, and simultaneously achieve very small energy loss (0.55 eV), very high open-circuit voltage (>1 V), and very high efficiency (>10%) in fullerene-free organic solar cells via an energy driver.

    5. Photonic Nanostructures Patterned by Thermal Nanoimprint Directly into Organo-Metal Halide Perovskites

      Neda Pourdavoud, Si Wang, André Mayer, Ting Hu, Yiwang Chen, André Marianovich, Wolfgang Kowalsky, Ralf Heiderhoff, Hella-Christin Scheer and Thomas Riedl

      Version of Record online: 19 JAN 2017 | DOI: 10.1002/adma.201605003

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      Photonic nanostructures are created in organo-metal halide perovskites by thermal nanoimprint lithography at a temperature of 100 °C. The imprinted layers are significantly smoothened compared to the initially rough, polycrystalline layers and the impact of surface defects is substantially mitigated upon imprint. As a case study, 2D photonic crystals are shown to afford lasing with ultralow lasing thresholds at room temperature.

    6. Initialization-Free Multilevel States Driven by Spin–Orbit Torque Switching

      Kuo-Feng Huang, Ding-Shuo Wang, Ming-Han Tsai, Hsiu-Hau Lin and Chih-Huang Lai

      Version of Record online: 18 JAN 2017 | DOI: 10.1002/adma.201601575

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      By engineering multidomain formation in Co/Pt multilayers, it is demonstrate how multilevel storage can be achieved by spin–orbit torque switching. It is rather remarkable that, by modulating the writing pulse conditions, the final magnetization states can be controlled, independent of the initial configurations. The initialization-free multilevel memory advances the spin–orbit-torque magnetic random access memory to higher storage density for practical applications.

    7. Reversible Formation of 2D Electron Gas at the LaFeO3/SrTiO3 Interface via Control of Oxygen Vacancies

      Pengfa Xu, Wei Han, Philip M. Rice, Jaewoo Jeong, Mahesh G. Samant, Katayoon Mohseni, Holger L. Meyerheim, Sergey Ostanin, Igor V. Maznichenko, Ingrid Mertig, Eberhard K. U. Gross, Arthur Ernst and Stuart S. P. Parkin

      Version of Record online: 16 JAN 2017 | DOI: 10.1002/adma.201604447

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      A conducting 2D electron gas (2DEG) is formed at the interface between epitaxial LaFeO3 layers >3 unit cells thick and the surface of SrTiO3 single crystals. The 2DEG is exquisitely sensitive to cation intermixing and oxygen nonstoichiometry. It is shown that the latter thus allows the controllable formation of the 2DEG via ionic liquid gating, thereby forming a nonvolatile switch.

    8. Topological, Valleytronic, and Optical Properties of Monolayer PbS

      Wenhui Wan, Yugui Yao, Liangfeng Sun, Cheng-Cheng Liu and Fan Zhang

      Version of Record online: 16 JAN 2017 | DOI: 10.1002/adma.201604788

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      A PbS monolayer is demonstrated to be a novel platform for topological, valleytronic, and optical phenomena. Compressive strain can turn the trivial monolayer into topological insulators. Optical pumping can facilitate charge, spin, and valley Hall effects tunable by external strain and light ellipticity. Similar results apply to other IV–VI semiconductors.

  14. Reviews

    1. Complex Hollow Nanostructures: Synthesis and Energy-Related Applications

      Le Yu, Han Hu, Hao Bin Wu and Xiong Wen (David) Lou

      Version of Record online: 16 JAN 2017 | DOI: 10.1002/adma.201604563

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      Hollow Nanostructures are of great interest in various current cutting edge innovations, especially as electrode materials for energy conversion and storage technologies including lithium-ion batteries, hybrid supercapacitors, lithium–sulfur batteries and electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions. Compared with conventional solid materials and simple hollow configurations, complex hollow nanostructures with tailorable architectures and compositions present multiple superiorities towards further optimized performance.

  15. Communications

    1. Biomimetic Supramolecular Polymer Networks Exhibiting both Toughness and Self-Recovery

      Ji Liu, Cindy Soo Yun Tan, Ziyi Yu, Yang Lan, Chris Abell and Oren A. Scherman

      Version of Record online: 16 JAN 2017 | DOI: 10.1002/adma.201604951

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      Biomimetic supramolecular dual networks: By mimicking the structure/function model of titin, integration of dynamic cucurbit[8]uril mediated host–guest interactions with a trace amount of covalent cross-linking leads to hierarchical dual networks with intriguing toughness, strength, elasticity, and energy dissipation properties. Dynamic host–guest interactions can be dissociated as sacrificial bonds and their facile reformation results in self-recovery of the dual network structure as well as its mechanical properties.

  16. Reviews

    1. Degradability and Clearance of Silicon, Organosilica, Silsesquioxane, Silica Mixed Oxide, and Mesoporous Silica Nanoparticles

      Jonas G. Croissant, Yevhen Fatieiev and Niveen M. Khashab

      Version of Record online: 13 JAN 2017 | DOI: 10.1002/adma.201604634

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      Degradability and clearance pathways are critical factors that dictate the applicability of new functional nanoparticles, although their design and synthesis is the focus of most of the reported work in this area. The most recent reports on the fate of silica-based hybrid materials are reviewed to help guide future designs, especially those targeting biomedical applications.

  17. Communications

    1. Nanocomposites from Solution-Synthesized PbTe-BiSbTe Nanoheterostructure with Unity Figure of Merit at Low-Medium Temperatures (500–600 K)

      Biao Xu, Matthias T. Agne, Tianli Feng, Thomas C. Chasapis, Xiulin Ruan, Yilong Zhou, Haimei Zheng, Je-Hyeong Bahk, Mercouri G. Kanatzidis, Gerald Jeffrey Snyder and Yue Wu

      Version of Record online: 13 JAN 2017 | DOI: 10.1002/adma.201605140

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      A scalable, low-temperature solution process is used to synthesize precursor material for Pb-doped Bi0.7Sb1.3Te3 thermoelectric nanocomposites. The controllable Pb-doping leads to the increase in the optical bandgap, thus delaying the onset of bipolar conduction. Furthermore, the solution synthesis enables nanostructuring, which greatly reduces thermal conductivity. As a result, this material exhibits a zT = 1 over the 513–613 K range.

  18. Research News

    1. Melt-Quenched Hybrid Glasses from Metal–Organic Frameworks

      Haizheng Tao, Thomas D. Bennett and Yuanzheng Yue

      Version of Record online: 13 JAN 2017 | DOI: 10.1002/adma.201601705

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      Recent discoveries in the glass formation of metal–organic frameworks via the conventional melt-quenching route are highlighted. In addition to the distinction and prevalence of this novel type of melt-quenched hybrid glass, potential technical advantages and applications together with its perspectives are described.

  19. Communications

    1. Direct Observations of Nanofilament Evolution in Switching Processes in HfO2-Based Resistive Random Access Memory by In Situ TEM Studies

      Chao Li, Bin Gao, Yuan Yao, Xiangxiang Guan, Xi Shen, Yanguo Wang, Peng Huang, Lifeng Liu, Xiaoyan Liu, Junjie Li, Changzhi Gu, Jinfeng Kang and Richeng Yu

      Version of Record online: 11 JAN 2017 | DOI: 10.1002/adma.201602976

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      Resistive switching processes in HfO2 are studied by electron holography and in situ energy-filtered imaging. The results show that oxygen vacancies are gradually generated in the oxide layer under ramped electrical bias, and finally form several conductive channels connecting the two electrodes. It also shows that the switching process occurs at the top interface of the hafnia layer.

    2. 3D Printing of Transparent and Conductive Heterogeneous Hydrogel–Elastomer Systems

      Kevin Tian, Jinhye Bae, Shannon E. Bakarich, Canhui Yang, Reece D. Gately, Geoffrey M. Spinks, Marc in het Panhuis, Zhigang Suo and Joost J. Vlassak

      Version of Record online: 11 JAN 2017 | DOI: 10.1002/adma.201604827

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      A hydrogel-dielectric elastomer system, polyacrylamide and poly(dimethylsiloxane) (PDMS), is adapted for extrusion printing for integrated device fabrication. A lithium-chloride-containing hydrogel printing ink is developed and printed onto treated PDMS with no visible signs of delamination and geometrically scaling resistance under moderate uniaxial tension and fatigue. A variety of designs are demonstrated, including a resistive strain gauge and an ionic cable.

  20. Reviews

    1. Photochemically Driven Polymeric Network Formation: Synthesis and Applications

      Eva Blasco, Martin Wegener and Christopher Barner-Kowollik

      Version of Record online: 11 JAN 2017 | DOI: 10.1002/adma.201604005

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      Photoinduced polymeric network formation is one of the most employed processes for network fabrication, since light provides ready access to temporal and spatial control. Recent light-induced modular reactions, such as photoinduced thiol-based reactions, Diels–Alder systems, 1,3-dipolar additions, or photodimerizations are successfully employed for the formation of precision polymeric networks with applications in a wide array of fields, entailing enticing prospects for future developments.

  21. Communications

    1. A Self-Powered Implantable Drug-Delivery System Using Biokinetic Energy

      Peiyi Song, Shuangyang Kuang, Nishtha Panwar, Guang Yang, Danny Jian Hang Tng, Swee Chuan Tjin, Wun Jern Ng, Maszenan Bin Abdul Majid, Guang Zhu, Ken-Tye Yong and Zhong Lin Wang

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/adma.201605668

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      The first triboelectric-nanogenerator (TENG)-based self-powered implantable drug-delivery system is presented. Pumping flow rates from 5.3 to 40 µL min−1 under different rotating speeds of the TENG are realized. The implantable drug-delivery system can be powered with a TENG device rotated by human hand motion. Ex vivo trans-sclera drug delivery in porcine eyes is demonstrated by utilizing the biokinetic energies of human hands.

  22. Progress Reports

    1. Nanocarbon for Oxygen Reduction Electrocatalysis: Dopants, Edges, and Defects

      Cheng Tang and Qiang Zhang

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/adma.201604103

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      Activity origins of nanocarbon-based oxygen reduction reaction (ORR) electrocatalysts are comprehensively discussed, considering the dopants, edges, and defects. They can effectively modify the charge/spin distribution on the sp2-conjugated carbon matrix, leading to similar activity origin. The specific doping at the defective edges is expected to bring the metal-free nanocarbon catalysts to practical applications.

  23. Communications

    1. 3D Ordered Macroporous MoS2@C Nanostructure for Flexible Li-Ion Batteries

      Zongnan Deng, Hao Jiang, Yanjie Hu, Yu Liu, Ling Zhang, Honglai Liu and Chunzhong Li

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/adma.201603020

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      A flexible and robust electrode is demonstrated by assembling the 3D ordered macroporous MoS2@C nanostructure on carbon cloth with ultrasmall few-layered MoS2 nanosheets homogenously embedded into the interconnected carbon wall. Such unique nanostructures are favorable for enhancing lithium storage capacity, directly applied as flexible electrode, demonstrating a very high electrochemical performance and superior cycling stability for lithium ion batteries.

    2. Highly Elastic and Self-Healing Composite Colloidal Gels

      Mani Diba, Huanan Wang, Thomas E. Kodger, Shima Parsa and Sander C. G. Leeuwenburgh

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/adma.201604672

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      Composite colloidal gels are formed by the pH-induced electrostatic assembly of silica and gelatin nanoparticles. These injectable and moldable colloidal gels are able to withstand substantial compressive and tensile loads, and exhibit a remarkable self-healing efficiency. This study provides new, critical insight into the structural and mechanical properties of composite colloidal gels and opens up new avenues for practical application of colloidal gels.

    3. Unleashing the Full Potential of Magnetoelectric Coupling in Film Heterostructures

      Haribabu Palneedi, Deepam Maurya, Gi-Yeop Kim, Venkateswarlu Annapureddy, Myoung-Sub Noh, Chong-Yun Kang, Jong-Woo Kim, Jong-Jin Choi, Si-Young Choi, Sung-Yoon Chung, Suk-Joong L. Kang, Shashank Priya and Jungho Ryu

      Version of Record online: 9 JAN 2017 | DOI: 10.1002/adma.201605688

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      A record-high, near-theoretical intrinsic magnetoelectric (ME) coupling of 7 V cm−1 Oe−1 is achieved in a heterostructure of piezoelectric Pb(Zr,Ti)O3 (PZT) film deposited on magnetostrictive Metglas (FeBSi). The anchor-like, nanostructured interface between PZT and Metglas, improved crystallinity of PZT by laser annealing, and optimum volume of crystalline PZT are found to be the key factors in realizing such a giant strain-mediated ME coupling.

    4. Strong, Tough, Stretchable, and Self-Adhesive Hydrogels from Intrinsically Unstructured Proteins

      Mark A. Gonzalez, Joseph R. Simon, Ali Ghoorchian, Zachary Scholl, Shaoting Lin, Michael Rubinstein, Piotr Marszalek, Ashutosh Chilkoti, Gabriel P. López and Xuanhe Zhao

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201604743

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      Strong, tough, stretchable, and self-adhesive hydrogels have been designed with intrinsically unstructured proteins. The extraordinary mechanical properties exhibited by these materials are enabled by an integration of toughening mechanisms that maintain high elasticity and dissipate mechanical energy within the protein networks.

    5. Intralayered Ostwald Ripening to Ultrathin Nanomesh Catalyst with Robust Oxygen-Evolving Performance

      Junfeng Xie, Xiaodong Zhang, Hao Zhang, Jiajia Zhang, Shuang Li, Ruoxing Wang, Bicai Pan and Yi Xie

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201604765

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      An etching-intralayered Ostwald ripening process is proposed, which leads to the formation of a β-Ni(OH)2 ultrathin nanomesh with abundant and uniformly distributed nanopores of 3–4 nm. The nanomesh catalyst exhibits outstanding oxygen evolution reaction performance, with high catalytic current density and superior long-term stability, making this Earth-abundant nanomesh catalyst a promising candidate for commercial water splitting.

  24. Progress Reports

    1. Single Nanoparticle Detection Using Optical Microcavities

      Yanyan Zhi, Xiao-Chong Yu, Qihuang Gong, Lan Yang and Yun-Feng Xiao

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201604920

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      Single nanoparticle detection is of critical importance in various fields from fundamental research to practical applications. Optical microcavities are excellent candidates to be employed in ultra-sensitive sensing due to significantly enhanced light-matter interaction. The sensing performance can be improved by obtaining better spectral resolution and temporal resolution, and techniques can be applied to realize practical and portable sensors using microcavities.

    2. Nonempirical Calculation of Superconducting Transition Temperatures in Light-Element Superconductors

      Ryotaro Arita, Takashi Koretsune, Shiro Sakai, Ryosuke Akashi, Yusuke Nomura and Wataru Sano

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201602421

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      Light elements often exhibit superconductivity at high temperature when they are placed under pressure or they form compounds. This study reviews recent progress in nonempirical calculation of Tc based on superconducting density functional theory, ab initio Migdal-Eliashberg theory, and multiscale ab initio scheme for correlated electrons, revealing nontrivial physics behind the high-Tc superconductivity in elemental Li, sulfur hydrides, and alkali-doped C60.

  25. Communications

    1. DNA-Origami-Driven Lithography for Patterning on Gold Surfaces with Sub-10 nm Resolution

      Isaac Gállego, Brendan Manning, Joan Daniel Prades, Mònica Mir, Josep Samitier and Ramon Eritja

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201603233

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      Sub-10 nm lithography of DNA patterns is achieved using the DNA-origami stamping method. This new strategy utilizes DNA origami to bind a preprogrammed DNA ink pattern composed of thiol-modified oligonucleotides on gold surfaces. Upon denaturation of the DNA origami, the DNA ink pattern is exposed. The pattern can then be developed by hybridization with complementary strands carrying gold nanoparticles.

    2. Inheriting the Characteristics of TADF Small Molecule by Side-Chain Engineering Strategy to Enable Bluish-Green Polymers with High PLQYs up to 74% and External Quantum Efficiency over 16% in Light-Emitting Diodes

      Guohua Xie, Jiajia Luo, Manli Huang, Tianheng Chen, Kailong Wu, Shaolong Gong and Chuluo Yang

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201604223

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      Thermally activated delayed fluorescence (TADF) polymers are designed and synthesized by grafting the TADF emitter to the side chain of the polycarbazole backbone. By employing these TADF polymers with large ratio of delayed fluorescence component and high photoluminescence quantum yield as the emitters, the solution-processed light-emitting diodes achieve a maximal external quantum efficiency of 16.1% at a luminance of around 100 cd m−2.

    3. Multimetallic Hierarchical Aerogels: Shape Engineering of the Building Blocks for Efficient Electrocatalysis

      Bin Cai, Arezoo Dianat, René Hübner, Wei Liu, Dan Wen, Albrecht Benad, Luisa Sonntag, Thomas Gemming, Gianaurelio Cuniberti and Alexander Eychmüller

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201605254

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      A new class of multimetallic hierarchical aerogels composed entirely of interconnected Ni-PdxPty nano-building blocks with in situ engineered morphologies and compositions is demonstrated. The underlying mechanism of the galvanic shape-engineering is elucidated in terms of nanowelding of intermediate nanoparticles. The hierarchical aerogels integrate two levels of porous structures, leading to improved electrocatalysis performance.

  26. Progress Reports

    1. Self-Assembled Peptide- and Protein-Based Nanomaterials for Antitumor Photodynamic and Photothermal Therapy

      Manzar Abbas, Qianli Zou, Shukun Li and Xuehai Yan

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201605021

      Thumbnail image of graphical abstract

      Self-assembled peptide- and protein-based nanomaterials are important and promising for the novel and emerging antitumor techniques of photodynamic therapy and photothermal therapy. Recent advances in fabrication and application of phototherapeutic nanomaterials based on peptide and protein self-assembly are highlighted, providing an increased understanding of the role of peptide and protein self-assembly in improving the efficiency of antitumor phototherapies.

  27. Communications

    1. Full Dynamic-Range Pressure Sensor Matrix Based on Optical and Electrical Dual-Mode Sensing

      Xiandi Wang, Miaoling Que, Mengxiao Chen, Xun Han, Xiaoyi Li, Caofeng Pan and Zhong Lin Wang

      Version of Record online: 6 JAN 2017 | DOI: 10.1002/adma.201605817

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      Pressure sensor matrix (PSM) with full dynamic range can accurately detect and spatially map pressure profile. A 100 × 100 large-scale PSM gives both electrical and optical signals by itself without applying an external power. The device represents a major step toward digital imaging and visible display of pressure distribution covers a large dynamic range.

    2. Nanopolymersomes with an Ultrahigh Iodine Content for High-Performance X-Ray Computed Tomography Imaging In Vivo

      Yan Zou, Yaohua Wei, Guanglin Wang, Fenghua Meng, Mingyuan Gao, Gert Storm and Zhiyuan Zhong

      Version of Record online: 5 JAN 2017 | DOI: 10.1002/adma.201603997

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      Biocompatible and biodegradable nanopolymersomes with an unprecedented iodine content, low viscosity, and iso-osmolality achieve significantly enhanced CT imaging of blood pool and the reticuloendothelial system. Moreover, in subcutaneous and orthotopic tumor models in mice, they show enhanced in vivo imaging when compared to iohexol, a clinically used small molecule contrast agent.

    3. Organometallic Perovskite Metasurfaces

      Behrad Gholipour, Giorgio Adamo, Daniele Cortecchia, Harish N. S. Krishnamoorthy, Muhammad. D. Birowosuto, Nikolay I. Zheludev and Cesare Soci

      Version of Record online: 5 JAN 2017 | DOI: 10.1002/adma.201604268

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      Organometallic perovskites, solution-processable materials with outstanding optoelectronic properties and high index of refraction, provide a platform for all-dielectric metamaterials operating at visible frequencies. Perovskite metasurfaces with structural coloring tunable across visible frequencies are realized through subwavelength structuring. Moreover, a threefold increase of the luminescence yield and comparable reduction of luminescence decay time are observed.

    4. In Situ Engineering of the Electrode–Electrolyte Interface for Stabilized Overlithiated Cathodes

      Tyler Evans, Daniela Molina Piper, Huaxing Sun, Timothy Porcelli, Seul Cham Kim, Sang Sub Han, Yong Seok Choi, Chixia Tian, Dennis Nordlund, Marca M. Doeff, Chunmei Ban, Sung-Jin Cho, Kyu Hwan Oh and Se-Hee Lee

      Version of Record online: 5 JAN 2017 | DOI: 10.1002/adma.201604549

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      The first-ever demonstration of stabilized Si/lithium–manganese-rich full cells, capable of retaining >90% energy over early cycling and >90% capacity over more than 750 cycles at the 1C rate (100% depth-of-discharge), is made through the utilization of a modified ionic liquid electrolyte capable of forming a favorable cathode–electrolyte interface.

    5. Bioinspired Coupling of Inorganic Layered Nanomaterials with Marine Polysaccharides for Efficient Aqueous Exfoliation and Smart Actuating Hybrids

      Lu Zong, Mingjie Li and Chaoxu Li

      Version of Record online: 5 JAN 2017 | DOI: 10.1002/adma.201604691

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      WS2 and marine alginate are perfectly coupled to ensure scalable production of exfoliated WS2 with unprecedented efficiency, further providing super mechanical properties and the photothermal effect to their composites. Combined with the water-intake and cation-binding capabilities of alginate, biomimetic soft devices are designed with stimuli-responsiveness and actuating properties, capable of serving as a photo-driven motor, walking robot and gripper.

    6. Chemically Robust Ambipolar Organic Transistor Array Directly Patterned by Photolithography

      Eun Kwang Lee, Cheol Hee Park, Junghoon Lee, Hae Rang Lee, Changduk Yang and Joon Hak Oh

      Version of Record online: 5 JAN 2017 | DOI: 10.1002/adma.201605282

      Thumbnail image of graphical abstract

      Organic ambipolar transistor arrays for chemical sensors are prepared on a flexible plastic substrate with a bottom-gate bottom-contact configuration to minimize the damage to the organic semiconductors, for the first time, using a photolithographically patternable polymer semiconductor. Well-balanced ambipolar charge transport has been achieved by introducing graphene electrodes because of the reduced contact resistance and energetic barrier for electron transport.

  28. Progress Reports

    1. Additive Manufacturing of Metal Structures at the Micrometer Scale

      Luca Hirt, Alain Reiser, Ralph Spolenak and Tomaso Zambelli

      Version of Record online: 4 JAN 2017 | DOI: 10.1002/adma.201604211

      Thumbnail image of graphical abstract

      To enable the additive manufacturing of metals at the micrometer scale, a variety of novel techniques are currently in use. The individual techniques are introduced, detailing their underlying principles. Furthermore, it critically compares their fabrication capabilities, in particular the minimum feature size, achievable geometry and obtained materials properties.

  29. Communications

    1. Molecular Crystal Engineering: Tuning Organic Semiconductor from p-type to n-type by Adjusting Their Substitutional Symmetry

      Hui Jiang, Peng Hu, Jun Ye, Yongxin Li, Henan Li, Xiaotao Zhang, Rongjin Li, Huanli Dong, Wenping Hu and Christian Kloc

      Version of Record online: 4 JAN 2017 | DOI: 10.1002/adma.201605053

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      Focusing on the bottleneck of molecularly engineered organic semiconductors, a breakthrough is made to tune the electronic properties of organic semiconductors from p-type to n-type by using fluorinated metal phthalocyanines as examples. The experimentally observed p-type to n-type transition characteristics of single-crystal field-effect devices result from a combination of extrinsic and intrinsic properties of materials with different fluoridation substitution.

    2. Hole Mobility and Electron Injection Properties of D-A Conjugated Copolymers with Fluorinated Phenylene Acceptor Units

      Ming Wang, Michael J. Ford, Alexander T. Lill, Hung Phan, Thuc-Quyen Nguyen and Guillermo C. Bazan

      Version of Record online: 4 JAN 2017 | DOI: 10.1002/adma.201603830

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      A novel wide-gap conjugated polymer PhF2,5 (Eg = 1.9 eV) is designed to contain alternating cyclopentadithiophene and difluorophenylene unit with the goal of favoring unipolar organic field effect transistor characteristics. The higher lowest unoccupied molecular orbital energy of PhF2,5 increases the barrier to electron injection, leading to unipolar transport and higher on/off ratios, without sacrificing desirable high hole mobilities.

    3. Porous 3D Few-Layer Graphene-like Carbon for Ultrahigh-Power Supercapacitors with Well-Defined Structure–Performance Relationship

      Jin Zhao, Yufei Jiang, Hao Fan, Meng Liu, Ou Zhuo, Xizhang Wang, Qiang Wu, Lijun Yang, Yanwen Ma and Zheng Hu

      Version of Record online: 3 JAN 2017 | DOI: 10.1002/adma.201604569

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      3D few-layer graphene-like carbon with hierarchical open porous architecture is obtained by a new in situ Cu template method, leading to top-level supercapacitive performance, especially state-of-the-art power density. An effective new approach is demonstrated, which can extend the understanding of structure–performance relationships for many electrochemical energy storage systems and form a significant complement to classical electrochemical impedance spectroscopy.

    4. A Facile Reduction Method for Roll-to-Roll Production of High Performance Graphene-Based Transparent Conductive Films

      Jing Ning, Long Hao, Meihua Jin, Xiongying Qiu, Yudi Shen, Jiaxu Liang, Xinghao Zhang, Bin Wang, Xianglong Li and Linjie Zhi

      Version of Record online: 2 JAN 2017 | DOI: 10.1002/adma.201605028

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      A facile roll-to-roll method is developed for fabricating reduced graphene oxide (rGO)-based flexible transparent conductive films. A Sn2+/ethanol reduction system and a rationally designed fast coating–drying–washing technique are proven to be highly efficient for low-cost continuous production of large-area rGO films and patterned rGO films, extremely beneficial toward the manufacture of flexible photoelectronic devices.

    5. Room-Temperature Quantum Transport Signatures in Graphene/LaAlO3/SrTiO3 Heterostructures

      Giriraj Jnawali, Mengchen Huang, Jen-Feng Hsu, Hyungwoo Lee, Jung-Woo Lee, Patrick Irvin, Chang-Beom Eom, Brian D'Urso and Jeremy Levy

      Version of Record online: 2 JAN 2017 | DOI: 10.1002/adma.201603488

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      High mobility graphene field-effect devices, fabricated on the complex-oxide heterostructure LaAlO3/SrTiO3, exhibit quantum interference signatures up to room temperature. The oxide material is believed to play a critical role in suppressing short-range and phonon contributions to scattering. The ability to maintain pseudospin coherence at room temperature holds promise for the realization of new classical and quantum information technologies.

    6. A Sulfur-Rich Copolymer@CNT Hybrid Cathode with Dual-Confinement of Polysulfides for High-Performance Lithium–Sulfur Batteries

      Guangjian Hu, Zhenhua Sun, Chao Shi, Ruopian Fang, Jing Chen, Pengxiang Hou, Chang Liu, Hui-Ming Cheng and Feng Li

      Version of Record online: 30 DEC 2016 | DOI: 10.1002/adma.201603835

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      A sulfur-rich copolymer@carbon nanotubes hybrid cathode is introduced for lithium–sulfur batteries produced by combining the physical and chemical confinement of polysulfides. The binder free and metal current collector free cathode of dual confinement enables an efficient pathway for the fabrication of high performance sulfur copolymer carbon matrix electrodes for lithium–sulfur batteries.

    7. Strain and Magnetic Field Induced Spin-Structure Transitions in Multiferroic BiFeO3

      A. Agbelele, D. Sando, C. Toulouse, C. Paillard, R. D. Johnson, R. Rüffer, A. F. Popkov, C. Carrétéro, P. Rovillain, J.-M. Le Breton, B. Dkhil, M. Cazayous, Y. Gallais, M.-A. Méasson, A. Sacuto, P. Manuel, A. K. Zvezdin, A. Barthélémy, J. Juraszek and M. Bibes

      Version of Record online: 30 DEC 2016 | DOI: 10.1002/adma.201602327

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      The magnetic field-dependent spin ordering of strained BiFeO3 films is determined using nuclear resonant scattering and Raman spectroscopy. The critical field required to destroy the cycloidal modulation of the Fe spins is found to be significantly lower than in the bulk, with appealing implications for field-controlled spintronic and magnonic devices.

  30. Research News

    1. Molecular Engineering of Conjugated Polymers for Solar Cells: An Updated Report

      Shengqiang Xiao, Qianqian Zhang and Wei You

      Version of Record online: 30 DEC 2016 | DOI: 10.1002/adma.201601391

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      Recent progress (2012-2016) in polymer:fullerene bulk heterojunction solar cells is reviewed. The intrinsic complexity of such solar cells urges the community to apply an integrated and comprehensive approach – including synthesis, morphology, and device physics – to elucidate the fundamental underlying principles that govern the device performance, in particular, in the context of disclosing structure–property correlations.

  31. Reviews

    1. Soft Actuators for Small-Scale Robotics

      Lindsey Hines, Kirstin Petersen, Guo Zhan Lum and Metin Sitti

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/adma.201603483

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      Ongoing soft-actuator development is reviewed in detail, highlighting approaches suitable for nanometer- to centimeter-scale robotic applications. These types of systems are often untethered and their actuation and sensing are often highly integrated. Soft, active materials are particularly well suited for these applications, with a wide range of stimulants, large deformations, high motion complexities, and varied multifunctionality.

  32. Progress Reports

    1. CVD Polymers for Devices and Device Fabrication

      Minghui Wang, Xiaoxue Wang, Priya Moni, Andong Liu, Do Han Kim, Won Jun Jo, Hossein Sojoudi and Karen K. Gleason

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/adma.201604606

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      Chemical vapor deposition (CVD) polymerization synthesizes conformal and pinhole-free organic thin films directly on substrates. Compared with solution-based techniques, the solvent-free nature of the CVD process avoids the undesirable monomer–solvent or polymer–solvent and solvent–substrate interactions. Thus, CVD is particularly suitable for synthesizing insoluble conductive polymers and robust crosslinked networks for organic devices.

    2. Critical Insight into the Relentless Progression Toward Graphene and Graphene-Containing Materials for Lithium-Ion Battery Anodes

      Rinaldo Raccichini, Alberto Varzi, Di Wei and Stefano Passerini

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/adma.201603421

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      The use of graphene and graphene-containing materials for lithium-ion battery anodes is reviewed. Through a specific focus on the evaluation of the most important parameters for lithium-ion battery applications, graphene and graphene-containing materials are critically assessed.

  33. Communications

    1. An Artificial Solid Electrolyte Interphase with High Li-Ion Conductivity, Mechanical Strength, and Flexibility for Stable Lithium Metal Anodes

      Yayuan Liu, Dingchang Lin, Pak Yan Yuen, Kai Liu, Jin Xie, Reinhold H. Dauskardt and Yi Cui

      Version of Record online: 29 DEC 2016 | DOI: 10.1002/adma.201605531

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      An artificial solid electrolyte interphase (SEI) is demonstrated for the efficient and safe operation of a lithium metal anode. Composed of lithium-ion-conducting inorganic nanoparticles within a flexible polymer binder matrix, the rationally designed artificial SEI not only mechanically suppresses lithium dendrite formation but also promotes homogeneous lithium-ion flux, significantly enhancing the efficiency and cycle life of lithium metal anode.

    2. Ternary NiCo2Px Nanowires as pH-Universal Electrocatalysts for Highly Efficient Hydrogen Evolution Reaction

      Rui Zhang, Xiangxue Wang, Shujun Yu, Tao Wen, Xiangwei Zhu, Fangxu Yang, Xiangnan Sun, Xiangke Wang and Wenping Hu

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/adma.201605502

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      A bimetallic-structured ternary phosphide (NiCo2Px) as a novel pH-universal electrocatalyst for hydrogen evolution reaction is presented. It exhibits both high activity and long-term stability in all the tested alkaline, neutral, and acidic media. The excellent catalytic performance endows it with a bright future in the large-scale electrochemical water splitting industry.

    3. Antibiotic Spider Silk: Site-Specific Functionalization of Recombinant Spider Silk Using “Click” Chemistry

      David Harvey, Philip Bardelang, Sara L. Goodacre, Alan Cockayne and Neil R. Thomas

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/adma.201604245

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      In a new, versatile approach to fun­ction­alizing recombinant spider silk, L-azidohomoalanine is introduced residue-specifically in the minispidroin protein 4RepCT through expression in an E. coli methionine auxotroph. Both fluorophores and the antibiotic levofloxacin are attached to this bio-orthogonal amino acid using copper-catalyzed click chemistry, either before or after the silk fibers are self-assembled.

    4. Epitaxial Growth and Air-Stability of Monolayer Antimonene on PdTe2

      Xu Wu, Yan Shao, Hang Liu, Zili Feng, Ye-Liang Wang, Jia-Tao Sun, Chen Liu, Jia-Ou Wang, Zhong-Liu Liu, Shi-Yu Zhu, Yu-Qi Wang, Shi-Xuan Du, You-Guo Shi, Kurash Ibrahim and Hong-Jun Gao

      Version of Record online: 28 DEC 2016 | DOI: 10.1002/adma.201605407

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      Monolayer antimonene is fabricated on PdTe2 by an epitaxial method. Monolayer antimonene is theoretically predicted to have a large bandgap for nanoelectronic devices. Air-exposure experiments indicate amazing chemical stability, which is great for device fabrication. A method to fabricate high-quality monolayer antimonene with several great properties for novel electronic and optoelectronic applications is provided.

    5. Paramagnetic Properties of Metal-Free Boron-Doped Graphene Quantum Dots and Their Application for Safe Magnetic Resonance Imaging

      Hui Wang, Richard Revia, Kui Wang, Rajeev J. Kant, Qingxin Mu, Zheng Gai, Kunlun Hong and Miqin Zhang

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201605416

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      A boron-doped graphene quantum dot (B-GQD) as a metal-free multimodal contrast agent (CA) for safe magnetic resonance imaging and fluorescence imaging is reported. In vivo T1-weighted magnetic resonance images show that B-GQDs induce significant contrast enhancement on heart, liver, spleen, and kidney, and sustain for more than 1 h, about 10 times longer than Gd-based CAs currently used in clinic.

  34. Reviews

    1. Nanoarchitectured Design of Porous Materials and Nanocomposites from Metal-Organic Frameworks

      Yusuf Valentino Kaneti, Jing Tang, Rahul R. Salunkhe, Xuchuan Jiang, Aibing Yu, Kevin C.-W. Wu and Yusuke Yamauchi

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201604898

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      Metal-organic framework (MOF)-derived nanostructures have attracted significant attention for a wide range of applications due to their tunable composition, structure and pore size. The recent developments, challenges and future directions in the fabrication of MOF-derived nanomaterials such as porous carbons, metal oxides, metal chalcogenides, metal carbides, metal phosphides and their composites are comprehensively reviewed.

  35. Communications

    1. Light-Enhancing Plasmonic-Nanopore Biosensor for Superior Single-Molecule Detection

      Ossama N. Assad, Tal Gilboa, Joshua Spitzberg, Matyas Juhasz, Elmar Weinhold and Amit Meller

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201605442

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      A stacked plasmonic nanowell–nanopore biosensor strongly suppresses the background fluorescence from the bulk and yields net more than tenfold enhancement of the fluorescence intensity. The device offers extremely high signal-to-background (S/B) ratio for single-molecule detection at ultralow excitation laser intensities, while maintaining extremely high temporal bandwidth for single-DNA sensing.

    2. Highly Reversible and Durable Na Storage in Niobium Pentoxide through Optimizing Structure, Composition, and Nanoarchitecture

      Jiangfeng Ni, Wencong Wang, Chao Wu, Haichen Liang, Joachim Maier, Yan Yu and Liang Li

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201605607

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      Amorphous, hydrogenated, and self-ordered nanoporous Nb2O5 films serve as an excellent binder-free electrode for sodium batteries, affording a high and sustainable capacity delivery and robust high-rate capability. This collaborative material engineering of structural order (amorphization), composition (hydrogenation), and architecture (ordered nanopore) opens up new possibilities to develop an energy storage solution that is more accessible, sustainable, and producible.

    3. Programmable Kiri-Kirigami Metamaterials

      Yichao Tang, Gaojian Lin, Shu Yang, Yun Kyu Yi, Randall D. Kamien and Jie Yin

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201604262

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      Programmable kirigami metamaterials with controllable local tilting orientations on demand through prescribed notches are constructed through a new approach of kiri-kirgami, and their actuation of pore opening via both mechanical stretching and temperature, along with their potential application as skins for energy saving building, is discussed.

  36. Reviews

    1. Materials with Giant Mechanocaloric Effects: Cooling by Strength

      Lluís Mañosa and Antoni Planes

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201603607

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      Materials with giant caloric properties are subject to intensive research due to expectations that they will contribute to a new efficient and environmentally friendly solid-state refrigeration technology. In the present review, the key properties of the most relevant mechanocaloric materials are critically examined, and some perspectives for further development in this field are provided.

  37. Communications

    1. Atomically and Electronically Coupled Pt and CoO Hybrid Nanocatalysts for Enhanced Electrocatalytic Performance

      Chao Meng, Tao Ling, Tian-Yi Ma, Hui Wang, Zhenpeng Hu, Yue Zhou, Jing Mao, Xi-Wen Du, Mietek Jaroniec and Shi-Zhang Qiao

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201604607

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      Atomically and electronically coupled Pt and CoO hybrid nanocatalysts are fabricated for electrocatalytic oxygen reduction reaction. The atomic coupling between the Pt and the CoO endows precise control of the atomic interface between the Pt and the CoO, which directly results in electron donation from the CoO to the Pt, and thus favorable tuning of the electronic structure of the Pt.

    2. Reversibly Photoswitchable Supramolecular Assembly and Its Application as a Photoerasable Fluorescent Ink

      Huang Wu, Yong Chen and Yu Liu

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201605271

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      A photoswitchable supramolecular assembly can efficiently and reversibly switch on/off the luminescence of the [Ru(bpy)3]2+ center upon irradiation by different wavelength light in solution and the solid state. The assembly possesses reversible photoisomerization and a high Förster resonance energy transfer efficiency, and when used as an ink it can be reversibly and repeatedly erased and recovered by altering the wavelength of irradiation light.

  38. Reviews

    1. Fuel-Free Synthetic Micro-/Nanomachines

      Tailin Xu, Wei Gao, Li-Ping Xu, Xueji Zhang and Shutao Wang

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201603250

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      Fuel-free synthetic micro-/nanomachines powered by external stimuli are able to swim efficiently in biologically relevant environments. Tremendous progress made in the past decade to develop different synthesis strategies for designing and fabricating fuel-free micro-/nanomotors with different functionalities is reviewed. These artificial nanomachines can achieve predetermined tasks in biomedical applications.

  39. Communications

    1. A Mixed-Extractor Strategy for Efficient Sorting of Semiconducting Single-Walled Carbon Nanotubes

      Dan Liu, Pan Li, Xiaoqing Yu, Jianting Gu, Jie Han, Shuchen Zhang, Hongbo Li, Hehua Jin, Song Qiu, Qingwen Li and Jin Zhang

      Version of Record online: 27 DEC 2016 | DOI: 10.1002/adma.201603565

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      A general strategy for sorting semiconducting single-walled carbon nanotubes (s-SWNTs) with high efficiency using a mixed-extractor has been reported. When the two extractors have a sufficient difference in binding energy with s-SWNTs, and skeleton flexibility, the mixture shows enhanced yield for sorting s-SWNTs. The strategy could be effective when applied to increase the sorting yield of other selective dispersion systems.

    2. Multistaged Nanovaccines Based on Porous Silicon@Acetalated Dextran@Cancer Cell Membrane for Cancer Immunotherapy

      Flavia Fontana, Mohammad-Ali Shahbazi, Dongfei Liu, Hongbo Zhang, Ermei Mäkilä, Jarno Salonen, Jouni T. Hirvonen and Hélder A. Santos

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201603239

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      Immunoadjuvant porous silicon (PSi)-based nanovaccines are prepared by nanoprecipitation in a glass capillary microfluidics device. Vesicles, derived from cancer cell membranes encapsulating thermally oxidized PSi nanoparticles or PSi-polymer nanosystems binding a model antigen, are biocompatible over a wide range of concentrations, and show immunostimulant properties in human cells, promoting the expression of co-stimulatory signals and the secretion of pro-inflammatory cytokines.

    3. Efficient Generation of Long-Lived Triplet Excitons in 2D Hybrid Perovskite

      Robert Younts, Hsin-Sheng Duan, Bhoj Gautam, Bayrammurad Saparov, Jie Liu, Cedric Mongin, Felix N. Castellano, David B. Mitzi and Kenan Gundogdu

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201604278

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      Triplet excitons form in quasi-2D hybrid inorganic-organic perovskites and diffuse over 100 nm before radiating with >11% PLQE at low temperatures.

    4. Multifunctional Carbon-Based Metal-Free Electrocatalysts for Simultaneous Oxygen Reduction, Oxygen Evolution, and Hydrogen Evolution

      Chuangang Hu and Liming Dai

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201604942

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      Rationally designed N, S co-doped graphitic sheets with stereoscopic holes (SHG) act as effective tri-functional catalysts for oxygen reduction reaction, hydrogen evolution reaction, and oxygen evolution reaction, simultaneously. The multifunctional electrocatalytic activities originate from a synergistic effect of the N, S heteroatom doping and unique SHG architecture, which provide a large surface area and efficient pathways for electron and electrolyte/reactant transports.

    5. Composite Yttrium-Carbonaceous Spheres Templated Multi-Shell YVO4 Hollow Spheres with Superior Upconversion Photoluminescence

      Lingbo Zong, Jie Xu, Shuaiyu Jiang, Kun Zhao, Zumin Wang, Porun Liu, Huijun Zhao, Jun Chen, Xianran Xing and Ranbo Yu

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201604377

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      Complex oxide YVO4 multi-shell hollow spheres with uniform morphologies and controllable shell numbers are successfully prepared by using a newly developed and general composite yttrium-carbonaceous sphere templated approach. The prominent upconversion luminous intensity of the YVO4:Yb3+/Er3+ hollow spheres might be attributed to the enhanced near-infrared excitation light harvesting efficiency originated from the multiple reflections.

    6. Surface-Driven Magnetotransport in Perovskite Nanocrystals

      Ha Le Thi N'Goc, Louis Donald Notemgnou Mouafo, Céline Etrillard, Almudena Torres-Pardo, Jean-François Dayen, Simon Rano, Gwenaëlle Rousse, Christel Laberty-Robert, Jose Gonzales Calbet, Marc Drillon, Clément Sanchez, Bernard Doudin and David Portehault

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201604745

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      Unique insights into magnetotransport in 20 nm ligand-free La0.67Sr0.33MnO3 perovskite nanocrystals of nearly perfect crystalline quality reveal a chemically altered 0.8 nm thick surface layer that triggers exceptionally large magnetoresistance at low temperature, independently of the spin polarization of the ferromagnetic core. This discovery shows how the nanoscale impacts magnetotransport in a material widely spread as electrode in hybrid spintronic devices.

    7. A Transparent, Self-Healing, Highly Stretchable Ionic Conductor

      Yue Cao, Timothy G. Morrissey, Eric Acome, Sarah I. Allec, Bryan M. Wong, Christoph Keplinger and Chao Wang

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201605099

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      Self-healing materials can repair damage caused by mechanical wear, thereby extending lifetime of devices. Here, a transparent, self-healing, highly stretchable ionic conductor is presented that autonomously heals after experiencing severe mechanical damage. The design of this self-healing polymer uses ion–dipole interactions as the dynamic motif. The unique properties of this material when used to electrically activate transparent artificial muscles are demonstrated.

    8. Direct Synthesis of Graphdiyne Nanowalls on Arbitrary Substrates and Its Application for Photoelectrochemical Water Splitting Cell

      Xin Gao, Jian Li, Ran Du, Jingyuan Zhou, Mao-Yong Huang, Rong Liu, Jie Li, Ziqian Xie, Li-Zhu Wu, Zhongfan Liu and Jin Zhang

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201605308

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      A general and simple route to fabricate graphdiyne nanowalls on arbitrary substrates is developed by using a copper envelope catalysis strategy. The GDY/BiVO4 system is but one example of combing the unique properites of GDY with those target substrates where GDY improves the photoelectrochemical performance dramatically.

    9. Nanosheets of an Organic Molecular Assembly from Aqueous Medium Exhibit High Solid-State Emission and Anisotropic Charge-Carrier Mobility

      Samrat Ghosh, Divya Susan Philips, Akinori Saeki and Ayyappanpillai Ajayaghosh

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201605408

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      A π-conjugated amphiphilic diketopyrrolopyrrole (PDPP-Amphi) forms crystalline 2D supramolecular nanosheets in water when compared to that from methyl cyclohexane. These nanosheets exhibit high fluorescence quantum yield in the solid-state with anisotropic charge-carrier mobility of 0.33 cm2 V–1 s–1.

    10. Green-Light-Emitting Diodes based on Tetrabromide Manganese(II) Complex through Solution Process

      Liang-Jin Xu, Cheng-Zhe Sun, Hui Xiao, Yue Wu and Zhong-Ning Chen

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201605739

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      Highly phosphorescent (Ph4P)2[MnBr4] as a low-cost and environmentally benign emitting material achieves peak current efficiency of 25.4 cd A−1 and external quantum efficiency (EQE) of 7.2% for nondoped organic light-emitting diodes, and peak current efficiency of 32.0 cd A−1 and EQE of 9.6% for doped devices with 20% (Ph4P)2[MnBr4]:27% TCTA:53% 6DCZPPY as a doping emitting layer.

    11. Humidity- and Photo-Induced Mechanical Actuation of Cross-Linked Liquid Crystal Polymers

      Yuyun Liu, Bo Xu, Shengtong Sun, Jia Wei, Limin Wu and Yanlei Yu

      Version of Record online: 23 DEC 2016 | DOI: 10.1002/adma.201604792

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      Azobenzene-containing cross-linked liquid crystal polymer films without hydrophilic groups exhibit dual-responsivity to humidity and UV light. The films realize not only a series of large and sophisticated contactless motions by utilizing moisture, including an inchworm walk, and tumbling locomotion, but also dual-mode actuation that can be applied in flexible electronics.

    12. 3D Chemical Patterning of Micromaterials for Encoded Functionality

      Hakan Ceylan, Immihan Ceren Yasa and Metin Sitti

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/adma.201605072

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      Programming local chemical properties of microscale soft materials with 3D complex shapes is indispensable for creating sophisticated functionalities, which has not yet been possible with existing methods. Here, precise spatiotemporal control of two-photon crosslinking is employed as an enabling tool for 3D patterning of microprinted structures for encoding versatile chemical moieties.

    13. Mineral Nano-Interconnectivity Stiffens and Toughens Nacre-like Composite Materials

      Madeleine Grossman, Florian Bouville, Florian Erni, Kunal Masania, Rafael Libanori and André R. Studart

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/adma.201605039

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      Bulk nacre-like composites with mineral nano-interconnectivity at the same length scale as in the biological material were produced using magnetic alignment and selective sintering techniques. These materials display stiffness and strength levels comparable to that of continuous fiber composites with the advantage of easier processability inherent of discontinuous composites. This opens new possibilities to produce parts with more complex designs.

    14. In-Plane Deformation Mechanics for Highly Stretchable Electronics

      Yewang Su, Xuecheng Ping, Ki Jun Yu, Jung Woo Lee, Jonathan A. Fan, Bo Wang, Ming Li, Rui Li, Daniel V. Harburg, YongAn Huang, Cunjiang Yu, Shimin Mao, Jaehoun Shim, Qinglin Yang, Pei-Yin Lee, Agne Armonas, Ki-Joong Choi, Yichen Yang, Ungyu Paik, Tammy Chang, Thomas J. Dawidczyk, Yonggang Huang, Shuodao Wang and John A. Rogers

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/adma.201604989

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      Scissoring in thick bars suppresses buckling behavior in serpentine traces that have thicknesses greater than their widths, as detailed in a systematic set of analytical and experimental studies. Scissoring in thick copper traces enables elastic stretchability as large as ≈350%, corresponding to a sixfold improvement over previously reported values for thin geometries (≈60%).

    15. Active Electrochemical Plasmonic Switching on Polyaniline-Coated Gold Nanocrystals

      Wenzheng Lu, Nina Jiang and Jianfang Wang

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/adma.201604862

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      High-performance electrochemical plasmonic switching is realized on both single-particle and ensemble levels by coating polyaniline on colloidal gold nanocrystals through surfactant-assisted oxidative polymerization. Under small applied potentials, the core@shell nanostructures exhibit reversible plasmon shifts as large as 150 nm, a switching time of less than 10 ms, and a high switching stability.

  40. Reviews

    1. Progress in Understanding Degradation Mechanisms and Improving Stability in Organic Photovoltaics

      William R. Mateker and Michael D. McGehee

      Version of Record online: 22 DEC 2016 | DOI: 10.1002/adma.201603940

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      Understanding the degradation mechanisms that reduce the long-term stability in organic photovoltaics is imperative. The present understanding of degradation mechanisms and strategies researchers can use to identify them in new materials are reviewed. Some of the relevant materials properties that can be tuned to improve the long-term performance of organic photovoltaics are identified.