112 results on '"Wilfried Sigle"'
Search Results
2. Experimental evidence of a size-dependent sign change of the Seebeck coefficient of Bi nanowire arrays
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Michael Florian Peter Wagner, Anna Sarina Paulus, Wilfried Sigle, Joachim Brötz, Christina Trautmann, Kay-Obbe Voss, Friedemann Völklein, and Maria Eugenia Toimil-Molares
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Medicine ,Science - Abstract
Abstract The electrical transport in bismuth nanowires is strongly influenced by both sample geometry and crystallinity. Compared to bulk bismuth, the electrical transport in nanowires is dominated by size effects and influenced by surface states, which gain increasing relevance with increasing surface-to-volume ratios, i.e. with decreasing wire diameter. Bismuth nanowires with tailored diameter and crystallinity constitute, therefore, excellent model systems, allowing to study the interplay of the different transport phenomena. Here, we present temperature-dependent Seebeck coefficient and relative electrical resistance measurements of parallel bismuth nanowire arrays with diameters between 40 and 400 nm synthesized by pulsed electroplating in polymer templates. Both electrical resistance and Seebeck coefficient exhibit a non-monotonic temperature dependence, with the sign of the Seebeck coefficient changing from negative to positive with decreasing temperature. The observed behavior is size-dependent and is attributed to limitations of the mean free path of the charge carriers within the nanowires. The observed size-dependent Seebeck coefficient and in particular the size-dependent sign change opens a promising avenue for single-material thermocouples with p- and n-legs made from nanowires with different diameters.
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- 2023
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3. Combined spectroscopy and electrical characterization of La:BaSnO3 thin films and heterostructures
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Arnaud P. Nono Tchiomo, Emanuela Carleschi, Aletta R. E. Prinsloo, Wilfried Sigle, Peter A. van Aken, Jochen Mannhart, Prosper Ngabonziza, and Bryan P. Doyle
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Physics ,QC1-999 - Abstract
For La-doped BaSnO3 thin films grown by pulsed laser deposition, we combine chemical surface characterization and electronic transport studies to probe the evolution of electronic states in the band structure for different La-doping contents. Systematic analyses of spectroscopic data based on fitting the core electron line shapes help to unravel the composition of the surface as well as the dynamics associated with increasing doping. These dynamics are observed with a more pronounced signature in the Sn 3d core level, which exhibits an increasing asymmetry to the high binding energy side of the peak with increasing electron density. The present results expand the current understanding of the interplay between the doping concentration, electronic band structure, and transport properties of epitaxial La:BaSnO3 films.
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- 2022
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4. Ruddlesden–Popper Faults in NdNiO3 Thin Films
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Chao Yang, Yi Wang, Daniel Putzky, Wilfried Sigle, Hongguang Wang, Roberto A. Ortiz, Gennady Logvenov, Eva Benckiser, Bernhard Keimer, and Peter A. van Aken
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Ruddlesden–Popper faults ,NNO thin films ,EELS ,HAADF image ,Mathematics ,QA1-939 - Abstract
The NdNiO3 (NNO) system has attracted a considerable amount of attention owing to the discovery of superconductivity in Nd0.8Sr0.2NiO2. In rare-earth nickelates, Ruddlesden–Popper (RP) faults play a significant role in functional properties, motivating our exploration of its microstructural characteristics and the electronic structure. Here, we employed aberration-corrected scanning transmission electron microscopy and spectroscopy to study a NdNiO3 film grown by layer-by-layer molecular beam epitaxy (MBE). We found RP faults with multiple configurations in high-angle annular dark-field images. Elemental intermixing occurs at the SrTiO3–NdNiO3 interface and in the RP fault regions. Quantitative analysis of the variation in lattice constants indicates that large strains exist around the substrate–film interface. We demonstrate that the Ni valence change around RP faults is related to a strain and structure variation. This work provides insights into the microstructure and electronic-structure modifications around RP faults in nickelates.
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- 2022
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5. Dopant size effects on novel functionalities: High-temperature interfacial superconductivity
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Y. Eren Suyolcu, Yi Wang, Federico Baiutti, Ameer Al-Temimy, Giuliano Gregori, Georg Cristiani, Wilfried Sigle, Joachim Maier, Peter A. van Aken, and Gennady Logvenov
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Medicine ,Science - Abstract
Abstract Among the range of complex interactions, especially at the interfaces of epitaxial oxide systems, contributing to the occurrence of intriguing effects, a predominant role is played by the local structural parameters. In this study, oxide molecular beam epitaxy grown lanthanum cuprate-based bilayers (consisting of a metallic (M) and an insulating phase (I)), in which high-temperature superconductivity arises as a consequence of interface effects, are considered. With the aim of assessing the role of the dopant size on local crystal structure and chemistry, and on the interface functionalities, different dopants (Ca2+, Sr2+ and, Ba2+) are employed in the M-phase, and the M–I bilayers are investigated by complementary techniques, including spherical-aberration-corrected scanning transmission electron microscopy. A series of exciting outcomes are found: (i) the average out-of-plane lattice parameter of the bilayers is linearly dependent on the dopant ion size, (ii) each dopant redistributes at the interface with a characteristic diffusion length, and (iii) the superconductivity properties are highly dependent on the dopant of choice. Hence, this study highlights the profound impact of the dopant size and related interface chemistry on the functionalities of superconducting oxide systems.
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- 2017
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6. High-temperature-grown buffer layer boosts electron mobility in epitaxial La-doped BaSnO3/SrZrO3 heterostructures
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Arnaud P. Nono Tchiomo, Wolfgang Braun, Bryan P. Doyle, Wilfried Sigle, Peter van Aken, Jochen Mannhart, and Prosper Ngabonziza
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Biotechnology ,TP248.13-248.65 ,Physics ,QC1-999 - Abstract
By inserting a SrZrO3 buffer layer between the film and the substrate, we demonstrate a significant reduction of the threading dislocation density with an associated improvement of the electron mobility in La:BaSnO3 films. A room temperature mobility of 140 cm2 V−1s−1 is achieved for 25-nm-thick films without any postgrowth treatment. The density of threading dislocations is only 4.9 × 109 cm−2 for buffered films prepared on (110) TbScO3 substrates by pulsed laser deposition.
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- 2019
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7. ZnO Nanowire Networks as Photoanode Model Systems for Photoelectrochemical Applications
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Liana Movsesyan, Albert Wouter Maijenburg, Noel Goethals, Wilfried Sigle, Anne Spende, Florent Yang, Bernhard Kaiser, Wolfram Jaegermann, Sun-Young Park, Guido Mul, Christina Trautmann, and Maria Eugenia Toimil-Molares
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etched ion-track membrane ,electrodeposition ,nanowire network ,core-shell nanowires ,ZnO ,TiO2 ,photoelectrochemical applications ,water splitting ,Chemistry ,QD1-999 - Abstract
In this work, the fabrication of zinc oxide (ZnO) nanowire networks is presented. By combining ion-track technology, electrochemical deposition, and atomic layer deposition, hierarchical and self-supporting three-dimensional (3D) networks of pure ZnO- and TiO2-coated ZnO nanowires were synthesized. Analysis by means of high-resolution transmission electron microscopy revealed a highly crystalline structure of the electrodeposited ZnO wires and the anatase phase of the TiO2 coating. In photoelectrochemical measurements, the ZnO and ZnO/TiO2 nanowire networks, used as anodes, generated higher photocurrents compared to those produced by their film counterparts. The ZnO/TiO2 nanowire network exhibited the highest photocurrents. However, the protection by the TiO2 coatings against chemical corrosion still needs improvement. The one-dimensionality of the nanowires and the large electrolyte-accessible area make these 3D networks promising photoelectrodes, due to the improved transport properties of photogenerated charge carriers and faster redox reactions at the surface. Moreover, they can find further applications in e.g., sensing, catalytical, and piezoelectric devices.
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- 2018
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8. Materials News: Interfacial chemistry and atomic arrangement of ZrO2 − La2/3Sr1/3MnO3 pillar-matrix structures
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Dan Zhou, Wilfried Sigle, Eiji Okunishi, Yi Wang, Marion Kelsch, Hanns-Ulrich Habermeier, and Peter A. van Aken
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Biotechnology ,TP248.13-248.65 ,Physics ,QC1-999 - Abstract
We studied ZrO2 − La2/3Sr1/3MnO3 pillar–matrix thin films which were found to show anomalous magnetic and electron transport properties. With the application of an aberration-corrected transmission electron microscope, interfacial chemistry, and atomic-arrangement of the system, especially of the pillar–matrix interface were revealed at atomic resolution. Minor amounts of Zr were found to occupy Mn positions within the matrix. The Zr concentration reaches a minimum near the pillar–matrix interface accompanied by oxygen vacancies. La and Mn diffusion into the pillar was revealed at atomic resolution and a concomitant change of the Mn valence state was observed.
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- 2014
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9. Numerical simulations of interference effects in photon-assisted electron energy-loss spectroscopy
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Nahid Talebi, Wilfried Sigle, Ralf Vogelgesang, and Peter van Aken
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Science ,Physics ,QC1-999 - Abstract
Although the electromagnetic resonances of individual nanostructures can be studied by electron or photon interactions alone, exciting new possibilities open up through the simultaneous use of both. In photon-induced near-field electron microscopy (PINEM), for example, single nanostructures are optically excited by short, intense pulses and concurrently imaged with high spatial resolution by fast electrons, which act as negligible probes of electric fields. Controlling their relative arrival time provides access to the dynamics of the electromagnetic response in the near field by recording images of the electron energy loss (or gain) spectra. In this paper, we investigate the transition from optically dominated PINEM to conventional, electron-dominated electron energy-loss spectroscopy (EELS). During the systematic reduction of optical excitation intensity to zero, a novel electro-optical interference effect emerges. It reveals itself at those optical field strengths that lead to prominently visible constructive and destructive interference patterns of the optical and electron radiation fields which are scattered by a nanostructure. The interference patterns reported here allow one to achieve higher temporal, energy and spatial resolutions of the modal dynamics in electron microscopy.
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- 2013
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10. Thickness-Dependent Interface Polarity in Infinite-Layer Nickelate Superlattices
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Chao Yang, Roberto A. Ortiz, Yi Wang, Wilfried Sigle, Hongguang Wang, Eva Benckiser, Bernhard Keimer, and Peter A. van Aken
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Mechanical Engineering ,General Materials Science ,Bioengineering ,General Chemistry ,Condensed Matter Physics - Published
- 2023
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11. Probing Grain-boundary Structure and Electrostatic Characteristics in a SrTiO3 Bi-crystal by 4D-STEM
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Chao Yang, Yi Wang, Wilfried Sigle, and Peter A van Aken
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Instrumentation - Published
- 2022
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12. Determination of Grain-Boundary Structure and Electrostatic Characteristics in a SrTiO3 Bicrystal by Four-Dimensional Electron Microscopy
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Chao Yang, Wilfried Sigle, Peter A. van Aken, and Yi Wang
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Letter ,Materials science ,Mechanical Engineering ,Bioengineering ,Charge (physics) ,General Chemistry ,oxygen vacancy ,Condensed Matter Physics ,law.invention ,Characterization (materials science) ,electrostatic characteristics ,grain boundary ,Chemical physics ,law ,Negative charge ,Electric field ,Scanning transmission electron microscopy ,General Materials Science ,Nanometre ,Grain boundary ,Electron microscope ,4D-STEM - Abstract
The grain boundary (GB) plays a critical role in a material’s properties and device performance. Therefore, the characterization of a GB’s atomic structure and electrostatic characteristics is a matter of great importance for materials science. Here, we report on the atomic structure and electrostatic analysis of a GB in a SrTiO3 bicrystal by four-dimensional scanning transmission electron microscopy (4D-STEM). We demonstrate that the Σ5 GB is Ti-rich and poor in Sr. We investigate possible effects on the variation in the atomic electrostatic field, including oxygen vacancies, Ti-valence change, and accumulation of cations. A negative charge resulting from a space-charge zone in SrTiO3 compensates a positive charge accumulated at the GB, which is in agreement with the double-Schottky-barrier model. It demonstrates the feasibility of characterizing the electrostatic properties at the nanometer scale by 4D-STEM, which provides comprehensive insights to understanding the GB structure and its concomitant effects on the electrostatic properties.
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- 2021
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13. Tuning the Size and Shape of NanoMOFs via Templated Electrodeposition and Subsequent Electrochemical Oxidation
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Dominik Weil, Rebekka Vogt, Francesco Caddeo, A. Wouter Maijenburg, Wilfried Sigle, and M. Eugenia Toimil-Molares
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Thermogravimetric analysis ,Materials science ,Scanning electron microscope ,Nanowire ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Amorphous solid ,Membrane ,Differential scanning calorimetry ,Chemical engineering ,Transmission electron microscopy ,General Materials Science ,Gas separation ,0210 nano-technology ,ddc:600 - Abstract
ACS applied materials & interfaces 11(28), 25378 - 25387 (2019). doi:10.1021/acsami.9b04449, Published by ACS, Washington, DC
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- 2019
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14. Effects of Size Reduction on the Electrical Transport Properties of 3D Bi Nanowire Networks
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Joachim Brötz, Anna Sarina Paulus, Kay-Obbe Voss, Christina Trautmann, F. Völklein, Michael Florian Peter Wagner, Maria Eugenia Toimil-Molares, and Wilfried Sigle
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Materials science ,business.industry ,ddc:621.3 ,Size reduction ,Ion track ,Nanowire ,chemistry.chemical_element ,Thermoelectric materials ,Electronic, Optical and Magnetic Materials ,Bismuth ,621.3 ,Electrical transport ,chemistry ,Optoelectronics ,Thin film ,business - Abstract
Advanced electronic materials 0, 2001069 (2021). doi:10.1002/aelm.202001069, Published by Wiley-VCH Verlag GmbH & Co. KG, Weinheim
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- 2021
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15. Secondary-Phase-Assisted Grain Boundary Migration in CuInSe2
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Peter A. van Aken, Karsten Albe, Marc-Daniel Heinemann, Dieter Greiner, Ekin Simsek Sanli, Wilfried Sigle, Chen Li, Daniel Barragan-Yani, Helena Stange, Daniel Abou-Ras, and Roland Mainz
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Materials science ,Condensed matter physics ,General Physics and Astronomy ,01 natural sciences ,Molecular dynamics ,Phase (matter) ,0103 physical sciences ,Scanning transmission electron microscopy ,Content (measure theory) ,Grain boundary ,Density functional theory ,Grain boundary migration ,010306 general physics ,Deposition (law) - Abstract
Significant structural evolution occurs during the deposition of ${\mathrm{CuInSe}}_{2}$ solar materials when the Cu content increases. We use in situ heating in a scanning transmission electron microscope to directly observe how grain boundaries migrate during heating, causing nondefected grains to consume highly defected grains. Cu substitutes for In in the near grain boundary regions, turning them into a Cu-Se phase topotactic with the ${\mathrm{CuInSe}}_{2}$ grain interiors. Together with density functional theory and molecular dynamics calculations, we reveal how this Cu-Se phase makes the grain boundaries highly mobile.
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- 2020
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16. Correcting the linear and nonlinear distortions for atomically resolved STEM spectrum and diffraction imaging
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Kersten Hahn, Peter A. van Aken, Vesna Srot, Yi Wang, Ute Salzberger, Y. Eren Suyolcu, and Wilfried Sigle
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spectrum image ,Diffraction ,Materials science ,02 engineering and technology ,Electron ,01 natural sciences ,Article ,Optics ,Structural Biology ,0103 physical sciences ,Scanning transmission electron microscopy ,Radiology, Nuclear Medicine and imaging ,Instrumentation ,Spectrum imaging ,010302 applied physics ,Shearing (physics) ,Pixel ,business.industry ,Spectrum (functional analysis) ,STEM ,021001 nanoscience & nanotechnology ,Nonlinear system ,Computer Science::Computer Vision and Pattern Recognition ,scanning image distortion ,0210 nano-technology ,business ,4D-STEM ,mapping at high resolution - Abstract
We report a software tool for post-correcting the linear and nonlinear image distortions of atomically resolved 3D spectrum imaging as well as 4D diffraction imaging. This tool improves the interpretability of distorted scanning transmission electron microscopy spectrum/diffraction imaging data., Specimen and stage drift as well as scan distortions can lead to a mismatch between true and desired electron probe positions in scanning transmission electron microscopy (STEM) which can result in both linear and nonlinear distortions in the subsequent experimental images. This problem is intensified in STEM spectrum and diffraction imaging techniques owing to the extended dwell times (pixel exposure time) as compared to conventional STEM imaging. As a consequence, these image distortions become more severe in STEM spectrum/diffraction imaging. This becomes visible as expansion, compression and/or shearing of the crystal lattice, and can even prohibit atomic resolution and thus limits the interpretability of the results. Here, we report a software tool for post-correcting the linear and nonlinear image distortions of atomically resolved 3D spectrum imaging as well as 4D diffraction imaging. This tool improves the interpretability of distorted STEM spectrum/diffraction imaging data.
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- 2018
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17. Interfacial reactions of crystalline Ni and amorphous SiC thin films
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Zumin Wang, Wilfried Sigle, E. J. Mittemeijer, and A.-S. Keita
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010302 applied physics ,Amorphous silicon ,Auger electron spectroscopy ,Materials science ,Mechanical Engineering ,chemistry.chemical_element ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Amorphous solid ,Nickel ,chemistry.chemical_compound ,Chemical engineering ,chemistry ,X-ray photoelectron spectroscopy ,Amorphous carbon ,Mechanics of Materials ,0103 physical sciences ,Silicide ,General Materials Science ,0210 nano-technology ,High-resolution transmission electron microscopy - Abstract
The initial interfacial reactions of crystalline nickel and amorphous silicon carbide (Ni/a-SiC) thin films were investigated by means of X-ray diffraction (XRD) analysis, high-resolution transmission electron microscopy [(HR)TEM], Auger electron spectroscopy (AES) and X-ray photoelectron spectroscopy (XPS). Upon annealing at 500 °C, in the initial stage (
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- 2018
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18. High-temperature superconductivity at the lanthanum cuprate/lanthanum–strontium nickelate interface
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Giuliano Gregori, Wilfried Sigle, Georg Cristiani, Federico Baiutti, Y. E. Suyolcu, Gennady Logvenov, P. A. van Aken, Yi Wang, and Joachim Maier
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Superconductivity ,Strontium ,High-temperature superconductivity ,Materials science ,Oxide ,chemistry.chemical_element ,Ionic bonding ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Electron spectroscopy ,law.invention ,Condensed Matter::Materials Science ,chemistry.chemical_compound ,chemistry ,law ,Chemical physics ,Condensed Matter::Superconductivity ,0103 physical sciences ,Lanthanum ,General Materials Science ,Cuprate ,010306 general physics ,0210 nano-technology - Abstract
The utilization of interface effects in epitaxial systems at the nanoscale has emerged as a very powerful approach for engineering functional properties of oxides. Here we present a novel structure fabricated by a state-of-the-art oxide molecular beam epitaxy method and consisting of lanthanum cuprate and strontium (Sr)-doped lanthanum nickelate, in which interfacial high-temperature superconductivity (Tc up to 40 K) occurs at the contact between the two phases. In such a system, we are able to tune the superconducting properties simply by changing the structural parameters. By employing electron spectroscopy and microscopy combined with dedicated conductivity measurements, we show that decoupling occurs between the electronic charge carrier and the cation (Sr) concentration profiles at the interface and that a hole accumulation layer forms, which dictates the resulting superconducting properties. Such effects are rationalized in the light of a generalized space-charge theory for oxide systems that takes account of both ionic and electronic redistribution effects.
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- 2018
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19. Ion transport in nanocrystalline CaF2 films
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Robert Usiskin, Marion Kelsch, Wilfried Sigle, Peter A. van Aken, and Joachim Maier
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Materials science ,Condensed matter physics ,Annealing (metallurgy) ,Transmission electron microscopy ,General Physics and Astronomy ,Grain boundary ,Substrate (electronics) ,Conductivity ,Nanocrystalline material ,Grain size ,Amorphous solid - Abstract
This work investigates the conductivity and structure of nanocrystalline CaF2 films grown at 200 °C by thermal evaporation. The in-plane conductivity is enhanced by several orders of magnitude compared to lightly doped bulk samples of CaF2, which independently confirms the finding of a previous work [Modine et al., J. Appl. Phys. 74, 2658 (1993)]. Upon heating above 200 °C, the enhancement is partially annealed out, and the activation energy increases continuously from 0.7 to 1.0 eV, which contradicts the annealing model proposed previously. The enhancement is seen only in an ∼20-nm thick region adjacent to the substrate, but this may be because the films show substantial porosity outside this region. A 5–10 nm grain size and a high density of grain boundaries are observed by high-resolution transmission electron microscopy. A 2–4 nm interfacial amorphous layer is seen in films grown on Al2O3, but such a layer is absent on MgO and evidently not responsible for the enhanced conduction. Overall, the evidence points to grain boundaries and/or dislocations as providing fast transport pathways. These results help to reconcile previous reports of enhanced ion transport in CaF2, and they are also relevant for understanding the enhancement mechanism in CaF2-based composites and antifluorite-structured materials such as Li2O.
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- 2021
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20. Secondary-Phase-Assisted Grain Boundary Migration in CuInSe_{2}
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Chen Li, Ekin Simsek Sanli, Daniel Barragan-Yani, Helena Stange, Marc-Daniel Heinemann, Dieter Greiner, Wilfried Sigle, Roland Mainz, Karsten Albe, Daniel Abou-Ras, and Peter A. van Aken
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Transmission electron microscope - Abstract
Significant structural evolution occurs during the deposition of CuInSe2 solar materials when the Cu content increases. We use in situ heating in a scanning transmission electron microscope to directly observe how grain boundaries migrate during heating, causing nondefected grains to consume highly defected grains. Cu substitutes for In in the near grain boundary regions, turning them into a Cu-Se phase topotactic with the CuInSe2 grain interiors. Together with density functional theory and molecular dynamics calculations, we reveal how this Cu-Se phase makes the grain boundaries highly mobile.
- Published
- 2019
21. Large thermopower anisotropy in PdCoO2 thin films
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Bernhard Keimer, P. Yordanov, Pinar Kaya, R. Pentcheva, Wilfried Sigle, H.-U. Habermeier, and Markus E. Gruner
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Thermoelectric transport ,Materials science ,Physics and Astronomy (miscellaneous) ,Condensed matter physics ,Lattice (group) ,02 engineering and technology ,engineering.material ,Physik (inkl. Astronomie) ,021001 nanoscience & nanotechnology ,Thermoelectric materials ,01 natural sciences ,Delafossite ,Seebeck coefficient ,0103 physical sciences ,Thermoelectric effect ,engineering ,General Materials Science ,Thin film ,010306 general physics ,0210 nano-technology ,Anisotropy - Abstract
The delafossite compound PdCoO${}_{2}$ is composed of highly conducting Pd and insulating CoO${}_{2}$ layers. As a consequence of this lattice architecture, the thermopower of PdCoO${}_{2}$ was predicted to be extremely anisotropic. Because of the limited size of available single crystals, however, these predictions had not been tested experimentally. The authors of this paper show that the electric and thermoelectric transport parameters of PdCoO${}_{2}$ along the main crystallographic directions can be determined from measurements on thin films grown on substrates with different offcut angles. The method is applicable to a wide range of thermoelectric materials. The experimental results confirm the predicted thermopower anisotropy of PdCoO${}_{2}$ and thus provide interesting perspectives for thermoelectric device applications.
- Published
- 2019
22. Silver nanowires with optimized silica coating as versatile plasmonic resonators
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Christoph Koch, Yan Lu, Matthias Ballauff, Günter Kewes, Peter A. van Aken, Wilfried Sigle, Oliver Benson, Zdravko Kochovski, Yuhang Zhao, and Martin Rothe
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0301 basic medicine ,Nanostructure ,Materials science ,Nanowire ,Nanoparticle ,lcsh:Medicine ,FOS: Physical sciences ,Nanotechnology ,Substrate (electronics) ,Dielectric ,engineering.material ,Article ,03 medical and health sciences ,0302 clinical medicine ,Coating ,lcsh:Science ,Plasmon ,Multidisciplinary ,lcsh:R ,030104 developmental biology ,ddc:540 ,engineering ,Institut für Chemie ,lcsh:Q ,Inhouse research on structure dynamics and function of matter ,Layer (electronics) ,030217 neurology & neurosurgery ,Physics - Optics ,Optics (physics.optics) - Abstract
Metal nanoparticles are the most frequently used nanostructures in plasmonics. However, besides nanoparticles, metal nanowires feature several advantages for applications. Their elongation offers a larger interaction volume, their resonances can reach higher quality factors, and their mode structure provides better coupling into integrated hybrid dielectric-plasmonic circuits. It is crucial though, to control the distance of the wire to a supporting substrate, to another metal layer or to active materials with sub-nanometer precision. A dielectric coating can be utilized for distance control, but it must not degrade the plasmonic properties. In this paper, we introduce a controlled synthesis and coating approach for silver nanowires to fulfill these demands. We synthesize and characterize silver nanowires of around 70 nm in diameter. These nanowires are coated with nm-sized silica shells using a modified Stöber method to achieve a homogeneous and smooth surface quality. We use transmission electron microscopy, dark-field microscopy and electron-energy loss spectroscopy to study morphology and plasmonic resonances of individual nanowires and quantify the influence of the silica coating. Thorough numerical simulations support the experimental findings showing that the coating does not deteriorate the plasmonic properties and thus introduce silver nanowires as usable building blocks for integrated hybrid plasmonic systems.
- Published
- 2018
23. Electron microscopy of polyoxometalate ions on graphene by electrospray ion beam deposition
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Suman Sen, Sabine Abb, Nilesh Vats, Klaus Kern, Marko Burghard, P. A. van Aken, Stephan Rauschenbach, Michael Dürr, André Portz, and Wilfried Sigle
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Materials science ,Graphene ,Nanotechnology ,02 engineering and technology ,Carbon nanotube ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,law.invention ,Characterization (materials science) ,Ion beam deposition ,law ,Transmission electron microscopy ,Polyoxometalate ,Deposition (phase transition) ,Molecule ,General Materials Science ,0210 nano-technology - Abstract
Aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM) has enabled atomically resolved imaging of molecules adsorbed on low-dimensional materials like carbon nanotubes, graphene oxide and few-layer-graphene. However, conventional methods for depositing molecules onto such supports lack selectivity and specificity. Here, we describe the chemically selective preparation and deposition of molecules-like polyoxometalate (POM) anions [PW12O40]3− using electrospray ion-beam deposition (ES-IBD) along with high-resolution TEM imaging. This approach provides access to sub-monolayer coatings of intact molecules on freestanding graphene, which enables their atomically resolved ex situ characterization by low-voltage AC-HRTEM. The capability to tune the deposition parameters in either soft or reactive landing mode, combined with the well-defined high-vacuum deposition conditions, renders the ES-IBD based method advantageous over alternative methods such as drop-casting. Furthermore, it might be expanded towards depositing and imaging large and nonvolatile molecules with complex structures.
- Published
- 2018
24. Sample tilt effects on atom column position determination in ABF–STEM imaging
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Dan Zhou, Wilfried Sigle, Florian F. Krause, Andreas Rosenauer, Peter A. van Aken, and Knut Müller-Caspary
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Materials science ,Atom position determination ,Phase (waves) ,02 engineering and technology ,Electron ,010402 general chemistry ,01 natural sciences ,Crystal ,Optics ,0103 physical sciences ,Atom ,Image simulation ,Instrumentation ,010302 applied physics ,Physics ,Sample tilt ,business.industry ,Zone axis ,Annular bright-field imaging ,021001 nanoscience & nanotechnology ,Crystallographic defect ,Atomic and Molecular Physics, and Optics ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,Tilt (optics) ,Cathode ray ,Atomic physics ,0210 nano-technology ,business - Abstract
The determination of atom positions from atomically resolved transmission electron micrographs is fundamental for the analysis of crystal defects and strain. In recent years annular bright-field (ABF) imaging has become a popular imaging technique owing to its ability to map both light and heavy elements. Contrast formation in ABF is partially governed by the phase of the electron wave, which renders the technique more sensitive to the tilt of the electron beam with respect to the crystal zone axis than high-angle annular dark-field imaging. Here we show this sensitivity experimentally and use image simulations to quantify this effect. This is essential for error estimation in future quantitative ABF studies.
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- 2016
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25. ZnO Nanowire Networks as Photoanode Model Systems for Photoelectrochemical Applications
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Guido Mul, Noel Goethals, Florent Yang, Bernhard Kaiser, Albert Wouter Maijenburg, Liana Movsesyan, Anne Spende, Maria Eugenia Toimil-Molares, Sun-Young Park, Wilfried Sigle, Christina Trautmann, Wolfram Jaegermann, and Photocatalytic Synthesis
- Subjects
Anatase ,Fabrication ,Materials science ,General Chemical Engineering ,Nanowire ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,water splitting ,Article ,nanowire network ,lcsh:Chemistry ,Atomic layer deposition ,TiO ,TiO2 ,etched ion-track membrane ,General Materials Science ,business.industry ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Anode ,lcsh:QD1-999 ,Transmission electron microscopy ,photoelectrochemical applications ,ddc:540 ,electrodeposition ,ZnO ,Water splitting ,Optoelectronics ,Charge carrier ,0210 nano-technology ,business ,core-shell nanowires - Abstract
Nanomaterials 8(9), 693 - (2018). doi:10.3390/nano8090693, Published by MDPI, Basel
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- 2018
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26. Evidence for Cu2–xSe platelets at grain boundaries and within grains in Cu(In,Ga)Se2 thin films
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P. A. van Aken, E. Simsek Sanli, Wilfried Sigle, Roland Mainz, Daniel Abou-Ras, Quentin M. Ramasse, and A. Weber
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Methods and concepts for material development ,Materials science ,Physics and Astronomy (miscellaneous) ,Recrystallization (metallurgy) ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Copper indium gallium selenide solar cells ,Grain growth ,Crystallography ,Vacuum deposition ,0103 physical sciences ,Scanning transmission electron microscopy ,Grain boundary ,Crystallite ,Thin film ,010306 general physics ,0210 nano-technology - Abstract
Cu(In,Ga)Se₂ (CIGS)-based solar cells reach high power-conversion efficiencies of above 22%. In this work, a three-stage co-evaporation method was used for their fabrication. During the growth stages, the stoichiometry of the absorbers changes from Cu-poor ([Cu]/([In] + [Ga]) 1) and finally becomes Cu-poor again when the growth process is completed. It is known that, according to the Cu-In-Ga-Se phase diagram, a Cu-rich growth leads to the presence of Cu₂–ₓSe (x = 0–0.25), which is assumed to assist in recrystallization, grain growth, and defect annihilation in the CIGS layer. So far, Cu₂–ₓSe precipitates with spatial extensions on the order of 10–100 nm have been detected only in Cu-rich CIGS layers. In the present work, we report Cu₂–ₓSe platelets with widths of only a few atomic planes at grain boundaries and as inclusions within grains in a polycrystalline, Cu-poor CIGS layer, as evidenced by high-resolution scanning transmission electron microscopy (STEM). The chemistry of the Cu–Se secondary phase was analyzed by electron energy-loss spectroscopy, and STEM image simulation confirmed the identification of the detected phase. These results represent additional experimental evidence for the proposed topotactical growth model for Cu–Se–assisted CIGS thin-film formation under Cu-rich conditions.
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- 2017
27. Towards atomically resolved EELS elemental and fine structure mapping via multi-frame and energy-offset correction spectroscopy
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Peter A. van Aken, Wilfried Sigle, Kersten Hahn, Yi Wang, Michael R. S. Huang, and Ute Salzberger
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010302 applied physics ,Offset (computer science) ,Chemistry ,business.industry ,Superlattice ,Nanotechnology ,02 engineering and technology ,Electron ,021001 nanoscience & nanotechnology ,01 natural sciences ,Atomic and Molecular Physics, and Optics ,Spectral line ,Electronic, Optical and Magnetic Materials ,Multi frame ,Structure mapping ,0103 physical sciences ,Scanning transmission electron microscopy ,Optoelectronics ,0210 nano-technology ,Spectroscopy ,business ,Instrumentation - Abstract
Electron energy-loss spectroscopy and energy-dispersive X-ray spectroscopy are two of the most common means for chemical analysis in the scanning transmission electron microscope. The marked progress of the instrumentation hardware has made chemical analysis at atomic resolution readily possible nowadays. However, the acquisition and interpretation of atomically resolved spectra can still be problematic due to image distortions and poor signal-to-noise ratio of the spectra, especially for investigation of energy-loss near-edge fine structures. By combining multi-frame spectrum imaging and automatic energy-offset correction, we developed a spectrum imaging technique implemented into customized DigitalMicrograph scripts for suppressing image distortions and improving the signal-to-noise ratio. With practical examples, i.e. SrTiO 3 bulk material and Sr-doped La 2 CuO 4 superlattices, we demonstrate the improvement of elemental mapping and the EELS spectrum quality, which opens up new possibilities for atomically resolved EELS fine structure mapping.
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- 2017
28. Dopant size effects on novel functionalities: High-temperature interfacial superconductivity
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Wilfried Sigle, Yi Wang, G. Logvenov, Giuliano Gregori, Peter A. van Aken, Joachim Maier, Federico Baiutti, Ameer Al-Temimy, Georg Cristiani, and Y. Eren Suyolcu
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Materials science ,Science ,Oxide ,02 engineering and technology ,01 natural sciences ,Article ,chemistry.chemical_compound ,Condensed Matter::Materials Science ,Lattice constant ,Phase (matter) ,Condensed Matter::Superconductivity ,0103 physical sciences ,Scanning transmission electron microscopy ,Cuprate ,010306 general physics ,Superconductivity ,Multidisciplinary ,Dopant ,021001 nanoscience & nanotechnology ,chemistry ,Chemical physics ,Medicine ,0210 nano-technology ,Molecular beam epitaxy - Abstract
Among the range of complex interactions, especially at the interfaces of epitaxial oxide systems, contributing to the occurrence of intriguing effects, a predominant role is played by the local structural parameters. In this study, oxide molecular beam epitaxy grown lanthanum cuprate-based bilayers (consisting of a metallic (M) and an insulating phase (I)), in which high-temperature superconductivity arises as a consequence of interface effects, are considered. With the aim of assessing the role of the dopant size on local crystal structure and chemistry, and on the interface functionalities, different dopants (Ca2+, Sr2+ and, Ba2+) are employed in the M-phase, and the M–I bilayers are investigated by complementary techniques, including spherical-aberration-corrected scanning transmission electron microscopy. A series of exciting outcomes are found: (i) the average out-of-plane lattice parameter of the bilayers is linearly dependent on the dopant ion size, (ii) each dopant redistributes at the interface with a characteristic diffusion length, and (iii) the superconductivity properties are highly dependent on the dopant of choice. Hence, this study highlights the profound impact of the dopant size and related interface chemistry on the functionalities of superconducting oxide systems.
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- 2017
29. Atomically Resolved EELS Elemental and Fine Structure Mapping via Multi-Frame and Energy-Offset Correction Acquisition
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Kersten Hahn, Ute Salzberger, Wilfried Sigle, Peter A. van Aken, Michael R. S. Huang, and Yi Wang
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010302 applied physics ,Materials science ,Offset (computer science) ,business.industry ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Multi frame ,Optics ,Structure mapping ,0103 physical sciences ,0210 nano-technology ,business ,Instrumentation - Published
- 2018
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30. In-situ observations of recrystallization in CuInSe2 solar cells via STEM
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Helena Strange, Roland Mainz, Marc-Daniel Heinemann, Daniel Abou-Ras, Wilfried Sigle, Peter A. van Aken, Chen Li, Ekin Simsek Sanli, and Dieter Greiner Schäfer
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In situ ,Materials science ,0103 physical sciences ,Metallurgy ,Recrystallization (metallurgy) ,02 engineering and technology ,021001 nanoscience & nanotechnology ,010306 general physics ,0210 nano-technology ,01 natural sciences ,Instrumentation - Published
- 2018
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31. STEM SI Warp: A Tool for Correcting the Linear and Nonlinear Distortions for Atomically Resolved STEM Spectrum and Diffraction Imaging
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Kersten Hahn, Ute Salzberger, Wilfried Sigle, Peter A. van Aken, Yi Wang, Vesna Srot, and Y. Eren Suyolcu
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010302 applied physics ,Diffraction ,Materials science ,business.industry ,Spectrum (functional analysis) ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Nonlinear system ,Optics ,0103 physical sciences ,0210 nano-technology ,business ,Instrumentation - Published
- 2018
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32. Probing Jahn-Teller Distortions at Superconducting La2CuO4 Interfaces
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Wilfried Sigle, Joachim Maier, Yi Wang, Federico Baiutti, Georg Cristiani, Gennady Logvenov, Peter A. van Aken, and Y. Eren Suyolcu
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0301 basic medicine ,Superconductivity ,03 medical and health sciences ,030104 developmental biology ,Materials science ,Condensed matter physics ,Jahn–Teller effect ,02 engineering and technology ,021001 nanoscience & nanotechnology ,0210 nano-technology ,Instrumentation - Published
- 2018
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33. Comparative study of LaNiO$_3$/LaAlO$_3$ heterostructures grown by pulsed laser deposition and oxide molecular beam epitaxy
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Georg Christiani, G. Logvenov, A. F. Mark, Eva Benckiser, H.-U. Habermeier, Wilfried Sigle, Bernhard Keimer, Friederike Wrobel, and P. A. van Aken
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Materials science ,Physics and Astronomy (miscellaneous) ,Band gap ,Superlattice ,Oxide ,FOS: Physical sciences ,Nanotechnology ,02 engineering and technology ,01 natural sciences ,Pulsed laser deposition ,Condensed Matter - Strongly Correlated Electrons ,chemistry.chemical_compound ,0103 physical sciences ,010306 general physics ,Condensed Matter - Materials Science ,Strongly Correlated Electrons (cond-mat.str-el) ,business.industry ,Materials Science (cond-mat.mtrl-sci) ,Heterojunction ,021001 nanoscience & nanotechnology ,Microstructure ,chemistry ,Transmission electron microscopy ,Optoelectronics ,0210 nano-technology ,business ,Molecular beam epitaxy - Abstract
Variations in growth conditions associated with different deposition techniques can greatly affect the phase stability and defect structure of complex oxide heterostructures. We synthesized superlattices of the paramagnetic metal LaNiO3 and the large band gap insulator LaAlO3 by atomic layer-by-layer molecular beam epitaxy (MBE) and pulsed laser deposition (PLD) and compared their crystallinity, microstructure as revealed by high-resolution transmission electron microscopy images and resistivity. The MBE samples show a higher density of stacking faults, but smoother interfaces and generally higher electrical conductivity. Our study identifies the opportunities and challenges of MBE and PLD growth and serves as a general guide for the choice of deposition technique for perovskite oxides., Comment: APL in press
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- 2017
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34. Structural and Chemical Investigations of Superconducting Lanthanum Cuprate Bilayer Interfaces
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Y. Eren Suyolcu, Yi Wang, Wilfried Sigle, Georg Cristiani, Gennady Logvenov, and Peter A. van Aken
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- 2016
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35. Investigation of Plasmonic Modes of Gold Tapers by EELS
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Surong Guo, Nahid Talebi, Wilfried Sigle, Ralf Vogelgesang, Martin Esmann, Simon F. Becker, Christoph Lienau, and Peter van Aken
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- 2016
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36. Precision and application of atom location in HAADF and ABF
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Yi Wang, Dan Zhou, Wilfried Sigle, Y. Eren Suyolcu, Knut Müller-Caspary, Florian F Krause, Andreas Rosenauer, and Peter van Aken
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- 2016
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37. Atomic-scale investigation of interface phenomena in two-dimensionally Sr-doped La2CuO4 and La2CuO4/ La2-xSrxNiO4 superlattices
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Yi Wang, Y. Eren Suyolcu, Wilfried Sigle, Ute Salzberger, Federico Baiutti, Giuliano Gregori, Georg Cristiani, Gennady Logvenov, Joachim Maier, and Peter van Aken
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- 2016
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38. Influence of Substrate Temperature and Dopant Distribution at Two-Dimensionally Doped Superconducting La2CuO4 Interfaces
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Federico Baiutti, Wilfried Sigle, Peter A. van Aken, Giuliano Gregori, Joachim Maier, Georg Cristiani, Gennady Logvenov, Y. Eren Suyolcu, and Yi Wang
- Subjects
0301 basic medicine ,Superconductivity ,Materials science ,Dopant ,business.industry ,Doping ,02 engineering and technology ,Substrate (electronics) ,021001 nanoscience & nanotechnology ,03 medical and health sciences ,030104 developmental biology ,Optoelectronics ,0210 nano-technology ,business ,Instrumentation - Published
- 2017
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39. Interaction between Relativistic Electrons and Mesoscopic Plasmonic Tapers
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Martin Esmann, Christoph Lienau, Nahid Talebi, Wilfried Sigle, Peter A. van Aken, Mathieu Kociak, Alfredo Campos, Ralf Vogelgesang, Simon F. Becker, and Surong Guo
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Physics ,0209 industrial biotechnology ,Mesoscopic physics ,020901 industrial engineering & automation ,Condensed matter physics ,02 engineering and technology ,Electron ,021001 nanoscience & nanotechnology ,0210 nano-technology ,Instrumentation ,Plasmon - Published
- 2017
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40. STEM SI Warp: a Digital Micrograph script tool for warping the image distortions of atomically resolved spectrum image
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Ute Salzberger, Wilfried Sigle, Peter A. van Aken, Yi Wang, and Vesna Srot
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010302 applied physics ,Materials science ,Micrograph ,business.industry ,Spectrum (functional analysis) ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Image (mathematics) ,Optics ,0103 physical sciences ,Image warping ,0210 nano-technology ,business ,Instrumentation - Published
- 2017
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41. Measuring the Cation and Oxygen Atomic Column Displacement at Picometer Precision
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Yi Wang, Benjamin Berkels, Peter A. van Aken, Lewys Jones, and Wilfried Sigle
- Subjects
010302 applied physics ,Chemistry ,Analytical chemistry ,Picometre ,chemistry.chemical_element ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Oxygen ,Column (database) ,0103 physical sciences ,Displacement (orthopedic surgery) ,0210 nano-technology ,Instrumentation - Published
- 2017
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42. Grain-boundary plane orientation dependence of electrical barriers at Σ5 boundaries in SrTiO3
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Yoon Ho Cho, Doh-Yeon Kim, Peter A. van Aken, Sung Bo Lee, Jong Heun Lee, Wilfried Sigle, and Fritz Phillipp
- Subjects
Materials science ,Polymers and Plastics ,Condensed matter physics ,Annealing (metallurgy) ,Electron energy loss spectroscopy ,Metals and Alloys ,Electron ,Microstructure ,Electron spectroscopy ,Electronic, Optical and Magnetic Materials ,Crystallography ,Transmission electron microscopy ,Ceramics and Composites ,Grain boundary ,Spectroscopy - Abstract
Dependence of the electrical properties on grain-boundary plane orientation is examined by a combination of high-resolution transmission electron microscopy, impedance spectroscopy, and electron energy-loss spectrometry using two kinds of SrTiO3 Σ5 ([1 0 0]/36.8°) bicrystalline grain boundaries: symmetric (3 1 0) (18.4°/18.4°) and asymmetric (8.4°/28.4°). While the symmetric grain boundary is observed to be straight with the symmetric (3 1 0)//(3 1 0) plane orientation, the asymmetric grain boundary is faceted into symmetric (3 1 0)//(3 1 0) and (2 1 0)//(2 1 0), and asymmetric (1 0 0)//(4 3 0). Grain-boundary impedance is observed only in the asymmetric grain boundary, and the electron energy-loss spectrometry quantification indicates that the asymmetric (1 0 0)//(4 3 0) facets are more oxygen-deficient than the symmetric ones. The results suggest that the asymmetric (1 0 0)//(4 3 0) facets are the most resistive among the three different facets.
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- 2008
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43. Fabrication of radial superlattices based on different hybrid materials
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Andrey Chuvilin, Wilfried Sigle, Ute Zschieschang, Christoph Deneke, Jürgen Thomas, Ronny Engelhard, Oliver G. Schmidt, Hagen Klauk, and Joachim Schumann
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Fabrication ,Materials science ,business.industry ,Superlattice ,Nanotechnology ,Heterojunction ,Condensed Matter::Mesoscopic Systems and Quantum Hall Effect ,Condensed Matter Physics ,Epitaxy ,Condensed Matter::Materials Science ,Semiconductor ,Planar ,Optoelectronics ,business ,Hybrid material ,Layer (electronics) - Abstract
The fabrication of radial superlattices is demonstrated for three different hybrid material systems. Inherently strained pseudomorphic InGaAs/Fe3Si bilayers are rolled-up to produce radial semiconductor/magnetic heterostructures. Apart from this epitaxially based material system, radial InAlGaAs/GaAs/Cr superlattices are investigated as an example for periodic semiconductor/metallic multilayers. Finally, rolled-up InGaAs/GaAs/1-hexadecanethiol layers are studied as a new class of semiconductor/organic short-period superlattices. The radial superlattices are examined structurally, and particular attention is paid to the interfaces of the periodic hybrid heterostructures. These investigations reveal that, except for the semiconductor/organic hybrid material system, always a new interface layer forms, modifying the initial rolled-up layer system. The study demonstrates the potential to fabricate periodic layer systems from pure single-crystalline material, single-crystalline/poly-crystalline material as well as single-crystalline/non-crystalline material, which cannot be realized by any planar growth techniques. (© 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)
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- 2008
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44. Elemental redistributions at structural defects in Cu In,Ga Se2 thin films for solar cells
- Author
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Hans-Joachim Kleebe, P. A. van Aken, A. Weber, Quentin M. Ramasse, Daniel Abou-Ras, Wilfried Sigle, E. Simsek Sanli, and Roland Mainz
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010302 applied physics ,Methods and concepts for material development ,Microstructural evolution ,Materials science ,General Physics and Astronomy ,02 engineering and technology ,Electron ,021001 nanoscience & nanotechnology ,01 natural sciences ,Crystallography ,Vacuum deposition ,0103 physical sciences ,Scanning transmission electron microscopy ,Grain boundary ,Dislocation ,Thin film ,0210 nano-technology ,Spectroscopy - Abstract
The microstructural evolution of Cu In,Ga Se2 absorber layers during a three stage type coevaporation process was studied to elucidate the effect of a Cu rich stage on the formation of extended structural defects. Defect densities for two Cu poor samples, one interrupted before and one after this crucial Cu rich composition stage, were investigated by scanning transmission electron microscopy STEM imaging. The structure and chemical nature of individual defects were investigated by aberration corrected high resolution STEM in combination with electron energy loss spectroscopy on the atomic scale. In spite of the different defect densities between the two samples, most of the individual defects exhibited similar chemistry. In particular, the elemental distributions ofatomic columns at 112 twin planes, which are very frequent in Cu In,Ga Se2 thin films, were found to be the same as in the defect free grain interiors. In contrast, within grain boundaries, dislocation cores, and other structurally more complex defects, elemental redistributions of Cu and In were observed. VC 2016 Author s . All article content, except where otherwise noted, is licensed under aCreative Commons Attribution CC BY license http creativecommons.org licenses by 4.0
- Published
- 2016
45. Unexpected plasticity of potassium niobate during compression between room temperature and 900 °C
- Author
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Wilfried Sigle, A. F. Mark, Miguel Castillo-Rodríguez, German Research Foundation, Consejo Superior de Investigaciones Científicas (España), and European Commission
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Potassium niobate ,Materials science ,Dislocations ,KNbO3 ,02 engineering and technology ,Slip (materials science) ,Plasticity ,Domain walls ,01 natural sciences ,law.invention ,chemistry.chemical_compound ,Brittleness ,law ,0103 physical sciences ,Materials Chemistry ,Electron microscopy ,Intermediate temperature ,Composite material ,010302 applied physics ,Mechanical behaviour ,021001 nanoscience & nanotechnology ,Cracking ,Crystallography ,chemistry ,Ceramics and Composites ,Electron microscope ,Dislocation ,0210 nano-technology - Abstract
Single crystals of potassium niobate were compressed over a range of temperatures (21 °C to 900 °C) and examined using electron microscopy. The material did not behave in a brittle manner; samples sustained up to 3.7% strain. There was a trend of decreasing strength with increasing temperature, with a (superimposed) increase between 300 °C and 500 °C. Characterization revealed slip lines consistent with slip on {110} planes, domain activity and cracking. Dislocations consistent with the {110} slip system were observed in all specimens, while dislocations most likely on the {100} system were also observed in specimens compressed at 900 °C. Domain walls were observed in large numbers only in specimens tested between 300 °C and 500 °C. It is proposed that the shape of the strength-temperature curve results from the combination of contributions from dislocation slip systems and mobility and a strong effect of domain walls only acting in the intermediate temperature range., This work was supported in part by DFG Project MR 22/4-2. M. C.-R. would like to acknowledge funding from a JAE/DOC contract awarded by the Spanish Consejo Superior de Investigaciones Cientificas (CSIC), co-financed by the European Social Fund.
- Published
- 2016
46. Comparative studies of microstructure and impedance of small-angle symmetrical and asymmetrical grain boundaries in SrTiO3
- Author
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Manfred Rühle, Wilfried Sigle, Zaoli Zhang, Joachim Maier, Roger A. De Souza, and Wolfgang Kurtz
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Materials science ,Polymers and Plastics ,Condensed matter physics ,Misorientation ,Metals and Alloys ,Microstructure ,Electronic, Optical and Magnetic Materials ,Crystal ,Condensed Matter::Materials Science ,Crystallography ,Transmission electron microscopy ,Ceramics and Composites ,Grain boundary ,Dislocation ,High-resolution transmission electron microscopy ,Grain boundary strengthening - Abstract
Several low-angle symmetrical [0 0 1]-tilt grain boundaries and an asymmetrical grain boundary with both tilt and twist components were examined by high-resolution transmission electron microscopy, conventional transmission electron microscopy, and impedance spectroscopy. The symmetrical tilt grain boundaries consist of isolated dislocation cores and the Burgers vectors are translation vectors of the crystal. Strain analysis shows that the strain fields around the dislocation cores overlap with increasing misorientation angle. The a.c. impedance response of the low-angle grain boundaries reveals a marked blocking effect for charge transport across the low-angle symmetrical grain boundaries, which increases with increasing misorientation angle. In the case of the mixed asymmetrical grain boundary, however, the blocking effect is low despite the large misorientation. The resistance and electrical potential of this grain boundary were calculated and compared with those obtained from the symmetrical grain boundaries. A relationship between microstructure and macroscopic electrical property can approximately be arrived by considering anion vacancies to be preferentially situated in highly distorted regions such as dislocation cores.
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- 2005
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47. In situ high-resolution transmission electron microscopy of dislocation formation and dynamics during the crystallization of amorphous SrTiO3
- Author
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D. Brunner, Fritz Phillipp, Wilfried Sigle, and Sung Bo Lee
- Subjects
Materials science ,Polymers and Plastics ,Condensed matter physics ,Annealing (metallurgy) ,Metals and Alloys ,Electronic, Optical and Magnetic Materials ,Amorphous solid ,Crystallography ,Transmission electron microscopy ,Ceramics and Composites ,Partial dislocations ,Grain boundary ,Dislocation ,High-resolution transmission electron microscopy ,Grain boundary strengthening - Abstract
In situ high-resolution TEM imaging of an ion-milled SrTiO3 sample during annealing at 925 and 940 °C is reported. Regions that were amorphized during the ion-milling at room temperature are observed to crystallize, forming low-angle grain boundaries. At the grain boundaries, perfect a〈0 0 1〉 dislocations and two climb-dissociated a/2〈0 1 1〉 dislocations were observed. The experimental observations also include dynamic dislocation phenomena, such as glide, climb, and annihilation. Interestingly, the separation of the two a/2〈0 1 1〉 partial dislocations in the low-angle grain boundaries is not constant, but temporarily fluctuates around a mean value of 2 nm.
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- 2005
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48. Microstructural studies on the reoxidation behavior of Nb-doped SrTiO3 ceramics
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Jürgen Fleig, B. Rahmati, Joachim Maier, Wilfried Sigle, Manfred Rühle, and E. Bischoff
- Subjects
Oxide ceramics ,Crystallography ,Nb doped ,Materials science ,Materials Chemistry ,Ceramics and Composites ,Charge compensation - Abstract
Donor-doped SrTiO3 ceramics have found application in sensors, varistors, grain boundary layer capacitors and catalysts. This wide range of applications is closely related to the defect chemistry of SrTiO3 and the fact that the properties can be strongly changed by varying the processing parameters. Oxidation of an initially reduced donor-doped SrTiO3 ceramics, for example, leads to a strongly enhanced resistivity, which is generally assumed to result from the formation of cation vacancies. This formation of cation vacancies, however, raises the question of the whereabout of the expelled Sr-ions. In this contribution, the structural and chemical phenomena observed after high temperature oxidation (at 1200°C for 30 hours) of 5 at.% Nb-doped polycrystalline SrTiO3 are reported. This reoxidation procedure leads to the formation of Sr-rich islands on the surface. These islands exhibit characteristic shapes, areal densities, and sizes, that depend on the surface orientation of the underlying grain. A correlation between grain orientation (determined by orientation imaging microscopy) and tendency towards island formation was found. The structure and the composition of the islands were investigated by transmission electron microscopy and significant differences were observed for different islands. The bulk interior was also investigated after reoxidation. Sr-rich secondary phases were found at the triple grain junctions and could be identified as a Ruddlesden-Popper phase. Moreover, surprising compositional gradients including Sr enrichment were observed in the grain interior beneath the surface. The results are discussed in terms of the defect chemistry of SrTiO3. Nb-dotiertes (5 At.%), polycrystallines SrTiO3, das in einer reduzierenden Atmosphare gesintert wurde, zeigt bei weiterer Temperaturbehandlung bei 1200°C unter Sauerstoffatmosphare (Reoxidation) erhebliche strukturelle und chemische Veranderungen. Diese erfolgen sowohl an der Oberflache, in den oberflachennahen Kornern und an den Korngrenzen. Auf der polierten Oberflache einer reduzierten, polykristallinen Probe bilden sich nach 30-stundiger Oxidation „Inseln“ mikrokristalliner Grose. Form, Haufungsdichte und laterale Anordnung der Inseln zeigen dabei eine charakteristische Abhangigkeit von der Orientierung der Oberflache. Mit Hilfe von OIM-Messungen konnten drei Klassen von Oberflachenorientierungen unterschieden werden, die sich hinsichtlich der Inselbildung signifikant unterscheiden: (111)-, (122)- und (112)-Oberflachen zeigen eine hohe Inseldichte. (001)-, (013)- und (114)-Oberflachen zeigen eine geringe Inseldichte. (011)-, (133)- und (012)-Oberflachen zeigen eine mittlere Inseldichte. Da die Haufungsdichte der Inseln als Mas fur die Oxidationsneigung der Oberflachen gelten kann, zeigt eine (111)-Oberflache die hochste, eine (001)-Oberflache die niedrigste und eine (011)-Oberflache eine mittlere Oxidationsneigung. Struktur und Zusammensetzung der Inseln unterscheiden sich in Abhangigkeit von der Oberflachenorientierung in signifikanter Weise. Dies wurde fur je eine Insel auf der (023)- bzw. (012)-Oberflache nachgewiesen. Die untersuchte Insel auf der (023)-Oberflache zeigte bei einer Hohe von 250 nm ein mit der Volumenphase identisches Elektronenbeugungsbild (mit einer hoheren Intensitat der 100 Super-Reflexe). Dies deutet darauf hin, dass die Insel eine Perowskit-Struktur besitzt. Die chemische Analyse mit Hilfe von XEDS-Messungen zeigen, dass die stochiometrische Zusammensetzung der Insel nahe der Grenzflache derjenigen des SrTiO3 Volumens entspricht. Die Zusammensetzung andert sich kontinuerlich in Wachstumsrichtung der Insel und wird dabei zunehmend Sr(2+)-reicher auf Kosten der Ti(4+)-Ionen. Die Perowskit-Struktur der Insel bleibt jedoch erhalten. Es ist anzunehmen, dass die Ti(4+)-Ionen in Wachstumsrichtung allmahlich durch Sr(2+)-Ionen in Form von Defekten ersetzt werden. Dies entspricht einer strukturellen und chemischen Veranderung der (023)-Insel in Wachstumsrichtung von SrTiO3 zu Sr2O2 durch Bildung von Sr(1)(Ti(1-x)Sr(x))O(3-x) (x wachst in Wachstumsrichtung). In diesem Modell wurden Sauerstoffleerstellen fur den Ladungsausgleich der -Defekte sorgen. Dagegen zeigt die untersuchte 900 nm hohe Insel auf der (012)-Oberflache ein vom SrTiO3-Volumen deutlich verschiedenes Elektronenbeugungsbild. Die gemessenen Gitterebenenabstande in der Insel stimmen gut mit den in der Literatur genannten Werten fur SrO uberein. Auch die XEDS-Analysen zeigen lediglich das Vorhandensein von Sr(2+)-Ionen in der Insel. Beides legt nahe, dass diese Insel aus SrO besteht mit der SrO-(260)-Ebene als Grenzflache zu SrTiO3. Das Wachstum der SrO-Inseln auf der SrTiO3-(012)-Oberflache resultiert in einer Gitterfehlpassung von 4% in [210]SrTiO3-Richtung beziehungsweise ~30% in [001]SrTiO3-Richtung der Grenzflache. Nach der Reoxidation bildet sich in der Nahe der Oberflache eine optisch transparente Schicht, deren Dicke etwa 50-70 mikrometer betragt. In dieser Schicht last sich eine ausgepragte Inhomogenitat der Kationen nachweisen. In der Nahe der Oberflache findet eine Anreicherung von Sr(2+)-Ionen statt. Anderseits liegt im tieferen Bereich der reoxidierten Schicht ein Ti(4+)-Uberschuss vor. Hinsichtlich Nb(5+) -Ionen lassen sich keine signifikante Konzentrationsunterschiede in der Oxidationsschicht nachweisen. Der starke Gradient des chemischen Potentials des Sauerstoffs zwischen Oberflache und Probeninneren wirkt jedoch als treibende Kraft fur eine kinetische Entmischung der Kationen. Voraussetzung fur die kinetische Entmischung sind unterschiedliche Beweglichkeiten der verschiedenen Kationen, wie dies in SrTiO3 der Fall ist. Die in dieser Arbeit beschriebenen Messungen stellen den ersten experimentellen Nachweis fur eine kinetische Entmischung in SrTiO3 dar. Es ist anzunehmen, dass in oberflachennahen Bereichen (hoherer p(O2)-Bereich) uberschussige Sr(2+)-Kationen die Ti(4+)-Gitterplatze besetzen und hierdurch -Defekte verursachen, die elektrische Ladung von kompensieren. An den Trippl punkten last sich nach der Reoxidation eine Sr(2+)-reiche zweite Phase (Sr2TiO4) nachweisen. Dies macht sich im TEM-Beugungsbild bei Projektion auf die [100] bzw. [210] Zonen-achse durch eine zusatzlichen Reflexion in [001]-Richtung bemerkbar. Sr2TiO4 gehort zur homologen Reihe Sr(n+1)Ti(n)O(3n+1), die als Ruddlesden-Popper Phasen bekannt sind. Auf Grund der bislang gewonnen Daten kann die Existenz der anderen Reihenmitglieder (n = 2, 3, ...) nicht ausgeschlossen werden. Damit konnte zum ersten Mal eine durch Reoxidation verursachte Korngrenzen-Phase in SrTiO3 nachgewiesen werden.
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- 2005
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49. Plasmons in Mesoscopic Gold Tapers
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Ralf Vogelgesang, Martin Esmann, Peter A. van Aken, Christian Knipl, Christoph Lienau, Surong Guo, Simon F. Becker, Nahid Talebi, and Wilfried Sigle
- Subjects
Physics ,0209 industrial biotechnology ,Mesoscopic physics ,020901 industrial engineering & automation ,Condensed matter physics ,02 engineering and technology ,021001 nanoscience & nanotechnology ,0210 nano-technology ,Instrumentation ,Plasmon - Published
- 2016
- Full Text
- View/download PDF
50. Electron-Beam-Induced Antiphase Boundary Reconstructions in ZrO2- La2/3Sr1/3MnO3 Pillar- Matrix Structures
- Author
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Wilfried Sigle, Peter A. van Aken, Marion Kelsch, Hanns-Ulrich Habermeier, and Dan Zhou
- Subjects
0301 basic medicine ,03 medical and health sciences ,Matrix (mathematics) ,030104 developmental biology ,Materials science ,Pillar ,Cathode ray ,Boundary (topology) ,02 engineering and technology ,021001 nanoscience & nanotechnology ,0210 nano-technology ,Instrumentation ,Molecular physics - Published
- 2016
- Full Text
- View/download PDF
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