A new method for dynamic chirality control of a magnetic vortex is demonstrated with micromagnetic simulations. Spin transfer torque and giant magnetoresistance in an asymmetric spin valve nanopillar provide fast, reliable, and compact single-bit manipulation and readout. Magnetization relaxation following chirality switching proceeds via formation and dissipation of spin wave eigenmodes. Combined time- and frequency-domain analysis reveals a novel radial eigenmode spectrum with large edge amplitudes and nonuniform phase in the fundamental mode, in contrast with existing analytical models and experimental precedents. With the aim to determine the sources of this departure, we implement signal processing methods to identify and characterize the effects of interlayer coupling and nanoscale spatial confinement on the magnetization dynamics. Variation of the interlayer coupling and relative chirality is found to modify the eigenfrequencies but not the eigenfunctions. Examination of the interlayer phase and dynamic stray field provides quantitative and qualitative explanation of frequency splitting with relative chirality. / Graduate / 0611, 0607

Nanoscale materials behave differently than their bulk counterparts due, in part, to the reduced length scales and the increased surface to core atom ratio. As the length scales decrease, the surface atoms become increasingly important as they make up a larger percentage of the total number of atoms. These surface atoms have magnetic properties that differ from the core atoms due to a surface anisotropy that alters the interparticle, intraparticle, and exchange interactions. In this work, we have synthesized three different nanoscale systems that will allow us to explore the physics of the different interactions. Cu/gamma-Fe2O3 core/shell nanoparticles were chosen because the gamma-Fe2O3 cores have vacancies in their B-sites, broken coordination at the surface, and experience superexchange interactions. As a comparison, multiphase undoped and V-doped SiO2/FeCo nanoparticles were chosen as these nanoparticles do not suffer from vacancies or surface disorder and experience both direct exchange interactions from the nanoparticle core and superexchange interactions between the FeCo core and the metal silicate interfacial phase. Finally, Fe nanocrystallites were grown in a Cu matrix as they present no vacancies or surface disorder, and they are single phase. We observed that the interfacial phases that form in these core/shell and nanocrystallite/matrix nanoscale systems alters significantly the physics of the magnetism. The overall magnetic properties, the elemental magnetism, and the atomic magnetism were all observed to be altered by this interfacial phase, along with the interparticle and intraparticle interactions. In addition, the thickness of this interfacial phase, and thus the strength of its affect, was controlled by controlling the thickness of the shells or the amount of intermixing in the case of the nanostructured thin film. / February 2016

Two-dimensional electron gases (2DEG) located at GaAs/Al0.33Ga0.67As heterojunctions are modulated by a periodic magnetic field generated by a magnetic grating fabricated at the surface of the heterostructure and are irradiated by microwaves. The devices were investigated for the detection of excitations of both paramagnetic and ferromagnetic spins in the magnetoresistance. Electron spin antiresonance was electrically detected, where spin flips are propelled by two transitions: one activated by snake orbit oscillations in the slanted magnetic field, the other by the microwaves. The double resonance forms a dark state which blocks spin flips, decreases Overhauser shift and freezes snake orbit drift, therefore changing the conduction in the 2DEG. The antiresonance is quantitatively described in the coherent population trapping framework. Collective and localised spin wave modes in dysprosium and cobalt gratings were detected as well in the 2DEG. Such effects were investigated as a function of microwave power, temperature, tilt angle of the applied magnetic field, and by varying the structural and material parameters to change the strength of dipolar interactions. The data reveal two types of spin waves. Dipolar magnetisation waves propagate across the grating through the magnetostatic interaction between stripes. An analytical expression of their dispersion curve was derived and a good fit of the ferromagnetic resonance broadening was obtained. The second type are dipolar edge spin waves which manifest through a series of sharp resonances at lower magnetic field. These waves are confined near the pole surfaces in spin wave ”wells”. The eigenfrequencies of the quantised modes were calculated and a qualitative explanation of the low field resonances was obtained. The experiments show that photovoltage measurements in hybrid semiconductor-ferromagnetic structures provide a sensitive and non-invasive tool for probing the spin waves of small magnets

One of the fundamental properties of bulk metals is the cancellation of electric fields. The free charges inside of a metal will move until they find an arrangement where the internal electric field is zero. This implies that the electric dipole moment of a metal particle should be exactly zero, because an electric dipole moment requires a net separation of charge and thus a nonzero internal electric field. This thesis is an experimental study to see if this property continues to hold for tiny sub- nanometer metal particles called clusters (2 - 200 atom, R < 1 nm). We have measured the electric dipole moments of metal clusters made from 15 pure elements using a molecular beam electric deflection technique. We find that the observed dipole moments vary a great deal across the periodic table. Alkali metals have zero dipole moments, while transition metals and lanthanides all have dipole moments which are highly size dependent. In most cases, the measured dipole moments are independent of temperature (T = 20 - 50 K), and when there is a strong temperature dependence this suggests that there is a new state of matter present. Our interpretation of these results are that those clusters which have a non- zero dipole moment are non-metallic, in the sense that their electrons must be localized and prevented from moving to screen the internal field associated with a permanent dipole moment. This interpretation gives insight to several related phenomena and applications. We briefly discuss an example cluster system RhN where the measured electric dipole moments appear to be correlated with a the N2O reactivity. Finally, we discuss a series of magnetic deflection experiments on lanthanide clusters (Pr, Ho, Tb, and Tm). The magnetic response of these clusters is very complex and highly sensitive to size and temperature. We find that PrN (which is non-magnetic in the bulk) becomes magnetic in clusters and TmN clusters have magnetic moments lower than the atomic value as well as the bulk saturation value implying that the magnetic order in the cluster involves non-collinear or antiferromagnetic order. HoN and TbN show very similar size dependent trends suggesting that these clusters have similar structures.

Le remplacement des technologies DRAM et SRAM des mémoires caches est un enjeu pour l’industrie microélectronique qui doit faire face à des demandes de miniaturisation, de réduction des amplitudes et des durées des courants d’écriture et de lecture des données. Les mémoires à accès direct magnétiques (MRAM) sont des candidates pour une future génération de mémoires et la découverte des couples de spin-orbite (SOT) a ouvert la voix à une combinaison des deux technologies appelée SOT-MRAM. Ces mémoires sont très prometteuses car elles allient non-volatilité et bonne fiabilité, mais de nombreux défis techniques et théoriques restent à relever.L’objectif de ce travail de thèse est d’étudier le retournement de l’aimantation par couple de spin-orbite avec des impulsions de courant sub-nanoseconde et de diminuer les courants d’écriture à couple de spin-orbite. Ce travail est préliminaire à la preuve de concept d’une mémoire SOT-MRAM écrite avec des impulsions de courant électrique ultra-courtes et des amplitudes relativement faibles.Pour cela nous avons étudié des cellules mémoire à base de Ta-CoFeB-MgO. Nous avons vérifié les dépendances du courant critique en durées d’impulsions et en un champ magnétique extérieur. Nous avons ensuite, sur une cellule type SOT-MRAM, prouvé l’écriture ultrarapide avec des impulsions de courant inférieures à la nanoseconde. Puis nous nous sommes intéressés à la diminution du courant d’écriture de SOT-MRAM à l’aide d’un champ électrique. Nous avons démontré que ce dernier permet de modulerl’anisotropie magnétique. Sa diminution lors d’une impulsion de courant dans la liste de tantale montre que la densité de courant critique pour le retournement de l’aimantation du CoFeB par SOT est réduite. Ces résultats sont très encourageants pour le développement des SOT-MRAM et incitent à approfondir ces études. Le mécanisme de retournement de l’aimantation semble être une nucléation puis une propagation de parois de domaines magnétiques. Cette hypothèse se fonde sur des tendances physiques observées lors des expériences ainsi que sur des simulations numériques. / They require smaller areas for bigger storage densities, non-volatility as well as reduced and shorter writing electrical currents. Magnetic Random Access Memory (MRAM) is one of the best candidates for the replacement of SRAM and DRAM. Moreover, the recent discovery of spin-orbit torques (SOT) may lead to a new technology called SOT-MRAM. These promising technologies combine non-volatility and good reliability but many challenges still need to be taken up.This thesis aims at switching magnetization by spin-orbit torques with ultra-fast current pulse and at reducing their amplitude. This preliminary work should enable one to proof the concept of SOT-MRAM written with short current pulses and low electrical consumption to write a memory cell.To do so, we studied Ta-CoFeB-MgO-based memory cells for which we verified current dependencies on pulse lengths and external magnetic field. Then we proved the ultrafast writing of a SOT-MRAM cell with pulses as short as 400 ps. Next, we focused on reducing the critical writing currents by SOT with the application of an electric field. We showed that magnetic anisotropy can be modulated by an electricfield. If it can be lowered while a current pulse is injected through the tantalum track, we observed a reduction of the critical current density for the switching of the CoFeB magnetization. Those results are very promising for the development of SOT-MRAM and encourage one to delve deeper into this study. The magnetization switching mechanism seems to be a nucleation followed by propagations of magneticdomain walls. This assumption is based on many physical tendencies we observed and also on numerical simulations.

This thesis will describe the magnetic behavior found in a scaling array of magnetic nanomaterials that have been uniquely designed, synthesized and characterised in order to better understand their properties with regards to potential future applications. Within Chapter 1 will be a detailed, yet accessible, introduction to nanomagnetism and the fundamental principles and practical techniques essential to the study of this unique mélange of physics and chemistry. This chapter will be designed to give the reader the necessary tools to understand key literature concepts found in Chapter 2, as well as the work presented in the following chapters. Chapter 2 will provide an overview of relevant literature in the field of magnetic nanomaterials, including: nanoparticles, single-molecule magnets, single-chain magnets and metal-organic frameworks. Chapter 3 will describe work performed on nanoparticles doped with lanthanide ions in order to explore their resulting size, shape, crystallinity and magnetic properties. The relevance of the chosen particles (NaYF4) pertains to their proposed use in a variety of applications due to their known luminescent properties, which we sought to hybridize with interesting magnetic properties, thus creating multimodal imaging capabilities. Doping with a variety of desired ratios of lanthanide ions (GdIII, TbIII, DyIII, ErIII and YbIII) was successful, producing crystalline nanoparticles with tunable size and shape. Magnetic measurements displayed a clear absence of superparamagnetic behavior, indicating that these materials have the potential to be well-suited to applications in biomedicine as multimodal imaging probes and MRI contrast agents. Chapter 4 will build on the previously explored doped nanomaterials through creating a hybrid nanomaterial by tethering lanthanide-based magnetic molecules to the surface of nanoparticles. This is performed through the synthetic design of a SMM with two anisotropic DyIII ions, which was synthesized and designed to bear terminal S-groups in order to promote the binding of the magnetic molecule to capping agent free gold nanoparticles. Upon confirmation of the successful surface attachment of the molecules, magnetic measurements displayed that the magnetic molecules maintained their static properties, however, their dynamic properties were altered. This system was the first example of this type of novel approach to the study of magnetic molecules on surfaces for data storage, spintronics, and quantum computing applications. Chapter 5 will expand on the previous study of ordering arrays of magnetic molecules on the surface of nanoparticles by tethering them into 1D chain networks. We successfully synthesized chain networks with YIII, EuIII, GdIII, TbIII and DyIII lanthanide ions. Magnetic characterisation revealed slow relaxation of the magnetization with no significant interactions between magnetic ions, thus these are discrete magnetic molecules in 1D. Rather surprisingly, the isotropic GdIII analogue displayed field induced slow relaxation of the magnetisation, necessitating the use of ab initio calculations in order to shed light on the potential causes of this unexpected behavior. Overall, through the formation and study of these structures, we observed a new potential method of SMM assembly for the study of ordered arrays of molecular magnets. Chapter 6 will focus on ordering of discrete magnetic systems in 3D. With this in mind, we successfully isolated the first Co8 cuboctahedron MOF. Magnetic measurements displayed that each SBU was well-isolated, with significant antiferromagnetic coupling between CoII ions, leading to an S = 0 ground state. These interactions were then modelled using density functional theory. This type of study promotes the future development of novel high-nuclearity MOF structures with interesting and tuneable magnetic properties, as well as the potential for assembly of discrete molecular magnetic units in 3D using MOFs. Chapter 7 utilizes the principles of Chapter 3, wherein magnetic ions are doped into a diamagnetic material; in this case, MOF-5. We sought to isolate one CoII ion in each SBU, and build upon this by adding additional magnetic ions and probing their interactions. Through magnetic measurements we observed a scaling magnetic moment with CoII content, and with higher dopant percentages we began to observe magnetic interactions occurring within the SBUs. Interestingly, we also observed a change in coordination environment with higher dopant percentages, likely as a result of the previously suggested capability of one ZnII ion within the MOF-5 SBU to become hexacoordinate, allowing CoII doping up to a maximum of 25%. Consequently, this study points to the cause of the structural instability that plagues MOF-5 in the presence of air and moisture. We probed this system further in Chapter 8 using FeIII as a dopant ion, and were able to obtain the first crystallographic evidence of the coordination change of ZnII in MOF-5. Furthermore, the structure obtained with FeIII was the first example of metal ion addition within a MOF that bound two interpenetrated frameworks together. This new MOF was found to have the potential to be a more practical material for gas storage and separation, and/or for catalysis. Thus, this study was informative in regards to the inherent instability of the parent framework, as well as a new method of metal addition to a known MOF structure. Chapter 9 will conclude the work with a discussion of what was performed in, and learned from, each thesis section, as well as provide an outlook and perspective on the novel work that may be derived from these projects going forward.

Methods of guiding magnetic particles in a controlled fashion through the arterial system in vivo using external magnetic fields are explored. Included are discussions of applications, magnetic field properties needed to allow guiding based on particle characteristics, hemodynamic forces, the uniformity of field and gradients, variable tissue characteristics, and imaging techniques employed to view these particles while in transport. These factors influence the type of magnetic guidance system that is needed for an effective drug delivery system. This thesis reviews past magnetic drug delivery work, variables, and concepts that needed to be understood for the development of an in vivo magnetic drug delivery system. The results of this thesis are the concise study and review of present methods for guided magnetic particles, aggregate theoretical work to allow proper hypotheses and extrapolations to be made, and experimental applications of these hypotheses to a working magnetic guidance system. The design and characterization of a magnetic guidance system was discussed and built. The restraint for this system that balanced multiple competing variables was primarily an active volume of 0.64 cm3, a workspace clearance of at least an inch on every side, a field of 0.3T, and a local axial gradient of 13 T/m. 3D electromagnetic finite element analysis modeling was performed and compared with experimental results. Drug delivery vehicles, a series of magnetic seeds, were successfully characterized using a vibrating sample magnetometer. Next, the magnetic seed was investigated under various flow conditions in vitro to analyze the effectiveness of the drug delivery system. Finally, the drug delivery system was successfully demonstrated under limiting assumptions of a specific magnetic field and gradient, seed material, a low fluid flow, and a small volume. / Master of Science

A recent International Technology Roadmap for Semiconductors (ITRS) report (2.0, 2015 edition) has shown that Moore’s law is unlikely to hold beyond 2028. There is a need for alternate devices to replace CMOS based devices, if further miniaturization and high energy efficiency is desired. The goal of this dissertation is to experimentally demonstrate the feasibility of nanomagnetic memory and logic devices that can be clocked with acoustic waves in an extremely energy efficient manner. While clocking nanomagnetic logic by stressing the magnetostrictive layer of a multiferroic logic element with with an electric field applied across the piezoelectric layer is known to be an extremely energy-efficient clocking scheme, stressing every nanomagnet separately requires individual contacts to each one of them that would necessitate cumbersome lithography. On the other hand, if all nanomagnets are stressed simultaneously with a global voltage, it will eliminate the need for individual contacts, but such a global clock makes the architecture non-pipelined (the next input bit cannot be written till the previous bit has completely propagated through the chain) and therefore, unacceptably slow and error prone. Use of global acoustic wave, that has in-built granularity, would offer the best of both worlds. As the crest and the trough propagate in space with a velocity, nanomagnets that find themselves at a crest are stressed in tension while those in the trough are compressed. All other magnets are relaxed (no stress). Thus, all magnets are not stressed simultaneously but are clocked in a sequentially manner, even though the clocking agent is global. Finally, the acoustic wave energy is distributed over billions of nanomagnets it clocks, which results in an extremely small energy cost per bit per nanomagnet. In summary, acoustic clocking of nanomagnets can lead to extremely energy efficient nanomagnetic computing devices while also eliminating the need for complex lithography. The dissertation work focuses on the following two topics: Acoustic Waves, generated by IDTs fabricated on a piezoelectric lithium niobate substrate, can be utilized to manipulate the magnetization states in elliptical Co nanomagnets. The magnetization switches from its initial single-domain state to a vortex state after SAW stress cycles propagate through the nanomagnets. The vortex states are stable and the magnetization remains in this state until it is ‘reset’ by an external magnetic field. 2. Acoustic Waves can also be utilized to induce 1800 magnetization switching in dipole coupled elliptical Co nanomagnets. The magnetization switches from its initial single-domain ‘up’ state to a single-domain ‘down’ state after SAW tensile/compressive stress cycles propagate through the nanomagnets. The switched state is stable and non-volatile. These results show the effective implementation of a Boolean NOT gate. Ultimately, the advantage of this technology is that it could also perform higher order information processing (not discussed here) while consuming extremely low power. Finally, while we have demonstrated acoustically clocked nanomagnetic memory and logic schemes with Co nanomagnets, materials with higher magnetostriction (such as FeGa) may ultimately improve the switching reliability of such devices. With this in mind we prepared and studied FeGa films using a ferromagnetic resonance (FMR) technique to extract properties of importance to magnetization dynamics in such materials that could have higher magneto elastic coupling than either Co or Ni.

Neste trabalho, pós magnéticos nanoestruturados de PrxFe94-xB6 (x = 6, 8, 10 e 12) foram preparados a partir da combinação do processo de hidrogenação, desproporção, dessorção e recombinação (HDDR) e moagem de alta energia entre uma liga em estado bruto de fusão (Pr14Fe80B6) e Fe-&alpha; em pó. As nanopartículas produzidas apresentaram propriedades magnéticas e microestruturais comparáveis aos estudos realizados em hipertermia. O tempo ideal para obtenção de nanopartículas magnéticas é de 5 horas (a 900 rpm). Foi constatado que quanto maior o tempo de moagem, maior o percentual de carbono nas partículas (0,05 - 3,43 % C). O carbono é proveniente do ácido oléico adicionado como surfactante na etapa de moagem. Os nanocompósitos obtidos exibiram forças coercivas entre 80 Oe (6,5 kAm-1) e 170 Oe (13,5 kAm-1), e momentos magnéticos variando entre 81 - 129 Am2kg-1. A partir da difração de raios X foram identificadas apenas duas fases em todas as amostras: Fe-&alpha; e a fase magnética Pr2Fe14B. Nanopartículas isoladas com diâmetro aproximado de 20nm foram analisadas. Todas as composições estudadas apresentaram aquecimento proveniente da exposição a um campo magnético alternado (f = 222 kHz e Hmax ~3,7 kAm-1) comparáveis aos reportados na literatura. As variações de temperaturas (&Delta;T) dos pós foram: 51 K referente à composição de Pr6Fe88B6, 41 K para Pr8Fe86B6, 38 K no composto com 10% at. Pr (Pr10Fe84B6) e 34 K em Pr12Fe82B6. As taxas de absorção específicas estimadas foram de 201 Wkg-1 para a composição Pr6Fe88B6, 158 Wkg-1 para a composição Pr8Fe86B6 e 114 Wkg-1 para as composições Pr10Fe84B6 e Pr12Fe82B6. / In this work, PrxFe94-xB6 (x = 6, 8, 10 and 12) nanostructured powders were prepared by a combination of hydrogenation, disproportionation, desorption and recombination (HDDR) process with high energy milling applied to the mixture of an as-cast alloy (Pr14Fe80B6) and &alpha;-Fe. The produced nanoparticles showed magnetic properties comparable to those reported in hyperthermia studies. The optimal time to obtain the magnetic nanoparticles is 5 hours (at 900 rpm). It was verified that longer milling times cause an increase in carbon percentage on the particles. The carbon is derived from oleic acid added as a surfactant in the milling step. The nanocomposites exhibit coercive force ranging from 80 Oe (6.5 kAm-1) to 170 Oe (13.5 kAm-1) and magnetic moments in the range of 81 129 Am2kg-1. From the x-ray diffraction analyses, only two phases were found in all samples: &alpha;-Fe and the magnetic phase Pr2Fe14B. Individual nanoparticles with diameter of about 20 nm were verified. The samples studied presented heating when exposed to an alternating magnetic field (f = 222 kHz e Hmax ~3.7 kAm-1) comparable to reported in literature. Temperature variations (&Delta;T) of the powders were: 51 K for Pr6Fe88B6, 41 K for Pr8Fe86B6, 38 K for Pr10Fe84B6 and T = 34 K for Pr12Fe82B6. The specific absorption rates (SARs) of the powders were 201 Wkg-1 for Pr6Fe88B6 composition, 158 Wkg-1 on the composition Pr8Fe86B6, and 114 Wkg-1 for Pr10Fe84B6 and Pr12Fe82B6 compositions.

Neste trabalho, pós magnéticos nanoestruturados de PrxFe94-xB6 (x = 6, 8, 10 e 12) foram preparados a partir da combinação do processo de hidrogenação, desproporção, dessorção e recombinação (HDDR) e moagem de alta energia entre uma liga em estado bruto de fusão (Pr14Fe80B6) e Fe-&alpha; em pó. As nanopartículas produzidas apresentaram propriedades magnéticas e microestruturais comparáveis aos estudos realizados em hipertermia. O tempo ideal para obtenção de nanopartículas magnéticas é de 5 horas (a 900 rpm). Foi constatado que quanto maior o tempo de moagem, maior o percentual de carbono nas partículas (0,05 - 3,43 % C). O carbono é proveniente do ácido oléico adicionado como surfactante na etapa de moagem. Os nanocompósitos obtidos exibiram forças coercivas entre 80 Oe (6,5 kAm-1) e 170 Oe (13,5 kAm-1), e momentos magnéticos variando entre 81 - 129 Am2kg-1. A partir da difração de raios X foram identificadas apenas duas fases em todas as amostras: Fe-&alpha; e a fase magnética Pr2Fe14B. Nanopartículas isoladas com diâmetro aproximado de 20nm foram analisadas. Todas as composições estudadas apresentaram aquecimento proveniente da exposição a um campo magnético alternado (f = 222 kHz e Hmax ~3,7 kAm-1) comparáveis aos reportados na literatura. As variações de temperaturas (&Delta;T) dos pós foram: 51 K referente à composição de Pr6Fe88B6, 41 K para Pr8Fe86B6, 38 K no composto com 10% at. Pr (Pr10Fe84B6) e 34 K em Pr12Fe82B6. As taxas de absorção específicas estimadas foram de 201 Wkg-1 para a composição Pr6Fe88B6, 158 Wkg-1 para a composição Pr8Fe86B6 e 114 Wkg-1 para as composições Pr10Fe84B6 e Pr12Fe82B6. / In this work, PrxFe94-xB6 (x = 6, 8, 10 and 12) nanostructured powders were prepared by a combination of hydrogenation, disproportionation, desorption and recombination (HDDR) process with high energy milling applied to the mixture of an as-cast alloy (Pr14Fe80B6) and &alpha;-Fe. The produced nanoparticles showed magnetic properties comparable to those reported in hyperthermia studies. The optimal time to obtain the magnetic nanoparticles is 5 hours (at 900 rpm). It was verified that longer milling times cause an increase in carbon percentage on the particles. The carbon is derived from oleic acid added as a surfactant in the milling step. The nanocomposites exhibit coercive force ranging from 80 Oe (6.5 kAm-1) to 170 Oe (13.5 kAm-1) and magnetic moments in the range of 81 129 Am2kg-1. From the x-ray diffraction analyses, only two phases were found in all samples: &alpha;-Fe and the magnetic phase Pr2Fe14B. Individual nanoparticles with diameter of about 20 nm were verified. The samples studied presented heating when exposed to an alternating magnetic field (f = 222 kHz e Hmax ~3.7 kAm-1) comparable to reported in literature. Temperature variations (&Delta;T) of the powders were: 51 K for Pr6Fe88B6, 41 K for Pr8Fe86B6, 38 K for Pr10Fe84B6 and T = 34 K for Pr12Fe82B6. The specific absorption rates (SARs) of the powders were 201 Wkg-1 for Pr6Fe88B6 composition, 158 Wkg-1 on the composition Pr8Fe86B6, and 114 Wkg-1 for Pr10Fe84B6 and Pr12Fe82B6 compositions.