Advanced Materials

Cover image for Vol. 28 Issue 24

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

  1. Communications

    1. 2D Protein Supramolecular Nanofilm with Exceptionally Large Area and Emergent Functions

      Dehui Wang, Yuan Ha, Jin Gu, Qian Li, Liangliang Zhang and Peng Yang

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201506476

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      2D nanofilms assembled by pure protein with a macroscopic area and multiple functions can be directly formed at the air/water interface or at the solid surface at a timescale of several minutes. The multifunctionality of the nanofilm coating is demonstrated by both top-down and bottom-up micro/nanoscale interfacial engineering, including surface modification, all-water-based photo/electron beam lithography, and electroless deposition.

    2. Alloy Acceptor: Superior Alternative to PCBM toward Efficient and Stable Organic Solar Cells

      Pei Cheng, Cenqi Yan, Yang Wu, Jiayu Wang, Meng Qin, Qiaoshi An, Jiamin Cao, Lijun Huo, Fujun Zhang, Liming Ding, Yanming Sun, Wei Ma and Xiaowei Zhan

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201602067

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      The alloy acceptor (indene-C60 bis-adduct (ICBA)/[6,6]-phenyl-C71-butyric acid-methyl-ester (PC71BM)) is employed to replace the widely used fullerene acceptor (PC71BM) in organic solar cells based on five different polymer donors, which exhibits a higher efficiency and much better device stability than the PC71BM counterpart.

    3. Controlling Synergistic Oxidation Processes for Efficient and Stable Blue Thermally Activated Delayed Fluorescence Devices

      Lin-Song Cui, Ya-Li Deng, Daniel Ping-Kuen Tsang, Zuo-Quan Jiang, Qisheng Zhang, Liang-Sheng Liao and Chihaya Adachi

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201602127

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      Efficient sky-blue organic light-emitting diodes (OLEDs) employing thermally activated delayed fluorescence (TADF) display a three orders of magnitude increase in lifetime, which is superior to those of controlled phosphorescent OLEDs used in this study. The combination of electro-oxidation and photo-oxidation of the TADF emitters in their triplet excited-states is suppressed through molecule design and device engineering.

    4. You have full text access to this OnlineOpen article
      Nanoscale Transformations in Metastable, Amorphous, Silicon-Rich Silica

      Adnan Mehonic, Mark Buckwell, Luca Montesi, Manveer Singh Munde, David Gao, Stephen Hudziak, Richard J. Chater, Sarah Fearn, David McPhail, Michel Bosman, Alexander L. Shluger and Anthony J. Kenyon

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201601208

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      Electrically biasing thin films of amorphous, substoichiometric silicon oxide drives surprisingly large structural changes, apparent as density variations, oxygen movement, and ultimately, emission of superoxide ions. Results from this fundamental study are directly relevant to materials that are increasingly used in a range of technologies, and demonstrate a surprising level of field-driven local reordering of a random oxide network.

    5. Efficient Visible Quasi-2D Perovskite Light-Emitting Diodes

      Jinwoo Byun, Himchan Cho, Christoph Wolf, Mi Jang, Aditya Sadhanala, Richard H. Friend, Hoichang Yang and Tae-Woo Lee

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201601369

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      Efficient quasi-2D-structure perovskite light-emitting diodes (4.90 cd A−1) are demonstrated by a mixing 3D-structured perovskite material (methyl ammonium lead bromide) and a 2D-structured perovskite material (phenylethyl ammonium lead bromide), which can be ascribed to better film uniformity, enhanced exciton confinement, and reduced trap density.

    6. In Situ Patterning of Microfluidic Networks in 3D Cell-Laden Hydrogels

      Nathalie Brandenberg and Matthias P. Lutolf

      Version of Record online: 23 JUN 2016 | DOI: 10.1002/adma.201601099

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      Focalized short-pulsed lasers have sufficient power to generate micrometer-sized cavities in various hydrogels. An in situ technique based on laser ablation to fabricate intricate microfluidic networks in biocompatible gels without manual handling is presented. This method is fully compatible with 3D cell culture and opens up unprecedented opportunities for cell biology, developmental biology, and stem-cell-based tissue engineering.

    7. In Situ Control of Separate Electronic Phases on SrTiO3 Surfaces by Oxygen Dosing

      Lenart Dudy, Michael Sing, Philipp Scheiderer, Jonathan D. Denlinger, Philipp Schütz, Judith Gabel, Mathias Buchwald, Christoph Schlueter, Tien-Lin Lee and Ralph Claessen

      Version of Record online: 22 JUN 2016 | DOI: 10.1002/adma.201600046

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      Insulating SrTiO3 (STO) can host 2D electron systems (2DESs) on its surfaces caused by oxygen defects. This study shows that the STO surface exhibits phase separation once the 2DES is formed. This study relates this inhomogeneity to recently reported magnetic order at STO surfaces and interfaces. The results open pathways to exploit oxygen defects for engineering the electronic and magnetic properties of oxides.

    8. Fabrication of Hydrogel Particles of Defined Shapes Using Superhydrophobic-Hydrophilic Micropatterns

      Ana I. Neto, Konstantin Demir, Anna A. Popova, Mariana B. Oliveira, João F. Mano and Pavel A. Levkin

      Version of Record online: 22 JUN 2016 | DOI: 10.1002/adma.201602350

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      High-throughput fabrication of freestanding hydrogel particles with defined geometry and size for 3D cell culture, cell screenings, and modular tissue engineering is reported here. The method employs discontinuous dewetting using superhydrophobic–hydrophilic micropatterns.

  2. Research News

    1. You have full text access to this OnlineOpen article
      Quenching of Charge and Spin Degrees of Freedom in Condensed Matter

      Fumitaka Kagawa and Hiroshi Oike

      Version of Record online: 21 JUN 2016 | DOI: 10.1002/adma.201601979

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      Quenched charge/spin/orbital states that are qualitatively different from the ground state can emerge under rapid cooling, such as 102–103 K s−1, and thus, the cooling rate is a control parameter of an electronic/magnetic state beyond the framework of the thermoequilibrium phase diagram. Such quenched states allow the design of an exotic class of phase-change memory.

    2. Self-Assembly of Chiral Plasmonic Nanostructures

      Xiang Lan and Qiangbin Wang

      Version of Record online: 21 JUN 2016 | DOI: 10.1002/adma.201600697

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      A large variety of chiral plasmonic nanostructures can be achieved with bottom-up self-assembly methods, including DNA-, peptide-, and cellulose-nanocrystal-directed chiral arrangement of nanoparticles. Self-assembled chiral plasmonic nanostructures exhibit novel optical activity in the visible wavelength region, and pave the way for the progress of chiral plasmonics.

  3. Communications

    1. Octopus-Inspired Smart Adhesive Pads for Transfer Printing of Semiconducting Nanomembranes

      Hochan Lee, Doo-Seung Um, Youngsu Lee, Seongdong Lim, Hyung-jun Kim and Hyunhyub Ko

      Version of Record online: 20 JUN 2016 | DOI: 10.1002/adma.201601407

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      By mimicking muscle actuation to control cavity-pressure-induced adhesion of octopus suckers, smart adhesive pads are developed in which the thermoresponsive actuation of a hydrogel layer on elastomeric microcavity pads enables excellent switchable adhesion in response to a thermal stimulus (maximum adhesive strength: 94 kPa, adhesion switching ratio: ≈293 for temperature change between 22 and 61 °C).

    2. Novel Air Stable Organic Radical Semiconductor of Dimers of Dithienothiophene, Single Crystals, and Field-Effect Transistors

      Hantang Zhang, Huanli Dong, Yang Li, Wei Jiang, Yonggang Zhen, Lang Jiang, Zhaohui Wang, Wei Chen, Angela Wittmann and Wenping Hu

      Version of Record online: 20 JUN 2016 | DOI: 10.1002/adma.201601502

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      Singly linked and vinyl linked dimer of dithienothiophenes exhibit different electronic behaviors. Single crystal of singly linked dimer shows high conductivity of 0.265 S cm−1, five orders of magnitude higher than that of vinyl linked dimer. The huge increase in the hole density of singly linked dimers results from formation of radicals, which can be reversibly tuned by facile thermal de-doping.

    3. 2D Layered Materials of Rare-Earth Er-Doped MoS2 with NIR-to-NIR Down- and Up-Conversion Photoluminescence

      Gongxun Bai, Shuoguo Yuan, Yuda Zhao, Zhibin Yang, Sin Yuk Choi, Yang Chai, Siu Fung Yu, Shu Ping Lau and Jianhua Hao

      Version of Record online: 20 JUN 2016 | DOI: 10.1002/adma.201601833

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      A 2D system of Er-doped MoS2 layered nanosheet has been developed. Structural studies indicate that the Er atoms can be substitutionally introduced into MoS2 to form stable doping. Density functional theory calculation implies that the system remains stable. Both NIR-to-NIR up-conversion and down-conversion light-emissions are observed in 2D transition metal dichalcogenides, ascribed to the energy transition from Er3+ dopants.

    4. Controllable Self-Assembly of RNA Tetrahedrons with Precise Shape and Size for Cancer Targeting

      Hui Li, Kaiming Zhang, Fengmei Pi, Sijin Guo, Luda Shlyakhtenko, Wah Chiu, Dan Shu and Peixuan Guo

      Version of Record online: 20 JUN 2016 | DOI: 10.1002/adma.201601976

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      RNA tetrahedral nanoparticles with two different sizes are successfully assembled by a one-pot bottom-up approach with high efficiency and thermal stability. The reported design principles can be extended to construct higher order polyhedral RNA architectures for various applications such as targeted cancer imaging and therapy.

    5. Towards the Nanosheet-Based Photonic Nose: Vapor Recognition and Trace Water Sensing with Antimony Phosphate Thin Film Devices

      Pirmin Ganter, Katalin Szendrei and Bettina V. Lotsch

      Version of Record online: 17 JUN 2016 | DOI: 10.1002/adma.201601992

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      A 2D nanosheet-based photonic nose for vapor identification is presented. A HSbP2O8 nanosheet thin film sensor with resistive readout is developed for the tracking of trace amounts of water, and a photonic HSbP2O8/TiO2 multilayer structure is effective at optically distinguishing between chemically similar solvent vapors through analyte-specific host-guest interactions.

    6. Wavelength-Tunable Microlasers Based on the Encapsulation of Organic Dye in Metal–Organic Frameworks

      Yanhui Wei, Haiyun Dong, Cong Wei, Wei Zhang, Yongli Yan and Yong Sheng Zhao

      Version of Record online: 17 JUN 2016 | DOI: 10.1002/adma.201601844

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      A wavelength-tunable microlaser has been realized based on the controlled intramolecular charge transfer (ICT) process in dye-encapsulated metal–organic framework (MOF) material. The confinement effect of MOFs is beneficial for low-threshold lasing. By effectively controlling the polarity of the MOF pores, the population distribution between the locally excited and ICT states is continuously modulated, thus achieving broadband tunable MOF-based microlasers.

    7. Heterostructured hBN-BP-hBN Nanodetectors at Terahertz Frequencies

      Leonardo Viti, Jin Hu, Dominique Coquillat, Antonio Politano, Christophe Consejo, Wojciech Knap and Miriam S. Vitiello

      Version of Record online: 17 JUN 2016 | DOI: 10.1002/adma.201601736

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      By reassembling the thin isolated atomic planes of hexagonal borum nitride (hBN) with a few layer phosphorene (black phosphorus BP), hBN/BP/hBN heterostructures were mechanically stacked to devise high efficiency THz photodetectors operating in the 0.3–0.65 THz range, from 4K to 300K, with a record signal-to-noise ratio of 20000.

    8. Superhydrophobic Diffusion Barriers for Hydrogels via Confined Interfacial Modification

      Xi Yao, Lie Chen, Jie Ju, Changhua Li, Ye Tian, Lei Jiang and Mingjie Liu

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601568

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      A ubiquitous strategy to superhydrophobize the surfaces of synthetic hydrogels is reported, creating heterogeneous wettability across the surface and the inner network. Such wetting disparity shows significant influence on preventing immediate diffusion of substances between the hydrogel and the aqueous environment on different scales.

    9. Phase-Transformation Engineering in Cobalt Diselenide Realizing Enhanced Catalytic Activity for Hydrogen Evolution in an Alkaline Medium

      Pengzuo Chen, Kun Xu, Shi Tao, Tianpei Zhou, Yun Tong, Hui Ding, Lidong Zhang, Wangsheng Chu, Changzheng Wu and Yi Xie

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601663

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      Phase-transformation engineering is successfully applied in designing an alkaline hydrogen evolution reaction (HER) electrocatalyst. Benefiting from phase-transformation engineering, which endows higher electrical conductivity, ideal water adsorption energy, and faster transformation efficiency of Hads into hydrogen, cubic-phase CoSe2 realizes an enhanced electrocatalytic activity for HER under alkaline conditions.

    10. Current Switching Coupled to Molecular Spin-States in Large-Area Junctions

      Constantin Lefter, Sylvain Rat, José Sánchez Costa, María D. Manrique-Juárez, Carlos M. Quintero, Lionel Salmon, Isabelle Séguy, Thierry Leichle, Liviu Nicu, Philippe Demont, Aurelian Rotaru, Gábor Molnár and Azzedine Bousseksou

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601420

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      The fabrication of large-area vertical junctions with a molecular spin crossover complex displaying concerted changes of spin degrees of freedom and charge transport properties is reported. Fabricated devices allow spin-state switching in the spin-crossover layer to be triggered and probed by optical means, while detecting associated changes in electrical resistance in the junctions.

    11. Self-Assembled PDINH Supramolecular System for Photocatalysis under Visible Light

      Di Liu, Jun Wang, Xiaojuan Bai, Ruilong Zong and Yongfa Zhu

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601168

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      A self-assembled perylene-3,4,9,10-tetracarboxylic diimide(PDINH) supramolecular system consisting of all-organic PDINH molecule building blocks through non-covalent interactions works as a visible light photocatalyst with high activity.

    12. Target Delivery of a Novel Antitumor Organoplatinum(IV)-Substituted Polyoxometalate Complex for Safer and More Effective Colorectal Cancer Therapy In Vivo

      Tiedong Sun, Wei Cui, Mei Yan, Geng Qin, Wei Guo, Hongxi Gu, Shaoqin Liu and Qiong Wu

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601778

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      An inactive organoplatinum(IV)-substituted polyoxometalate is developed as an efficient and nontoxic prodrug with significant potential for treating human colorectal cancers. Further encapsulation of PtIV-PW11 with DSPE-PEG2000 nanoparticles (NPs) enables targeted delivery and controlled release of inactive prodrug. Such PtIV-PW11-DSPE-PEG2000 NPs are highly efficient in inhibiting cellular growth of HT29 cells and treating human colorectal cancer in mice, superior to classic cisplatin.

    13. Implementing Room-Temperature Multiferroism by Exploiting Hexagonal-Orthorhombic Morphotropic Phase Coexistence in LuFeO3 Thin Films

      Seungwoo Song, Hyeon Han, Hyun Myung Jang, Young Tae Kim, Nam-Suk Lee, Chan Gyung Park, Jeong Rae Kim, Tae Won Noh and James F. Scott

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601989

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      Room-temperature multiferroism in LuFeO3 (LFO) films is demonstrated by exploiting the orthorhombic-hexagonal (o-h) morphotrophic phase coexistence. The LFO film further reveals magnetoelectric coupling effect that is not shown in single-phase (h- or o-) LFO. The observed multiferroism is attributed to the combination of sufficient polarization from h-LFO and net magnetization from o-LFO.

    14. High-Performance Polymer Solar Cells with PCE of 10.42% via Al-Doped ZnO Cathode Interlayer

      Xiaohui Liu, Xiaodong Li, Yaru Li, Changjian Song, Liping Zhu, Wenjun Zhang, Hai-Qiao Wang and Junfeng Fang

      Version of Record online: 16 JUN 2016 | DOI: 10.1002/adma.201601814

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      High performance polymer solar cells incorporating the low-temperature processed aluminum-doped zinc oxide (AZO) cathode interlayer are constructed with power conversion efficiency (PCE) of 10.42% based on PTB7-Th:PC71BM blends (insensitive to AZO thickness). Moreover, flexible devices on PET/ITO substrates with PCE of 8.93% are also obtained and well distributed efficiency and good device stability are demonstrated as well.

    15. Nanoscale Positioning of Single-Photon Emitters in Atomically Thin WSe2

      Johannes Kern, Iris Niehues, Philipp Tonndorf, Robert Schmidt, Daniel Wigger, Robert Schneider, Torsten Stiehm, Steffen Michaelis de Vasconcellos, Doris E. Reiter, Tilmann Kuhn and Rudolf Bratschitsch

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201600560

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      Single-photon emitters in monolayer WSe2 are created at the nanoscale gap between two single-crystalline gold nanorods. The atomically thin semiconductor conforms to the metal nanostructure and is bent at the position of the gap. The induced strain leads to the formation of a localized potential well inside the gap. Single-photon emitters are localized there with a precision better than 140 nm.

    16. Subzero-Temperature Cathode for a Sodium-Ion Battery

      Ya You, Hu-Rong Yao, Sen Xin, Ya-Xia Yin, Tong-Tong Zuo, Chun-Peng Yang, Yu-Guo Guo, Yi Cui, Li-Jun Wan and John B. Goodenough

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201600846

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      A subzero-temperature cathode material is obtained by nucleating cubic prussian blue crystals at inhomogeneities in carbon nanotubes. Due to fast ionic/electronic transport kinetics even at −25 °C, the cathode shows an outstanding low-temperature performance in terms of specific energy, high-rate capability, and cycle life, providing a practical sodium-ion battery powering an electric vehicle in frigid regions.

    17. Sliding Hydrogels with Mobile Molecular Ligands and Crosslinks as 3D Stem Cell Niche

      Xinming Tong and Fan Yang

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201601484

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      Here, the development of a sliding hydrogel with mobile crosslinks and biochemical ligands as a 3D stem cell niche is reported. The molecular mobility of this sliding hydrogel allows stem cells to reorganize the surrounding ligands and change their morphology in 3D. Without changing matrix stiffness, sliding hydrogels support efficient stem cell differentiation toward multiple lineages including adipogenesis, chondrogenesis, and osteogenesis.

    18. Aqueous Solution Processed Photoconductive Cathode Interlayer for High Performance Polymer Solar Cells with Thick Interlayer and Thick Active Layer

      Li Nian, Zhenhui Chen, Stefanie Herbst, Qingyuan Li, Chengzhuo Yu, Xiaofang Jiang, Huanli Dong, Fenghong Li, Linlin Liu, Frank Würthner, Junwu Chen, Zengqi Xie and Yuguang Ma

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201601615

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      An aqueous solution processed photoconductive cathode interlayer is developed, in which the photoinduced charge transfer brings multiple advantages such as increased conductivity and electron mobility as well as reduced work function. Average power conversion efficiency over 10% is achieved even when the thickness of the cathode interlayer and active layer is up to 100 and 300 nm, respectively.

    19. Triboelectric Nanogenerator Accelerates Highly Efficient Nonviral Direct Conversion and In Vivo Reprogramming of Fibroblasts to Functional Neuronal Cells

      Yoonhee Jin, Jungmok Seo, Jung Seung Lee, Sera Shin, Hyun-Ji Park, Sungjin Min, Eunji Cheong, Taeyoon Lee and Seung-Woo Cho

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201601900

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      Triboelectric nanogenerators (TENGs) can be an effective cell reprogramming platform for producing functional neuronal cells for therapeutic applications. Triboelectric stimulation accelerates nonviral direct conversion of functional induced neuronal cells from fibroblasts, increases the conversion efficiency, and induces highly matured neuronal phenotypes with improved electrophysiological functionalities. TENG devices may also be used for biomedical in vivo reprogramming.

  4. Reviews

    1. Nanoscale Engineering of Heterostructured Anode Materials for Boosting Lithium-Ion Storage

      Gen Chen, Litao Yan, Hongmei Luo and Shaojun Guo

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201600164

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      The concept of materials engineering and design is exceptionally important in the development of electrode materials with high energy and power densities and good stability, as well as other features such as light weight and flexibility. Nanoscale engineering brings new visions into the fabrication of novel heterostructured electrode materials with specific features, which can provide the anticipated electrochemical performance. Therefore they are promising for next-generation lithium-ion batteries.

  5. Communications

    1. Activatable Fluorescent Nanoprobe with Aggregation-Induced Emission Characteristics for Selective In Vivo Imaging of Elevated Peroxynitrite Generation

      Zhegang Song, Duo Mao, Simon H. P. Sung, Ryan T. K. Kwok, Jacky W. Y. Lam, Deling Kong, Dan Ding and Ben Zhong Tang

      Version of Record online: 15 JUN 2016 | DOI: 10.1002/adma.201601214

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      An activatable fluorescent nanoprobe with aggregation-induced emission signature is developed. The nanoprobe is nonfluorescent, but can be induced to emit intensely after reaction with peroxynitrite forming an intramolecular hydrogen bond. Excellent performance for selective in vivo imaging of inflammation with elevated peroxynitrite generation and efficient visualization of in vivo treatment efficacy of anti-inflammatory agents is demonstrated.

    2. Fast and Sensitive Solution-Processed Visible-Blind Perovskite UV Photodetectors

      Valerio Adinolfi, Olivier Ouellette, Makhsud I. Saidaminov, Grant Walters, Ahmed L. Abdelhady, Osman M. Bakr and Edward H. Sargent

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201601196

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      The first visible-blind UV photodetector based on MAPbCl3 integrated on a substrate exhibits excellent performance, with responsivities reaching 18 A W−1 below 400 nm and imaging-compatible response times of 1 ms. This is achieved by using substrate-integrated single crystals, thus overcoming the severe limitations affecting thin films and offering a new application of efficient, solution-processed, visible-transparent perovskite optoelectronics.

    3. A Universal Soaking Strategy to Convert Composite Hydrogels into Extremely Tough and Rapidly Recoverable Double-Network Hydrogels

      Yanyu Yang, Xing Wang, Fei Yang, Hong Shen and Decheng Wu

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201601742

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      Soak n' Boost: A universal strategy to manufacture hybrid double-network hydrogels with eminent mechanical properties is developed by postformation of the chitosan microcrystalline and chain-entanglement physical networks via simple treatment of the chitosan composite hydrogels using alkaline and saline solutions. The strategy may open an avenue to fabricate multifarious double-network hydrogels for promising applications in antifouling materials, drug delivery, and tissue engineering.

    4. Defect-Engineered Graphene for High-Energy- and High-Power-Density Supercapacitor Devices

      Jingyi Zhu, Anthony S. Childress, Mehmet Karakaya, Sushmita Dandeliya, Anurag Srivastava, Ye Lin, Apparao M. Rao and Ramakrishna Podila

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201602028

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      Defects are often written off as performance limiters. Contrary to this notion, it is shown that controlling the defect configuration in graphene is critical to overcome a fundamental limitation posed by quantum capacitance and opens new channels for ion diffusion. Defect-engineered graphene flexible pouch capacitors with energy densities of 500% higher than the state-of-the-art supercapacitors are demonstrated.

    5. Bright Stretchable Alternating Current Electroluminescent Displays Based on High Permittivity Composites

      Flurin Stauffer and Klas Tybrandt

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201602083

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      A high permittivity composite is developed to enhance the brightness of stretchable electroluminescent displays. The unique two-step assembly process yields dense layers, in which the voids around the electroluminescent particles are filled with smaller high dielectric particles. A stretchable seven-segment display based on the composite is bright enough to be used under standard indoor lighting conditions.

    6. PGMA-Based Star-Like Polycations with Plentiful Hydroxyl Groups Act as Highly Efficient miRNA Delivery Nanovectors for Effective Applications in Heart Diseases

      Rui-Quan Li, Yina Wu, Ying Zhi, Xinchao Yang, Yulin Li, Jie Du and Fu-Jian Xu

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201602319

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      Poly(glycidyl methacrylate)-based star-like polycations with rich hydrophilic hydroxyl groups can efficiently transfer miRNA into primary cardiac fibroblasts for effective applications in cardiac diseases, such as inhibition of cardiac fibrosis and hypertrophy.

  6. Progress Reports

    1. Smart Gating Multi-Scale Pore/Channel-Based Membranes

      Xu Hou

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201600797

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      Smart gating membranes are important and promising in membrane science and technology. Rapid progress in developing smart membranes is transforming technology in many different fields, from energy and environmental to the life sciences. How a specific smart behavior for controllable gating of porous membranes can be obtained, especially for nano- and micrometer-sized multi-scale pore/channel-based membrane systems is addressed.

  7. Communications

    1. Metal–Organic Covalent Network Chemical Vapor Deposition for Gas Separation

      Nicolas D. Boscher, Minghui Wang, Alberto Perrotta, Katja Heinze, Mariadriana Creatore and Karen K. Gleason

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201601010

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      The chemical vapor deposition (CVD) polymerization of metalloporphyrin building units is demonstrated to provide an easily up-scalable one-step method toward the deposition of a new class of dense and defect-free metal–organic covalent network (MOCN) layers. The resulting hyper-thin and flexible MOCN layers exhibit outstanding gas-separation performances for multiple gas pairs.

    2. Highly Conductive, Air-Stable Silver Nanowire@Iongel Composite Films toward Flexible Transparent Electrodes

      Weiwei Xiong, Hongliang Liu, Yongzhen Chen, Meiling Zheng, Yuanyuan Zhao, Xiangbin Kong, Ying Wang, Xiqi Zhang, Xiangyu Kong, Pengfei Wang and Lei Jiang

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201600358

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      A new type of flexible transparent electrode is designed, by employing wettability-induced selective electroless-welding of silver nanowire (AgNW) networks, together with a thin conductive iongel as the protective layer. The obtained electrode exhibits high optical transmittance, and excellent air-stability without sacrificing conductivity.

    3. Superaerophilic Carbon-Nanotube-Array Electrode for High-Performance Oxygen Reduction Reaction

      Zhiyi Lu, Wenwen Xu, Jun Ma, Yingjie Li, Xiaoming Sun and Lei Jiang

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201504652

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      A micro-/nanostructured “superaerophilic” electrode constructed by direct growth of cobalt-incorporated and nitrogen-doped carbon-nanotube arrays with subsequent hydrophobic modification is demonstrated for a high-performance oxygen-reduction-reaction electrode, superior to the Pt/C–air electrode. This high performance is attributed to the simultaneously accelerated gas-diffusion and electron-transport processes induced by the unique structural advantages.

    4. Visualizing Light Scattering in Silicon Waveguides with Black-Phosphorus Photodetectors

      Tianjiao Wang, Shuren Hu, Bhim Chamlagain, Tu Hong, Zhixian Zhou, Sharon M. Weiss and Ya-Qiong Xu

      Version of Record online: 14 JUN 2016 | DOI: 10.1002/adma.201506277

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      A black-phosphorus photodetector is utilized to investigate the light-scattering patterns of a silicon waveguide through wavelength- and polarization-dependent scanning photocurrent measurements. The photocurrent signals exhibit similar patterns to the light-intensity distribution of the waveguide calculated by finite-difference time-domain simulations, suggesting that photoexcited electron–hole pairs in the silicon waveguide can be injected into phosphorene to induce its photoresponse.

    5. Construction of 3D Metallic Nanostructures on an Arbitrarily Shaped Substrate

      Fei Chen, Jingning Li, Fangfang Yu, Di Zhao, Fan Wang, Yanbin Chen, Ru-Wen Peng and Mu Wang

      Version of Record online: 13 JUN 2016 | DOI: 10.1002/adma.201602049

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      Constructing conductive/magnetic nanowire arrays with 3D features by electrodeposition remains challenging. An unprecedented fabrication approach that allows to construct metallic (cobalt) nanowires on an arbitrarily shaped surface is reported. The spatial separation of nanowires varies from 70 to 3000 nm and the line width changes from 50 to 250 nm depending on growth conditions.

    6. Self-Junctioned Copper Nanofiber Transparent Flexible Conducting Film via Electrospinning and Electroplating

      Seongpil An, Hong Seok Jo, Do-Yeon Kim, Hyun Jun Lee, Byeong-Kwon Ju, Salem S. Al-Deyab, Jong-Hyun Ahn, Yueling Qin, Mark T. Swihart, Alexander L. Yarin and Sam S. Yoon

      Version of Record online: 13 JUN 2016 | DOI: 10.1002/adma.201506364

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      Self-junctioned copper nanofiber transparent flexible films are produced using electrospinning and electroplating processes that provide high performances of T = 97% and Rs = 0.42 Ω sq−1 by eliminating junction resistance at wire intersections. The film remains conductive after being stretched by up to 770% (films with T = 76%) and after 1000 cycles of bending to a 5 mm radius.

    7. Intelligent Albumin–MnO2 Nanoparticles as pH-/H2O2-Responsive Dissociable Nanocarriers to Modulate Tumor Hypoxia for Effective Combination Therapy

      Qian Chen, Liangzhu Feng, Jingjing Liu, Wenwen Zhu, Ziliang Dong, Yifan Wu and Zhuang Liu

      Version of Record online: 10 JUN 2016 | DOI: 10.1002/adma.201601902

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      A unique type of pH/H2O2 dual-responsive intelligent nanoscale delivery system based on albumin-coated MnO2 is presented, which is capable of modulating the tumor microenvironment (TME) by relieving hypoxia. Additionally, TME-responsive size changes enable effective intratumor diffusion. A highly effective combined photodynamic and chemotherapy is realized with these nanoparticles in a mouse tumor model.

    8. Superior Chemical Sensing Performance of Black Phosphorus: Comparison with MoS2 and Graphene

      Soo-Yeon Cho, Youhan Lee, Hyeong-Jun Koh, Hyunju Jung, Jong-Seon Kim, Hae-Wook Yoo, Jihan Kim and Hee-Tae Jung

      Version of Record online: 10 JUN 2016 | DOI: 10.1002/adma.201601167

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      Superior chemical sensing performance of black phosphorus (BP) is demonstrated by comparison with MoS2 and graphene. Dynamic sensing measurements of multichannel detection show that BP displays highly sensitive, selective, and fast-responsive NO2 sensing performance compared to the other representative 2D sensing materials.

  8. Reviews

    1. Carbon Nanomembranes

      Andrey Turchanin and Armin Gölzhäuser

      Version of Record online: 9 JUN 2016 | DOI: 10.1002/adma.201506058

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      Carbon nanomembranes (CNMs) are made by radiation-induced crosslinking of aromatic self-assembled monolayers and their subsequent release from the substrate. CNMs are molecularly thin, mechanically stable, and chemically functionalizable films with tunable electrical, mechanical, and biofunctional properties. Large-area CNMs can be prepared with sizes of up to 25 cm × 25 cm on solid supports, and 500 µm × 500 µm free-standing.

  9. Communications

    1. Effect of Internal Electric Fields on Charge Carrier Dynamics in a Ferroelectric Material for Solar Energy Conversion

      Madeleine R. Morris, Stephanie R. Pendlebury, Jongin Hong, Steve Dunn and James R. Durrant

      Version of Record online: 9 JUN 2016 | DOI: 10.1002/adma.201601238

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      Spontaneous polarization is shown to enhance the lifetimes of photogenerated species in BaTiO3. This is attributed to polarization-induced surface band bending acting as a thermal barrier to electron/hole recombination. The study indicates that the efficiencies of solar cells and solar fuels devices can be enhanced by the use of ferroelectric materials.

    2. Low-Temperature Chemical Vapor Deposition Synthesis of Pt–Co Alloyed Nanoparticles with Enhanced Oxygen Reduction Reaction Catalysis

      Dong Sung Choi, Alex W. Robertson, Jamie H. Warner, Sang Ouk Kim and Heeyeon Kim

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201600469

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      Novel Pt–Co alloyed nanocatalysts are generated via chemical vapor deposition-assisted facile one-pot synthesis. The method guarantees highly monodisperse Pt–Co alloy nanoparticles with precise control of metallic compositions within 1 at%. A significant features is that a perfectly alloyed single-crystal structure is obtained at temperatures as low as 500 °C, which is much lower than conventional alloying temperatures.

    3. Peapod-Like Carbon-Encapsulated Cobalt Chalcogenide Nanowires as Cycle-Stable and High-Rate Materials for Sodium-Ion Anodes

      Chao Wu, Yu Jiang, Peter Kopold, Peter A. van Aken, Joachim Maier and Yan Yu

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201600964

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      Peapod-like carbon-encapsulated cobalt chalcogenide nanowires are designed and synthesized by a facile method. The nanowires show excellent electrochemical performance for sodium storage, suggesting that chalcogenides, especially selenides, have potential as advanced anodes for sodium-ion batteries.

    4. Unveiling the Switching Riddle of Silver Tetracyanoquinodimethane Towards Novel Planar Single-Crystalline Electrochemical Metallization Memories

      Fangxu Yang, Qiang Zhao, Chunhui Xu, Ye Zou, Huanli Dong, Yonggang Zheng and Wenping Hu

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201600902

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      It is unveiled that the switching riddle of AgTCNQ is caused by the solid electrolyte mechanism. Both factors of bulk phase change and contact issue play key roles in the efficient work of the devices. An effective strategy is developed to locate the formation/disruption of Ag conductive filaments using the planar asymmetric configuration of Au/AgTCNQ/AlOx/Al. These novel electrochemical metallization memories demonstrate many promising properties.

    5. Catalase-Loaded TaOx Nanoshells as Bio-Nanoreactors Combining High-Z Element and Enzyme Delivery for Enhancing Radiotherapy

      Guosheng Song, Yuyan Chen, Chao Liang, Xuan Yi, Jingjing Liu, Xiaoqi Sun, Sida Shen, Kai Yang and Zhuang Liu

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201602111

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      A novel type of bio-nanoreactor with catalase loaded inside TaOx hollow nanoshells is fabricated via a mild one-step method. Such bio-nanoreactors could efficiently improve the tumor oxygenation by supplying oxygen via decomposition of endogenic H2O2 in a tumor microenvironment, and thus synergistically enhance the efficacy of cancer radiotherapy by both depositing radiation energy within the tumor and overcoming hypoxia-induced radiotherapy resistance.

    6. Utilization of Electrochromically Luminescent Transition-Metal Complexes for Erasable Information Recording and Temperature-Related Information Protection

      Kenneth Yin Zhang, Xiaojiao Chen, Guanglan Sun, Taiwei Zhang, Shujuan Liu, Qiang Zhao and Wei Huang

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201601978

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      Transition metal complexes containing pyrazinium or pyridinium moieties display reversible luminescence changes in response to electrical stimuli, which is useful in the development of erasable information recording electric devices. These complexes are also suitable for temperature-related information protection, since chemically-induced luminescence turn-on is temperature-dependent.

    7. Ultrahigh Thermal Conductivity of Interface Materials by Silver-Functionalized Carbon Nanotube Phonon Conduits

      Daewoo Suh, Choong Man Moon, Duckjong Kim and Seunghyun Baik

      Version of Record online: 8 JUN 2016 | DOI: 10.1002/adma.201600642

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      An ultrahigh thermal conductivity (κ = 160 W m−1K−1) of thermal interface materials is achieved with a high enhancement factor (96). A small amount (2.3 vol%) of 1D multiwalled carbon nanotubes (MWNTs) with high κ constructs effective phonon transport pathways between microscale silver-flake islands, and a solid phonon transport junction is realized by the coalescence of silver nanoparticles pre-functionalized on the MWNTs.

    8. Modulate Organic-Metal Oxide Heterojunction via [1,6] Azafulleroid for Highly Efficient Organic Solar Cells

      Chang-Zhi Li, Jiang Huang, Huanxin Ju, Yue Zang, Jianyuan Zhang, Junfa Zhu, Hongzheng Chen and Alex K.-Y. Jen

      Version of Record online: 7 JUN 2016 | DOI: 10.1002/adma.201601161

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      By creating an effective π-orbital hybridization between the fullerene cage and the aromatic anchor (addend), the azafulleroid interfacial modifiers exhibit enhanced electronic coupling to the underneath metal oxides. High power conversion efficiency of 10.3% can be achieved in organic solar cells using open-cage phenyl C61 butyric acid methyl ester (PCBM)-modified zinc oxide layer.

    9. Strong Electron-Deficient Polymers Lead to High Electron Mobility in Air and Their Morphology-Dependent Transport Behaviors

      Yu-Qing Zheng, Ting Lei, Jin-Hu Dou, Xin Xia, Jie-Yu Wang, Chen-Jiang Liu and Jian Pei

      Version of Record online: 7 JUN 2016 | DOI: 10.1002/adma.201600541

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      Planar backbone, locked conformation, and low lowest unoccupied molecular orbital level provide polymer F4BDOPV-2T with ultrahigh electron mobilities of up to 14.9 cm2 V−1 s−1 and good air stability. It is found that the nonlinear transfer curves can be tuned to near-ideal ones by changing fabrication conditions, indicating that film morphology largely contributes to the nonlinear transfer curves in high-mobility conjugated polymers.

  10. Review

    1. 2D-Crystal-Based Functional Inks

      Francesco Bonaccorso, Antonino Bartolotta, Jonathan N. Coleman and Claudia Backes

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201506410

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      An overview on the process chain of 2D crystals is provided from the exfoliation of layered bulk counterparts in liquid to yield nanosheets, with controlled lateral sizes and thicknesses, to ink formulation and their printing/coating processes on different substrates for the realization of printed devices.

  11. Reviews

    1. Multifunctional Nanoparticles Self-Assembled from Small Organic Building Blocks for Biomedicine

      Pengyao Xing and Yanli Zhao

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201600906

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      Nanoparticles self-assembled from small organic building blocks show a promising application potential for biomedical applications such as cancer theranostics. The dynamic property of rationally designed building blocks enables self-assembled nanoparticles with high performance in biosensors, bioimaging, and drug delivery.

  12. Communications

    1. Hierarchical Manipulation of Block Copolymer Patterns on 3D Topographic Substrates: Beyond Graphoepitaxy

      Sungjune Park, Xiao Cheng, Alexander Böker and Larisa Tsarkova

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201601098

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      Templates of complex nanopatterns in a form of hierarchically sequenced dots and stripes can be generated in block copolymer films on lithography-free 3D topographic substrates. The approach exploits thickness- and swelling-responsive morphological behavior of block copolymers, and demonstrates novel possibilities of topography-guided registration of nanopatterns due to periodic confinement and spontaneous orthogonal flow-fields.

    2. Hydration and Thermal Expansion in Anatase Nanoparticles

      He Zhu, Qiang Li, Yang Ren, Longlong Fan, Jun Chen, Jinxia Deng and Xianran Xing

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201600973

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      A tunable thermal expansion is reported in nanosized anatase by taking advantage of surface hydration. The coefficient of thermal expansion of 4 nm TiO2 along a-axis is negative with hydrated surface and is positive without hydrated surface. High-energy synchrotron X-ray pair distribution function analysis combining with ab initio calculations on the specific hydrated surface have been carried out to reveal the local structure distortion that is responsible for the unusual negative thermal expansion.

    3. Mechanical Isolation of Highly Stable Antimonene under Ambient Conditions

      Pablo Ares, Fernando Aguilar-Galindo, David Rodríguez-San-Miguel, Diego A. Aldave, Sergio Díaz-Tendero, Manuel Alcamí, Fernando Martín, Julio Gómez-Herrero and Félix Zamora

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201602128

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      Antimonene fabricated by mechanical exfoliation is highly stable under atmospheric conditions over periods of months and even immersed in water. Density functional theory confirms the experiments and predicts an electronic gap of ≈1 eV. These results highlight the use of antimonene for optoelectronics applications.

    4. Band Engineering by Controlling vdW Epitaxy Growth Mode in 2D Gallium Chalcogenides

      Hui Cai, Emmanuel Soignard, Can Ataca, Bin Chen, Changhyun Ko, Toshihiro Aoki, Anupum Pant, Xiuqing Meng, Shengxue Yang, Jeffrey Grossman, Frank D. Ogletree and Sefaattin Tongay

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201601184

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      Atomically thin quasi-2D GaSe flakes are synthesized via van-der-Waals (vdW) epitaxy on a polar Si (111) surface. The band gap is continuously tuned from its commonly accepted value at 620 down to 700 nm range, which was only attained previously by alloying Te into GaSe (GaSexTe1−x). This is accomplished by manipulating various vdW epitaxy kinetic factors, which allows us to choose between screw-dislocation driven and layer-by-layer growth, and design different morphologies with different material–substrate interaction (strain) energies.

    5. Sky-Blue Organic Light Emitting Diode with 37% External Quantum Efficiency Using Thermally Activated Delayed Fluorescence from Spiroacridine-Triazine Hybrid

      Ting-An Lin, Tanmay Chatterjee, Wei-Lung Tsai, Wei-Kai Lee, Meng-Jung Wu, Min Jiao, Kuan-Chung Pan, Chih-Lung Yi, Chin-Lung Chung, Ken-Tsung Wong and Chung-Chih Wu

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201601675

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      Extremely efficient sky-blue organic electroluminescence with external quantum efficiency of ≈37% is achieved in a conventional planar device structure, using a highly efficient thermally activated delayed fluorescence emitter based on the spiroacridine-triazine hybrid and simultaneously possessing nearly unitary (100%) photoluminescence quantum yield, excellent thermal stability, and strongly horizontally oriented emitting dipoles (with a horizontal dipole ratio of 83%).

    6. Enhanced Singlet Oxygen Generation in Oxidized Graphitic Carbon Nitride for Organic Synthesis

      Hui Wang, Shenlong Jiang, Shichuan Chen, Dandan Li, Xiaodong Zhang, Wei Shao, Xianshun Sun, Junfeng Xie, Zhi Zhao, Qun Zhang, Yupeng Tian and Yi Xie

      Version of Record online: 6 JUN 2016 | DOI: 10.1002/adma.201601413

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      Experimental data reveal that the incorporation of carbonyl groups into polymer matrix can significantly enhance singlet oxygen (1O2) generation and suppress other reactive oxygen species production. Excitonic processes interrogated with phosphorescence spectroscopy reveal enhanced triplet-exciton generation in the modified g-C3N4, which facilitate 1O2 generation through energy transfer process. Benefiting from this, the modified g-C3N4 shows excellent conversion and selectivity in organic synthesis.

  13. Reviews

    1. Sodium-Oxygen Batteries: A Comparative Review from Chemical and Electrochemical Fundamentals to Future Perspective

      Hossein Yadegari, Qian Sun and Xueliang Sun

      Version of Record online: 3 JUN 2016 | DOI: 10.1002/adma.201504373

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      Various aspects of Na-O2 cell from fundamental (electro)chemistry of sodium and oxygen to the chemical and electrochemical reaction mechanisms of the cell are discussed. Specifically, effects of various factors, e.g. physicochemical and kinetic parameters, humidity, air electrode, binders, electrolyte, and electrocatalysis on the performance of Na-O2 cell are reviewed over the recent studies and future research perspectives are accordingly proposed.

  14. Communications

    1. Piezotronic Effect Modulated Heterojuction Electron Gas in AlGaN/AlN/GaN Heterostructure Microwire

      Xingfu Wang, Ruomeng Yu, Chunyan Jiang, Weiguo Hu, Wenzhuo Wu, Yong Ding, Wenbo Peng, Shuti Li and Zhong Lin Wang

      Version of Record online: 3 JUN 2016 | DOI: 10.1002/adma.201601721

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      The piezotronic effect is applied to modulate the physical properties of heterojunction electron gas and thus tune the electric transport in AlGaN/AlN/GaN heterostructure microwires. At room temperature, the conductance is increased by 165% under −1.78% compressive strains, and reduced by 48% under 1.78% tensile strains; at 77 K, this modulating effect is further improved by 890% and 940% under compressive and tensile strains, respectively.

  15. Reviews

    1. Hierarchical Targeting Strategy for Enhanced Tumor Tissue Accumulation/Retention and Cellular Internalization

      Sheng Wang, Peng Huang and Xiaoyuan Chen

      Version of Record online: 3 JUN 2016 | DOI: 10.1002/adma.201601498

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      Hierarchical targeting, which combines the advantages of both enhanced tumor tissue accumulation/retention and enhanced cellular internalization, is a promising strategy to improve the tumor targeting efficiency of nanoparticles. The different strategies are summarized including the exploitation of changeable particle sizes, switchable surface charges and activatable surface ligands to develop hierarchical targeting nanoplatforms.

    2. Synthesis of Two-Dimensional Materials for Capacitive Energy Storage

      Beatriz Mendoza-Sánchez and Yury Gogotsi

      Version of Record online: 2 JUN 2016 | DOI: 10.1002/adma.201506133

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      Advances in the synthesis and applications of 2D nanomaterials for capacitive energy storage are reviewed. Graphene, transition metal oxides, dichalcogenides, and carbides, which are being explored are described, and key factors that influence their performance are analyzed. Challenges and opportunities in synthesis, electrochemical stability, electrode design, and architecture are thoroughly discussed, and future research opportunities are outlined.

  16. Communications

    1. Traumatic Brain Injury Imaging in the Second Near-Infrared Window with a Molecular Fluorophore

      Xiao-Dong Zhang, Huasen Wang, Alexander L. Antaris, Lulin Li, Shuo Diao, Rui Ma, Andy Nguyen, Guosong Hong, Zhuoran Ma, Joy Wang, Shoujun Zhu, Joseph M. Castellano, Tony Wyss-Coray, Yongye Liang, Jian Luo and Hongjie Dai

      Version of Record online: 2 JUN 2016 | DOI: 10.1002/adma.201600706

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      Traumatic brain injury (TBI) is a leading cause of death and disability worldwide. A bright, renal-excreted, and biocompatible near-infrared II fluorophore for in vivo imaging of TBI is designed. A transient hypoperfusion in the injured cerebral region, followed by fluorophore leakage, is observed. NIR-II fluorophores can provide noninvasive assessment of TBI.

    2. Resistive Switching in All-Oxide Ferroelectric Tunnel Junctions with Ionic Interfaces

      Qi Hang Qin, Laura Äkäslompolo, Noora Tuomisto, Lide Yao, Sayani Majumdar, Jaianth Vijayakumar, Arianna Casiraghi, Sampo Inkinen, Binbin Chen, Asier Zugarramurdi, Martti Puska and Sebastiaan van Dijken

      Version of Record online: 1 JUN 2016 | DOI: 10.1002/adma.201504519

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      Universal, giant and nonvolatile resistive switching is demonstrated for oxide tunnel junctions with ferroelectric PbZr0.2Ti0.8O3, ferroelectric BaTiO3, and paraelectric SrTiO3 tunnel barriers. The effects are caused by reversible migration of oxygen vacancies between the tunnel barrier and bottom La2/3Sr1/3MnO3 electrode. The switching process, which is driven by large electric fields, is efficient down to a temperature of 5 K.

    3. Gelatin–Graphene Nanocomposites with Ultralow Electrical Percolation Threshold

      Hoda Nassira, Antoni Sánchez-Ferrer, Jozef Adamcik, Stephan Handschin, Hossein Mahdavi, Nader Taheri Qazvini and Raffaele Mezzenga

      Version of Record online: 1 JUN 2016 | DOI: 10.1002/adma.201601115

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      Gelatin–graphene conductive biopolymer nanocomposites (CPCs) with ultralow percolation threshold are designed by reducing in situ graphene oxide nanosheets with ascorbic acid and suppressing the aggregation of the graphene nanosheets. The resulting conductive nanocomposites show a record-low electrical percolation threshold of 3.3 × 10−2 vol%, which arises from the homogeneous dispersion of the graphene nanosheets within the gelatin matrix.

    4. Improving the Stability and Performance of Perovskite Light-Emitting Diodes by Thermal Annealing Treatment

      Jae Choul Yu, Dae Woo Kim, Da Bin Kim, Eui Dae Jung, Jong Hyun Park, Ah-Young Lee, Bo Ram Lee, Daniele Di Nuzzo, Richard H. Friend and Myoung Hoon Song

      Version of Record online: 30 MAY 2016 | DOI: 10.1002/adma.201601105

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      A perovskite LED with a perovskite film treated under optimum thermal annealing conditions exhibited a significantly enhanced long-term stability with full coverage of the green electroluminescence emission due to the highly uniform morphology of the perovskite film.

    5. A Sinusoidally Architected Helicoidal Biocomposite

      Nicholas A. Yaraghi, Nicolás Guarín-Zapata, Lessa K. Grunenfelder, Eric Hintsala, Sanjit Bhowmick, Jon M. Hiller, Mark Betts, Edward L. Principe, Jae-Young Jung, Leigh Sheppard, Richard Wuhrer, Joanna McKittrick, Pablo D. Zavattieri and David Kisailus

      Version of Record online: 30 MAY 2016 | DOI: 10.1002/adma.201600786

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      A fibrous herringbone-modified helicoidal architecture is identified within the exocuticle of an impact-resistant crustacean appendage. This previously unreported composite microstructure, which features highly textured apatite mineral templated by an alpha-chitin matrix, provides enhanced stress redistribution and energy absorption over the traditional helicoidal design under compressive loading. Nanoscale toughening mechanisms are also identified using high-load nanoindentation and in situ transmission electron microscopy picoindentation.

    6. Molecular Order in Buried Layers of TbPc2 Single-Molecule Magnets Detected by Torque Magnetometry

      Mauro Perfetti, Michele Serri, Lorenzo Poggini, Matteo Mannini, Donella Rovai, Philippe Sainctavit, Sandrine Heutz and Roberta Sessoli

      Version of Record online: 27 MAY 2016 | DOI: 10.1002/adma.201600791

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      Cantilever torque magnetometry is used to elucidate the orientation of magnetic molecules in thin films. The technique allows depth-resolved investigations by intercalating a layer of anisotropic magnetic molecules in a film of its isotropic analogues. The proof-of-concept is here demonstrated with the single-molecule magnet TbPc2 evidencing also an exceptional long range templating effect on substrates coated by the organic molecule perylene-3,4,9,10-tetracarboxylic dianhydride.

    7. Ultrafast Nanocrystalline-TiO2(B)/Carbon Nanotube Hyperdispersion Prepared via Combined Ultracentrifugation and Hydrothermal Treatments for Hybrid Supercapacitors

      Katsuhiko Naoi, Takayuki Kurita, Masayuki Abe, Takumi Furuhashi, Yuta Abe, Keita Okazaki, Junichi Miyamoto, Etsuro Iwama, Shintaro Aoyagi, Wako Naoi and Patrice Simon

      Version of Record online: 27 MAY 2016 | DOI: 10.1002/adma.201600798

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      Anisotropically-grown (b-axis short) single-nano TiO2(B), uniformly hyper-dispersed on the surface of multiwalled carbon nanotubes (MWCNT), was successfully synthesized via an in situ ultracentrifugation (UC) process coupled with a follow-up hydrothermal treatment. The uc-TiO2(B)/MWCNT composite materials enable ultrafast Li+ intercalation especially along the b-axis, resulting in a capacity of 235 mAh g–1 per TiO2(B) even at 300C (1C = 335 mA g–1).

    8. Mesoporous Titanium Nitride-Enabled Highly Stable Lithium-Sulfur Batteries

      Zhiming Cui, Chenxi Zu, Weidong Zhou, Arumugam Manthiram and John B. Goodenough

      Version of Record online: 27 MAY 2016 | DOI: 10.1002/adma.201601382

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      The TiN-S composite cathode exhibits superior performance because of higher electrical conductivity and the capture of the soluble intermediate species of the electrode reactions by 2–5 nm mesopores and strong N–S surface bonding.

    9. Bioinspired 1D Superparamagnetic Magnetite Arrays with Magnetic Field Perception

      Xiangyu Jiang, Jiangang Feng, Lei Huang, Yuchen Wu, Bin Su, Wensheng Yang, Liqiang Mai and Lei Jiang

      Version of Record online: 27 MAY 2016 | DOI: 10.1002/adma.201601609

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      Superparamagnetic magnetite nanoparticles can be assembled into 1D arrays by a capillary-bridge mediate assembly approach, inspired by the Earth's magnetic field perception in nature. These 1D arrays possess strict alignment, precise position and high aspect ratio, yielding highly anisotropic magnetization characteristic.

    10. Efficient All-Vacuum Deposited Perovskite Solar Cells by Controlling Reagent Partial Pressure in High Vacuum

      Sheng-Yi Hsiao, Hong-Lin Lin, Wei-Hung Lee, Wei-Lun Tsai, Kai-Ming Chiang, Wei-Yu Liao, Chen-Zheng Ren-Wu, Chien-Yu Chen and Hao-Wu Lin

      Version of Record online: 25 MAY 2016 | DOI: 10.1002/adma.201601505

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      All-vacuum deposited perovskite solar cells produced by controlling reagent partial pressure in high vacuum with newly developed multi-layer electron and hole transporting structures show outstanding power conversion efficiency of 17.6% and smooth, pinhole-free, micrometer-sized perovskite crystal grains.

    11. Preparation and Characterization of Newly Discovered Fibrous Aggregates of Single-Walled Carbon Nanohorns

      Ryota Yuge, Fumiyuki Nihey, Kiyohiko Toyama and Masako Yudasaka

      Version of Record online: 25 MAY 2016 | DOI: 10.1002/adma.201602022

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      Fibrous aggregates composed of radially assembled graphene-based single-walled nanotubules are prepared, named here as fibrous aggregates of single-walled carbon nanohorns (fib-CNHs), whose structure resembles that of chenille stems. The newly discovered fib-CNHs are 30–100 nm in diameter and 1–10 μm in length. The fib-CNHs show high dispersibility and conductivity. The fib-CNHs increase the advantages of nanocarbons in various fields.

    12. You have full text access to this OnlineOpen article
      Unraveling Unprecedented Charge Carrier Mobility through Structure Property Relationship of Four Isomers of Didodecyl[1]benzothieno[3,2-b][1]benzothiophene

      Yusuke Tsutsui, Guillaume Schweicher, Basab Chattopadhyay, Tsuneaki Sakurai, Jean-Baptiste Arlin, Christian Ruzié, Almaz Aliev, Artur Ciesielski, Silvia Colella, Alan R. Kennedy, Vincent Lemaur, Yoann Olivier, Rachid Hadji, Lionel Sanguinet, Frédéric Castet, Silvio Osella, Dmytro Dudenko, David Beljonne, Jérôme Cornil, Paolo Samorì, Shu Seki and Yves H. Geerts

      Version of Record online: 25 MAY 2016 | DOI: 10.1002/adma.201601285

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      The structural and electronic properties of four isomers of didodecyl[1]-benzothieno[3,2-b][1]benzothiophene (C12-BTBT) have been investigated. Results show the strong impact of the molecular packing on charge carrier transport and electronic polarization properties. Field-induced time-resolved microwave conductivity measurements unravel an unprecedented high average interfacial mobility of 170 cm2 V−1 s−1 for the 2,7-isomer, holding great promise for the field of organic electronics.

    13. 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.

    14. 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.

    15. 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.

    16. 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.

    17. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.