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In this work we study thin epilayers of new antiferromagnetic semimetal CuMnAs by time- resolved magneto-optical experiments. In 10 nm layers of CuMnAs, we observed a harmonic dependence of the dynamical magneto-optical signal on the orientation of probe pulse linear polarization. This shows that in this 10 nm layer there is an in-plane uniaxial magnetic anisotropy which can be detected due to a quadratic magneto-optical effect - magnetic linear dichroism. From the measured data we also estimated the Néel temperature and the spectral variation of the magneto-optical coefficient describing the magnitude of the magnetic linear dichroism in this sample.

In processing and data storage mainly ferromagnetic (FM) materials are being used. Approaching physical limits, new concepts have to be found for faster, smaller switches, for higher data densities and more energy efficiency. Some of the discussed new concepts involve the material classes of correlated oxides and materials with antiferromagnetic coupling. Their applicability depends critically on their switching behavior, i.e., how fast and how energy efficient material properties can be manipulated. This thesis presents investigations of ultrafast non-equilibrium phase transitions on such new materials. In transition metal oxides (TMOs) the coupling of different degrees of freedom and resulting low energy excitation spectrum often result in spectacular changes of macroscopic properties (colossal magneto resistance, superconductivity, metal-to-insulator transitions) often accompanied by nanoscale order of spins, charges, orbital occupation and by lattice distortions, which make these material attractive. Magnetite served as a prototype for functional TMOs showing a metal-to-insulator-transition (MIT) at T = 123 K. By probing the charge and orbital order as well as the structure after an optical excitation we found that the electronic order and the structural distortion, characteristics of the insulating phase in thermal equilibrium, are destroyed within the experimental resolution of 300 fs. The MIT itself occurs on a 1.5 ps timescale. It shows that MITs in functional materials are several thousand times faster than switching processes in semiconductors. Recently ferrimagnetic and antiferromagnetic (AFM) materials have become interesting. It was shown in ferrimagnetic GdFeCo, that the transfer of angular momentum between two opposed FM subsystems with different time constants leads to a switching of the magnetization after laser pulse excitation. In addition it was theoretically predicted that demagnetization dynamics in AFM should occur faster than in FM materials as no net angular momentum has to be transferred out of the spin system. We investigated two different AFM materials in order to learn more about their ultrafast dynamics. In Ho, a metallic AFM below T ≈ 130 K, we found that the AFM Ho can not only be faster but also ten times more energy efficiently destroyed as order in FM comparable metals. In EuTe, an AFM semiconductor below T ≈ 10 K, we compared the loss of magnetization and laser-induced structural distortion in one and the same experiment. Our experiment shows that they are effectively disentangled. An exception is an ultrafast release of lattice dynamics, which we assign to the release of magnetostriction. The results presented here were obtained with time-resolved resonant soft x-ray diffraction at the Femtoslicing source of the Helmholtz-Zentrum Berlin and at the free-electron laser in Stanford (LCLS). In addition the development and setup of a new UHV-diffractometer for these experiments will be reported. / In der Datenspeichertechnologie werden bisher hauptsächlich ferromagnetische Materialien eingesetzt. Da mit diesen aber physikalische Grenzen erreicht werden, werden neue Konzepte gesucht, um schnellere und kleinere Schalter, größere Datendichten und eine höherere Energieeffizienz zu erzeugen. Unter den diskutierten Materialklassen finden sich komplexen Übergangsmetalloxide und Materialien mit antiferromagnetischer Kopplung. Die Anwendbarkeit solcher Materialien hängt stark davon ab, wie schnell sich deren Eigenschaften verändern lassen und wieviel Energie dafür eingesetzt werden muss. Die vorliegende Arbeit beschäftigt sich mit ultraschnellen, Nicht-Gleichgewicht-Phasenübergängen genau in solchen Materialien. In Übergangsmetalloxiden führt die enge Kopplung zwischen den unterschiedlichen Freiheitsgraden zu einem effektiven niederenergetischen Anregungsspektrum. Diese Anregungen sind oft verknüpft mit spektakulären makroskopischen Eigenschaften, wie z.B. dem kolossalen Magnetowiderstand, Hochtemperatur-Supraleitung, Metall- Isolator-Übergang, die oft von nanoskaliger Ordnung von Spins, Ladungen, orbitaler Besetzung sowie Gitterverzerrungen begleitet sind. Dadurch werden diese Materialien interessant für Anwendbarkeit. Magnetit, ein Prototyp eines solchen funktionalen Materials zeigt einen Metall-Isolator-Übergang bei T = 123 K. Untersucht man die Ladungs- und orbitale Ordnung sowie die Struktur nach einer optischen Anregung, so findet man, dass die elektronische Struktur und Gitterverzerrung, die kennzeichnend für die Tieftemperaturphase sind, innerhalb der Zeitauflösung des Experiments von 300 fs zerstört wird. Der eigentliche Metall-Isolator-Übergang zeigt sich erst nach 1.5 ps. Die Ergebnisse zeigen, dass MITs in funktionalen Materialien bis zu tausend Mal schneller geschaltet werden können als in vorhandenen Halbleiter-Schaltern. Seit kurzem rücken auch ferrimagnetische und antiferromagnetische Materialen in den Fokus des Interesses. Es wurde im Ferrimagnet GdFeCo gezeigt, dass der Transfer von Drehimpuls zwischen zwei entgegengesetzten Subsystemen mit unterschiedlichen Zeitkonstanten zu einem Umschalten der Magnetisierung führt. Zudem wurde vorhergesagt, dass Demagnetisierungsdynamiken in antiferromagnetischen Materialien schneller ablaufen soll als in ferromagnetischen, da kein Drehimpuls aus dem Spinsystem abgeführt werden muss. Damit wir mehr über antiferromagnetische Dynamik erfahren haben wir zwei unterschiedliche Antiferromagneten untersucht, um sie mit den bekannten FM zu vergleichen. Im metallischen AFM Holmium fanden wir, dass die magnetische Ordnung schneller und zehnmal energieeffizienter zerstört werden kann als in vergleichbaren FM Metallen. In Europium-Tellurid, einem antiferromagnetischem Halbleiter, haben wir den Zerfall der magnetischen Ordnung im Hinblick auf Wechselwirkungen mit der Struktur untersucht. Wir fanden auf kurzen Zeitskalen eine eher entkoppelte Dynamik. Eine Ausnahme ist ein schneller Beitrag zur Gitterdynamik, den wir mit dem Wegfall von Magnetostriktion erklären. Die hier gezeigten Ergebnisse wurden mit Hilfe zeitaufgelöster resonanter weicher Röntgenbeugung an der Femtoslicing Strahlungsquelle des Helmholtz-Zentrums Berlin und am freien Elektronenlaser LCLS gemessen. Zusätzlich wird über die Entwicklung und den Bau eines UHV-Diffraktometers für diese Experimente berichtet.

Made available in DSpace on 2014-10-09T12:40:47Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:08:00Z (GMT). No. of bitstreams: 1 02947.pdf: 6721410 bytes, checksum: 6b8fd88ede9d8533a129cf94a67a4313 (MD5) / Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP / FAPESP:92/02990-0

Made available in DSpace on 2016-12-12T20:15:50Z (GMT). No. of bitstreams: 1 Douglas Nascimento.pdf: 4060178 bytes, checksum: 878a0a0c64fd603563f3de3e4f166d98 (MD5) Previous issue date: 2013-03-14 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / The Kondo lattice model,also known as the double exchange model, is used to describe materials that have magnetic moments localized and conduction electrons.We consider an antiferromagnetic material composed of two sublattices forming an interpenetrating simple cubic lattice. Assuming a ferromagnetic coupling JK > 0 between the conduction electrons and the localized magnetic moments, the magnetization of the conduction electrons is obtained through the Green functions by means of the equation of motion and the magnetization of the localized spins is determined via the Brillouin function in the approximation molecular field. In the mean field approximation, the phase diagrams JK −n e h−T, including the phases ferromagnetic (FM) and antiferromagnetic (AF), are obtained. The curves ΔS exhibit differents behavior for differents intensities of the applied magnetic field, these behaviors are analyzed using diagrams JK − n e h − T. / O modelo da rede de Kondo, também conhecido como modelo da dupla troca, é utilizado para descrever materiais que possuem momentos magnéticos localizados e elétrons de condução. É considerado um material antiferromagnético composto por duas subredes interpenetrantes formando uma rede cúbica simples. Assumindo um acoplamento ferromagnético JK > 0 entre os elétrons de condução e os momentos magnéticos localizados, a magnetização dos elétrons de condução é obtida através das funções de Green por meio da equação de movimento e a magnetização dos spins localizados é determinada via função de Brillouin na aproximação de campo molecular. Na aproximação de campo médio, os diagramas de fases JK − n e h − T, incluindo as fases ferromagnetica (FM) e antiferromagnética (AF), são obtidos. As curvas de ΔS exibem comportamentos distintos para diferentes intensidades de campo magnético aplicado, sendo estes comportamentos analisados por meio dos diagramas JK − n e h − T.

Made available in DSpace on 2014-10-09T12:40:47Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:08:00Z (GMT). No. of bitstreams: 1 02947.pdf: 6721410 bytes, checksum: 6b8fd88ede9d8533a129cf94a67a4313 (MD5) / Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP / FAPESP:92/02990-0

<p> The magnetic properties of MnP2O7, CuP2O7, Co2P2O7 and Ni2P2O7 were studied. They were investigated using magnetic susceptibility and magnetic resonance techniques. They were all found to become magnetically ordered between 10°K and 30°K. In all the predominant exchange interaction was antiferromagnetic. Ni2P2O7 however did show a resultant moment at low temperatures which was attributed to weak ferrornagnetism. The experimental results were analysed in the molecular field approxmation which accounted for their behaviour except in the case of Cu2P2O7 where the High Temperature Series Expansion method was necessary to explain the temperature dependence of its paramagnetic susceptibility. </p> / Thesis / Doctor of Philosophy (PhD)

Manipulation of ferromagnetic (FM) spins (and spin textures) using an antiferromagnet (AFM) as an active element in exchange coupled AFM/FM heterostructures is a promising branch of spintronics. Recent ground-breaking experimental demonstrations, such as electrical manipulation of the interfacial exchange coupling and FM spins, as well as ultrafast control of the interfacial exchange-coupling torque in AFM/FM heterostructures, have paved the way towards ultrafast spintronic devices for data storage and neuromorphic computing device applications.[5,6] To achieve electrical manipulation of FM spins, AFMs offer an efficient alternative to passive heavy metal electrodes (e.g., Pt, Pd, W, and Ta) for converting charge current to pure spin current. However, AFM thin films are often integrated into complex heterostructured thin film architectures resulting in chemical, structural, and magnetic disorder. The structural and magnetic disorder in AFM/FM-based spintronic devices can lead to highly undesirable properties, namely thermal dependence of the AFM anisotropy energy barrier, fluctuations in the magnetoresistance, non-linear operation, interfacial spin memory loss, extrinsic contributions to the effective magnetic damping in the adjacent FM, decrease in the effective spin Hall angle, atypical magnetotransport phenomena and distorted interfacial spin structure. Therefore, controlling the magnetic order down to the nanoscale in exchange coupled AFM/FM-based heterostructures is of fundamental importance. However, the impact of fractional variation in the magnetic order at the nanoscale on the magnetization reversal, magnetization dynamics, interfacial spin transport, and the interfacial domain structure of AFM/FM-based heterostructures remains a critical barrier. To address the aforementioned challenges, we conduct a comprehensive experimental investigation of chemical, structural, magnetization reversal (integral and element-specific), magnetization dynamics, and magnetotransport properties, combined with high-resolution magnetic imaging of the exchange coupled Ni3Fe/IrMn3-based heterostructures. Initially, we study the chemical, structural, electrical, and magnetic properties of epitaxially textured MgO(001)/IrMn3(0-35 nm)/Ni3Fe(15 nm)/Al2O3(2.0 nm) heterostructures. We reveal the impact of magnetic field annealing on the interdiffusion at the IrMn3/Ni3Fe interface, electrical resistivity, and magnetic properties of the heterostructures. We further present an AFM IrMn3 film thickness dependence of the exchange bias field, coercive field, magnetization reversal, and magnetization dynamics of the exchange coupled heterostructures. These experiments reveal a strong correlation between the chemical, structural and magnetic properties of the IrMn3-based heterostructures. We find a significant decrease in the spin-mixing conductance of the chemically-disordered IrMn3/Ni3Fe interface compared to the chemically-ordered counterpart. Independent of the AFM film thickness, we unveil that thermally disordered AFM grains exist in all the samples (measured up to 35-nm-thick IrMn3 films). We develop an iterative magnetic field cooling procedure to systematically manipulate the orientation of the thermally disordered and reversible AFM moments and thus, achieve tunable magnetic, and magnetotransport properties of exchange coupled AFM-based heterostructures. Subsequently, we investigate the impact of fractional variation in the AFM order on the magnetization reversal and magnetotransport properties of the epitaxially textured ɣ-phase IrMn3/Ni3Fe, Ni3Fe/IrMn3/Ni3Fe, and Ni3Fe/IrMn3/Ni3Fe/CoO heterostructures. We probe the element-specific (FM: Ni and Co, and AFM: Mn) magnetization reversal properties of the exchange coupled Ni3Fe/IrMn3/Ni3Fe/Co/CoO heterostructures in various magnetic field cooled states. We present a detailed procedure for separating the spin and orbital moment contributions for magnetic elements using the XMCD sum rule. We address whether Mauri-type domain walls can develop at the (polycrystalline) exchange coupled Ni3Fe/IrMn3/Ni3Fe interfaces. We further study the impact of magnetic field cooling on the AFM Mn (near L2,3-edges) X-ray absorption spectra. Finally, we employ a combination of in-field high-resolution magnetic force microscopy, magnetooptical Kerr effect magnetometry with micro-focused beam, and micromagnetic simulations to study the magnetic vortex structures in exchange coupled FM/AFM and AFM/FM/AFM disk structures. We examine the magnetic vortex annihilation mechanism mediated by the emergence and subsequent annihilation of the vortex-antivortex (V-AV) pairs in simple FM and exchange coupled FM/AFM as well as AFM/FM/AFM disk structures. We image the distorted magnetic vortex structures in exchange coupled FM/AFM disks proposed by Gilbert and coworkers. We further emphasize crucial magnetic vortex properties, such as handedness, effective vortex core radius, core displacement at remanence, nucleation field, annihilation field, and exchange bias field. Our experimental inquiry offers profound insight into the interfacial exchange interaction, magnetization reversal, magnetization dynamics, and interfacial spin transport of the AFM/FM-based heterostructures. Moreover, our results pave the way towards nanoscale control of the magnetic properties in AFM-based heterostructures and point towards future opportunities in the field of AFM spintronic devices.:1. Introduction 2. Magnetic Interactions and Exchange Bias Effect 3. Materials 4. Experimental Methods 5. Structural, Electrical, and Magnetization Reversal Properties of Epitaxially Textured ɣ-IrMn3/ Ni3Fe Heterostructures 6. Magnetization Dynamics of MgO(001)/IrMn3/Ni3Fe Heterostructures in the Frequency Domain 7. Tunable Magnetic and Magnetotransport Properties of MgO(001)/Ni3Fe/IrMn3/Ni3Fe/ CoO/Pt Heterostructures 8. Element-Specific XMCD Study of the Exchange Couple Ni3Fe/IrMn3/Ni3Fe/Co/CoO Heterostructures 9. Distorted Vortex Structure and Magnetic Vortex Reversal Processes in Exchange Coupled Ni3Fe/IrMn3 Disk Structures 10. Conclusions and Outlook Addendum Acronyms Symbols Publication List Author Information Acknowledgments Statement of Authorship

The process of assembling metal nanoparticles at the interface of two liquids has received a great interest over the past few years due to a wide range of important applications and their unusual properties compared to bulk materials. The work in this thesis presents a low cost, simple and cheap synthesis of metal nanoparticles, core/shell structures and semiconductors followed by assembly of these particles between immiscible liquids. The aim of this thesis is divided to three parts (Summary of the experimental work of this thesis is in Table A1):1) To achieve a closed loop recycling for producing cadmium sulfide as powders and/or nanostructured thin films for solar cells or other optoelectronic devices applications. A series of bis(dialkyldithiocarbamato)cadmium(II) were used for this approach. Bis(dioctyldithiocarbamato)cadmium(II) complexes proved to be the optimal alkyl chain for this process. The approach can be extended to other metal sulfides such as those of Zn, Pb, Cu, or Fe and many transition metals and oxides.2) To explore the phenomena of exchange bias in very small size particles (5 nm) of Ni/NiO (core/shell structure) obtained by solution phase synthesis. Ferromagnetism (FM) due to exchange bias is well established in the case of larger particles with diameters over 10 nm. However, sub 10 nm magnetic structures synthesized by solution phase have never been found to be ferromagnetic at room temperature. These Ni/NiO nanocrystals with ferromagnetic properties at room temperature were among the smallest and strongest magnets made in solution. Similar magnets can be obtained using a rare class of high anisotropy materials nearly all of which feature precious metals. This work would lead to significantly cheaper magnetic particles suited for the mass market. The applications of this work can be applied to produce viable storage devices and the other possibility is to disperse these nanocrystals in solution and use it to make ferrofluids which have a number of mature applications. Functional device architectures of these particles were rapidly and inexpensively produced as thin films using self-assembly of liquid/liquid interface process at room temperature by using octylamine as a surfactant.3) To synthesise and assemble submicron particles of silver, cobalt and nickel by using polyol methods and liquid/liquid interface, respectively. The effect of reaction conditions (solvent, precursor concentration, temperature, etc.) on synthesis and assembly of the particles was studied. Assembled cobalt and nickel as films are promising materials for spintronics, magnetic and magneto-electronics and biomedics. The nature and characteristics of the particles and their films were studied by a number of techniques such as SEM, EDX, TEM, p-XRD, UV-Vis, PL, FTIR, DLS and SQUID for magnetic measurements.

Neste trabalho, apresentamos estudos sobre o transporte eletrônico de cargas e diagramas de fase no plano ns-B em bicamadas eletrônicas ou poços quânticos duplos, formados de ligas semiconductoras de AlxGa1-xAs e GaAs, assim como também em poços quânticos triplos de GaAs. Para esta finalidade, amostras de poços duplos com diferentes concentrações de Al (x) dentro de cada poço e triplos de GaAs foram crescidas. Inicialmente, se apresenta um estudo teórico, o qual mostrou que, em poços quânticos duplos em que em cada poço a concetração de Al é diferente, a aplicação de tensões de porta permite a modulação do fator g de Landé dos elétrons confinados nesses poços. Em especial, estudou-se o caso de concentrações de Al que correspondem a valores do fator g com sinal oposto, em cada poço. Posteriormente se faz um estudo teórico da estrutura eletrônica das amostras de poços duplos e triplos, em seguida apresenta-se os fundamentos teóricos que serão de base para a interpretação de nosso resultados experimentais. Na primeira parte de nosso trabalho, medidas de magnetotransporte (Shubnikov-de Haas (SdH) e Hall), foram realizadas em todas as amostras de estudo. Na amostra de poço duplo 3242, com fator g de Landé de sinais opostos foi encontrado o colapso do gap de spin nas oscilações SdH com o incremento do campo magnético, ou seja, a soma da energia de Zeeman mais a energia de troca e correlação é igual ao potencial de desordem. Este colapso é atribuido à competição entre as energias de troca, intracamadas e intercamadas. Foi realizada uma análise das oscilações SdH através da transformada de Fourier (FFT), para mostrar que as propriedades eletrônicas tais como a concentração e mobilidade dos elétrons, nas amostras de poços duplos, decrescem à medida que aumenta a concentracão de Al. As propriedades eletrônicas nas amostras de poços triplos dependem dos parâmetros de crescimento, tal como a largura dos poços e barreira. Na segunda parte, são apresentados diagramas de fase ns-B, obtidos através da justaposição dos espectros de magnetorresistência, em amostras de poços duplos e triplos em campo magnético perpendicular e certos valores de campo inclinado. Mostra-se que, em campo magnético perpendicular, o modelo de uma partícula sem interações descreve com boa aproximação o aparecimento dos anéis no diagrama de fase para a amostra de poço duplo com g = -0,44. No entanto, na amostra com g ~ 0 o modelo não descreve em boa aproximação os diagramas de fase em campo magnético perpendicular e inclinado, precisando de um modelo que inclua termos de interação de muitos corpos para uma possível explicação. Também se prediz a existência de um estado canted antiferromagnético. O modelo também mostrará que os diagramas de fase das amostras de poços triplos têm um comportamento semelhante ao das amostras de poços duplos, quando a densidade de elétrons do poço central é baixa comparada com a densidade dos poços laterais. / In this work, we present studies about the electronic transport of charges and phase diagrams in the ns-B plane in electronic bilayers or double quantum wells formed of both AlxGa1-xAs and GaAs semiconductor alloys, also in GaAs triple quantum wells. For this purpose, double quantum wells with different aluminium compositions (Al(x)) in each well and triple quantum wells samples were growth. Firstly, a theoretical study was presented, which showed that in double quantum wells with different Al compositions, the aplication of gate voltages allow the modulation of the Landé g factor of the electrons confined within each well. In particular, the case where the quantum wells have different Al compositions was studied, which lead to the opposite signs of the electronic g-factor in each well. After this, a theoretical study of the electronic structure has been presented of both double and triple quantum wells, then, a basic theory has been presented, which will be the base for the interpretation of our experimental results. At the frst part of our work, magnetotransport measurements (Shubnikov-de Haas (SdH) and Hall) were performed in all the studied samples. In the double quantum well sample (3242), wich has Landé g-factor with opposite signs in each well, was found the spin gap collapse at the Shubnikov-de Haas oscillations with an increase in the magnetic field, that is, the sum of the bare Zeeman energy and exchange potencial energy has the same magnitude of the disorder potencial. This collapse was attributed to the competition between the interlayer and intralayer exchange energies. Fast Fourier transform (FFT) of the Shubnikov-de Haas oscillations was performed in the double and triple quantum well samples to show that the electronic properties, such as electron density and mobility decrease with the increase of the Al compositions. On the other hand, the electronic properties on the triple quantum well samples depend on growth parameters, such as width and heigh barriers of the wells. At the second part ns- B phase diagrams were determined through the superposed longitudinal magnetoresistance, in the double and triple quantum wells samples at the perpendicular magnetic field and certain values of tilted magnetic fields. It has been shown that in a perpendicular magnetic field a single particle model describes in a good aproximation the appearance of ring structures in the phase diagram of the double quantum well with g = -0:44. Meanwhile, at the sample with vanishing Landé g-factor (g ~ 0) the single particle model can not describe in a good approximation the phase diagram, being a requirement a many particle model for an possivel explanation. It has also been predicted the existence of a canted antiferromagnetic state. Finally, the model will also showed the phase diagram of triple quantum wells are similar to double quantum wells, when the electron density of the middle well is low compared to the side wells.