Oxide heterostructures are attracting huge interest in recent years due to the special functionalities of quasi two-dimensional quantum gases. In this thesis, the electronic states at the interface between perovskite oxides and pyrite compounds have been studied by first-principles calculations based on density functional theory. Optimization of the atomic positions are taken into account, which is considered very important at interfaces, as observed in the case of LaAlO3/SrTiO3. The creation of metallic states at the interfaces thus is explained in terms of charge transfer between the transition metal and oxygen atoms near the interface. It is observed that with typical thicknesses of at least 10-12 °A the gases still extend considerably in the third dimension, which essentially determines the magnitude of quantum mechanical effects. To overcome this problem, we propose incorporation of highly electronegative cations (such as Ag) in the oxides. A fundamental interest is also the thermodynamic stability of the interfaces due to the possibility of atomic intermixing in the interface region. Therefore, different cation intermixed configurations are taken into account for the interfaces aiming at the energetically stable state. The effect of O vacancies is also discussed for both polar and non-polar heterostructures. The interface metallicity is enhanced for the polar system with the creation of O vacancies, while the clean interface at the non-polar heterostructure exhibits an insulating state and becomes metallic in presence of O vacancy. The O vacancy formation energies are calculated and explained in terms of the increasing electronegativity and effective volume of A the side cation. Along with these, the electronic and magnetic properties of an interface between the ferromagnetic metal CoS2 and the non-magnetic semiconductor FeS2 is investigated. We find that this contact shows a metallic character. The CoS2 stays quasi half metallic at the interface, while the FeS2 becomes metallic. At the interface, ferromagnetic ordering is found to be energetically favorable as compared to antiferromagnetic ordering. Furthermore, tensile strain is shown to strongly enhance the spin polarization so that a virtually half-metallic interface can be achieved, for comparably moderate strain. Our detailed study is aimed at complementing experiments on various oxide interfaces and obtaining a general picture how factors like cations, anions, their atomic weights and elecronegativities, O vacancies, lattice mismatch, lattice relaxation, magnetism etc play a combined role in device design.

Crystalline systems formed with transition metal elements tend to exhibit strong magneto-structural coupling that gives rise to unusual but exciting physical phenomena in these materials. In this dissertation, we present our findings from the studies of structural and physical properties of single phase compounds Co2MnSi, Ni16Mn6Si7 and Mn(Ni0.6Si0.4)2. In addition, the stability of a Ni2MnSi composition in a multiphase system is discussed by both theoretical and experimental approaches. All the works have been conducted with a focus on explaining the fundamental behaviors of these systems that have not been adequately addressed by other studies in the literature. We present an experimental and theoretical investigation of the half-metallic Heusler compound, Co2MnSi to address disorder occupancies and magnetic interactions in the material. Contrary to previous studies, our neutron diffraction refinement of the polycrystalline sample reveals almost identical amount of Mn and Co antisite disorders of ~6.5% and ~7.6%, respectively which is also supported explicitly by our first-principles calculations on the system with defects. A reduction of the net moment of Co2MnSi due to an antiferromagnetic interaction introduced by disordered Mn is observed by our theoretical study. The neutron refinements at 298 K, 100 K, and 4 K further supports such reduction of moments. The work also reports the growth of single crystal by the Czochralski method and determination of a Curie temperature of ~1014 K measured by both the electrical resistivity and dilatometry measurement. Studies of a Ni2MnSi Heusler system reveal two new systems i.e., the Ni16Mn6Si7 G-phase and the Mn(Ni0.6Si0.4)2 based Laves phase with complex crystal structures. These systems exhibit strong magneto-structural coupling that could lead to interesting physical behaviors. The lack of thorough understanding of the properties of these materials inspired us to undertake the present studies. We address the geometrically frustrated two-dimensional magnetic structure and spin canted weak ferromagnetic behavior of Ni16Mn6Si7. Our magnetization and specific heat measurements on a Czochralski grown single crystal sample depicts the paramagnetic to antiferromagnetic transition at 197 K, and a second phase change at 50 K. Furthermore, a gradual drop of zero field cooled magnetic susceptibility is observed below 6 K that is associated with the spin freezing effect. The neutron diffraction on the polycrystalline powder samples at the temperatures of interest reveals that the antiferromagnetism is governed by the magnetic ordering of the Mn ions in the octahedral network. Below the Néel temperature of 197 K, the 2/3 of Mn atom moments form a two-dimensional magnetic arrangement, while the 1/3 moments remain geometrically frustrated. The phase transition at 50 K is found to be associated with the reorientation of the 2D moments to a canted antiferromagnetic state and development of ordering of the frustrated paramagnetic ions. Magnetization measurements as a function of temperature and magnetic field in principal directions, permit to determine the anisotropic magnetic behavior of Ni16Mn6Si7 in terms of the magnetic structure obtained by the neutron diffraction measurements. We also report an irreversible smeared spin-flop type transition for the system at a higher magnetic field. The diffuse scattering due to the short-range ordering is a commonly occurring phenomenon in Laves phase materials. The occurrence of such distinct atomic arrangement can considerably influence the physical behavior of the material. Nevertheless, no structural reconstruction of such atomic distribution in Laves phase has ever been reported in the literature. In this work, we present the structural ordering, and the associated physical behavior of an antiferromagnetic Ni-Mn-Si Laves phase with a composition Mn(Ni0.6Si0.4)2. The possibility of unique short-range ordering in the material is first concluded based on our single crystal diffraction analysis. With the high-resolution transmission electron microscopy and electron energy loss spectroscopy analysis, our work resolves the distinct atomic ordering of the Laves phase system. The investigations reveal the origin of the short-range ordering to arise from a unique arrangement between Ni and Si. The study also presents the atomic resolution mapping of the Si atoms which has never been reported by any previous studies. With further electrical conductivity measurement, we find one of the consequences of the unique ordering reflected in a semiconducting like temperature dependence of the compound. The neutron diffraction at 298 K suggests Mn(Ni0.6Si0.4)2 to be a strong antiferromagnetic system, which is further supported by the successive magnetic susceptibility measurement. The Néel temperature is determined to be 550 K. We also address the stability of the hypothetical ferromagnetic Heusler compound Ni2MnSi which has been proposed to be a stable system by numerous theoretical studies. Our first-principles work corroborates those studies with a negative formation enthalpy of -1.46 eV/formula unit. However, after numerous attempts to synthesize the composition, we conclude that a single phase Heusler Ni2MnSi compound cannot form under ambient conditions. Our results show that the system crystallizes as a mixture of the two Ni-Mn-Si compounds, i.e., the Ni16Mn6Si7 type G-phase and Mn(Ni0.6Si0.4)2 based Laves phase. Our work provides a possible explanation for the unstable Ni2MnSi Heusler compound with the calculation of formation enthalpy of the hypothetical Heusler system in terms of the computed energies of the neighboring phases Ni16Mn6Si7 and Mn(Ni0.6Si0.4)2. / Thesis / Doctor of Philosophy (PhD)

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Das Co2FeSi/GaAs-Hybridsystem wurde hinsichtlich seiner Eignung für Anwendungen in der Spintronik untersucht. Die Heusler-Legierung Co2FeSi ist ein aussichtsreicher Kandidat für derartige Anwendungen, weil der vollständig geordneten Kristallphase Halbmetallizität, d. h. eine Spinpolarisation von 100% an der Fermi-Energie, vorhergesagt wird. Zunächst wurde im Rahmen dieser Arbeit die elektrische Spininjektion und Spindetektion in lateralen Transportstrukturen in der sogenannten nicht-lokalen Konfiguration sowohl für die vollständig geordnete, als auch für eine teilweise ungeordnete Kristallphase mittels Spinventil- und Hanle-Messungen nachgewiesen. Die Abhängigkeiten der Spinsignale vom Strom und von der Temperatur konnten erklärt werden und eine Spininjektionsefizienz von 16 bzw. 9% wurde ermittelt. Für den praktischen Einsatz werden allerdings lokale Spinventile benötigt, deren Funktionsfähigkeit für beide kristallinen Ordnungen demonstriert wurde. Der Magnetowiderstand, der ein Maß für die Güte der lokalen Spinventile darstellt, beträgt 0.03% und liegt im Bereich des theoretisch zu erwartenden Wertes. Anhand des sogenannten Fert-Kriteriums konnten die Gründe für diesen niedrigen Wert aufgezeigt werden. Des Weiteren ließ ein Vergleich der lokalen und nicht-lokalen Spinsignale auf eine hohe Spinpolarisation des Co2FeSi schließen. Die Spinextraktion bietet neben der Spininjektion eine weitere Möglichkeit zur Erzeugung einer Spinakkumulation in einem Halbleiter. Die Stromabhängigkeiten von Spininjektion und Spinextraktion unterscheiden sich für beide kristallinen Phasen des Co2FeSi. Das stark unterschiedliche Verhalten konnte anhand des Einflusses der jeweiligen Bandstruktur auf die Spinerzeugung erklärt werden. Des Weiteren konnte aus dem Vergleich zwischen der Messungen und der theoretisch vorhergesagten Bandstruktur der halbmetallische Charakter der vollständig geordneten Kristallphase nachgewiesen werden. / The Co2FeSi/GaAs hybrid system was investigated regarding its suitability for spintronic applications. The Heusler-compound Co2FeSi is a promissing canditate for these kind of applications due to the predicted half-metallicity, i. e. a 100% spin polarisation at the Fermi energy, for its fully ordered crystall phase. The electrical spin injection and detection was demonstrated in lateral tranpost structures in the so called non-local geometry for the fully ordered and for a partly disordered crystall phase by observing spin valve signatures and Hanle characteristics. The current and temperature dependence of the spin signals was explained and a respective spin injection efficiencies of 16 and 9% determined. For practical use one needs local spin valves, which where demonstrated for both crystalline phases. The magnetoresistance, a measure of the goodness of a local spin valve, was 0.03%, i. e. in the theoretically expected range. Making use of the so-called Fert criterion the reasons for this low value could be pointed out. Further the quotient of the local and non-local spin signals implied a high spin polarisation of the Co2FeSi. Spin extraction is another method to create a spin accumulation in a semiconductor. The current dependece of the spin injection and the spin extraction signals strongly depends on the degree of ordering in the Co2FeSi lattice. The different behavior is explanied by the crucial influence of the respective electronic band structure on the spin generation processes. Further, the comparison between the measured signals and the theoretically calculated electronic band structure hints towards the half-metalicity of the fully ordered crystall phase of Co2FeSi.