Photon-assisted Spectroscopy of Electronic Interface States in Perovskite Oxide Heterostructures

Photon-assisted Spectroscopy of Electronic Interface States in Perovskite Oxide Heterostructures
Author:
Publisher:
Total Pages:
Release: 2007
Genre:
ISBN:

Complex oxides are an intriguing field of solid-state research, as they can exhibit a wide variety of functional properties, such as ferroelasticity, ferroelectricity, ferro- and antiferromagnetism or an even more complicated type of magnetic ordering, the combination or interaction of those ferroic properties (multiferroicity), high spin polarization, or high-temperature superconductivity. Thus they are prospective candidates for future materials in microelectronics. It is a matter of fact that the performance of such oxide-based devices depends mainly on transport properties, which in turn depend on the distribution and density of intrinsic or extrinsic electronic interface states across the device structure. The present thesis focuses on the identification and characterization of such electronic properties by two different photoassisted spectroscopy techniques: surface photovoltage spectroscopy and photoelectron spectroscopy. This work especially deals with perovskite oxides, namely with the model perovskite strontium titanate (SrTiO3) as a substrate and three differently doped lanthanum manganite thin films (10-15 nm thickness) grown by pulsed laser deposition (PLD) on the SrTiO3 substrate(La0.7Sr0.3MnO3, La0.7Ca0.3MnO3, La0.7Ce0.3MnO3). The first part aims at the identification of electronic surface and interface states at the free SrTiO3 surface as well as at the three different lanthanum manganite/SrTiO3 interfaces. For that purpose three different experimental realizations of the surface photovoltage spectroscopy technique were implemented and employed: photoelectron spectroscopy under additional optical excitation, the capacitive detection of the photoinduced displacement current in a parallel-plate capacitor geometry under modulated optical excitation, and the classical Kelvin probe technique. The methods are evaluated comparatively with respect to their suitability to analyze the given oxidic interfaces. The main result of this first part is a map of the.

Atomic-Scale Studies Of Structure And Bonding At Perovskite Oxide Heterointerfaces

Atomic-Scale Studies Of Structure And Bonding At Perovskite Oxide Heterointerfaces
Author: Lena Fitting Kourkoutis
Publisher:
Total Pages: 0
Release: 2009
Genre:
ISBN:

Perovskite oxides exhibit an almost universal range of ground states including insulator, semiconductor, metal, superconductor, ferromagnet, antiferromagnet, spin glass, ferroelectric, and piezoelectric. Many of these phenomena occur in materials that are lattice-matched within a few percent of one another, giving rise to the possibility of heteroepitaxial structures using perovskite oxides, accessing these multiple degrees of freedom. The existence of interfaces can, however, greatly affect the macroscopic properties of these heterostructures, leading on the one hand to exotic new phases stabilized at the interface or on the other hand to the degradation of bulk-like properties. Here scanning transmission electron microscopy (STEM) in combination with electron energy loss spectroscopy (EELS) is used to study interface phenomenon in perovskite-oxide heterostructures. In STEM the self-focusing of the probe electron wavepacket by channeling along a zone axis in a crystalline material can strongly affect the annular dark field (ADF) image contrast. By exploiting these channeling effects, atomically thin, buried SrTiO3 layers on Si were imaged in plan view, revealing a nonuniform coverage by epitaxial SrTiO3 islands and 2x1 Sr-covered regions. The dewetting of thin SrTiO3 films grown on Si(100) is caused by a phase-separation instability as predicted by density functional theory calculations. Improved coverage was obtained by choosing growth conditions away from equilibrium. Atomically abrupt interfaces have been demonstrated for all-oxides heterostructures. However, for most systems there are intrinsic limitations to the abruptness of an interface. Polar discontinuities at oxide interfaces can cause atomic reconstruction. In LaVO3 /SrTiO3 multilayers a second effect, preferential Sr surface segregation, is shown to dominate. The vanadate layers exhibit a growth asymmetry, with diffuse lower and atomically-abrupt upper interfaces. This suggests that segregation processes can set an upper limit to the obtainable interface sharpness in perovskite oxide heterostructures. Starting with an abrupt interface between LaVO3 and LaVO4 , spatially resolved EELS is used to probe how the transition from V 3d2 in LaVO3 to V 3d0 in LaVO4 is made. Although no bulk phase of LaVO x with V 3d1 configuration exists, a nanometer-wide region of V 3d1 is found at the LaVO3 /LaVO4 interface, rather than a mixture of V 3d0 and V 3d2 . This two-dimensional sheet of 3d1 electrons is an example for electronic reconstruction at a complex oxide interface, which can be used to induce and stabilize non-bulk-like valence states. How does the presence of interfaces affect the physical properties of the complex oxide heterostructure? La0.7 Sr0.3 MnO3 is a conducting ferromagnet at room temperature. However, in manganite/titanate tunnel junctions interface spin and charge modulations are thought to create an interfacial dead layer, thus fundamentally limiting the use of this material in small dimensions. Here, the degradation of the magnetic and transport properties of La0.7 Sr0.3 MnO3 /SrTiO3 multilayers is found to correlate with a higher degree of intermixing at the interfaces and the presence of extended cation defects in the La0.7 Sr0.3 MnO3 layers. When these extrinsic defects are eliminated, metallic ferromagnetism at room temperature can be stabilized in ultrathin manganite layers.

Characterization of Perovskite Oxide/semiconductor Heterostructures

Characterization of Perovskite Oxide/semiconductor Heterostructures
Author: HsinWei Wu
Publisher:
Total Pages: 137
Release: 2018
Genre: Electronic dissertations
ISBN:

Integrated oxide/semiconductor heterostructures have attracted intense interest for device applications which require sharp interfaces and controlled defects. The research of this dissertation has focused on the characterization of perovskite oxide/oxide and oxide/semiconductor heterostructures, and the analysis of interfaces and defect structures, using scanning transmission electrom microscopy (STEM) and related techniques. The SrTiO3/Si system was initially studied to develop a basic understanding of the integration of perovskite oxides with semiconductors, and successful integration with abrupt interfaces was demonstrated. Defect analysis showed no misfit dislocations but only anti-phase boundaries (APBs) in the SrTiO3 (STO) films. Similar defects were later observed in other perovskite oxide heterostructures. Ferroelectric BaTiO3 (BTO) thin films deposited directly onto STO substrates, or STO buffer layers with Ge substrates, were grown by molecular beam epitaxy (MBE) in order to control the polarization orientation for field-effect transistors (FETs). STEM imaging and elemental mapping by electron energy-loss spectroscopy (EELS) showed structurally and chemically abrupt interfaces, and the BTO films retained the c-axis-oriented tetragonal structure for both BTO/STO and BTO/STO/Ge heterostructures. The polarization displacement in the BTO films of TiN/BTO/STO heterostructures was investigated. The Ti4+ atomic column displacements and lattice parameters were measured directly using HAADF images. A polarization gradient, which switched from upwards to downwards, was observed in the BTO thin film, and evidence was found for positively-charged oxygen vacancies. Heterostructures grown on Ge substrates by atomic layer deposition (ALD) were characterized and compared with MBE-grown samples. A two-step process was needed to overcome interlayer reaction at the beginning of ALD growth. A-site-rich oxide films with thicknesses of at least 2-nm had to be deposited and then crystallized before initiating deposition of the following perovskite oxide layer in order to suppress the formation of amorphous oxide layers on the Ge surface. BTO/STO/Ge, BTO/Ge, SrHfTiO3/Ge and SrZrO3/Ge thin films with excellent crystallinity were grown using this process. Metal-insulator-metal (MIM) heterostructures were fabricated as ferroelectric capacitors and then electrically stressed to the point of breakdown to correlate structural changes with electrical and physical properties. BaTiO3 on Nb:STO was patterned with different top metal electrodes by focused-ion-beam milling, Au/Ni liftoff, and an isolation-defined approach.

Extreme Electron Density Perovskite Oxide Heterostructures for Field Effect Transistors

Extreme Electron Density Perovskite Oxide Heterostructures for Field Effect Transistors
Author: Omor Faruk Shoron
Publisher:
Total Pages: 99
Release: 2015
Genre:
ISBN:

Perovskite oxides are an interesting group of materials with diverse and unique electronic, photonic, optical and magnetic properties. One of the recent discoveries in perovskite oxide is the extreme high electron density at polar and non-polar oxide heterojunction interfaces. GdTiO3/SrTiO3 heterostructure shows an electron density of 3x1014 cm-2 at the interface that is around one order higher than any conventional semiconductor heterostructures. In this work, GdTiO3/SrTiO3 heterostructures were used to demonstrate field effect transistors. This is the first demonstration of transistor with such high charge density. We also investigated the factors that limit the charge modulation in this heterostructure, and developed an analytical model that can predict charge control characteristics of this heterostructure. Three methods were proposed and demonstrated to improve the modulation, leading to record charge modulation of 1.5x1014 cm-2, which is the highest to date for any semiconductor system using electronic gating.

Spectroscopy of Complex Oxide Interfaces

Spectroscopy of Complex Oxide Interfaces
Author: Claudia Cancellieri
Publisher: Springer
Total Pages: 326
Release: 2018-04-09
Genre: Technology & Engineering
ISBN: 3319749897

This book summarizes the most recent and compelling experimental results for complex oxide interfaces. The results of this book were obtained with the cutting-edge photoemission technique at highest energy resolution. Due to their fascinating properties for new-generation electronic devices and the challenge of investigating buried regions, the book chiefly focuses on complex oxide interfaces. The crucial feature of exploring buried interfaces is the use of soft X-ray angle-resolved photoemission spectroscopy (ARPES) operating on the energy range of a few hundred eV to increase the photoelectron mean free path, enabling the photons to penetrate through the top layers – in contrast to conventional ultraviolet (UV)-ARPES techniques. The results presented here, achieved by different research groups around the world, are summarized in a clearly structured way and discussed in comparison with other photoemission spectroscopy techniques and other oxide materials. They are complemented and supported by the most recent theoretical calculations as well as results of complementary experimental techniques including electron transport and inelastic resonant X-ray scattering.

Electronic Transitions in Perovskite Oxide Heterostructures

Electronic Transitions in Perovskite Oxide Heterostructures
Author: Franklin Wong
Publisher:
Total Pages: 312
Release: 2011
Genre:
ISBN:

The focus of this dissertation is on tuning electronic phase transitions in perovskite oxide heterostructures. The recurring theme is the exploitation of characteristics inherent to heteroepitaxy that are unavailable in the bulk materials of identical chemistry; these inherent characteristics are epitaxial strain and interfacial electronic reconstruction. In contrast, the effects of chemical substitution, for example, are not defining traits of heterostructures as they can be routinely studied in bulk materials, and therefore will not be included in this work. Heteroepitaxial lattice deformation is identified to be crucial in two systems: coherently strained LaTiO3 films on SrTiO3 substrates and La2/3Sr1/3MnO3 films on LaAlO3 substrates. One the other hand, interfacial charge transfer is the responsible for the insulator-metal transitions in LaAlO3 films on SrTiO3 substrates, or LaAlO3/SrTiO3 heterointerfaces. The charge, orbital, spin, and lattice "degrees of freedom" are intimately linked in perovskite oxides, particularly those containing transition metals. The lattice can be modified through heteroepitaxial strain, and the charge state can be modified through interfacial electronic reconstruction. It is shown that epitaxial strain can induce an insulator-metal transition in LaTiO3, which is a Mott insulator in the bulk that is near an electronic instability owing to its orbital disorder. It is confirmed that metallic conduction occurs throughout the entire thicknesses of the LaTiO3 films, as opposed to being confined to the surfaces or interfaces. It is possible to exploit heteroepitaxial strain as a knob to modulate the electronic bandwidth. Strain values that can be introduced routinely in thin films are greater than those which are easily accessible in hydrostatic or uniaxial stress studies of bulk materials. Epitaxial strain also is explicitly linked to the enhanced magnetoresistive properties of La2/3Sr1/3MnO3 films, particularly at low temperatures. The key effect appears to be the stabilization of a more insulating phase that may coexist with the double-exchange metallic ferromagnetic phase, which is stable in the bulk. The more insulating phase in turn becomes unstable upon the application of a magnetic field, resulting in higher magnetoresistance over a wide range of temperatures. While such a mechanism is certainly believed to be pertinent for many bulk manganites, it is not expected to be relevant for the specific chemical composition studied. Similar to the case of LaTiO3, the orbital degrees of freedom in La2/3Sr1/3MnO3 are important for the tunability of such an electronic transition controlled by thin-film lattice deformation; an added ingredient is that there exist two competing magnetic exchange mechanisms that are sensitive to chemical bonding. Both the orbital degree of freedom and competing exchange interactions make the electronic properties of manganite films very sensitive to external lattice perturbations. Finally, metallic LaAlO & euro;3/SrTiO3 heterointerfaces between two nominally undoped insulators are examined. Interfacial polarity is believed to induce electron transfer from LaAlO3 to SrTiO3. Low temperature magnetotransport studies reveal signatures of strong spin-orbit interaction in this quasi-two-dimensional metallic channel. The spin-orbit coupling in the heterostructures is enhanced greatly by interfacial electric fields; hence, it represents a property that is fundamentally non-bulk-like. The transport data presented in this work suggest that disorder and carriers are introduced concurrently at the heterointerface, and also shed light on the origin of metallicity.

Hard X-ray Photoelectron Spectroscopy (HAXPES)

Hard X-ray Photoelectron Spectroscopy (HAXPES)
Author: Joseph Woicik
Publisher: Springer
Total Pages: 576
Release: 2015-12-26
Genre: Science
ISBN: 3319240439

This book provides the first complete and up-to-date summary of the state of the art in HAXPES and motivates readers to harness its powerful capabilities in their own research. The chapters are written by experts. They include historical work, modern instrumentation, theory and applications. This book spans from physics to chemistry and materials science and engineering. In consideration of the rapid development of the technique, several chapters include highlights illustrating future opportunities as well.

First-Principles Study of Two-Dimensional Electron Gas in Perovskite Oxide Heterostructures

First-Principles Study of Two-Dimensional Electron Gas in Perovskite Oxide Heterostructures
Author: Jianli Cheng
Publisher:
Total Pages: 185
Release: 2018
Genre:
ISBN:

Two-dimensional electron gas (2DEG) formed at the interface between two insulating perovskite oxides has provided a versatile playground to explore emergent interfacial electronic and magnetic properties. In this thesis our efforts centered on studying the electronic and structural properties of different 2DEG heterostructures (HS), with the goal of designing novel 2DEG HS using first-principles methods. In the first project we studied the [delta]-doping effects on the electronic and energetic properties of LaAlO3/SrTiO3 HS with 23 transition-metal (TM) dopants. It has been found that there is a trade-off between achieving small electron effective mass and obtaining an energetically favorable TM-doped LaAlO3/SrTiO3 system. More importantly, in addition to the experimentally confirmed Mn dopant, we proposed that Fe, Co, Ni, Ru, Rh, Pd, Os and Ir elements can also be promising dopants to yield light effective mass bands and good energetic stability. In the second project we compared the electronic and energetic properties of TiO2/LaAlO3 and LaAlO3/TiO2 HS. We found that TiO2/LaAlO3 is intrinsically metallic and has a larger interfacial charge carrier density, smaller electron effective mass and a stronger interface cohesion than LaAlO3/TiO2, which shows an insulator-to-metal transition at 4 unit cells of LaAlO3. In the third project we introduced a hitherto unknown 2DEG formed at the interface between spinel MgAl2O4 and SrTiO3. Our integrated approach combining experimental measurements and first-principles calculations reveals that an atomic-thin interfacial Ti-Al-O layer with a thickness of about 4Å is key to the observed metallic transport. The 2DEG observed at spinel/perovskite interface implies the existence of emergent phenomena at the interfaces between spinel group minerals and perovskite oxides. In the fourth and fifth project we explored the possibility of creating 2DEG in nonpo- lar/nonpolar perovskite oxide HS. We found that the lattice-mismatch-induced compression strain from the substrate leads to a large polarization in the film, which then drives the charge transfer from the film to the substrate and results in a 2DEG at the interface. In addition, by using high-throughput first-principles calculations and a group of combinatory descriptors, we rapidly designed more than 300 novel nonpolar/nonpolar 2DEG HS. In the final project we introduced Grain Boundary Maker (GBMaker), an efficient and open-source Python library for generating atomic coordinates in periodic grain boundary models. It is designed to construct various grain boundary structures from cubic and non-cubic initial configurations. GBMaker is expected to greatly accelerate the theoretical investigation of grain boundary properties and facilitate the experimental analysis of grain boundary structures as well.

Photoelectron Spectroscopy

Photoelectron Spectroscopy
Author: Stefan Hüfner
Publisher: Springer Science & Business Media
Total Pages: 525
Release: 2013-11-11
Genre: Science
ISBN: 3662031507

An up-to-date introduction to the field, treating in depth the electronic structures of atoms, molecules, solids and surfaces, together with brief descriptions of inverse photoemission, spin-polarized photoemission and photoelectron diffraction. Experimental aspects are considered throughout and the results carefully interpreted by theory. A wealth of measured data is presented in tabullar for easy use by experimentalists.