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Quantitative Statistical Analysis of Atomic Scale Structural and Chemical Variations in Complex Oxides Interfaces

Quantitative Statistical Analysis of Atomic Scale Structural and Chemical Variations in Complex Oxides Interfaces PDF Author: Hao Yang
Publisher:
ISBN: 9781303541285
Category :
Languages : en
Pages :

Book Description
Grain boundaries (GBs) are known to have far-reaching effects on the electrical and mechanical properties of materials. Understanding the atomic scale mechanisms behind these effects requires an accurate determination of the interplay between GB structure and composition. Based on the analysis of a range of grain boundaries using aberration corrected scanning transmission electron microscopy (STEM), a general structural units model has been derived for the structure of grain boundaries in various dense packing cubic materials including FCC metals, perovskites and fluorites. The similarities in the observed grain boundary structures of these materials originate from related space (and point) group symmetries of the parent structures. The presence of structural variations away from the general structural units model may be caused by frustrations of certain symmetry operations that result from the incorporation of point defects (vacancies and impurities). A clear understanding of the similarity and variation in grain boundary atomic structures will not only provide a means to infer the structure-property relationships in broad classes of materials, but also enables us eventually to effectively manipulate the GB structures to achieve better materials properties.To understand these chemical induced variations, and further quantify exactly how atomic scale variations at the boundary plane extend to the practical mesoscale operating length of the system, statistical analysis has been applied to the aberration corrected STEM Z-contrast images acquired from a series of undoped and doped SrTiO3 GBs. In order to understand the effects of oxygen vacancies incorporation, in-situ characterization of GB atomic structures were performed using the Environmental TEM under the reduced gas and heating environment. This analysis of GB similarity and variation provides insights into the structure-composition relationship in GBs to understand the influence of nonstoichiometry and dopant segregations. It also helps to determine experimentally the energetics behind the formation of grain boundary structures to predict GB formation in various materials.

Quantitative Statistical Analysis of Atomic Scale Structural and Chemical Variations in Complex Oxides Interfaces

Quantitative Statistical Analysis of Atomic Scale Structural and Chemical Variations in Complex Oxides Interfaces PDF Author: Hao Yang
Publisher:
ISBN: 9781303541285
Category :
Languages : en
Pages :

Book Description
Grain boundaries (GBs) are known to have far-reaching effects on the electrical and mechanical properties of materials. Understanding the atomic scale mechanisms behind these effects requires an accurate determination of the interplay between GB structure and composition. Based on the analysis of a range of grain boundaries using aberration corrected scanning transmission electron microscopy (STEM), a general structural units model has been derived for the structure of grain boundaries in various dense packing cubic materials including FCC metals, perovskites and fluorites. The similarities in the observed grain boundary structures of these materials originate from related space (and point) group symmetries of the parent structures. The presence of structural variations away from the general structural units model may be caused by frustrations of certain symmetry operations that result from the incorporation of point defects (vacancies and impurities). A clear understanding of the similarity and variation in grain boundary atomic structures will not only provide a means to infer the structure-property relationships in broad classes of materials, but also enables us eventually to effectively manipulate the GB structures to achieve better materials properties.To understand these chemical induced variations, and further quantify exactly how atomic scale variations at the boundary plane extend to the practical mesoscale operating length of the system, statistical analysis has been applied to the aberration corrected STEM Z-contrast images acquired from a series of undoped and doped SrTiO3 GBs. In order to understand the effects of oxygen vacancies incorporation, in-situ characterization of GB atomic structures were performed using the Environmental TEM under the reduced gas and heating environment. This analysis of GB similarity and variation provides insights into the structure-composition relationship in GBs to understand the influence of nonstoichiometry and dopant segregations. It also helps to determine experimentally the energetics behind the formation of grain boundary structures to predict GB formation in various materials.

Atomic Scale Characterization of Complex Oxide Thin Films

Atomic Scale Characterization of Complex Oxide Thin Films PDF Author: Meng Gu
Publisher:
ISBN: 9781267240491
Category :
Languages : en
Pages :

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.

Atomic Scale Chemical and Structural Characterization of Ceramic Oxide Heterostructure Interfaces

Atomic Scale Chemical and Structural Characterization of Ceramic Oxide Heterostructure Interfaces PDF Author: R. K. Singh
Publisher:
ISBN:
Category :
Languages : en
Pages : 5

Book Description
The research plan was divided into three tasks: (a) growth of oxide heterostructures for interface engineering using standard thin film deposition techniques, (b) atomic level characterization of oxide heterostructure using such techniques as STEM-2 combined with AFM/STM and conventional high-resolution microscopy (HRTEM), and (c) property measurements of aspects important to oxide heterostructures using standard characterization methods, including dielectric properties and dynamic cathodoluminescence measurements. Each of these topics were further classified on the basis of type of oxide heterostructure. Type I oxide heterostructures consisted of active dielectric layers, including the materials Ba{sub x}Sr{sub 1-x}TiO{sub 3} (BST), Y{sub 2}O{sub 3} and ZrO{sub 2}. Type II heterostructures consisted of ferroelectric active layers such as lanthanum manganate and Type III heterostructures consist of phosphor oxide active layers such as Eu-doped Y{sub 2}O{sub 3}.

Atomic Resolution Studies of Oxide Superlattices and Ultrathin Films

Atomic Resolution Studies of Oxide Superlattices and Ultrathin Films PDF Author: Amish B. Shah
Publisher:
ISBN:
Category :
Languages : en
Pages :

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.

Handbook of Nanoscopy, 2 Volume Set

Handbook of Nanoscopy, 2 Volume Set PDF Author: Gustaaf van Tendeloo
Publisher: John Wiley & Sons
ISBN: 3527317066
Category : Technology & Engineering
Languages : en
Pages : 1484

Book Description
This completely revised successor to the Handbook of Microscopy supplies in-depth coverage of all imaging technologies from the optical to the electron and scanning techniques. Adopting a twofold approach, the book firstly presents the various technologies as such, before going on to cover the materials class by class, analyzing how the different imaging methods can be successfully applied. It covers the latest developments in techniques, such as in-situ TEM, 3D imaging in TEM and SEM, as well as a broad range of material types, including metals, alloys, ceramics, polymers, semiconductors, minerals, quasicrystals, amorphous solids, among others. The volumes are divided between methods and applications, making this both a reliable reference and handbook for chemists, physicists, biologists, materials scientists and engineers, as well as graduate students and their lecturers.

Data Science for Nano Image Analysis

Data Science for Nano Image Analysis PDF Author: Chiwoo Park
Publisher: Springer Nature
ISBN: 3030728226
Category : Business & Economics
Languages : en
Pages : 376

Book Description
This book combines two distinctive topics: data science/image analysis and materials science. The purpose of this book is to show what type of nano material problems can be better solved by which set of data science methods. The majority of material science research is thus far carried out by domain-specific experts in material engineering, chemistry/chemical engineering, and mechanical & aerospace engineering. The book could benefit materials scientists and manufacturing engineers who were not exposed to systematic data science training while in schools, or data scientists in computer science or statistics disciplines who want to work on material image problems or contribute to materials discovery and optimization. This book provides in-depth discussions of how data science and operations research methods can help and improve nano image analysis, automating the otherwise manual and time-consuming operations for material engineering and enhancing decision making for nano material exploration. A broad set of data science methods are covered, including the representations of images, shape analysis, image pattern analysis, and analysis of streaming images, change points detection, graphical methods, and real-time dynamic modeling and object tracking. The data science methods are described in the context of nano image applications, with specific material science case studies.

Scientific and Technical Aerospace Reports

Scientific and Technical Aerospace Reports PDF Author:
Publisher:
ISBN:
Category : Aeronautics
Languages : en
Pages : 704

Book Description


Stanford Bulletin

Stanford Bulletin PDF Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 716

Book Description


The Surface Science of Metal Oxides

The Surface Science of Metal Oxides PDF Author:
Publisher: Royal Society of Chemistry
ISBN:
Category : Science
Languages : en
Pages : 498

Book Description
The surface science of metal oxides is studied using a variety of experimental and theoretical techniques, allowing the geometry, electronic structure, dynamics and the behaviour of the metal oxide-metal interface to be explored. Faraday Discussions documents a long-established series of Faraday Discussion meetings which provide a unique international forum for the exchange of views and newly acquired results in developing areas of physical chemistry, biophysical chemistry and chemical physics. The papers presented are published in the Faraday Discussion volume together with a record of the discussion contributions made at the meeting. Faraday Discussions therefore provide an important record of current international knowledge and views in the field concerned.

Energy Research Abstracts

Energy Research Abstracts PDF Author:
Publisher:
ISBN:
Category : Power resources
Languages : en
Pages : 442

Book Description