New semiconductor materials may enable next-generation â spintronicâ devices which exploit both the spin and charge of an electron for data processing, storage, and transfer. The realization of such devices would benefit greatly from room temperature ferromagnetic dilute magnetic semiconductors. Theoretical predictions have suggested that room temperature ferromagnetism may be possible in the wide bandgap semiconductors GaMnN and ZnMnO, though the existing models require input from the growth of high-quality materials. This work focuses on an experimental effort to develop high-quality materials in both of these wide bandgap materials systems. ZnMnO and ZnCoO single crystals have been grown by a modified melt growth technique. X-ray diffraction was used to examine the structural quality and demonstrate the single crystal character of these devices. Substitutional transition metal incorporation has been verified by optical transmission and electron paramagnetic resonance measurements. No indications of ferromagnetic hysteresis are observed from the bulk single crystal samples, and temperature dependent magnetization studies demonstrate a dominant antiferromagnetic exchange interaction. Efforts to introduce ferromagnetic ordering were only successful through processing techniques which significantly degraded the material quality. GaMnN thin films were grown by metalorganic chemical vapor deposition. Good crystalline quality and a consistent growth mode with Mn incorporation were verified by several independent characterization techniques. Substitutional incorporation of Mn on the Ga lattice site was confirmed by electron paramagnetic resonance. Mn acted as a deep acceptor in GaN. Nevertheless, ferromagnetic hysteresis was observed in the GaMnN films. The apparent strength of the magnetization correlated with the relative ratio of trivalent to divalent Mn. Valence state control through codoping with additional donors such as silicon was observed. Additional studies on GaFeN also showed a magnetic hysteresis. A comparison with implanted samples showed that the common origin to the apparent strong ferromagnetic hysteresis related to contribution from Mn substitutional ions. The observed magnetic hysteresis is due to the formation of Mn-rich regions during the growth process. This work demonstrated that the original intrinsic models for room temperature ferromagnetism in the wide bandgap semiconductors do not hold and the room temperature ferromagnetism in these materials results from extrinsic contributions.

Thesis (Ph. D.)--Oregon State University, 2008. / Printout. Includes bibliographical references (leaves 102-108). Also available on the World Wide Web.

No description available.

<p>The present thesis is concerned to the application of first-principles self-consistent total-energy calculations within the density functional theory on different topics in materials science.</p><p>Crystallographic phase-transitions under high-pressure has been study for TiO2, FeI2, Fe3O4, Ti, the heavy alkali metals Cs and Rb, and C3N4. A new high-pressure polymorph of TiO2 has been discovered, this new polymorph has an orthorhombic OI (Pbca) crystal structure, which is predicted theoretically for the pressure range 50 to 100 GPa. Also, the crystal structures of Cs and Rb metals have been studied under high compressions. Our results confirm the recent high-pressure experimental observations of new complex crystal structures for the Cs-III and Rb-III phases. Thus, it is now certain that the famous isostructural phase transition in Cs is rather a new crystallographic phase transition.</p><p>The elastic properties of the new superconductor MgB2 and Al-doped MgB2 have been investigated. Values of all independent elastic constants (c11, c12, c13, c33, and c55) as well as bulk moduli in the a and c directions (Ba and Bc respectively) are predicted. Our analysis suggests that the high anisotropy of the calculated elastic moduli is a strong indication that MgB2 should be rather brittle. Al doping decreases the elastic anisotropy of MgB2 in the a and c directions, but, it will not change the brittle behaviour of the material considerably.</p><p>The three most relevant battery properties, namely average voltage, energy density and specific energy, as well as the electronic structure of the Li/LixMPO4 systems, where M is either Fe, Mn, or Co have been calculated. The mixing between Fe and Mn in these materials is also examined. Our calculated values for these properties are in good agreement with recent experimental values. Further insight is gained from the electronic density of states of these materials, through which conclusions about the physical properties of the various phases are made.</p><p>The electronic and magnetic properties of the dilute magnetic semiconductor Mn-doped ZnO has been calculated. We have found that for an Mn concentration of 5.6%, the ferromagnetic configuration is energetically stable in comparison to the antiferromgnetic one. A half-metallic electronic structure is calculated by the GGA approximation, where Mn ions are in a divalent state leading to a total magnetic moment of 5 μB per Mn atom.</p>

The present thesis is concerned to the application of first-principles self-consistent total-energy calculations within the density functional theory on different topics in materials science. Crystallographic phase-transitions under high-pressure has been study for TiO2, FeI2, Fe3O4, Ti, the heavy alkali metals Cs and Rb, and C3N4. A new high-pressure polymorph of TiO2 has been discovered, this new polymorph has an orthorhombic OI (Pbca) crystal structure, which is predicted theoretically for the pressure range 50 to 100 GPa. Also, the crystal structures of Cs and Rb metals have been studied under high compressions. Our results confirm the recent high-pressure experimental observations of new complex crystal structures for the Cs-III and Rb-III phases. Thus, it is now certain that the famous isostructural phase transition in Cs is rather a new crystallographic phase transition. The elastic properties of the new superconductor MgB2 and Al-doped MgB2 have been investigated. Values of all independent elastic constants (c11, c12, c13, c33, and c55) as well as bulk moduli in the a and c directions (Ba and Bc respectively) are predicted. Our analysis suggests that the high anisotropy of the calculated elastic moduli is a strong indication that MgB2 should be rather brittle. Al doping decreases the elastic anisotropy of MgB2 in the a and c directions, but, it will not change the brittle behaviour of the material considerably. The three most relevant battery properties, namely average voltage, energy density and specific energy, as well as the electronic structure of the Li/LixMPO4 systems, where M is either Fe, Mn, or Co have been calculated. The mixing between Fe and Mn in these materials is also examined. Our calculated values for these properties are in good agreement with recent experimental values. Further insight is gained from the electronic density of states of these materials, through which conclusions about the physical properties of the various phases are made. The electronic and magnetic properties of the dilute magnetic semiconductor Mn-doped ZnO has been calculated. We have found that for an Mn concentration of 5.6%, the ferromagnetic configuration is energetically stable in comparison to the antiferromgnetic one. A half-metallic electronic structure is calculated by the GGA approximation, where Mn ions are in a divalent state leading to a total magnetic moment of 5 μB per Mn atom.

The properties of dilute magnetic semiconductors have been studied by combined ab initio, Monte Carlo, and experimental techniques. This class of materials could be very important for future spintronic devices, that offer enriched functionality by making use of both the spin and the charge of the electrons. The main part of the thesis concerns the transition metal doped ZnO. The role of defects on the magnetic interactions in Mn-doped ZnO was investigated. In the presence of acceptor defects such as zinc vacancies and oxygen substitution by nitrogen, the magnetic interactions are ferromagnetic. For dilute concentrations of Mn (~ 5%) the ordering temperature of the system is low, due to the short ranged character of the exchange interactions and disorder effects. The clustering tendency of the Co atoms in a ZnO matrix was also studied. The electronic structure, and in turn the magnetic interactions among the Co atoms, is strongly dependent on the exchange-correlation functional used. It is found that Co impurities tend to form nanoclusters and that the interactions among these atoms are antiferromagnetic within the local spin density approximation + Hubbard U approach. The electronic structure, as well as the chemical and magnetic interactions in Co and (Co,Al)-doped ZnO, was investigated by joined experimental and theoretical techniques. For a good agreement between the two, approximations beyond the local density approximation must be used. It is found that the Co atoms prefer to cluster within the semiconducting matrix, a tendency which is increased with Al co-doping. We envision that it is best to describe the system as superparamagnetic due to the formation of  Co nanoclusters within which the interactions are antiferromagnetic. The magnetic anisotropy and evolution of magnetic domains in Fe81Ni19/Co(001) superlattices were investigated both experimentally, as well as using model spin dynamics. A magnetic reorientation transition was found.

This work presents the development of a GaN-based dilute magnetic semiconductor (DMS) by metal organic chemical vapor deposition (MOCVD) that is ferromagnetic at room temperature (RT), electrically conductive, and possesses magnetic properties that can be tuned by n- and p-doping. The transition metal series (TM: Cr, Mn, and Fe) along with the rare earth (RE) element, Gd, was investigated in this work as the magnetic ion source for the DMS. Single- phase and strain-free GaTMN films were obtained. Optical measurements revealed that Mn is a deep acceptor in GaN, while Hall measurements showed that these GaTMN films were semi-insulating, making carrier mediated exchange unlikely. Hysteresis curves were obtained for all the GaTMN films, and by analyzing the effect of n- and p-dopants on the magnetic properties of these films it was determined that the magnetization is due to magnetic clusters. These findings are supported by the investigation of the effect of TM dopants in GaN nanostructures which reveal that TMs enhance nucleation resulting in superparamagnetic nanostructures. Additionally, this work presents the first report on the development of GaGdN by MOCVD providing an alternate route to developing a RT DMS. Room temperature magnetization results revealed that the magnetization strength increases with Gd concentration and can be enhanced by n- and p-doping, with holes being more efficient at stabilizing the ferromagnetic signal. The GaGdN films obtained in this work are single-phase, unstrained, and conductive making them suitable for the development of multifunctional devices that integrate electrical, optical, and magnetic properties.

Nuclear magnetic resonance force microscopy (NMRFM) is a technique that combines aspects of scanning probe microscopy (SPM) and nuclear magnetic resonance (NMR) to obtain 3 dimensional nanoscale spatial resolution and perform spectroscopy. We describe the components of a helium-3 NMRFM probe and studies of ammonium sulfate ((NH₄)₂SO₄) and magnesium diboride (MgB₂). For our room temperature (NH₄)₂SO₄ studies we were able to perform a 1-D scan and perform nutation and spin echo experiments. In our 77 K MgB₂ we demonstrate a 1-D scan of a 30 micron powder sample. In addition, we describe magnetic measurements of the possible dilute semiconductors Mn[subscript x]Sc[subscript 1-x]N and Fe₀.₁Sc₀.₉N. / text

Submitted by Regina Correa (rehecorrea@gmail.com) on 2016-09-21T18:57:01Z No. of bitstreams: 1 TeseLKSH.pdf: 62711757 bytes, checksum: dd2b481497af4493346131729910c613 (MD5) / Approved for entry into archive by Marina Freitas (marinapf@ufscar.br) on 2016-09-23T18:36:35Z (GMT) No. of bitstreams: 1 TeseLKSH.pdf: 62711757 bytes, checksum: dd2b481497af4493346131729910c613 (MD5) / Approved for entry into archive by Marina Freitas (marinapf@ufscar.br) on 2016-09-23T18:36:40Z (GMT) No. of bitstreams: 1 TeseLKSH.pdf: 62711757 bytes, checksum: dd2b481497af4493346131729910c613 (MD5) / Made available in DSpace on 2016-09-23T18:36:47Z (GMT). No. of bitstreams: 1 TeseLKSH.pdf: 62711757 bytes, checksum: dd2b481497af4493346131729910c613 (MD5) Previous issue date: 2015-12-14 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) / Defects play a fundamental issue on physical properties of wide bandgap semiconductors (WBS) due to the possibility of application in high temperature. This work shows the features of the defects in di erent kind of WBS grown/synthesized by solid state reaction, Pechini method and Molecular Beam Epitaxy. First we investigated the structural and optical properties of erbium- and manganese-doped strontium aluminates (SrAl2O4). The fundamental optical transitions due to Er3+ and Mn2+ are typical features of the well-diluted doping process. A signi cant enhancement of the Er3+ optical emission band at 1530 nm was observed when the matrix is co-doped with Mn. A model of energy transfer mechanism from Mn2+ to Er3+ is proposed to explain the experimental results. We present also the e ect of preparation and annealing conditions on the properties of Nb2O5. The increase of oxygen vacancies causes an inrreversible phase transition from pseudohexagonal to orthorhombic phase, and they are responsible for the increase in the e ective magnetic moments related to paramagnetic behavior. Finally, we explore the e ects of the interfaces imperfections of quantum wells of cubic GaN alloys. An indication of localized states in low temperature is observed. A decrease of this e ects happens when we increase the number of interfaces. Furthermore, magneto-PL measurements show a higher spin polarizations in the donor-acceptor impurities in the bulk of c-GaN corroborate for the importance of the defects. This work shows that the defects engineering in WBS are fundametal for developing new technologies in spintronics and optoelectronic eld. / Os defeitos em semicondutores acarretam mudanças nas propriedades físicas do material, tendo uma grande importância nos semicondutores que possuem alta energia de gap devido à possibilidade de aplicação em alta temperatura. No presente trabalho, estudamos as características atribuídas à presença de defeitos em diferentes semicondutores de gap largo, crescidos/sintetizados por reação de estado sólido, método de Pechini e epitaxia de feixes moleculares. Primeiramente, investigamos as propriedades ópticas e estruturais do aluminato de estrôncio (SrAl2O4) dopado com érbio e co-dopado com manganês. Neste caso, um aumento na emissão do Er3+ na região do infravermelho (1530 nm) foi observado na matriz com co-dopagem de manganês. Atribuímos este efeito ao mecanismo de transferência de energia do íon de Mn2+ para o Er3+. Também estudamos os efeitos das condições de preparação e tratamento térmico nas propriedades de pentóxido de nióbio (Nb2O5). Nossa investigação, mostra que vacâncias de oxigênio causam transições irreversíveis da fase pseudo-hexagonal para a ortorrômbica. Além disso, esses defeitos são responsáveis por um acréscimo de momentos magnéticos efetivos, relacionados com o comportamento paramagnético. Por último, averiguamos os efeitos de imperfeições entre as interfaces de poços quânticos de ligas de nitreto de gálio cúbico (cGaN). Esse estudo indicou uma diminuição de estados localizados, em baixa temperatura, com a mudança na quantidade de interfaces do QW. No caso do c GaN bulk, foi observado uma maior polarização de spin na emissão óptica da impureza doadora-aceitadora. Este trabalho evidencia a importância da engenharia de defeitos em semicondutores de gap largo para o aperfeiçoamento de tecnologias ligadas à área de optoeletrônica e spintrônica.

Nanotechnology is the science and engineering of creating functional materials by precise control of matter at nanometer (nm) length scale and exploring novel properties at that scale. It is vital to understand the quantum mechanical phenomena manifested at nanometer scale dimensions since that will enable us to precisely engineer quantum mechanical properties to realize novel device functionalities. This dissertation investigates optical and electronic properties of compound and transition metal doped compound semiconductor nanowires with a view to exploiting them for a wide range of applications in semiconductor electronic and optical devices. In this dissertation work, basic concepts of optical and electronic properties at low dimensional structures will be discussed in chapter 1. Chapter 2 discusses the nanofabrication technique employed to fabricate highly ordered nanowires. Using this method, which is based on electrochemical self-assembly techniques, we can fabricate highly ordered and size controlled nanowires and quantum dots of different materials. In Chapter 3, we report size dependent fluorescence spectroscopy of ZnSe and Mn doped ZnSe nanowires fabricated by the above method. The nanowires exhibit blue shift in the emission spectrum due to quantum confinement effect, which increases the effective bandgap of the semiconductor. We found that the fluorescence spectrum of Mn doped ZnSe nanowires shows high luminescence efficiency, which seems to increase with increasing Mn concentration. These results are highly encouraging for applications in multi spectral displays. Chapter 4 investigates field emission results of highly ordered 50 nm tapered ZnO nanowires that were also fabricated by electrochemical self-assembly. Subsequent to fabrication, the nanowires tips are exposed by chemical etching which renders the tips conical in shape. This tapered shape concentrates the electric field lines at the tip of the wires, and that, in turn, increases the emission current density while lowering the threshold field for the onset of field emission. Measurement of the Fowler-Nordheim tunneling current carried out in partial vacuum indicates that the threshold electric field for field emission in 50-nm diameter ZnO nanowires is 15 V/µm. In this study we identified the key constraint that can increase the threshold field and reduce emission current density. In Chapter 5 we report optical and magnetic measurement of Mn-doped ZnO nanowires. Hysterisis measurements carried out at various temperatures show a ferromagnetic behavior with a Curie temperature of ~ 200 K. We also studied Mn-doping of the ZnO nanowires. The room temperature fluorescence spectroscopy of Mn-doped ZnO nanowires shows a red-shift in the spectra compared to the undoped ZnO nanowires possibly due to strain introduced by the dopants in the nanowires. Finally, in Chapter 6, we report our study of the ensemble averaged transverse spin relaxation time (T2*) in InSb thin films and nanowires using electron spin resonance (ESR) measurement. Unfortunately, the nanowires contained too few spins to produce a detectable signal in our apparatus, but the thin films contained enough spins (> 109/cm2) to produce a measurable ESR signal. We found that the T2* decreases rapidly with increasing temperature between 3.5 K and 20 K, which indicates that spin-dephasing is primarily caused by spin-phonon interactions.