Advanced Materials

Cover image for Vol. 26 Issue 9

March 5, 2014

Volume 26, Issue 9

Pages 1309–1467

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      Electronic Skin: Silk-Molded Flexible, Ultrasensitive, and Highly Stable Electronic Skin for Monitoring Human Physiological Signals (Adv. Mater. 9/2014) (page 1309)

      Xuewen Wang, Yang Gu, Zuoping Xiong, Zheng Cui and Ting Zhang

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470054

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      Flexible ultrasensitive electronic skin is fabricated by combining silk-molded micro-patterned polydimethylsiloxane (PDMS) with a single-walled carbon nanotube (SWNT) ultrathin film, as reported by T. Zhang and co-workers on page 1336. These E-skin devices might be used for applications in monitoring human physiological signals for disease diagnosis and health assessment.

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      Conducting Polymers: Stretchable Polymeric Multielectrode Array for Conformal Neural Interfacing (Adv. Mater. 9/2014) (page 1310)

      Liang Guo, Mingming Ma, Ning Zhang, Robert Langer and Daniel G. Anderson

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470055

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      D. G. Anderson and co-workers demonstrate on page 1427 a highly stretchable polymeric multielectrode array (SPMEA) that is applied as an epimysial interface to treat muscle denervation atrophy through electrical stimulation during the course of nerve repair. Meanwhile, the SPMEA is capable of monitoring the re innervation process by recording an electromyogram. This SPMEA is developed with a conducting polymer film as the sole conductor for both electrodes and leads, offering the benefits of conducting polymer electrodes in a demanding stretchable format, including low electrode impedance, high charge-injection capacity, and good biocompatibility.

  3. Inside Back Cover

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      Graphene: Near-Equilibrium Chemical Vapor Deposition of High-Quality Single-Crystal Graphene Directly on Various Dielectric Substrates (Adv. Mater. 9/2014) (page 1471)

      Jianyi Chen, Yunlong Guo, Lili Jiang, Zhiping Xu, Liping Huang, Yunzhou Xue, Dechao Geng, Bin Wu, Wenping Hu, Gui Yu and Yunqi Liu

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470059

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      Via a small-carbon-flow, long-time, near-equilibrium chemical vapor deposition method, single-crystal graphene grains larger than 10 μm are grown directly on various dielectric substrates, successfully practicing the Chinese saying of Image (slow work yields a fine product). The high mobility, exceeding 5000 cm2 V−1 s−1, is comparable to that of metal-catalyzed graphene. Further details can be found in the article by Y. Liu and co-workers on page 1348.

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      Phononic Crystals: Phononic Crystal with Adaptive Connectivity (Adv. Mater. 9/2014) (page 1472)

      Andrea Bergamini, Tommaso Delpero, Luca De Simoni, Luigi Di Lillo, Massimo Ruzzene and Paolo Ermanni

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470060

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      Phononic crystals are structures with discontinuous dispersion relations, such as crystals made of atoms. A. Bergamini and co-workers show on page 1343 that in adaptively augmented phononic crystals, existing bandgaps can be canceled at specific frequencies by modifying the mechanical connectivity of the unit cell. Photography: Wolfram Raither, ETH Zürich Photo Design: Beat Geyer, Empa and Wolfram Raither, ETH Zürich.

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      Masthead: (Adv. Mater. 9/2014)

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470057

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  7. Reviews

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      25th Anniversary Article: Organic Field-Effect Transistors: The Path Beyond Amorphous Silicon (pages 1319–1335)

      Henning Sirringhaus

      Version of Record online: 20 JAN 2014 | DOI: 10.1002/adma.201304346

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      The mobility of organic field-effect transistors (OFETs) has improved dramatically over the past 25 years, and now exceeds that of amorphous silicon. OFETs are being used in products such as flexible electronic paper displays. Current understanding of the charge transport physics that allows such unexpectedly high mobilities to be reached in van der Waals-bonded molecular and polymeric semiconductors is reviewed.

  8. Communications

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    1. Silk-Molded Flexible, Ultrasensitive, and Highly Stable Electronic Skin for Monitoring Human Physiological Signals (pages 1336–1342)

      Xuewen Wang, Yang Gu, Zuoping Xiong, Zheng Cui and Ting Zhang

      Version of Record online: 17 DEC 2013 | DOI: 10.1002/adma.201304248

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      Flexible and transparent E-skin devices are achieved by combining silk-molded micro-patterned polydimethylsiloxane (PDMS) with single-walled carbon nanotube (SWNT) ultrathin films. The E-skin sensing device demonstrates superior sensitivity, a very low detectable pressure limit, a fast response time, and a high stability for the detection of superslight pressures, which may broaden their potential use as cost-effective wearable electronics for healthcare applications.

    2. Phononic Crystal with Adaptive Connectivity (pages 1343–1347)

      Andrea Bergamini, Tommaso Delpero, Luca De Simoni, Luigi Di Lillo, Massimo Ruzzene and Paolo Ermanni

      Version of Record online: 19 DEC 2013 | DOI: 10.1002/adma.201305280

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      The band structure of a phononic crystal can be controlled by tuning the mechanical stiffness of the links connecting its constituting elements. The first implementation of a phononic crystal with adaptive connectivity is obtained by using piezoelectric resonators as variable stiffness elements, and its wave-propagation properties are experimentally characterized.

    3. Near-Equilibrium Chemical Vapor Deposition of High-Quality Single-Crystal Graphene Directly on Various Dielectric Substrates (pages 1348–1353)

      Jianyi Chen, Yunlong Guo, Lili Jiang, Zhiping Xu, Liping Huang, Yunzhou Xue, Dechao Geng, Bin Wu, Wenping Hu, Gui Yu and Yunqi Liu

      Version of Record online: 12 DEC 2013 | DOI: 10.1002/adma.201304872

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      By using near-equilibrium chemical vapor deposition, it is demonstrated that high-quality single-crystal graphene can be grown on dielectric substrates. The maximum size is about 11 μm. The carrier mobility can reach about 5650 cm2 V−1 s−1, which is comparable to those of some metal-catalyzed graphene crystals, reflecting the good quality of the graphene lattice.

    4. High Contrast Fluorescence Patterning in Cyanostilbene-Based Crystalline Thin Films: Crystallization-Induced Mass Flow Via a Photo-Triggered Phase Transition (pages 1354–1359)

      Jin Wook Park, Shusaku Nagano, Seong-Jun Yoon, Tomoki Dohi, Jangwon Seo, Takahiro Seki and Soo Young Park

      Version of Record online: 28 NOV 2013 | DOI: 10.1002/adma.201304250

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      A facile and innovative method for the fabrication of highly fluorescent micro-patterns is presented, which operates on the principle of phototriggered phase transition and physical mass migration in the crystalline film of a cyanostilbene-type aggregation-induced enhanced emission (AIEE) molecule ((Z)-2,3-bis(3,4,5-tris(dodecyloxy)phenyl) acrylonitrile) with liquid-crystalline (LC) mesomorphic behavior.

    5. Carbonized Eggshell Membrane as a Natural Polysulfide Reservoir for Highly Reversible Li-S Batteries (pages 1360–1365)

      Sheng-Heng Chung and Arumugam Manthiram

      Version of Record online: 27 NOV 2013 | DOI: 10.1002/adma.201304365

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      Carbonized sucrose-coated eggshell membranes (CSEMs) consisting of natural micropores function well as a polysulfide reservoir in Li/dissolved polysulfide cells. The bottom CSEM current collector encapsulates the active material, while the upper CSEM inhibitor intercepts the migrating polysulfides. This design with CSEM allows the dissolved polysulfides to be localized and the electrochemical reactions within the cathode region to be stabilized, resulting in high discharge capacity, long-term cycle stability, and high sulfur loading.

    6. Nanostructured Singlet Fission Photovoltaics Subject to Triplet-Charge Annihilation (pages 1366–1371)

      Nicholas J. Thompson, Eric Hontz, Daniel N. Congreve, Matthias E. Bahlke, Sebastian Reineke, Troy Van Voorhis and Marc A. Baldo

      Version of Record online: 27 NOV 2013 | DOI: 10.1002/adma.201304588

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      Singlet exciton fission is an efficient multiple-exciton generation process that is vulnerable to a characteristic loss process: triplet-charge annihilation. This loss process is characterized in singlet-fission photovoltaics and losses as high as 40% are observed in poorly designed devices. Techniques are demonstrated to improve charge extraction and reduce triplet-charge annihilation to negligible levels at short-circuit conditions.

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      On-Chip Photonic Memory Elements Employing Phase-Change Materials (pages 1372–1377)

      Carlos Rios, Peiman Hosseini, C. David Wright, Harish Bhaskaran and Wolfram H. P. Pernice

      Version of Record online: 2 DEC 2013 | DOI: 10.1002/adma.201304476

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      Phase-change materials integrated into nanophotonic circuits provide a flexible way to realize tunable optical components. Relying on the enormous refractive-index contrast between the amorphous and crystalline states, such materials are promising candidates for on-chip photonic memories. Nonvolatile memory operation employing arrays of microring resonators is demonstrated as a route toward all-photonic chipscale information processing.

    8. Graphene/Graphene-Tube Nanocomposites Templated from Cage-Containing Metal-Organic Frameworks for Oxygen Reduction in Li–O2 Batteries (pages 1378–1386)

      Qing Li, Ping Xu, Wei Gao, Shuguo Ma, Guoqi Zhang, Ruiguo Cao, Jaephil Cho, Hsing-Lin Wang and Gang Wu

      Version of Record online: 26 NOV 2013 | DOI: 10.1002/adma.201304218

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      Nitrogen-doped graphene/graphene-tube nanocomposites are prepared by a hightemperature approach using a newly designed cage-containing metal-organic framework (MOF) to template nitrogen/carbon (dicyandiamide) and iron precursors. The resulting N-Fe-MOF catalysts universally exhibit high oxygen-reduction activity in acidic, alkaline, and non-aqueous electrolytes and superior cathode performance in Li-O2 batteries.

    9. Controlling Structural Symmetry of a Hybrid Nanostructure and its Effect on Efficient Photocatalytic Hydrogen Evolution (pages 1387–1392)

      Qian Zhao, Muwei Ji, Hongmei Qian, Baosong Dai, Lin Weng, Jing Gui, Jiatao Zhang, Min Ouyang and Hesun Zhu

      Version of Record online: 12 DEC 2013 | DOI: 10.1002/adma.201304652

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      The existence of lattice strain between two different materials can be used to control the fine structural configuration in a hybrid colloidal nanostructure. Enabled by such, the relative position change of Au and CdX in Au-CdX from a symmetric to an asymmetric configuration is demonstrated, which can further lead to fine tuning of plasmon-exciton coupling and different hydrogen photocatalytic performance. These results provide new insight into plasmon enhanced photocatalytic mechanisms and provide potential catalysts for photoreduction reactions.

    10. One-Step Two-Dimensional Microfluidics-Based Synthesis of Three-Dimensional Particles (pages 1393–1398)

      Navid Hakimi, Scott S. H. Tsai, Chil-Hung Cheng and Dae Kun Hwang

      Version of Record online: 11 DEC 2013 | DOI: 10.1002/adma.201304378

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      Synthesis of three-dimensional anisotropic microparticles using a simple one-step microfluidic-based method is described. The method exploits the nonuniformity of the polymerizing UV light, UV absorption by opaque nanoparticles in the precursor solution, and discontinuous photomask patterns to make magnetic and non-magnetic microparticles in a twodimensional microchannel. Numerical simulations of monomer conversion in the microfluidic channel are performed to predict the manufactured particle shape.

    11. 2-Dimensional Transition Metal Dichalcogenides with Tunable Direct Band Gaps: MoS2(1–x)Se2x Monolayers (pages 1399–1404)

      John Mann, Quan Ma, Patrick M. Odenthal, Miguel Isarraraz, Duy Le, Edwin Preciado, David Barroso, Koichi Yamaguchi, Gretel von Son Palacio, Andrew Nguyen, Tai Tran, Michelle Wurch, Ariana Nguyen, Velveth Klee, Sarah Bobek, Dezheng Sun, Tony. F. Heinz, Talat S. Rahman, Roland Kawakami and Ludwig Bartels

      Version of Record online: 12 DEC 2013 | DOI: 10.1002/adma.201304389

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      MoS2(1−x) Se2x single-layer films are prepared using a mixture of organic selenium and sulfur precursors as well as a solid molybdenum source. The direct bandgaps are found to scale nearly linearly with composition in the range of 1.87 eV (pure single-layer MoS2) to 1.55 eV (pure single-layer MoSe2) permitting straightforward bandgap engineering.

    12. Activated Solutions Enabling Low-Temperature Processing of Functional Ferroelectric Oxides for Flexible Electronics (pages 1405–1409)

      Iñigo Bretos, Ricardo Jiménez, Aiying Wu, Angus I. Kingon, Paula M. Vilarinho and M. Lourdes Calzada

      Version of Record online: 12 DEC 2013 | DOI: 10.1002/adma.201304308

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      Functional ferroelectric oxides for flexible electronics are achieved from activated solutions enabling low-temperature processing and large-area deposition directly on polymeric substrates. This processing technology reaches the lower limit temperature of crystallization at 300 °C, using a strategy that combines seeded diphasic precursors and photochemical solution deposition. Properties of these materials are comparable to those of high-temperature-processed counterparts and organic ferroelectrics.

    13. Fabrication of Silicon Nanowire Arrays by Macroscopic Galvanic Cell-Driven Metal Catalyzed Electroless Etching in Aerated HF Solution (pages 1410–1413)

      Lin Liu, Kui-Qing Peng, Ya Hu, Xiao-Ling Wu and Shuit-Tong Lee

      Version of Record online: 10 DEC 2013 | DOI: 10.1002/adma.201304327

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      Macroscopic galvanic cell-driven metal catalyzed electroless etching (MCEE) of silicon in aqueous hydrofluoric acid (HF) solution is devised to fabricate silicon nanowire (SiNW) arrays with dissolved oxygen acting as the one and only oxidizing agent. The key aspect of this strategy is the use of a graphite or other noble metal electrode that is electrically coupled with silicon substrate.

    14. A Multilevel Intermediate-Band Solar Cell by InGaN/GaN Quantum Dots with a Strain-Modulated Structure (pages 1414–1420)

      Liwen Sang, Meiyong Liao, Qifeng Liang, Masaki Takeguchi, Benjamin Dierre, Bo Shen, Takashi Sekiguchi, Yasuo Koide and Masatomo Sumiya

      Version of Record online: 6 DEC 2013 | DOI: 10.1002/adma.201304335

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      Multiple stacked InGaN/GaN quantum dots are embedded into an InGaN p-n junction to develop multilevel intermediateband (MIB) solar cells. An IB transition is evidenced from both experiment and theoretical calculations. The MIB solar cell shows a wide photovoltaic response from the UV to the near-IR region. This work opens up an interesting opportunity for high-efficiency IB solar cells in the photovoltaics field.

  9. Frontispiece

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      Hierarchical Structures: 3D Hierarchical Architectures Prepared by Single Exposure Through a Highly Durable Colloidal Phase Mask (Adv. Mater. 9/2014) (page 1421)

      Tae Yoon Jeon, Hwan Chul Jeon, Su Yeon Lee, Tae Soup Shim, Jung-Dae Kwon, Sung-Gyu Park and Seung-Man Yang

      Version of Record online: 4 MAR 2014 | DOI: 10.1002/adma.201470058

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      A simple and cost-effective fabrication of 3D hierarchical architectures is demonstrated by S.-M. Yang, S.-G. Park, and co-workers on page 1422. 3D nanoarchitectures with hole and dot repeating layers can be used as efficient photonic and plasmonic sensors.

  10. Communications

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    1. 3D Hierarchical Architectures Prepared by Single Exposure Through a Highly Durable Colloidal Phase Mask (pages 1422–1426)

      Tae Yoon Jeon, Hwan Chul Jeon, Su Yeon Lee, Tae Soup Shim, Jung-Dae Kwon, Sung-Gyu Park and Seung-Man Yang

      Version of Record online: 9 DEC 2013 | DOI: 10.1002/adma.201304317

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      Three-dimensional hierarchical architectures are fabricated using a simple, cost-effective, durable colloidal phase mask containing a colloidal monolayer embedded in a flexible polydimethylsiloxane (PDMS) membrane. These structures give rise to a photonic bandgap that can be tuned over a wide spectral range from the visible to the near-infrared regions.

    2. Stretchable Polymeric Multielectrode Array for Conformal Neural Interfacing (pages 1427–1433)

      Liang Guo, Mingming Ma, Ning Zhang, Robert Langer and Daniel G. Anderson

      Version of Record online: 22 OCT 2013 | DOI: 10.1002/adma.201304140

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      A highly stretchable neural interface of concurrent robust electrical and mechanical properties is developed with a conducting polymer film as the sole conductor for both the electrodes and the leads. This neural interface offers the benefits of conducting polymer electrodes in a demanding stretchable format, including low electrode impedance and high chargeinjection capacity, due to the large electroactive surface area of the electrode.

    3. Control of Functional Responses Via Reversible Oxygen Loss in La1-xSrxFeO3-δ Films (pages 1434–1438)

      Yujun Xie, Mark D. Scafetta, Rebecca J. Sichel-Tissot, Eun Ju Moon, Robert C. Devlin, Hanqi Wu, Alex L. Krick and Steven J. May

      Version of Record online: 27 NOV 2013 | DOI: 10.1002/adma.201304374

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      La0.3 Sr0.7 FeO3-δ films undergo dramatic changes in electronic and optical properties due to reversible oxygen loss induced by low-temperature heating. This mechanism to control the functional properties may serve as a platform for new devices or sensors in which external stimuli are used to dynamically control the composition of complex oxide heterostructures.

    4. Alignment-Free Three-Dimensional Optical Metamaterials (pages 1439–1445)

      Yang Zhao, Jinwei Shi, Liuyang Sun, Xiaoqin Li and Andrea Alù

      Version of Record online: 5 DEC 2013 | DOI: 10.1002/adma.201304379

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      Three-dimensional optical metamaterials based on multilayers typically rely on critical vertical alignment to achieve the desired functionality. Here the conditions under which three-dimensional metamaterials with different functionalities may be realized without constraints on alignment are analyzed and demonstrated experimentally. This study demonstrates that the release of alignment constraints for multilayered metamaterials is allowed, while their anomalous interaction with light is preserved.

    5. Thin Film Metal Nanocluster Light-Emitting Devices (pages 1446–1449)

      Bjoern Niesen and Barry P. Rand

      Version of Record online: 20 DEC 2013 | DOI: 10.1002/adma.201304725

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      Light-emitting devices that utilize thin films of metal nanoclusters as quantum emitters are presented. Implementing Ag as well as Au nanoclusters, the versatility of the approach is demonstrated, and it is shown that the electroluminescence measured from these devices is tunable by the choice of nanocluster. Ultimately, it is demonstrated that metal nanoclusters represent an additional option for future light-generating applications.

    6. High-Performance Electrocatalysts for Oxygen Reduction Derived from Cobalt Porphyrin-Based Conjugated Mesoporous Polymers (pages 1450–1455)

      Zhong-Shuai Wu, Long Chen, Junzhi Liu, Khaled Parvez, Haiwei Liang, Jie Shu, Hermann Sachdev, Robert Graf, Xinliang Feng and Klaus Müllen

      Version of Record online: 29 NOV 2013 | DOI: 10.1002/adma.201304147

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      A cobalt-nitrogen-doped porous carbon that exhibits a ribbon-shape morphology, high surface area, mesoporous structure, and high nitrogen and cobalt content is fabricated for high-performance self-supported oxygen reduction electrocatalytsts through template-free pyrolysis of cobalt porphyrin-based conjugated mesoporous polymer frameworks.

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      Bio-Inspired Hierarchical Polymer Fiber–Carbon Nanotube Adhesives (pages 1456–1461)

      Zhuxia Rong, Yanmin Zhou, Bingan Chen, John Robertson, Walter Federle, Stephan Hofmann, Ullrich Steiner and Pola Goldberg-Oppenheimer

      Version of Record online: 11 DEC 2013 | DOI: 10.1002/adma.201304601

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      Hierarchical pillar arrays consisting of micrometer-sized polymer setae covered by carbon nanotubes are engineered to deliver the role of spatulae, mimicking the fibrillar adhesive surfaces of geckos. These biomimetic structures conform well and achieve better attachment to rough surfaces, providing a new platform for a variety of applications.

    8. Room Temperature Formation of High-Mobility Two-Dimensional Electron Gases at Crystalline Complex Oxide Interfaces (pages 1462–1467)

      Y. Z. Chen, N. Bovet, T. Kasama, W. W. Gao, S. Yazdi, C. Ma, N. Pryds and S. Linderoth

      Version of Record online: 12 DEC 2013 | DOI: 10.1002/adma.201304634

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      Well-controlled sub-unit-cell layer-bylayer epitaxial growth of spinel alumina is achieved at room temperature on a TiO2-terminated SrTiO3 single-crystalline substrate. By tailoring the interface redox reaction, 2D electron gases with mobilities exceeding 3000 cm 2 V−1 s−1 are achieved at this novel oxide interface.

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