Advanced Materials

Cover image for Vol. 24 Issue 10

March 8, 2012

Volume 24, Issue 10

Pages 1281–1346, OP1–OP83

  1. Cover Picture

    1. Top of page
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    3. Inside Front Cover
    4. Masthead
    5. Contents
    6. Review
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    8. Communications
    9. Cover Picture: Advanced Optical Materials
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    13. Editorial: Advanced Optical Materials
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    1. Graphene Films: Solution-Processed Ultrathin Chemically Derived Graphene Films as Soft Top Contacts for Solid-State Molecular Electronic Junctions (Adv. Mater. 10/2012) (page 1281)

      Tao Li, Jonas Rahlf Hauptmann, Zhongming Wei, Søren Petersen, Nicolas Bovet, Tom Vosch, Jesper Nygård, Wenping Hu, Yunqi Liu, Thomas Bjørnholm, Kasper Nørgaard and Bo W. Laursen

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290048

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      Nondestructive fabrication of solid-state molecular junctions using ultrathin chemically derived graphene films as soft top-contacts and protection layers is described by K. Nørgaard, B. W. Laursen, and co-workers on page 1333. The graphene is placed on top of a layer of short conjugated molecules or alkanethiols, protecting it during deposition of a gold top-contact on the layer. Chemically derived graphene can also act as a conductive interconnection between junctions in series, having molecular features such as non-linear charge-transport properties and molecular length dependence of the junction resistance.

  2. Inside Front Cover

    1. Top of page
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    4. Masthead
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    6. Review
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    8. Communications
    9. Cover Picture: Advanced Optical Materials
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    1. Multicompartmental Microparticles: Controlled Synthesis of 3D Multi-Compartmental Particles with Centrifuge-Based Microdroplet Formation from a Multi-Barrelled Capillary (Adv. Mater. 10/2012) (page 1282)

      Kazuki Maeda, Hiroaki Onoe, Masahiro Takinoue and Shoji Takeuchi

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290049

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      Multi-compartmental particles and a centrifuge-based droplet shooting device (CDSD) are described on page 1340 by S. Takeuchi and co-workers. Sodium alginate solutions introduced in a multi-barreled capillary form droplets at the capillary orifice under ultra-high gravity, and are solidified in a CaCl2 solution. The size, shape, and compartmentalization of the particles are con-trolled. All of the fabrication procedures can be conducted on a lab bench within a few minutes using commercially available components.

  3. Masthead

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    1. Masthead: (Adv. Mater. 10/2012)

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290050

  4. Contents

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    1. Contents: (Adv. Mater. 10/2012) (pages 1283–1286)

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290046

  5. Review

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    1. Anisotropic Wetting Surfaces with One-Dimesional and Directional Structures: Fabrication Approaches, Wetting Properties and Potential Applications (pages 1287–1302)

      Deying Xia, Leah M. Johnson and Gabriel P. López

      Article first published online: 9 FEB 2012 | DOI: 10.1002/adma.201104618

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      New developments in anisotropic wetting on 1D and directional patterned surfaces in recent years (i.e., 2005–2011) are reviewed in this paper. Both natural surfaces and fabricated surfaces using various approaches with 1D patterned surfaces or directional nanostructures exhibit obvious anisotropic static or dynamic wetting behavior. Some modeling and simulation methods are proposed to interpret the observed anisotropic wetting. Many potential applications exist for anisotropic wetting surfaces.

  6. Frontispiece

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    1. Microfluidics: Two-Photon Continuous Flow Lithography (Adv. Mater. 10/2012) (page 1303)

      Simona C. Laza, Marco Polo, Antonio A. R. Neves, Roberto Cingolani, Andrea Camposeo and Dario Pisignano

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290047

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      Polymeric fibers and helical and bow-tie particles are generated by A. Camposeo, D. Pisignano and co-workers on page 1304, using the combination of two-photon lithog-raphy and microfluidics. The two-photon continuous flow lithography enables the creation of polymeric micro-objects with 3D features and sub-diffraction resolution. The particle synthesis throughput is improved, thanks to the combination of polymerization by multiple laser beams under continuous flow.

  7. Communications

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    9. Cover Picture: Advanced Optical Materials
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    1. Two-Photon Continuous Flow Lithography (pages 1304–1308)

      Simona C. Laza, Marco Polo, Antonio A. R. Neves, Roberto Cingolani, Andrea Camposeo and Dario Pisignano

      Article first published online: 3 FEB 2012 | DOI: 10.1002/adma.201103357

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      A new approach for microfluidics-based production of polymeric particles, namely two-photon continuous flow lithography, is reported. This technique takes advantage of two-photon lithography to create objects with sub-micrometer and 3D features, and overcomes the traditional process limitations of two-photon lithography by using multiple beam production under continuous flow. Polymeric fibers, helical and bow-tie particles with sub-diffraction resolution and surface roughness as low as 10 nm are demonstrated.

    2. Synthesis and Optical Properties of Mesoporous β-Co(OH)2/Brilliant Blue G (G250) Hybrid Hierarchical Structures (pages 1309–1315)

      Huai-Ping Cong, Xiao-Chen Ren, Hong-Bin Yao, Ping Wang, Helmut Cölfen and Shu-Hong Yu

      Article first published online: 2 FEB 2012 | DOI: 10.1002/adma.201104605

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      New mesoporous β-Co(OH)2/brilliant blue G (G250) hybrid hierarchical structures constructed by thin mesocrystal nanosheets can be synthesized by a one-step refluxing process under the synergistic effect of CTAB and G250 (see Figure). This approach opens up an avenue to access new novel inorganic/dye hybrid materials with hierarchical structures for pigment and electrocatalytic application.

    3. Digital Microfluidic High-Throughput Printing of Single Metal-Organic Framework Crystals (pages 1316–1320)

      Daan Witters, Nicolas Vergauwe, Rob Ameloot, Steven Vermeir, Dirk De Vos, Robert Puers, Bert Sels and Jeroen Lammertyn

      Article first published online: 2 FEB 2012 | DOI: 10.1002/adma.201104922

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      The first microfluidic method for accurately depositing monodisperse single MOF crystals is presented, enabling unprecedented high-throughput, yet flexible single-crystal printing. Individual droplets of MOF precursor solutions are actuated over a matrix of hydrophilic-in-hydrophobic micropatterns for the controlled generation of femtoliter droplets. As such, thousands of monodisperse single MOF crystals are printed per second in a desired pattern, without the use of impractically expensive equipment.

    4. Compliant Silver Nanowire-Polymer Composite Electrodes for Bistable Large Strain Actuation (pages 1321–1327)

      Sungryul Yun, Xiaofan Niu, Zhibin Yu, Weili Hu, Paul Brochu and Qibing Pei

      Article first published online: 3 FEB 2012 | DOI: 10.1002/adma.201104101

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      A new compliant electrode-based on silver nanowire-polymer composite has been developed. The composite electrode has low sheet resistance (as low as 10 Ω/sq), remains conductive (102–103 Ω/sq) at strains as high as 140%, and can support Joule heating. The combination of the composite and a bistable electroactive polymer produces electrically-induced, large-strain actuation and relaxation, reversibly without the need of mechanical programming.

    5. Polarization-Induced Charge Distribution at Homogeneous Zincblende/Wurtzite Heterostructural Junctions in ZnSe Nanobelts (pages 1328–1332)

      Luying Li, Lei Jin, Jianbo Wang, David J. Smith, Wan-Jian Yin, Yanfa Yan, Hongqian Sang, Wallace C. H. Choy and Martha R. McCartney

      Article first published online: 2 FEB 2012 | DOI: 10.1002/adma.201103920

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      Homogeneous heterostructural wurtzite (WZ)/zincblende (ZB) junctions are successfully fabricated in ZnSe nanobelts. Polarity continuity across the ZB/WZ interface is demonstrated. The saw-tooth-like potential profile induced by spontaneous polarization across the WZ/ZB/WZ interfaces is identified directly at the nanoscale. The polarization-induced charge distribution across the homogeneous heterostructural interfaces is proposed as a viable alternative approach towards charge tailoring in semiconductor nanostructures.

    6. Solution-Processed Ultrathin Chemically Derived Graphene Films as Soft Top Contacts for Solid-State Molecular Electronic Junctions (pages 1333–1339)

      Tao Li, Jonas Rahlf Hauptmann, Zhongming Wei, Søren Petersen, Nicolas Bovet, Tom Vosch, Jesper Nygård, Wenping Hu, Yunqi Liu, Thomas Bjørnholm, Kasper Nørgaard and Bo W. Laursen

      Article first published online: 6 FEB 2012 | DOI: 10.1002/adma.201104550

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      A novel method using solution-processed ultrathin chemically derived graphene films as soft top contacts for the non-destructive fabrication of molecular junctions is demonstrated. We believe this protocol will greatly enrich the solid-state test beds for molecular electronics due to its low-cost, easy-processing and flexible nature.

    7. Controlled Synthesis of 3D Multi-Compartmental Particles with Centrifuge-Based Microdroplet Formation from a Multi-Barrelled Capillary (pages 1340–1346)

      Kazuki Maeda, Hiroaki Onoe, Masahiro Takinoue and Shoji Takeuchi

      Article first published online: 6 FEB 2012 | DOI: 10.1002/adma.201102560

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      Controlled synthesis of micro multi-compartmental particles using a centrifuge droplet shooting device (CDSD) is reported. Sodium alginate solutions introduced in a multi-barreled capillary form droplets at the capillary orifice under ultrahigh gravity and gelify in a CaCl2 solution. The size, shape, and compartmentalization of the particles are controlled. Co-encapsulation of Jurkat cells and magnetic colloids into Janus particles is demonstrated. The Janus particles present sensitive reaction toward magnetic fields, while the viability of the encapsulated cells is 91%.

  8. Cover Picture: Advanced Optical Materials

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    1. Electro-optical Materials: Efficient Poling of Electro-Optic Polymers in Thin Films and Silicon Slot Waveguides by Detachable Pyroelectric Crystals (Adv. Mater. 10/2012) (page OP1)

      Su Huang, Jingdong Luo, Hin-Lap Yip, Ali Ayazi, Xing-Hua Zhou, Michael Gould, Antao Chen, Tom Baehr-Jones, Michael Hochberg and Alex K.-Y. Jen

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290057

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      This first ever Advanced Optical Materials cover design shows a silicon–polymer hybrid slot waveguide ring-resonator modulator being poled by two pyroelectric crystals. Each of the three images, from top to bottom, indicates one stage of the poling—before, during, and after—with the device configuration in the front and the dipole alignment state represented in the background. For details on how this was achieved, check out the article by A. K.-Y. Jen and co-workers on page OP42.

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    1. Plasmonics: High Magneto-Optical Activity and Low Optical Losses in Metal-Dielectric Au/Co/Au–SiO2 Magnetoplasmonic Nanodisks (Adv. Mater. 10/2012) (page OP2)

      Juan Carlos Banthí, David Meneses-Rodríguez, Fernando García, María Ujué González, Antonio García-Martín, Alfonso Cebollada and Gaspar Armelles

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290058

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      The internal architecture of metal-dielectric Au/Co/Au–SiO2 magnetoplasmonic nanodisks provides control over the internal electromagnetic field distribu on by varying the relative contributions of the magneto-optically active layers and the optically lossy layers. This allows simultaneous tuning of the magneto-optical activity and the absorption. On page OP36, A. Cebollada and co-workers show how placing the dielectric between the upper Au layer and the Co produces a configuration of sizeable magneto-optical activity and low optical loss. If the dielectric is placed below the Co, the magneto-optical activity is maintained, but the optical losses are larger.

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    1. Masthead: (Adv. Mater. 10/2012)

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290059

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      Contents: (Adv. Mater. 10/2012) (pages OP4–OP7)

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290054

  12. Editorial: Advanced Optical Materials

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    1. Nanopillars: Large Area Fabrication of Leaning Silicon Nanopillars for Surface Enhanced Raman Spectroscopy (Adv. Mater. 10/2012) (page OP10)

      Michael Stenbæk Schmidt, Jörg Hübner and Anja Boisen

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290051

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      M. S. Schmidt et al. describe on page OP11 a simple, two-step fabrication process to as-semble flexible, freestanding nanopillars into large-area substrates. These substrates can be made using readily available silicon-processing equipment and are suitable for SERS, having a large, uniform Raman enhancement.

  14. Communications: Advanced Optical Materials

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      Large Area Fabrication of Leaning Silicon Nanopillars for Surface Enhanced Raman Spectroscopy (pages OP11–OP18)

      Michael Stenbæk Schmidt, Jörg Hübner and Anja Boisen

      Article first published online: 22 NOV 2011 | DOI: 10.1002/adma.201103496

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      Using a simple two step fabrication process substrates with a large and uniform Raman enhancement, based on flexible free standing nanopillars can be manufactured over large areas using readily available silicon processing equipment.

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      Giant Optical Gain in a Rare-Earth-Ion-Doped Microstructure (pages OP19–OP22)

      Dimitri Geskus, Shanmugam Aravazhi, Sonia M. García-Blanco and Markus Pollnau

      Article first published online: 24 OCT 2011 | DOI: 10.1002/adma.201101781

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      Modal gain per unit length versus launched pump power is predicted and measured in a 47.5 at.% Yb3+-doped potassium double tungstate channel waveguide. The highest measured gain exceeds values previously reported for rare-earth-ion-doped materials by two orders of magnitude.

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      A 3D Optical Metamaterial Made by Self-Assembly (pages OP23–OP27)

      Silvia Vignolini, Nataliya A. Yufa, Pedro S. Cunha, Stefan Guldin, Ilia Rushkin, Morgan Stefik, Kahyun Hur, Ulrich Wiesner, Jeremy J. Baumberg and Ullrich Steiner

      Article first published online: 24 OCT 2011 | DOI: 10.1002/adma.201103610

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      Optical metamaterials have unusual optical characteristics that arise from their periodic nanostructure. Their manufacture requires the assembly of 3D architectures with structure control on the 10-nm length scale. Such a 3D optical metamaterial, based on the replication of a self-assembled block copolymer into gold, is demonstrated. The resulting gold replica has a feature size that is two orders of magnitude smaller than the wavelength of visible light. Its optical signature reveals an archetypal Pendry wire metamaterial with linear and circular dichroism.

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    1. Plasmonics: Plasmon-Enhanced Sub-Wavelength Laser Ablation: Plasmonic Nanojets (Adv. Mater. 10/2012) (page OP28)

      Ventsislav K. Valev, Denitza Denkova, Xuezhi Zheng, Arseniy I. Kuznetsov, Carsten Reinhardt, Boris N. Chichkov, Gichka Tsutsumanova, Edward J. Osley, Veselin Petkov, Ben De Clercq, Alejandro V. Silhanek, Yogesh Jeyaram, Vladimir Volskiy, Paul A. Warburton, Guy A. E. Vandenbosch, Stoyan Russev, Oleg A. Aktsipetrov, Marcel Ameloot, Victor V. Moshchalkov and Thierry Verbiest

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290052

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      When a droplet hits the surface of water, it is often observed that a water column, or ‘back-jet’, surges upwards. Counterintuitive though it might be, a similar phenomenon can occur when ultrafast light pulses shine on a nanostructured metal surface. These sub-wavelength ‘nanojets’ occur in the regions of highest local field enhancements. For more details, see the article by V. K. Valev et al. on page OP29.

  16. Communications: Advanced Optical Materials

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      Plasmon-Enhanced Sub-Wavelength Laser Ablation: Plasmonic Nanojets (pages OP29–OP35)

      Ventsislav K. Valev, Denitza Denkova, Xuezhi Zheng, Arseniy I. Kuznetsov, Carsten Reinhardt, Boris N. Chichkov, Gichka Tsutsumanova, Edward J. Osley, Veselin Petkov, Ben De Clercq, Alejandro V. Silhanek, Yogesh Jeyaram, Vladimir Volskiy, Paul A. Warburton, Guy A. E. Vandenbosch, Stoyan Russev, Oleg A. Aktsipetrov, Marcel Ameloot, Victor V. Moshchalkov and Thierry Verbiest

      Article first published online: 9 JAN 2012 | DOI: 10.1002/adma.201103807

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      In response to the incident light's electric field, the electron density oscillates in the plasmonic hotspots producing an electric current. Associated Ohmic losses raise the temperature of the material within the plasmonic hotspot above the melting point. A nanojet and nanosphere ejection can then be observed precisely from the plasmonic hotspots.

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      High Magneto-Optical Activity and Low Optical Losses in Metal-Dielectric Au/Co/Au–SiO2 Magnetoplasmonic Nanodisks (pages OP36–OP41)

      Juan Carlos Banthí, David Meneses-Rodríguez, Fernando García, María Ujué González, Antonio García-Martín, Alfonso Cebollada and Gaspar Armelles

      Article first published online: 23 DEC 2011 | DOI: 10.1002/adma.201103634

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      Metal-dielectric Au-Co-SiO2 magnetoplasmonic nanodisks are found to exhibit large magneto-optical activity and low optical losses. The internal architecture of the nanodisks is such that, in resonant conditions, the electromagnetic field undertakes a particular spatial distribution. This makes it possible to maximize the electromagnetic field at the magneto-optically active layers and minimize it in the other, optically lossy ones.

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      Efficient Poling of Electro-Optic Polymers in Thin Films and Silicon Slot Waveguides by Detachable Pyroelectric Crystals (pages OP42–OP47)

      Su Huang, Jingdong Luo, Hin-Lap Yip, Ali Ayazi, Xing-Hua Zhou, Michael Gould, Antao Chen, Tom Baehr-Jones, Michael Hochberg and Alex K.-Y. Jen

      Article first published online: 28 DEC 2011 | DOI: 10.1002/adma.201102874

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      Pyroelectric crystals are used as a conformal and detachable electric field source to efficiently pole electro-optic (E-O) polymers in both parallel-plate (transverse) and in-plane (quasi-longitudinal) configurations. Large Pockels coefficients in poled thin films and high tunability of resonance wavelength shift in hybrid polymer silicon slot waveguide ring-resonator modulators have been achieved using this method.

  17. Frontispiece: Advanced Optical Materials

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    1. Photodetection: Spatially Resolved Photodetection in Leaky Ferroelectric BiFeO3 (Adv. Mater. 10/2012) (page OP48)

      Won-Mo Lee, Ji Ho Sung, Kanghyun Chu, Xavier Moya, Donghun Lee, Cheol-Joo Kim, Neil D. Mathur, S.-W. Cheong, C.-H. Yang and Moon-Ho Jo

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290053

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      On page OP49, M.-H. Jo and co-workers describe a method of control over photocurrent detection by manipulating ferroelectric domain configurations. The magnitude is spectrally centered around charged domain walls that are associated with oxygen vacancy migration in BiFeO3, where potential gradients caused by spontaneous polarization yield asymmetric and nonlinear photocarrier dynamics.

  18. Communications: Advanced Optical Materials

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      Spatially Resolved Photodetection in Leaky Ferroelectric BiFeO3 (pages OP49–OP53)

      Won-Mo Lee, Ji Ho Sung, Kanghyun Chu, Xavier Moya, Donghun Lee, Cheol-Joo Kim, Neil D. Mathur, S.-W. Cheong, C.-H. Yang and Moon-Ho Jo

      Article first published online: 27 JAN 2012 | DOI: 10.1002/adma.201102816

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      Potential gradients due to the spontaneous polarization of BiFeO3 yield asymmetric and nonlinear photocarrier dynamics. Photocurrent direction is determined by local ferroelectric domain orientation, whereas magnitude is spectrally centered around charged domain walls that are associated with oxygen vacancy migration. Photodetection can be electrically controlled by manipulating ferroelectric domain configurations.

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      Homoepitaxial Growth of Single Crystal Diamond Membranes for Quantum Information Processing (pages OP54–OP59)

      Igor Aharonovich, Jonathan C. Lee, Andrew P. Magyar, Bob B. Buckley, Christopher G. Yale, David D. Awschalom and Evelyn L. Hu

      Article first published online: 31 JAN 2012 | DOI: 10.1002/adma.201103932

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      Homoepitaxial growth of single crystal diamond membranes is demonstrated employing a microwave plasma chemical vapor deposition technique. The membranes possess excellent structural, optical, and spin properties, which make them suitable for fabrication of optical microcavities for applications in quantum information processing, photonics, spintronics, and sensing.

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      Self-Assembled Flexible Microlasers (pages OP60–OP64)

      Van Duong Ta, Rui Chen and Han Dong Sun

      Article first published online: 10 FEB 2012 | DOI: 10.1002/adma.201103409

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      Hemispherical microresonators with tunable sizes are obtained based on the hydrophobic effect on distributed Bragg reflectors. Under optical excitation, whispering gallery mode lasing is observed from the dye-doped microresonators at room temperature. The results indicate the potential application of the flexible microresonators in photonic integrated circuits.

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      Ultrafast Polymerization Inhibition by Stimulated Emission Depletion for Three-dimensional Nanolithography (pages OP65–OP69)

      Joachim Fischer and Martin Wegener

      Article first published online: 10 FEB 2012 | DOI: 10.1002/adma.201103758

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      To identify the depletion mechanism in the stimulated-emission-depletion (STED) inspired photoresist composed of a ketocoumarin photoinitiator in pentaerythritol tetraacrylate, we perform lithography with pulsed excitation and tunable delayed depletion. A fast component can unambiguously be assigned to stimulated emission. Our results allow the systematical optimization of the conditions in next-generation STED direct-laser-writing optical lithography.

  19. Frontispiece: Advanced Optical Materials

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    1. Graphene: Plasmonic Graphene Transparent Conductors (Adv. Mater. 10/2012) (page OP70)

      Guowei Xu, Jianwei Liu, Qian Wang, Rongqing Hui, Zhijun Chen, Victor A. Maroni and Judy Wu

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201290055

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      Plasmonic graphene has been fabricated by G. Xu et al. using thermally assisted self-assembly of Ag nanoparticles on graphene. The localized surface-plasmonic effect is demonstrated with the resonance frequency shifting from 446 to 495 nm when the lateral dimension of the Ag nanopar-ticles increases from about 50 to 150 nm. Both the resonance frequency and amplitude decrease with increasing graphene thickness. In addition, plasmonic graphene shows much improved electrical conductance by a factor of 2–4 as compared to the original graphene.

  20. Communication: Advanced Optical Materials

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      Plasmonic Graphene Transparent Conductors (pages OP71–OP76)

      Guowei Xu, Jianwei Liu, Qian Wang, Rongqing Hui, Zhijun Chen, Victor A. Maroni and Judy Wu

      Article first published online: 6 MAR 2012 | DOI: 10.1002/adma.201104846

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      Plasmonic graphene is fabricated using thermally assisted self-assembly of silver nanoparticles on graphene. Tuning of the surface plasmonic resonance frequency and amplitude in plasmonic graphene is demonstrated.

  21. Full Paper: Advanced Optical Materials

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      Certain Biominerals in Leaves Function as Light Scatterers (pages OP77–OP83)

      Assaf Gal, Vlad Brumfeld, Steve Weiner, Lia Addadi and Dan Oron

      Article first published online: 31 JAN 2012 | DOI: 10.1002/adma.201104548

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      Leaf minerals function as internal light scatterers inside leaves. They transfer light from the saturated upper tissue into the light deprived lower tissue. This eases the steep light gradient inside the leaf and improves photosynthetic efficiency on the tissue scale.

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