A photonic crystal is any material which exhibits a photonic band gap (PBG) and is comprised of a periodic arrangement of alternating layers of different dielectric constant. It has been found recently that an interesting route to approach such materials is via the synthesis of block copolymers which are able to microphase separate. This thesis describes the synthetic methods, in particular anionic polymerization, used to prepare such copolymers which exhibit photonic properties in the visible region of the electromagnetic spectrum.

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De nombreuses études ont déjà montré que les composés pharmaceutiques cristallins pouvaient subir des transformations cristal-->verre sous broyage mécanique. Dans ce mémoire, nous nous intéressons aux effets du broyage mécanique sur le verre lui même, obtenu de manière classique par trempe thermique du liquide. Les résultats ont été essentiellement obtenus par calorimétries standard et modulée, calorimétrie à dissolution et diffraction des rayons X. Les expériences ont été menées sur deux excipients pharmaceutiques réputés bons formateurs de verres: le tréhalose et le maltitol. Les résultats mettent en évidence trois effets majeurs du broyage sur les propriétés physiques des verres: 1. Un dédoublement du saut de chaleur spécifique à Tg. L'origine de ce double saut a été clairement identifiée et attribuée à l'évolution microstructurale du matériau broyé lors du passage de la transition vitreuse. 2. Une augmentation continue de l'enthalpie libre du matériau. Cette augmentation entraîne, non seulement, un rajeunissement du verre, mais aussi la formation d'un verre de haute énergie semblable aux verres obtenus par hypertrempe du liquide. 3. Une modification de la stabilité physique du verre. Le changement de stabilité se manifeste en particulier par une recristallisation au réchauffage. Cette recristallisation n'est cependant que transitoire dans la mesure où elle se développe pour les temps de broyage courts, puis disparaît progressivement pour des temps de broyage plus longs. L'ensemble des résultats permet d'avoir une vue cohérente des évolutions microstructurales, structurales et dynamiques du verre au cours d'une opération de broyage mécanique. / Many studies have already reported that crystalline pharmaceutical materials could undergo crystal-to-glass transformations upon mechanical milling. In this thesis we study the effects of milling on the glass itself, as obtained by quench of the melt. The results are mainly obtained by modulated and standard calorimetries, dissolution calorimetry and X-ray diffraction. Two good glass formers have been used for the experiments: tréhalose and maltitol. The results reveal three main effects of milling on the physical properties of glasses: 1. A two-step Cp jump at Tg. The origin of these two steps was clearly identified and attributed to the microstructural evolution of the milled material when passing through the glass transition zone. 2. A continuous increase of the free enthalpy of the material. This increase leads to the rejuvenation of the glass in a first stage and to the formation of a high energy glass in a second step. The final material has then physical properties similar to those of hyper quenched glasses. 3. A modification of the physical stability of the glass. The stability change appears, in particular, through a recrystallization upon heating. However, this recrystallization is only transient since it develops during the early stage of the milling process and then progressively decays during the late stage of the milling process. The overall results provide a coherent global view of structural, microstructural and dynamical evolutions of a glass during a high energy milling process.

In this thesis we study elliptic PDEs and PDE systems with e-pcriodic coeffi- cients, for small E, using the theory of two-scale homogenisation. We study a class of PDEs of partially degenerating type: PDEs with coefficients that are not uniformly elliptic with respect to E, and become degenerate in the limit E -t O. We review a recently developed theory of homogenisation for a general class of partially degenerating PDEs via the theory of two-scale convergence, and study two such problems from physics. The first problem arises from the study of a linear elastic composite with periodically dispersed inclusions that are isotropic and (soft' in shear: the shear modulus is of order E2. By passing to the two- scale limit as E -t 0 we find the homogenised limit equations to be a genuinely two-scale system in terms of both the macroscopic variable x and the micro- scopic variable y. We discover that the corresponding two-scale limit solutions must satisfy the incompressibility condition in y and therefore the composite only undergoes microscopic deformations when a (microscopically rotational' force is applied. We analyse the corresponding limit spectral problem and find that, due to the y-incompressibility, the spectral problem is an uncoupled two-scale prob- lem in terms of x and y. This gives a simple representation of the two-scale limit spectrum. We prove the spectral compactness result that states: the spectrum of the original operator converges to the spectrum of the limit operator in the sense of Hausdorff. The second problem we study is the propagation of electro- magnetic waves down a photonic fibre with a periodic cross section. We seek solutions to Maxwell's equations, propagating down the waveguide with wave number k E2-close to some (critical' value. In this setting, Maxwell's equations are reformulated as a partially degenerating PDE system with z-periodic coeffi- cients. Using the theory of homogenisation we pass to the limit as E -t 0 to find a non-standard two-scale homogenised limit and prove that the spectral compact- ness result holds. We finally prove that there exist gaps in the limit spectrum for two particular examples: a one-dimensionally periodic 'multilayer ' photonic crystal and a two-dimensionally periodic two-phase photonic crystal with the in- clusion phase consisting of arbitrarily small circles. Therefore, we prove that these photonic fibres have photonic band gaps for certain k.

The increasing demand for nearline storage capacity in data centers calls for a continued enhancement in hard disk drive recording density far beyond one terabit per square inch. The thermal stability limit forces the drive manufacturers to develop new concepts in order to achieve this in the long term. Potential solutions are microwave-assisted magnetic recording (MAMR), heat-assisted magnetic recording (HAMR) and bit-patterned media (BPM). A simple example of BPM based on sputter-deposited Co/Pd multilayers and prepatterned substrates at hypothetical recording densities up to one terabit per square inch was studied by magnetic force microscopy (MFM). This system achieved promising results at lower densities, but an actual application for data storage, especially at one terabit per square inch and higher densities, requires elaborate optimizations. For some time now, FePt thin films have attracted much attention as prospective recording layers for high-density magnetic data storage due to their high magnetic anisotropy. The use of FePt films in HAMR is especially promising. This application has been tested successfully by Seagate and its key customers in recent years and is about to be introduced into the nearline hard disk drive market. It requires a tuning of the magnetic properties of FePt, especially of its Curie temperature. The addition of Cu proved to be effective in this regard and can also facilitate the formation of the crucial L10 structure and (001) texture during rapid thermal annealing of sputter-deposited thin films. Such films were prepared as bilayers of Cu and FePt on Si substrates, annealed for 30 s, and analyzed by X-ray diffraction (XRD) and SQUID vibrating sample magnetometry (SQUID-VSM). The influence of large Cu additions on important properties like lattice parameters, mosaicity, magnetic anisotropy and Curie temperature is discussed. The chemical long-range order was calculated from the XRD data, and a dedicated chapter of this thesis covers the most important factors to be considered in such calculations for textured thin films and other samples. The feasibility of creating patterned Fe-Cu-Pt films with perpendicular magnetic anisotropy, as needed for a combination of HAMR and BPM, by deposition through a PMMA mask, a lift-off process and subsequent annealing was investigated as well. The results indicate that the chosen approach might not lead to the required (001) texture when the nanostructures are small enough to compete with today's recording densities, so that either a continuous film might need to be etched after annealing or a seed layer might be required to induce the texture.:1. Motivation: Magnetic Data Storage 2. Experimental Techniques 3. Co/Pd Multilayers on Prepatterned Substrates 4. Fe-Pt and Fe-Cu-Pt Alloys 5. Rapid Thermal Annealing of FePt and FePt/Cu Films 6. Order Parameter Calculation 7. Summary

Par rapport aux détecteurs de rayons X couramment utilisés pour la cristallographie, les détecteurs à pixels hybrides apportent des avantages majeurs qui proviennent principalement de l’utilisation d'une chaîne de comptage propre à chaque pixel permettant de compter les photons individuellement et très rapidement. Les principales innovations de ces détecteurs sont les suivantes : (1) Suppression quasi totale du bruit ; (2) Obturateur électronique ultra rapide (de l'ordre de 100 ns) ; (3) Vitesse d'acquisition de 500 images par seconde. Ces avantages déjà mis à profit depuis une petite dizaine d’années sur les lignes synchrotron, sont également très prometteurs pour les diffractomètres de laboratoire. L’objet de la thèse a été de développer un diffractomètre expérimental de laboratoire équipé d’un détecteur à pixels hybrides, XPAD, et de réaliser les premières mesures de diffraction sur monocristal. Ces mesures ont permis de déterminer les corrections et calibrations du détecteur nécessaires pour les mesures sur monocristaux. Conjointement, les méthodes et techniques de traitement des images pour intégrer les intensités de diffraction ont été étudiées. L’intérêt du très faible bruit du détecteur pour l’étude de modèles de densité électronique a été démontré ; le prototype avec le détecteur XPAD a donné de meilleurs résultats que les diffractomètres usuels. Une deuxième application a consisté à utiliser les qualités de vitesse du détecteur pixel pour la mise en œuvre de mesures résolues en temps à l’échelle de la milliseconde. Des mesures sous champs électrique commuté ont permis de montrer le potentiel de ce type de détecteur dans ce domaine de recherche / Compared to X-ray detectors commonly used for crystallography, hybrid pixels detectors provide major advantages primarily due to the use of a counting system proper to each pixel allowing for very fast and individual photon counting. The main innovations of these detectors are: (1) Almost total suppression of noise ; (2) Ultra-fast electronic shutter (about 100 ns) ; (3) Acquisition rate of 500 images per second. These advantages have already been exploited over the past ten years on synchrotron beam lines and are also very promising for laboratory diffractometers. The thesis work was to realize a prototype laboratory diffractometer equipped with such a detector, XPAD, and to achieve single crystal X-ray diffraction measurements. The necessary corrections and calibrations of the detector required for diffraction measurements on single crystals were determined. The methods and image processing techniques to integrate the diffraction intensities were studied. Benefits of the very low noise of the detector for electron density models study were demonstrated; the prototype diffractometer equipped with an XPAD detector gave better results than conventional diffractometers. A second type of application was to use the pixel detector for the implementation of time-resolved diffraction measurements at millisecond timescale. Measurements under switched electric fields have shown the potential of this type of detector in this area of research

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