Author: Amish B. Shah
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
The ability to grow ultrathin films layer-by-layer with well-defined epitaxial relationships has allowed research groups worldwide to grow a range of artificial films and superlattices, first for semiconductors, and now with oxides. In the oxides thin film research community, there have been concerted efforts recently to develop a number of epitaxial oxide systems grown on single crystal oxide substrates that display a wide variety of novel interfacial functionality, such as enhanced ferromagnetic ordering, increased charge carrier density, increased optical absorption, etc, at interfaces. The magnitude of these novel properties is dependent upon the structure of thin films, especially interface sharpness, intermixing, defects, and strain, layering sequence in the case of superlattices and the density of interfaces relative to the film thicknesses. To understand the relationship between the interfacial thin film oxide atomic structure and its properties, atomic scale characterization is required. Transmission electron microscopy (TEM) offers the ability to study interfaces of films at high resolution. Scanning transmission electron microscopy (STEM) allows for real space imaging of materials with directly interpretable atomic number contrast. Electron energy loss spectroscopy (EELS), together with STEM, can probe the local chemical composition as well as local electronic states of transition metals and oxygen. Both techniques have been significantly improved by aberration correctors, which reduce the probe size to 1 ©5, or less. Aberration correctors have thus made it possible to resolve individual atomic columns, and possibly probe the electronic structure at atomic scales. Separately, using electron probe forming lenses, structural information such as the crystal structure, strain, lattice mismatches, and superlattice ordering can be measured by nanoarea electron diffraction (NED). The combination of STEM, EELS, and NED techniques allows us to gain a fundamental understanding of the properties of oxide superlattices and ultrathin films and their relationship with the corresponding atomic and electronic structure. In this dissertation, I use the aforementioned electron microscopy techniques to investigate several oxide superlattice and ultrathin film systems. The major findings are summarized below. These results were obtained with stringent specimen preparation methods that I developed for high resolution studies, which are described in Chapter 2. The essential materials background and description of electron microscopy techniques are given in Chapter 1 and 2. In a LaMnO3-SrMnO3 superlattice, we demonstrate the interface of LaMnO3-SrMnO3 is sharper than the SrMnO3-LaMnO3 interface. Extra spectral weights in EELS are confined to the sharp interface, whereas at the rougher interface, the extra states are either not present or are not confined to the interface. Both the structural and electronic asymmetries correspond to asymmetric magnetic ordering at low temperature. In a short period LaMnO3-SrTiO3 superlattice for optical applications, we discovered a modified band structure in SrTiO3 ultrathin films relative to thick films and a SrTiO3 substrate, due to charge leakage from LaMnO3 in SrTiO3. This was measured by chemical shifts of the Ti L and O K edges using atomic scale EELS. The interfacial sharpness of LaAlO3 films grown on SrTiO3 was investigated by the STEM/EELS technique together with electron diffraction. This interface, when prepared under specific conditions, is conductive with high carrier mobility. Several suggestions for the conductive interface have been proposed, including a polar catastrophe model, where a large built-in electric field in LaAlO3 films results in electron charge transfer into the SrTiO3 substrate. Other suggested possibilities include oxygen vacancies at the interface and/or oxygen vacancies in the substrate. The abruptness of the interface as well as extent of intermixing has not been thoroughly investigated at high resolution, even though this can strongly influence the electrical transport properties. We found clear evidence for cation intermixing through the LaAlO3-SrTiO3 interface with high spatial resolution EELS and STEM, which contributes to the conduction at the interface. We also found structural defects, such as misfit dislocations, which leads to increased intermixing over coherent interfaces.
Author: Gianfranco Pacchioni
Publisher: John Wiley & Sons
ISBN: 3527640193
Category : Technology & Engineering
Languages : en
Pages : 368
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Book Description
A wealth of information in one accessible book. Written by international experts from multidisciplinary fields, this in-depth exploration of oxide ultrathin films covers all aspects of these systems, starting with preparation and characterization, and going on to geometrical and electronic structure, as well as applications in current and future systems and devices. From the Contents: Synthesis and Preparation of Oxide Ultrathin Films Characterization Tools of Oxide Ultrathin Films Ordered Oxide Nanostructures on Metal Surfaces Unusual Properties of Oxides and Other Insulators in the Ultrathin Limit Silica and High-K Dielectrics Thin Films in Microelectronics Oxide Passive Films and Corrosion Protection Oxide Films as Catalytic Materials and as Models of Real Catalysts Oxide Films in Spintronics Oxide Ultrathin Films in Solid Oxide Fuel Cells Transparent Conducting and Chromogenic Oxide Films as Solar Energy Materials Oxide Ultrathin Films in Sensor Applications Ferroelectricity in Ultrathin Film Capacitors Titania Thin Films in Biocompatible Materials and Medical Implants Oxide Nanowires for New Chemical Sensor Devices
Author: Meng Gu
Publisher:
ISBN: 9781267240491
Category :
Languages : en
Pages :
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Book Description
Materials with the ABO3 perovskite structure possess a wide variety of properties including superconductivity, ferroelectric, and magnetic properties. These properties are highly tunable due to the fact that the B site cation can assume multiple valence states and its high structural stability allows for large scale doping and strain. Due to a reduced dimensionality, two dimensional thin films and superlattices grown using techniques such as pulsed laser deposition (PLD) often possess novel properties which differ from the bulk perovskite materials. The origins of these novel properties can be traced to interfacial chemical intermixing, electronic reconstruction, strain as well as defect formation, which cause significant changes in the electronic structures. Therefore, it is crucially important to investigate the atomic and electronic structures of the functional materials in order to understand the correlation between microstructures and physical properties. Chemically-sensitive Z-contrast imaging and bonding-sensitive electron energy loss spectroscopy (EELS) in aberration corrected scanning transmission electron microscopes (STEM) can directly characterize the local structure, strain, composition and bonding on the atomic scale. Determination of the atomic and electronic structures of the interfaces and defects in the thin films can then be correlated with the magnetic and transport properties. Therefore, the understanding of the structure-property relationship for several different systems of perovskite oxide thin films and superlattices were developed on the atomic scale. Multifunctional superlattices composed of ferromagnetic (FM) La(0.7)Sr(0.3)MnO3 (LSMO) and antiferromagnetic (AFM) La(0.7)Sr(0.3)FeO3 (LSFO) have potential applications for next generation data storage and logic devices. Defect formation, driven by strain relaxation in the LSMO/LSFO superlattices can modify not only the structure and surface sharpness, but also the functional properties of the superlattice. Stacking faults were found as one efficient way of strain relaxation while maintaining robust antiferromagnetic properties for a thin [3LSMO][6LSFO] superlattice (repeating motif composed of 3 unit-cell LSMO sublayer and 6 unit-cell LSFO sublayer). On the other hand, for a fully strained [3LSMO][6LSFO], large inter-diffusion across the interface between the LSMO and LSFO layers was detected in EELS line scans, resulting in deteriorated AFM properties. When a [6LSMO][6LSFO] superlattice with one micron thickness, a high density of nanoflowers and cracks/pinholes were observed to result from strain relaxation. The formation of these nanoflowers and cracks/pinholes was suppressed by increasing the growth rate and thereby reducing the growth time and overall thermal treatment of the sample. Strain relaxation was shown to be directly related to the growth conditions and have a large effect on both the structure and functional properties of the superlattices. A series of superlattices composed of non-magnetic La(0.5)Sr(0.5)TiO3 (LSTO) and ferromagnetic LSMO were grown on single crystal oxide substrates with different amounts of misfit strain. No significant electronic structure changes along the interfaces was observed in this series of superlattices as revealed by atomic resolution EELS. In comparison, charge transfer effect was reported for the LSMO/STO superlattices and was shown to cause an ultrathin magnetic dead layer along the interfaces. Thus, compared with the LSMO/STO superlattice, composition tuning of the sublayers was proven to be efficient in controlling the interfacial charge transfer effects in a superlattice. In addition, tetragonal distortion was found to reduce the ferromagnetic ordering, decrease the Tc, increase the resistivity, and even lead to metal-insulator transitions of the superlattices. The strain relaxation defects such as dislocations and low angle grain boundaries serve as important pinning sites for magnetic domains, leading to enhanced coercive field strength. In order to determine the properties of an intermixed interface layer, we have performed a detailed study of the solid solution between LSMO and LSFO, i.e. La(0.7)Sr(0.3)Mn(0.5)Fe(0.5)O3 (LSMFO). A large target-substrate distance during the PLD growth led to cation segregation in the LSMFO film. Cation segregation could cause the formation of diverse local magnetic ordering and B site valence states due to the different local stoichiometry and coordination environment. For the cation segregated LSFMO films, robust ferromagnetic and antiferromagnetic coupling was observed at 150K and room temperature. Decreasing the target-substrate distance resulted to a homogeneous cation distribution in the film, without any ferromagnetic ordering as expected. This result suggests the important role of target-substrate distance and the kinetic energy of the plume species on the crystalline quality and functional properties of perovskite oxide thin films. La(x)Sr(1-x)TiO3 possesses a wide range of functional properties which make it an attractive candidate material for applications such as the conductive buffer for high temperature superconductor growth, transparent conductors, and anodes in solid oxide fuel cells. La(0.5)Sr(0.5)TiO3 thin films were grown using PLD and the resistivity was found to be highly dependent on the O2 background pressure used in the deposition. However, a thin film which was deposited as a single phase film was transformed into a semi-ordered superlattice with TiO2 rich stacking faults and distorted lattices upon exposure to high oxygen pressure (~200torr) during the cooling procedure after deposition. This phase change stabilized Ti4+ ions and dramatically increased the resistivity of the film. In addition, a two dimensional free electron gas could be constructed by confining a few unit cells of La doped STO with STO spacer layers. Our study showed that charge transfer over a distance of ~2 u.c. was present in Sr(0.75)La(0.25)TiO3/STO superlattices. This thickness defined the lower limit for the thickness of the STO spacers in order to confine the charge carriers into two dimensions; secondly, the La dopants were shown to be less localized in thicker superlattice (~100nm) due to interdiffusion upon extended thermal exposure. This information provided important feedback on the fabrication and utilization of this material.In conclusion, several perovskite thin film systems with fascinating properties have been explored in this thesis. Strain states and strain relaxations, defect formation, interfacial atomic mixing, charge transfer, and cation segregation were shown to have profound effect on the functional properties of complex oxide thin film systems. Atomic resolution Z-contrast imaging and EELS provide extremely useful information on the structural and electronic structure variations, which enable us to see the whole picture of growth, structure and properties' interactions.
Author: Miroslav Kotrla
Publisher: Springer Science & Business Media
ISBN: 9401003912
Category : Science
Languages : en
Pages : 588
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Book Description
Epitaxial growth lies at the heart of a wide range of industrial and technological applications. Recent breakthroughs, experimental and theoretical, allow actual atom-by-atom manipulation and an understanding of such processes, opening up a totally new area of unprecedented nanostructuring. The contributions to Atomistic Aspects of Epitaxial Growth are divided into five main sections, taking the reader from the atomistic details of surface diffusion to the macroscopic description of epitaxial systems. many of the papers contain substantial background material on theoretical and experimental methods, making the book suitable for both graduate students as a supplementary text in a course on epitaxial phenomena, and for professionals in the field.
Author: J. Matharu
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
The properties of metal oxide surfaces are key to their diverse technological applications. However, the semiconducting nature of metal oxides presents a problem - many surface science techniques are electron based and thus require samples to be conducting. As such, bulk crystal studies of metal oxides by techniques such as photoemission spectroscopy (PES) and scanning tunneling microscopy (STM) are limited to reduced surfaces. Alternatively, thin films of a metal oxide can be synthesised on a suitable conducting substrate that mimic the bulk crystal surface whilst having sufficient conducting character to use these techniques. CeO2 is an important material found in three-way catalysts that remove pollutants from the exhaust gas of modern automobiles. Key to this application is the ability of reduced ceria to store and release oxygen depending on the composition of the exhaust. The addition of noble metals such as Pd to the ceria surface greatly improves the efficiency of pollutant conversion evidenced by X-ray photoelectron spectroscopy (XPS) by reducing the ceria. Resonance photoemission spectroscopy (RESPES) has been used to investigate the eect of Pd on ceria CeO2-x(110) thin films grown on a Pt(111) substrate. RESPES is more surface specific than XPS and thus reveals more information on the surface layers of ceria films. TiO2(110) is the most studied metal oxide surface, and has a multitude of applications. Its chemistry with two of the most abundant chemical species - water (H2O) and oxygen (O2) - is thus very important. H2O has been shown to dissociate on TiO2 surfaces. TiO2 thin films grown on W(100) were used as model system to study the chemistry of the reaction between TiO2 and H2O, and subsequently the reaction of hydrated surfaces with O2 using XPS. STM was used to examine the morphology of TiO2(110) films grown on W(100)-(2 x 1)-O, changes with film thickness and methods of improving surface smoothness. The first detailed STM images showing row structure of TiO2(110) films grown on W are shown.
Author: Falko P. Netzer
Publisher: Springer
ISBN: 3319283324
Category : Technology & Engineering
Languages : en
Pages : 403
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Book Description
This book summarizes the current knowledge of two-dimensional oxide materials. The fundamental properties of 2-D oxide systems are explored in terms of atomic structure, electronic behavior and surface chemistry. The concept of polarity in determining the stability of 2-D oxide layers is examined, charge transfer effects in ultrathin oxide films are reviewed as well as the role of defects in 2-D oxide films. The novel structure concepts that apply in oxide systems of low dimensionality are addressed, and a chapter giving an overview of state-of-the-art theoretical methods for electronic structure determination of nanostructured oxides is included. Special emphasis is given to a balanced view from the experimental and the theoretical side. Two-dimensional materials, and 2-D oxides in particular, have outstanding behavior due to dimensionality and proximity effects. Several chapters treat prototypical model systems as illustrative examples to discuss the peculiar physical and chemical properties of 2-D oxide systems. The chapters are written by renowned experts in the field.
Author:
Publisher:
ISBN:
Category : Power resources
Languages : en
Pages : 762
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Book Description
Semiannual, with semiannual and annual indexes. References to all scientific and technical literature coming from DOE, its laboratories, energy centers, and contractors. Includes all works deriving from DOE, other related government-sponsored information, and foreign nonnuclear information. Arranged under 39 categories, e.g., Biomedical sciences, basic studies; Biomedical sciences, applied studies; Health and safety; and Fusion energy. Entry gives bibliographical information and abstract. Corporate, author, subject, report number indexes.
Author:
Publisher:
ISBN:
Category : Aeronautics
Languages : en
Pages : 702
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Author:
Publisher: Elsevier
ISBN: 0128098945
Category : Science
Languages : en
Pages : 5276
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Book Description
Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry, Seven Volume Set summarizes current, fundamental knowledge of interfacial chemistry, bringing readers the latest developments in the field. As the chemical and physical properties and processes at solid and liquid interfaces are the scientific basis of so many technologies which enhance our lives and create new opportunities, its important to highlight how these technologies enable the design and optimization of functional materials for heterogeneous and electro-catalysts in food production, pollution control, energy conversion and storage, medical applications requiring biocompatibility, drug delivery, and more. This book provides an interdisciplinary view that lies at the intersection of these fields. Presents fundamental knowledge of interfacial chemistry, surface science and electrochemistry and provides cutting-edge research from academics and practitioners across various fields and global regions
Author: Tamalika Banerjee
Publisher: CRC Press
ISBN: 0429886896
Category : Science
Languages : en
Pages : 225
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Book Description
Oxide materials have been used in mainstream semiconductor technology for several decades and have served as important components, such as gate insulators or capacitors, in integrated circuits. However, in recent decades, this material class has emerged in its own right as a potential contender for alternative technologies, generally designated as ‘beyond Moore’. The 2004 discovery by Ohtomo and Hwang was a global trendsetter in this context. It involved observing a two-dimensional, high-mobility electron gas at the heterointerface between two insulating oxides, LaAlO3 and SrTiO3, supported by the rise of nascent deposition and growth-monitoring techniques, which was an important direction in materials science research. The quest to understand the origin of this unparalleled physical property and to find other emergent properties has been an active field of research in condensed matter that has united researchers with expertise in diverse fields such as thin-film growth, defect control, advanced microscopy, semiconductor technology, computation, magnetism and electricity, spintronics, nanoscience, and nanotechnology.
