Advanced Materials

Cover image for Vol. 25 Issue 34

September 14, 2013

Volume 25, Issue 34

Pages 4681–4813

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      Metal-Organic Frameworks: Combining UV Lithography and an Imprinting Technique for Patterning Metal-Organic Frameworks (Adv. Mater. 34/2013) (page 4681)

      Cara M. Doherty, Gianluca Grenci, Raffaele Riccò, James I. Mardel, Julien Reboul, Shuhei Furukawa, Susumu Kitagawa, Anita J. Hill and Paolo Falcaro

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370212

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      Patterning metal-organic frameworks (MOFs) using cheap, fast, and versatile methods is a key enabling technology for multifunctional miniaturized device fabrication. A collaborative work led by Paolo Falcaro (CSIRO - Australia) demonstrates on page 4701 how a combination of existing lithographic approaches, such as photolithography and imprinting, can be efficiently used for positioning different already-prepared ultraporous crystals. Cover Image by Paolo Falcaro.

  2. Inside Front Cover

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      Field-Effect Transistors: Sub-10 nm Graphene Nanoribbon Array Field-Effect Transistors Fabricated by Block Copolymer Lithography (Adv. Mater. 34/2013) (page 4682)

      Jeong Gon Son, Myungwoo Son, Kyeong-Joo Moon, Byoung Hun Lee, Jae-Min Myoung, Michael S. Strano, Moon-Ho Ham and Caroline A. Ross

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370213

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      Arrays of field-effect transistors are described by Caroline Ross, Moon-Ho Ham and co-workers on page 4723. These are based on highly aligned sub-10 nm graphene nanoribbons that are fabricated over large areas by etching CVD-grown graphene, using a mask made by the directed self-assembly of a cylindrical PS-block-PDMS block copolymer under solvent annealing guided by a removable template.

  3. Back Cover

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      Supercapacitors: Bacterial-Cellulose-Derived Carbon Nanofiber@MnO2 and Nitrogen-Doped Carbon Nanofiber Electrode Materials: An Asymmetric Supercapacitor with High Energy and Power Density (Adv. Mater. 34/2013) (page 4816)

      Li-Feng Chen, Zhi-Hong Huang, Hai-Wei Liang, Qing-Fang Guan and Shu-Hong Yu

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370214

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      A new kind of high-performance asymmetric supercapacitor is designed with pyrolyzed bacterial cellulose (p-BC)-coated MnO2 as the positive electrode material and nitrogen-doped p-BC as the negative electrode material, via an easy, efficient, large-scale, and green fabrication approach as described by Shu-Hong Yu and co-workers, on page 4746. The optimal asymmetric device possesses an excellent supercapacitive behavior with quite high energy and power density.

  4. Masthead

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      Masthead: (Adv. Mater. 34/2013)

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370215

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  6. Correction

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      Correction: High-Performance ZnO Transistors Processed Via an Aqueous Carbon-Free Metal Oxide Precursor Route at Temperatures Between 80–180 °C (page 4689)

      Yen-Hung Lin, Hendrik Faber, Kui Zhao, Qingxiao Wang, Aram Amassian, Martyn McLachlan and Thomas D. Anthopoulos

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201303701

      This article corrects:
  7. Communications

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    1. Line Patterns from Cylinder-Forming Photocleavable Block Copolymers (pages 4690–4695)

      Weiyin Gu, Hui Zhao, Qingshuo Wei, E. Bryan Coughlin, Patrick Theato and Thomas P. Russell

      Version of Record online: 19 JUL 2013 | DOI: 10.1002/adma.201301556

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      A robust route for the preparation of nanoscopic line patterns from polystyrene-block-poly(ethylene oxide) featuring a photocleavable o-nitrobenzyl ester junction is demonstrated. After mild UV (λ = 365 nm) exposure and selective removal of the PEO microdomains, the polymer trench patterns are used as scaffold to fabricate highly ordered arrays of silica or Au line patterns.

    2. A New Diamond Biosensor with Integrated Graphitic Microchannels for Detecting Quantal Exocytic Events from Chromaffin Cells (pages 4696–4700)

      Federico Picollo, Sara Gosso, Ettore Vittone, Alberto Pasquarelli, Emilio Carbone, Paolo Olivero and Valentina Carabelli

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201300710

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      An MeV ion-microbeam lithographic technique can be successfully employed for the fabrication of an all-carbon miniaturized cellular biosensor based on graphitic microchannels embedded in a single-crystal diamond matrix. The device is functionally characterized for the in vitro recording of quantal exocytic events from single chromaffin cells, with high sensitivity and signal-to-noise ratio, opening promising perspectives for the realization of monolithic all-carbon cellular biosensors.

    3. Combining UV Lithography and an Imprinting Technique for Patterning Metal-Organic Frameworks (pages 4701–4705)

      Cara M. Doherty, Gianluca Grenci, Raffaele Riccò, James I. Mardel, Julien Reboul, Shuhei Furukawa, Susumu Kitagawa, Anita J. Hill and Paolo Falcaro

      Version of Record online: 24 JUL 2013 | DOI: 10.1002/adma.201301383

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      Thin metal-organic framework (MOF) films are patterned using UV lithography and an imprinting technique. A UV lithographed SU-8 film is imprinted onto a film of MOF powder forming a 2D MOF patterned film. This straightforward method can be applied to most MOF materials, is versatile, cheap, and potentially useful for commercial applications such as lab-on-a-chip type devices.

  8. Frontispiece

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      Scalable Manufacture of Built-to-Order Nanomedicine: Spray-Assisted Layer-by-Layer Functionalization of PRINT Nanoparticles (Adv. Mater. 34/2013) (page 4706)

      Stephen W. Morton, Kevin P. Herlihy, Kevin E. Shopsowitz, Zhou J. Deng, Kevin S. Chu, Charles J. Bowerman, Joseph M. DeSimone and Paula T. Hammond

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370217

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      Scalable methods, PRINT particle fabrication, and spray-assisted layer-by-layer deposition, are combined by Paula Hammond, Joseph DeSimone and co-workers on page 4707 to generate uniform and functional nanotechnologies with precise control over composition, size, shape, and surface functionality. A modular and tunable approach toward the design of built-to-order nanoparticle systems, spray coatings on PRINT particles are demonstrated to achieve technologies capable of targeted interactions with cancer cells for applications in drug delivery.

  9. Communications

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    1. Scalable Manufacture of Built-to-Order Nanomedicine: Spray-Assisted Layer-by-Layer Functionalization of PRINT Nanoparticles (pages 4707–4713)

      Stephen W. Morton, Kevin P. Herlihy, Kevin E. Shopsowitz, Zhou J. Deng, Kevin S. Chu, Charles J. Bowerman, Joseph M. DeSimone and Paula T. Hammond

      Version of Record online: 1 JUL 2013 | DOI: 10.1002/adma.201302025

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      Scalable methods, PRINT particle fabrication, and spray-assisted Layer-by-Layer deposition are combined to generate uniform and functional nanotechnologies with precise control over composition, size, shape, and surface functionality. A modular and tunable approach towards design of built-to-order nanoparticle systems, spray coating on PRINT particles is demonstrated to achieve technologies capable of targeted interactions with cancer cells for applications in drug delivery.

    2. A Triggered DNA Hydrogel Cover to Envelop and Release Single Cells (pages 4714–4717)

      Juan Jin, Yongzheng Xing, Yanli Xi, Xueli Liu, Tao Zhou, Xinxin Ma, Zhongqiang Yang, Shutao Wang and Dongsheng Liu

      Version of Record online: 9 JUL 2013 | DOI: 10.1002/adma.201301175

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      We develop an enzyme-triggered permeable DNA hydrogel cover to envelop and release single cells in microwells. The porous structure of the DNA hydrogel allows nutrients and waste to pass through, leading to a cell viability as high as 98%. The design provides a general method to culture, monitor, and manipulate single cells, and has potential applications in cell patterning and studying cell communication.

    3. Novel Conjugation of Tumor-Necrosis-Factor-Related Apoptosis-Inducing Ligand (TRAIL) with Monomethyl Auristatin E for Efficient Antitumor Drug Delivery (pages 4718–4722)

      Li-Qiang Pan, Hai-Bin Wang, Zhang-Ming Xie, Zhao-Hui Li, Xiao-Jing Tang, Ying-Chun Xu, Chen Zhang, Hua Naranmandura and Shu-Qing Chen

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201301385

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      Monomethyl auristatin E (MMAE) is conjugated with TNF-related apoptosis-inducing ligand (TRAIL) via a linker that is stable in extracellular fluid, while it is cleaved by cathepsin once the conjugate has entered a tumor cell, thus activating the antimitotic mechanism of MMAE. The TRAIL-MMAE conjugate is a conceptually viable therapeutic strategy with improved in vitro antitumor activity, cell circle arrest and specific accumulation in tumor to treat TRAIL-resistant tumors.

    4. Sub-10 nm Graphene Nanoribbon Array Field-Effect Transistors Fabricated by Block Copolymer Lithography (pages 4723–4728)

      Jeong Gon Son, Myungwoo Son, Kyeong-Joo Moon, Byoung Hun Lee, Jae-Min Myoung, Michael S. Strano, Moon-Ho Ham and Caroline A. Ross

      Version of Record online: 25 JUN 2013 | DOI: 10.1002/adma.201300813

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      Sub-10 nm Graphene Nanoribbon Arrays are fabricated over large areas by etching CVD-grown graphene. A mask is used made by the directed self-assembly of a cylindrical PS-b-PDMS block copolymer under solvent annealing guided by a removable template. The optimized solvent annealing process, surface-modified removable polymeric templates, and high Flory-Huggins interaction parameters of the block copolymer enable a highly aligned array of nanoribbons with low line edge roughness to be formed. This leads to a higher on/off ratio and stronger temperature dependence of the current for nanoribbon FETs, and a photocurrent which is 30 times larger compared to unpatterned graphene.

    5. Foldable Graphene Electronic Circuits Based on Paper Substrates (pages 4729–4734)

      Woo Jin Hyun, O Ok Park and Byung Doo Chin

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201302063

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      Graphene electronic circuits are prepared on paper substrates by using graphene nanoplates and applied to foldable paper-based electronics. The graphene circuits show a small change in conductance under various folding angles and maintain an electronic path on paper substrates after repetition of folding and unfolding. Foldable paper-based applications with graphene circuits exhibit excellent folding stability.

    6. Enhancing Electron Mobility at the LaAlO3/SrTiO3 Interface by Surface Control (pages 4735–4738)

      Yanwu Xie, Christopher Bell, Yasuyuki Hikita, Satoshi Harashima and Harold Y. Hwang

      Version of Record online: 15 JUL 2013 | DOI: 10.1002/adma.201301798

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      Mobility of electrons confined at the LaAlO3/SrTiO3 interface is significantly enhanced by surface control using surface charges and adsorbates, reaching a low temperature value more than 20 000 cm2 V−1s−1. A uniform trend that mobility increases with decreasing sheet carrier density is observed.

    7. Ultrathin Limit of Exchange Bias Coupling at Oxide Multiferroic/Ferromagnetic Interfaces (pages 4739–4745)

      M. Huijben, P. Yu, L. W. Martin, H. J. A. Molegraaf, Y.-H. Chu, M. B. Holcomb, N. Balke, G. Rijnders and R. Ramesh

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201300940

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      Exchange bias coupling at the multiferroic- ferromagnetic interface in BiFeO3/La0.7Sr0.3MnO3 heterostructures exhibits a critical thickness for ultrathin BiFeO3 layers of 5 unit cells (2 nm). Linear dichroism measurements demonstrate the dependence on the BiFeO3 layer thickness with a strong reduction for ultrathin layers, indicating diminished antiferromagnetic ordering that prevents interfacial exchange bias coupling.

    8. Bacterial-Cellulose-Derived Carbon Nanofiber@MnO2 and Nitrogen-Doped Carbon Nanofiber Electrode Materials: An Asymmetric Supercapacitor with High Energy and Power Density (pages 4746–4752)

      Li-Feng Chen, Zhi-Hong Huang, Hai-Wei Liang, Qing-Fang Guan and Shu-Hong Yu

      Version of Record online: 29 MAY 2013 | DOI: 10.1002/adma.201204949

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      A new kind of high-performance asymmetric supercapacitor is designed with pyrolyzed bacterial cellulose (p-BC)-coated MnO2 as a positive electrode material and nitrogen-doped p-BC as a negative electrode material via an easy, efficient, large-scale, and green fabrication approach. The optimal asymmetric device possesses an excellent supercapacitive behavior with quite high energy and power density.

    9. Large Magnetoresistance in Magnetically Coupled SrRuO3 –CoFe2O4 Self-Assembled Nanostructures (pages 4753–4759)

      Heng-Jui Liu, Vu-Thanh Tra, Ying-Jiun Chen, Rong Huang, Chun-Gang Duan, Ying-Hui Hsieh, Hong-Ji Lin, Jiunn-Yuan Lin, Chien-Te Chen, Yuichi Ikuhara and Ying-Hao Chu

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201301461

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      A new way to induce a large magnetoresistance has been achieved by self-assembled nanostructures consisting of ferromagnetic spinel CoFe2O4 (CFO) and metallic perovskite SrRuO3 (SRO). The interdiffused Fe3+ ions in SRO have paved the way to strong magnetic couplings with CFO nanopillars, resulting in the suppression of spin-polarized electron scattering.

    10. Spatially-Resolved In-Situ Structural Study of Organic Electronic Devices with Nanoscale Resolution: The Plasmonic Photovoltaic Case Study (pages 4760–4765)

      B. Paci, D. Bailo, V. Rossi Albertini, J. Wright, C. Ferrero, G. D. Spyropoulos, E. Stratakis and E. Kymakis

      Version of Record online: 24 JUL 2013 | DOI: 10.1002/adma.201301682

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      A novel high spatial resolution synchrotron X-ray diffraction stratigraphy technique has been applied in-situ to an integrated plasmonic nanoparticle-based organic photovoltaic device. This original approach allows for the disclosure of structure-property relations linking large scale organic devices to length scales of local nano/hetero structures and interfaces between the different components.

    11. Fullerene Derivative-Doped Zinc Oxide Nanofilm as the Cathode of Inverted Polymer Solar Cells with Low-Bandgap Polymer (PTB7-Th) for High Performance (pages 4766–4771)

      Sih-Hao Liao, Hong-Jyun Jhuo, Yu-Shan Cheng and Show-An Chen

      Version of Record online: 13 AUG 2013 | DOI: 10.1002/adma.201301476

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      Modification of a ZnO cathode by doping it with a hydroxyl-containing derivative — giving a ZnO-C60 cathode — provides a fullerene-derivative-rich surface and enhanced electron conduction. Inverted polymer solar cells with the ZnO-C60 cathode display markedly improved power conversion efficiency compared to those with a pristine ZnO cathode, especially when the active layer includes the low-bandgap polymer PTB7-Th.

  10. Frontispiece

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      Flexible High-Performance All-Inkjet-Printed Inverters: Organo-Compatible and Stable Interface Engineering (Adv. Mater. 34/2013) (page 4772)

      Seungjun Chung, Mi Jang, Seon-Beom Ji, Hwarim Im, Narkhyeon Seong, Jewook Ha, Soon-Ki Kwon, Yun-Hi Kim, Hoichang Yang and Yongtaek Hong

      Version of Record online: 9 SEP 2013 | DOI: 10.1002/adma.201370218

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      On page 4773 Yongtaek Hong, Hoichang Yang, and co-workers demonstrate high-performance, flexible, all-inkjet-printed organic thin-film transistor (OTFT) inverters showing full up-down switching. They are implemented by introducing organic-compatible, hydroxylfree, end-functionalized polystyrene at the interfaces of the channel and source/drain contact.

  11. Communications

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    1. Flexible High-Performance All-Inkjet-Printed Inverters: Organo-Compatible and Stable Interface Engineering (pages 4773–4777)

      Seungjun Chung, Mi Jang, Seon-Beom Ji, Hwarim Im, Narkhyeon Seong, Jewook Ha, Soon-Ki Kwon, Yun-Hi Kim, Hoichang Yang and Yongtaek Hong

      Version of Record online: 5 JUL 2013 | DOI: 10.1002/adma.201301040

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      High-performance all-inkjet-printed organic inverters are fabricated on flexible substrates. By introducing end-functionalized polystyrene on both surfaces of inkjet-printed source/drain Ag electrodes and poly(4-vinylphenol) dielectrics, organic-compatible and hydroxyl-free interfaces between those layers and 6,13-bis(triisopropylsilylethynyl)pentacene drastically reduce the interfacial trap and contact resistance. The resulting organic inverters show a full up-down switching performance and a high voltage gain of 19.8.

    2. Molecular Layer-by-Layer Assembled Thin-Film Composite Membranes for Water Desalination (pages 4778–4782)

      Joung-Eun Gu, Seunghye Lee, Christopher M. Stafford, Jong Suk Lee, Wansuk Choi, Bo-Young Kim, Kyung-Youl Baek, Edwin P. Chan, Jun Young Chung, Joona Bang and Jung-Hyun Lee

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201302030

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      Molecular layer-by-layer (mLbL) assembled thin-film composite membranes fabricated by alternating deposition of reactive monomers on porous supports exhibit both improved salt rejection and enhanced water flux compared to traditional reverse osmosis membranes prepared by interfacial polymerization. Additionally, the well-controlled structures achieved by mLbL deposition further lead to improved antifouling performance.

    3. Enhanced Efficiency of Single and Tandem Organic Solar Cells Incorporating a Diketopyrrolopyrrole-Based Low-Bandgap Polymer by Utilizing Combined ZnO/Polyelectrolyte Electron-Transport Layers (pages 4783–4788)

      Jang Jo, Jean-Rémi Pouliot, David Wynands, Samuel D. Collins, Jin Young Kim, Thanh Luan Nguyen, Han Young Woo, Yanming Sun, Mario Leclerc and Alan J. Heeger

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201301288

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      Power conversion efficiency up to 8.6% is achieved for a solution-processed tandem solar cell based on a diketopyrrolopyrrole-containing polymer as the low-bandgap material after using a thin polyelectrolyte layer to modify the electron-transport ZnO layers, indicating that interfacial engineering is a useful approach to further enhancing the efficiency of tandem organic solar cells.

    4. High-Performance and Low-Power Rewritable SiOx 1 kbit One Diode–One Resistor Crossbar Memory Array (pages 4789–4793)

      Gunuk Wang, Adam C. Lauchner, Jian Lin, Douglas Natelson, Krishna V. Palem and James M. Tour

      Version of Record online: 8 JUL 2013 | DOI: 10.1002/adma.201302047

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      An entire 1-kilobit crossbar device based upon SiOx resistive memories with integrated diodes has been made. The SiOx-based one diode–one resistor device system has promise to satisfy the prerequisite conditions for next generation non-volatile memory applications.

    5. Nitrogen and Sulfur Dual-Doped Non-Noble Catalyst Using Fluidic Acrylonitrile Telomer as Precursor for Efficient Oxygen Reduction (pages 4794–4799)

      Yuanqin Chang, Fei Hong, Chuanxin He, Qianling Zhang and Jianhong Liu

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201301002

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      In order to make polyacrylonitrile (PAN) fluidic, acrylonitrile telomer (ANT) is synthesized by radical telomerization and used as a nitrogen and carbon precursor to prepare a non-noble oxygen reduction reaction (ORR) catalyst. This fluidic precursor greatly increases the contact between Fe salt aggregates and the polymer so that more active sites are formed during stabilization and carbonization. Such prepared catalysts and the commercial Pt/C catalyst have comparable ORR performance and stability.

    6. A Promising Mid-Temperature Thermoelectric Material Candidate: Pb/Sn-Codoped In4PbxSnySe3 (pages 4800–4806)

      Zhi-Sheng Lin, Ling Chen, Li-Min Wang, Jing-Tai Zhao and Li-Ming Wu

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201302038

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      A facile polycrystalline Pb/Sn-codoped In4Pb0.01SnySe3 material is obtained, its thermoelectric performance is evaluated, and the intrinsic reasons have been studied. This material shows an excellent ZT value of 1.4 at 733 Kelvin, among the best values of the relative materials, thus making it a promising candidate for the mid-temperature thermoelectric application.

    7. A Photochromic Diode With a Continuum of Intermediate States: Towards High Density Multilevel Storage (pages 4807–4813)

      R. Clayton Shallcross, Peter O. Körner, Eduard Maibach, Anne Köhnen and Klaus Meerholz

      Version of Record online: 12 JUL 2013 | DOI: 10.1002/adma.201301286

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      A continuum of intermediate states (current levels) is demonstrated for an organic diode utilizing a photochromic (dithienylethene) switching layer. Specific intermediate states can be attained by controlling the fraction of closed isomer (X) in the transduction layer, affording a novel methodology for multilevel storage applications. The analog response of the device is discussed in terms of the concentration and morphology of closed dithienylethene isomer, which can be accessed via optical and electrical switching reactions.

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