Advanced Materials

Cover image for Vol. 24 Issue 23

June 19, 2012

Volume 24, Issue 23

Pages 3081–3142, OP89–OP180

  1. Cover Picture

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    18. Full Paper “Advanced Optical Materials”
    1. Organic Semiconductors: Thiazole-Based Organic Semiconductors for Organic Electronics (Adv. Mater. 23/2012) (page 3081)

      Yuze Lin, Haijun Fan, Yongfang Li and Xiaowei Zhan

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290133

      Thumbnail image of graphical abstract

      Thiazole-based organic semiconductors exhibit high performance in organic field-effect transistors (OFETs), which are a key element in materials such as the electronic paper shown in the image. On page 3087, Y. Li, X. Zhan, and co-workers review recent developments to thiazole-based organic semiconductors, particularly thiazole, bithiazole, thiazolothiazole, and benzobisthiazole-based small molecules and polymers, for applications in OFETs, solar cells, and light-emitting diodes.

  2. Inside Front Cover

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    16. Communications “Advanced Optical Materials”
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    18. Full Paper “Advanced Optical Materials”
    1. Template Patterning: Flexible Control of Block Copolymer Directed Self-Assembly using Small, Topographical Templates: Potential Lithography Solution for Integrated Circuit Contact Hole Patterning (Adv. Mater. 23/2012) (page 3082)

      He Yi, Xin-Yu Bao, Jie Zhang, Christopher Bencher, Li-Wen Chang, Xiangyu Chen, Richard Tiberio, James Conway, Huixiong Dai, Yongmei Chen, Subhasish Mitra and H.-S. Philip Wong

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290134

      Thumbnail image of graphical abstract

      The image depicts the flexible control over the directed self-assembly of block copolymers that can be achieved using small topographical templates. On page 3107, H.-S. P. Wong and co-workers explain how differently shaped templates cause the block copolymer to self-assemble to form corresponding nanopatterns, providing a potential solution to contact-hole patterning for integrated circuits beyond the 22 nm technology node.

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    1. Masthead: (Adv. Mater. 23/2012)

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290135

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    18. Full Paper “Advanced Optical Materials”
  5. Progress Report

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    1. Thiazole-Based Organic Semiconductors for Organic Electronics (pages 3087–3106)

      Yuze Lin, Haijun Fan, Yongfang Li and Xiaowei Zhan

      Version of Record online: 11 MAY 2012 | DOI: 10.1002/adma.201200721

      Thumbnail image of graphical abstract

      Thiazole is an electron-accepting heterocycle due to electron-withdrawing nitrogen of imine, several thiazole related moieties have been widely introduced into organic semiconductors and yielded high performance in organic electronic devices. This article reviews recent developments in thiazole, bithiazole, thiazolothiazole and benzobisthiazole-based small molecule and polymer semiconductors for applications in organic field-effect transistors, solar cells and light-emitting diodes.

  6. Communications

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    1. Flexible Control of Block Copolymer Directed Self-Assembly using Small, Topographical Templates: Potential Lithography Solution for Integrated Circuit Contact Hole Patterning (pages 3107–3114)

      He Yi, Xin-Yu Bao, Jie Zhang, Christopher Bencher, Li-Wen Chang, Xiangyu Chen, Richard Tiberio, James Conway, Huixiong Dai, Yongmei Chen, Subhasish Mitra and H.-S. Philip Wong

      Version of Record online: 2 MAY 2012 | DOI: 10.1002/adma.201200265

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      Block copolymer directed self-assembly (DSA) using small guiding templates for contact hole patterning in integrated circuits is reported. Flexible and precise DSA control of 25 nm contact holes guided by 66 nm templates for industry-standard 22 nm static random access memory cells is experimentally demonstrated. For 22 nm random logic circuits a DSA-aware design methodology is developed and the contact holes are achieved with a critical dimension of 15 nm and overylay accuracy of 1 nm.

    2. Micelle-Templated Mesoporous Films of Magnesium Carbonate and Magnesium Oxide (pages 3115–3119)

      B. Eckhardt, E. Ortel, J. Polte, D. Bernsmeier, O. Görke, P. Strasser and R. Kraehnert

      Version of Record online: 9 MAY 2012 | DOI: 10.1002/adma.201104984

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      Ordered mesoporous MgO films are synthesized via micelle-templating for the first time. The problems of low melting points, insolubility and excessive crystallization of the metal oxide precursors are overcome by synthesizing in-situ a magnesium nitrate-citric acid complex. The stepwise thermal transformation into magnesium carbonate and then MgO was studied as well as the evolution of the mesopore structure.

    3. Strong Hard X-ray Magnetochiral Dichroism in Paramagnetic Enantiopure Molecules (pages 3120–3123)

      Marcelo Ceolín, Sara Goberna-Ferrón and José Ramón Galán-Mascarós

      Version of Record online: 16 MAY 2012 | DOI: 10.1002/adma.201200786

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      Experimental evidence of magnetochiral dichroism is found in the hard X-ray absorption spectra of paramagnetic enantiopure molecules. An isotropic sample of a {Tb[Ni(pro)2]6}3+ salt (pro = L- or D-prolinate) shows up to a 1% difference in absorbance when a magnetic field (1 T) is applied parallel or anti-parallel to the incident X-ray beam at room temperature. This represents the largest magnetochiral dichroism ever observed in absolute and relative value.

    4. A Membrane Device for Substrate-Free Photovoltaic Characterization of Quantum Dot Based p-i-n Solar Cells (pages 3124–3129)

      Philipp Löper, David Stüwe, Matthias Künle, Martin Bivour, Christian Reichel, Rainer Neubauer, Manuel Schnabel, Martin Hermle, Oliver Eibl, Stefan Janz, Margit Zacharias and Stefan W. Glunz

      Version of Record online: 16 MAY 2012 | DOI: 10.1002/adma.201200539

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      A membrane based silicon nanocrystal p-i-n diode is presented that enables the photovoltaic characterization of silicon quantum dots produced by high-temperature routes. The membrane p-i-n diode decouples silicon nanocrystal formation from the formation of selective contacts and therefore enables extraction of the full photovoltaic potential. Open-circuit voltages of up to 370 mV are shown, which is encouraging for future tandem solar cells.

    5. Accessible Surface Area of Porous Materials: Understanding Theoretical Limits (pages 3130–3133)

      Lev Sarkisov

      Version of Record online: 9 MAY 2012 | DOI: 10.1002/adma.201104708

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      In this article, computational tools are applied to establish a theoretical limit of the accessible surface area in porous structures. For both crystalline and disordered structures the theoretical limit of the surface area is estimated at about 15000 m2/g. For models of disordered carbons based on random packings of platelets, this limit is estimated at about 6400 m2/g.

    6. Graphene Oxide Filled Nanocomposite with Novel Electrical and Dielectric Properties (pages 3134–3137)

      Zepu Wang, J. Keith Nelson, Henrik Hillborg, Su Zhao and Linda S. Schadler

      Version of Record online: 9 MAY 2012 | DOI: 10.1002/adma.201200827

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      Graphene oxide filled polymer nanocomposites are found to possess excellent nonlinear electrical conductivity, low conductivity at low field and a good combination of increased dielectric constant and low loss factor. Those outstanding electrical properties are achieved at filler loading of 3% and controllable by adjusting the oxidation state of graphene oxide.

    7. Hybrid Organic/Inorganic Optical Up-Converter for Pixel-Less Near-Infrared Imaging (pages 3138–3142)

      Jun Chen, Jianchen Tao, Dayan Ban, Michael G. Helander, Zhibin Wang, Jacky Qiu and Zhenghong Lu

      Version of Record online: 18 MAY 2012 | DOI: 10.1002/adma.201200587

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      A hybrid organic/inorganic up-converter for pixel-less near-infrared (NIR) imaging has been designed and demonstrated. The device is fabricated by direct tandem integration of an organic light-emitting diode with an i-InGaAs substrate. A good-quality 1.5 μm NIR to 520 nm visible green light up-conversion image with a spatial resolution of better than 6 μm is achieved.

  7. Cover Picture “Advanced Optical Materials”

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    1. Photonic Crystals: Photoresponsive Block Copolymer Photonic Gels with Widely Tunable Photosensitivity by Counter-Ions (Adv. Mater. 23/2012) (page OP89)

      Youshin Ahn, Eunjoo Kim, Jinho Hyon, Changjoon Kang and Youngjong Kang

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290136

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      Block copolymer photonic gels exhibiting multiple colors in response to near-UV radiation are demonstrated by Y. Kang and co-workers on page OP 127. The counterions pairing with the polyelectrolyte in the gel layers determine the photosensitivity of photonic gels. The simple replacement of ions can make the photonic gels either highly sensitive or insensitive to near-UV. The illustration shows ionic signaling giving “STOP” and “GO” cues for the photoresponse of these photonic gels.

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    1. Microlens Arrays: Fabrication of Microlens Arrays with Well-controlled Curvature by Liquid Trapping and Electrohydrodynamic Deformation in Microholes (Adv. Mater. 23/2012) (page OP90)

      Xiangming Li, Yucheng Ding, Jinyou Shao, Hongmiao Tian and Hongzhong Liu

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290137

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      Y. C. Ding, J. Y. Shao, and co-workers demonstrate a creative and economic method for manufacturing large-area microlens arrays (MLAs) with controllable curvature and supersmooth surfaces. On page OP 165, the production of a concave MLA is achieved by electrohydrodynamically deforming the surface of a photocurable prepolymer trapped in microhole array which has been etched onto a doped silicon wafer. The concave MLA is then used as a master to generate the convex MLA via vacuum micromoulding.

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    1. Metamaterial Electromagnetic Wave Absorbers (Adv. Mater. 23/2012) (page OP181)

      Claire M. Watts, Xianliang Liu and Willie J. Padilla

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290138

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      The image shows a dual-band metamaterial perfect absorber. The structure, described on page OP98 by W. J. Padilla and co-workers, is made of a checkerboard pattern of two gold crosses on a ground plane separated by a dielectric. The crosses of different sizes resonate at two frequencies, causing an impedance match condition and hence unity absorption at those frequencies. In this rendering, the incoming light (white) and the reflected white (red) are seen where green and blue light have been absorbed.

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    1. Masthead: (Adv. Mater. 23/2012)

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290139

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  13. Progress Report “Advanced Optical Materials”

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      Metamaterial Electromagnetic Wave Absorbers (pages OP98–OP120)

      Claire M. Watts, Xianliang Liu and Willie J. Padilla

      Version of Record online: 25 MAY 2012 | DOI: 10.1002/adma.201200674

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      A review of metamaterial perfect absorbers, their applications (both potential and realized) and an overview and critique of current work taking place in the field is presented.

  14. Frontispiece “Advanced Optical Materials”

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    1. Electrochromic Materials: Electrochemical Optical-Modulation Device with Reversible Transformation Between Transparent, Mirror, and Black (Adv. Mater. 23/2012) (page OP121)

      Shingo Araki, Kazuki Nakamura, Kanae Kobayashi, Ayako Tsuboi and Norihisa Kobayashi

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290142

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      A novel electrochromic device with three optical states - transparent, specular mirror, and black - is demonstrated by N. Kobayashi and co-workers on page OP 122. The cell is constructed by sandwiching gel electrolyte-containing silver nitrate between one flat and one particle-modified in-dium thin oxide electrode. The optical states can be switched by altering the potential across the two electrodes.

  15. Communications “Advanced Optical Materials”

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      Electrochemical Optical-Modulation Device with Reversible Transformation Between Transparent, Mirror, and Black (pages OP122–OP126)

      Shingo Araki, Kazuki Nakamura, Kanae Kobayashi, Ayako Tsuboi and Norihisa Kobayashi

      Version of Record online: 10 MAY 2012 | DOI: 10.1002/adma.201200060

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      A novel electrochromic device with three optical states, transparent, specular mirror, and black, is demonstrated. The cell is constructed by sandwiching gel electrolyte containing silver nitrate between one flat and one particle-modified indium thin oxide electrode. The optical states can be switched by altering the potential across the two electrodes. All changes are reversible and show good stability over 2500 cycles of testing.

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      Photoresponsive Block Copolymer Photonic Gels with Widely Tunable Photosensitivity by Counter-Ions (pages OP127–OP130)

      Youshin Ahn, Eunjoo Kim, Jinho Hyon, Changjoon Kang and Youngjong Kang

      Version of Record online: 10 FEB 2012 | DOI: 10.1002/adma.201103767

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      Block copolymer photonic crystals comprising polyelectrolyte hydrogels exhibit strong reflective multicolors in response to near-UV radiation. Due to unique volume transition of swollen gels, the photonic gels show high photosensitivity, and which can be widely tunable by exchanging counter-anions. Multicolor photonic patterns created by photolithography can be repeatedly fixated and reactivated by sequentially exchanging counter-anions with different photosensitivity.

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      Light-Driven Plasmonic Color Filters by Overlaying Photoresponsive Liquid Crystals on Gold Annular Aperture Arrays (pages OP131–OP135)

      Yan Jun Liu, Guang Yuan Si, Eunice S. P. Leong, Ning Xiang, Aaron J. Danner and Jing Hua Teng

      Version of Record online: 21 MAR 2012 | DOI: 10.1002/adma.201104440

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      Light-driven plasmonic color filters are demonstrated by integrating gold annular aperture arrays with photoresponsive liquid crystals (LCs). Upon photoirradiation, a nematic−isotropic phase transition of the LCs arises from the transcis photoisomerization of photochromic LCs. As a consequence, the effective refractive index experienced by the impinging light changes, modulating the transmission intensity.

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      Metal–Polymer–Metal Split-Dipole Nanoantennas (pages OP136–OP142)

      Deirdre M. O'Carroll, James S. Fakonas, Dennis M. Callahan, Martin Schierhorn and Harry A. Atwater

      Version of Record online: 22 MAR 2012 | DOI: 10.1002/adma.201103396

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      The conjugated polymer semiconductor poly(3-hexylthiophene), (P3HT), is integrated directly into the slot region of resonant plasmonic split-dipole nanoantennas. The P3HT radiative emission rate is enhanced by a factor of up to 29, in experiment, and 550 for the ideal case, due to the large local density of optical states in the nanoantenna slot region. Additionally, the theoretical modified luminescence quantum efficiency is shown to increase from 1% to 45% for optimized nanoantenna parameters.

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      Realization of Variable Three-Dimensional Terahertz Metamaterial Tubes for Passive Resonance Tunability (pages OP143–OP147)

      Chen Zaichun, Mohsen Rahmani, Gong Yandong, Chong Tow Chong and Hong Minghui

      Version of Record online: 22 MAR 2012 | DOI: 10.1002/adma.201104575

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      A three-dimensional metamaterial tube is fabricated by rolling up 2D metamaterials on flexible PEN substrate. This novel 3D design of metamaterials can be used to effectively tune the resonance frequency by varying its diameter. Meanwhile, it can also be applied in material identification with a solid-core metamaterials tube.

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      Label-Free, Coupler-Free, Scalable and Intracellular Bio-imaging by Multimode Plasmonic Resonances in Split-Ring Resonators (pages OP148–OP152)

      Yueh-Chun Lai, Hsin-Cheng Lee, Shu-Wen Kuo, Cheng-Kuang Chen, Hsieh-Ting Wu, Oscar K. Lee and Ta-Jen Yen

      Version of Record online: 15 MAY 2012 | DOI: 10.1002/adma.201200291

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      Intracellular imaging by exciting multimode resonances in spilt-ring resonators (SRRs) is presented. With advantages such as being label-free, coupler-free, having a tunable spectrum range and intracellular detection length, SRR microscopy is a strong competitor for surface plasmon resonance microscopy for observing cells. Its capability for constructing refractive index distribution images of cells is demonstrated. SRR microscopy offers a much simpler optical configuration and better penetration depth for truly whole-cell imaging applications.

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      Radiative Lifetime Modification of LaF3:Nd Nanoparticles Embedded in 3D Silicon Photonic Crystals (pages OP153–OP158)

      Hailong Ning, Agustin Mihi, Joseph B. Geddes III, Masao Miyake and Paul V. Braun

      Version of Record online: 9 MAY 2012 | DOI: 10.1002/adma.201104769

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      The photonic density of states (DOS) of a silicon inverse photonic crystal is probed using the radiative emission of LaF3:Nd nanoparticles. These emitters are embedded as a thin planar defect within the interior of photonic crystals with varying silicon filling fractions. The alignment of the narrow emission of the particles with the high and low photonic DOS regions is achieved. The time-resolved measurements reveal that the radiative lifetime of the embedded Nd3+ is strongly influenced by the surrounding DOS provided by the silicon inverse opals.

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      Low Threshold, Amplified Spontaneous Emission from Core-Seeded Semiconductor Nanotetrapods Incorporated into a Sol–Gel Matrix (pages OP159–OP164)

      Yile Liao, Guichuan Xing, Nimai Mishra, Tze Chien Sum and Yinthai Chan

      Version of Record online: 18 MAY 2012 | DOI: 10.1002/adma.201200121

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      Wet-chemically synthesized CdSe seeded CdS nanotetrapods incorporated into silica matrices have been explored as high performance nanocrystal-based optical amplifiers. Varying the physical dimensions of the tetrapods allowed for room temperature biexcitonic amplified spontaneous emission (ASE) at wavelengths corresponding to either the CdSe core or CdS arms, while higher pump intensities resulted in ASE from a higher CdSe excited state. These results collectively indicate that such heterostructured tetrapods can facilitate tunable, multiple-wavelength lasing across a wide spectral range from a single nanostructure.

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      Fabrication of Microlens Arrays with Well-controlled Curvature by Liquid Trapping and Electrohydrodynamic Deformation in Microholes (pages OP165–OP169)

      Xiangming Li, Yucheng Ding, Jinyou Shao, Hongmiao Tian and Hongzhong Liu

      Version of Record online: 22 MAR 2012 | DOI: 10.1002/adma.201104625

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      The microlens array (MLA) or micromirror array (MMA) is one of the most important units in many optical devices and photoelectronic systems. The paper presents a process for fabricating an MLA with well-controlled curvature by liquid trapping and electrohydrodynamic deformation in microholes. The approach has been shown capable of generating large-area and high-quality MLAs or MMAs economically.

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      Can Nanotubes Make a Lens Array? (pages OP170–OP173)

      Ranjith Rajasekharan, Haider Butt, Qing Dai, Timothy D. Wilkinson and Gehan A. J. Amaratunga

      Version of Record online: 9 MAY 2012 | DOI: 10.1002/adma.201200296

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      Reflective binary Fresnel lenses fabricated so far all suffer from reflections from the opaque zones and hence degradation in focusing and lensing properties. Here a solution is found to this problem by developing a carbon nanotube Fresnel lens, where the darkest man-made material ever, i.e., low-density vertically aligned carbon nanotube arrays, are exploited.

  16. Frontispiece “Advanced Optical Materials”

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    1. Hierarchical Electrohydrodynamic Structures for Surface-Enhanced Raman Scattering (Adv. Mater. 23/2012) (page OP174)

      Pola Goldberg-Oppenheimer, Sumeet Mahajan and Ullrich Steiner

      Version of Record online: 12 JUN 2012 | DOI: 10.1002/adma.201290143

      Thumbnail image of graphical abstract

      On page OP 175, U. Steiner and co-workers destabilise polymer trilayer films using an electric field to generate separated micrometre-sized core-shell pillars, which are further modified by selective polymer dissolution to yield polymer core columns surrounded by a rim and micro-volcano rim structures. When coated with gold and decorated with Raman active probes, all three structure types give rise to substantial enhancement in surface-enhanced Raman scattering (SERS). Since this SERS enhancement arises from each of the isolated structures in the array, these surface patterns are an ideal platform for multiplexed SERS detection.

  17. Full Paper “Advanced Optical Materials”

    1. Top of page
    2. Cover Picture
    3. Inside Front Cover
    4. Masthead
    5. Contents
    6. Progress Report
    7. Communications
    8. Cover Picture “Advanced Optical Materials”
    9. Inside Front Cover “Advanced Optical Materials”
    10. Back Cover “Advanced Optical Materials”
    11. Masthead “Advanced Optical Materials”
    12. Contents “Advanced Optical Materials”
    13. Editorial “Advanced Optical Materials”
    14. Progress Report “Advanced Optical Materials”
    15. Frontispiece “Advanced Optical Materials”
    16. Communications “Advanced Optical Materials”
    17. Frontispiece “Advanced Optical Materials”
    18. Full Paper “Advanced Optical Materials”
    1. You have free access to this content
      Hierarchical Electrohydrodynamic Structures for Surface-Enhanced Raman Scattering (pages OP175–OP180)

      Pola Goldberg-Oppenheimer, Sumeet Mahajan and Ullrich Steiner

      Version of Record online: 4 APR 2012 | DOI: 10.1002/adma.201104159

      Thumbnail image of graphical abstract

      Electrohydrodynamic (EHD) instabilities are employed to create hierarchical structures including, pillars, coaxial morphologies and rims with sub-micrometer edges, which are further used as substrates for surface-enhanced Raman scattering (SERS). 1.0 × 107 SERS enhancements from isolated rims and coaxial patterns are observed. Since SERS enhancement arises from each of the isolated structures in the array, EHD-patterned substrates provide optimal platforms for high-throughput SERS detection, where each of the individual EHD structures can be used to detect a different molecular component.

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