Understanding Electrically Active Interface Formation on Wide Bandgap Semiconductors through Molecular Beam Epitaxy Using Fe3O 4 for Spintronics as a Base Cas

Nanoelectronics, complex heterostructures, and engineered 3D matrix materials are quickly advancing from research possibilities to manufacturing challenges for applications ranging from high-power devices to solar cells to any number of novel multifunctional sensors and controllers. Formation of an abrupt and effective interface is one of the basic requirements for integration of functional materials on different types of semiconductors (from silicon to the wide bandgaps) which can significantly impact the functionality of nanoscale electronic devices. To realize the potential of next-generation electronics, the understanding and control of those initial stages of film layer formation must be understood and translated to a process that can control the initial stages of film deposition.;Thin film Fe3O4 has attracted much attention as a material for exploring the potential of spintronics in next-generation information technologies. Synthesis of highly spin-polarized material as spin sources, in combination with wide bandgap semiconductors which have a long spin relaxation time in addition to functionality in high-temperature, high-power, and high-frequency environments, would enhance the performance of today's spintronic devices. Spinel ferrite Fe3O4 has a high Curie temperature of 858 K and it is predicted to possess half-metallic properties, i.e. ~ 100% spin polarization at the Fermi level, which can lead to ultrahigh tunneling magnetoresistance at room temperature. However, these properties have been very difficult to realize in thin film form, and device design strategies require high-quality thin films of Fe3O4. The most common reason reported in literature for the failure of the films to achieve theoretical performance is that the growth techniques used today produce films with antiphase boundaries (APB). These APBs have a strong antiferromagnetic coupling that negatively impact the magnetic and transport properties of epitaxial Fe 3O4 films.;Therefore, greater understanding of how to reduce APB density is of essential importance for applications of Fe3O4 films, and understanding the complex chemical and structural influences on the initial stages of film deposition is the key to eliminating APB density. This work used molecular beam epitaxy (MBE) to further understand the nucleation and growth mechanism needed to ensure single crystal film formation in a controlled orientation directly on a semiconductor (SiC) and then also on an insulating layer (MgO) that can not only align crystal structure but also provide an effective spin-aligned tunnel junction material.;The starting substrate surface proved critical to effective integration, and the role of atomic hydrogen seems to be key in controlling the starting surface. We have investigated 1) the hydrogen furnace cleaning at 1600 °C of 6H-SiC (0001) substrates surfaces to produce a smooth, uniformly stepped surface and a √3x√3 R30° surface reconstruction with less than 10 at% residual oxygen contamination, 2) the atomic hydrogen cleaning of 6H-SiC (0001) substrates to produce a (1x1) surface structure with less than 7 at% residual oxygen contamination at relatively low temperature of 700 °C, 3) the atomic hydrogen cleaning of Ge (100) to produce smooth surface (RMS < 0.5 nm over a 1 mum2 area), and 4) the oxygen plasma cleaning of MgO (111) substrates. Each of these starting surfaces, in addition to single crystalline MgO (111) films deposited on SiC (0001) by MBE, produced different initial growth mechanisms for MgO and Fe3 O4.;The highest quality single crystalline, epitaxial Fe 3O4 (111) films were deposited by MBE on the √3x√3 R30 surface reconstruction with less than 10 at% residual oxygen contamination 6H-SiC. The Fe3O4 film exhibits high structural order with sharp interfaces and an easy axis in-plane magnetization with a coercivity of 200 Oe. The MgO deposited by MBE on SiC prepared by the hydrogen furnace was found to have two-dimensional features that transitioned from 2D to 3D when the thickness exceeded 2nm; the structure changed from hexagonal to rock-salt due to relaxation as the layer thickness increased. MgO deposited by MBE on atomic hydrogen cleaned SiC had the rock-salt structure from the beginning due to the more thermodynamically stable arrangement on the non-reconstructed starting surface. This is one example of how we have shown the ability to balance kinetic and thermodynamic drivers through the use of starting surface chemistry and structure and processing techniques. This understanding enables the development of processing strategies to reduce APBs in Fe3O 4 on SiC and ultimately lead to the next generation of spintronic devices.