Le travail présenté dans cette thèse porte sur le bruit d'intensité du laser Brillouin à fibre ainsi que sur le brûlage de trou spectral du processus de diffusion Brillouin stimulée (DBS) dans les fibres. Le bruit d'intensité du laser Brillouin provient principalement de deux sources : les fluctuations du coefficient de réinjection et le bruit d'intensité du laser de pompe. L'influence de chacune d'elles sur le bruit d'intensité du laser Brillouin est évaluée au moyen d'une fonction de transfert. Une étude théorique de ces deux fonctions a été réalisée puis validée expérimentalement. Nous montrons ensuite théoriquement que le brûlage de trou spectral, déjà observé expérimentalement pour le générateur et l'amplificateur Brillouin, peut être interprété en supposant que l'élargissement spectral du processus de DBS est de nature homogène. Le brûlage de trou provient de la saturation du gain conjuguée au couplage entre les variations de l'amplitude des champs optiques.

Le cadre général dans lequel s'insère ce travail de thèse est celui de l'étude de la diffusion Brillouin dans une nouvelle génération de fibres optiques à cristaux photoniques (PCFs). Ces fibres, qui présentent un arrangement périodique de micro-canaux d'air parallèles le long de la fibre, possèdent en effet des propriétés optiques et acoustiques remarquables et inédites par rapport aux fibres conventionnelles. De façon plus précise, nous montrons dans ce travail, par le biais de simulations numériques et de données expérimentales, que les fibres à cristaux photoniques offrent la possibilité de supprimer ou, à contrario, augmenter les interactions entre les photons et les phonons. Dans une première partie, nous présentons une méthode de cartographie des fluctuations longitudinales de la microstructure des fibres PCFs à l'aide d'un capteur distribué basé sur une méthode innovante d'écho Brillouin. Cette méthode, très sensible et à haute résolution, est directement intéressante pour caractériser et améliorer l'uniformité des PCFs lors de leur fabrication et également pour la détection des différentes contraintes de température et étirement induites le long des fibres. Sur le plan fondamental, notre système de mesure distribuée à haute résolution nous a également permis d'observer, pour la première fois à notre connaissance, le temps de vie des ondes acoustiques dans les fibres à cristaux photoniques et les fibres standard. Par ailleurs, sur le plan technique, nous avons développé une architecture simplifiée de capteur distribué combinant la technique des échos Brillouin et celle de la modulation différentielle par déplacement de phase avec un seul modulateur d'intensité. Nos résultats montrent une résolution centimétrique dans la zone de soudure entre deux fibres optiques à l'aide d'une impulsion de phase de 500 ps. Nous démontrons dans une deuxième partie la suppression directe et passive de la rétrodiffusion Brillouin stimulée dans une fibre optique micro structurée en faisant varier périodiquement le diamètre de la microstructure. Une augmentation de 4 dB du seuil de puissance Brillouin a été obtenue avec une variation de seulement 7% sur une période de 30m. Ce résultat est très intéressant car la diffusion Brillouin est un facteur limitant dans les systèmes de télécommunications par fibre optique et les lasers à fibre. La troisième et dernière partie est consacrée à l'étude numérique et expérimentale de la diffusion Brillouin en avant dans les fibres à cristaux photoniques. En plus de la suppression de la plupart des modes acoustiques transverses, nous montrons que cette diffusion Brillouin est fortement augmentée pour certains modes acoustiques à haute fréquence qui sont piégés au cœur de la microstructure. Nous avons également étudié une fibre à structure multi-échelle qui révèle l'excitation sélective de plusieurs phonons acoustiques à des fréquences allant jusqu'a 2GHz. Ces mesures ont étés confirmées par des simulations numériques basées sur une méthode vectorielle aux éléments finis. L'impact des irrégularités de la microstructure a aussi été mis en évidence.Mots clés : optique non linéaire, diffusion Brillouin, fibres optiques microstructurées, seuil Brillouin, capteurs Brillouin distribués.

The sub-surface region of chemical vapour deposition (CVD) diamond was transformed by C+ ion implantation followed by isochronal annealing up to 1200 oC. Different implantation regimes and with different energies at different implantation temperatures would give different thicknesses were studied. This enabled a study in the evolution of the stiffness of the damaged layer as a function of annealing. The technique of choice for this study was the non-destructive Brillouin light scattering (BLS) utilizing two scattering geometries; indirectly scattered phonons (Kr¨uger-type geometry) for temperature anneals up to 600 oC, and the conventional surface ripple mechanism up to 1200 oC. It has been argued that surface acoustic waves (SAW) on a transparent medium are enhanced by applying a thin metallic reflective layer on the surface, this study has showed that opacity of the substrate is key. In fact, bulk modes with SAW-like characteristics emanating from indirect photon scattering off phonons after reflection at the smooth reflective back of the sample dominated down to transmission below 5% which was observed after annealing between 500-600 oC (low annealing temperatures). The other complementing techniques employed to understand the changing structure of the ion implanted diamond were Raman spectroscopy, electromagnetic transmission in the visible range, electron energy loss spectroscopy (EELS) and high-resolution transmission electron microscopy (HRTEM) in addition to theoretical techniques: transport of ions in matter (TRIM), finite element modelling (FEM) and elastodynamic Green’s functions. Although the electronic techniques showed a structurally changing material at the low annealing temperatures, the optical ones did not show significant changes in the ion-damaged material possibly due to lack of distinct interface between the pristine diamond and the ion irradiated region at these lower annealing temperatures.

by Yip Sung-tat. / Bibliography: leaves 120-123 / Thesis (M.Ph.)--Chinese University of Hong Kong, 1984

Despite the advent of alternative dosage forms, solid dosage forms constitute a major proportion of dosage forms not only on the market, but also in many pharmaceutical companies’ pipelines. This is because of their superior stability and ease of manufacturing relative to other dosage forms. Although solid dosage forms have been the topic of discussion for decades, the process of compaction of these dosage forms is considered an art rather than science because of the empiricism that exists in this area. With the introduction of Quality by Design (QbD), it is imperative that the drug development process is guided by structured scientific principles. It has been hypothesized that crystal structure of organic solids plays a pivotal role in understanding the properties, processing and eventually performance of solids. In this regard, the intermolecular interactions within a solid play a paramount role in dictating the materials response to stress. One important parameter that is weakly addressed in the literature is the concept of strength of intermolecular interactions. In the current work, we utilize the concept of elasticity as a metric for strength of intermolecular interactions. We introduce powder Brillouin light scattering; an inelastic light scattering technique to measure the elasticity of organic solids and try to correlate the mechanical moduli extracted from the spectra to the compaction performance of solids. We hypothesize that any redistribution of intermolecular interactions would be reflected in the BLS spectrum of these materials and the material properties can be used to explain the differences in compaction performance. Before we tested our hypothesis, we validated our powder BLS technique using aspirin as model system. We then applied the same analysis to four model systems that involved different ways of reorganizing the intermolecular interactions upon subtle modifications to the molecular structure. In Chapter 4, we investigated the effect of alkyl chain length and crystal structure on the mechanical properties and compaction performance of p-aminobenzoic acid (PABA) and its esters. For the entire ester series, a similar hydrogen bonding pattern was observed with strong N-H…O (carbonyl) and supportive N-H…N interactions. While the ethyl and butyl esters exhibited a layered structure, the methyl ester displayed a 3-D isotropic structure. The crystal structure for PABA exhibited a three-dimensional, quasi-isotropic distribution of the hydrogen-bonding interactions that connected the PABA dimers. The powder BLS spectra for these materials revealed low velocity shear modes for the layered structures and a spectrum consistent with an isotropic structure for Me-PABA and PABA. This was in good agreement with the compressibility behavior under load, with Et-PABA and Bu-PABA more compressible than PABA. However, due to greater particle-particle adhesion, PABA compacts showed greater tensile strength at higher pressures. The moduli calculated also showed that both Et-PABA and Bu-PABA had lower shear and Young’s modulus relative to the other materials. Attachment energies corroborated the above results. These studies showed that weak dispersive forces play an important role in understanding material properties. In Chapter 5, a series of nitrobenzoic derivatives were used to study the effect of secondary interactions on the crystal reorganization and material properties. The materials used in the study include p-nitrobenzoic acid (4-NBA), m-nitrobenzoic acid (3-NBA, 4-chloro-3-nitrobenzoic acid (Cl-NBA), 4-bromo-3-nitrobenzoic acid (Br-NBA), and 4-methyl-3-nitrobenzoic acid (Me-NBA). Crystal structures of the materials revealed different organization of C-H…O interactions. Two types of C-H…O interactions were prevalent namely C-H…O (nitro) and C-H…O (carboxy). The reorganization of these two types of interactions led to different packing motifs and different mechanical behavior. These structural features were reflected in their mechanical properties assessed by powder Brillouin light scattering. Cl-NBA and Br-NBA displayed an isotropic spectrum similar to polystyrene and aspirin. 3-NBA, 4-NBA and Me-NBA displayed different spectra from Cl-NBA and Br-NBA with high frequency tailing in the longitudinal mode distribution indicating a specific direction of extended molecular interactions. The Young’s modulus and shear modulus followed the order: 3-NBA < Me-NBA< 4-NBA < Cl-NBA < Br-NBA. The maximum longitudinal modulus Mmax was the highest for 3-NBA and was significantly greater than rest of the materials. From the compaction studies, it was observed that the tabletability followed the rank order 3-NBA > 4-NBA > Me-NBA ≈ Br-NBA ≈ Cl-NBA which is the same order as Mmax. 3-NBA by virtue of its low shear and Young’s modulus to be the most compressible material, but the compressibility rank order was 4-NBA > Me-NBA ≈ 3-NBA > Cl-NBA > Br-NBA. However, 3-NBA by virtue of its greater particle-particle adhesion was the most compactable material. The yield pressures obtained from Heckel plots revealed that 4-NBA and Me-NBA were relatively more plastic when compared to the other materials. This study demonstrated that subtle changes to the molecular structure can result in drastically different crystal packing which in turn would influence the mechanical properties and the compaction performance of organic solids. In Chapter 6, we investigated the effect of cocrystallization on the compaction performance of caffeine(CAF). The series of halo-nitrobenzoic acids (F-NBA, Cl-NBA and 3-NBA) were used as coformers. The cocrystals CAF: F-NBA, CAF: Cl-NBA and CAF: NBA Form 1 adopted a flat layered structure that can undergo deformation with ease. This increased the compressibility of the cocrystals relative to CAF. In addition to the improved compressibility, by virtue of increased particle-particle contacts, the cocrystals also displayed superior tabletability. In contrast to the layered structures adopted by the three cocrystals, the CAF: NBA Form 2 displayed a columnar structure that exhibited resistance to stress. The compressibility and the tabletability of CAF: NBA Form 2 was significantly compromised when compared to that of Form1. All the compaction characteristics of the cocrystals were in good agreement with moduli and parameters obtained from powder BLS spectra. The layered materials showed the presence of low velocity shear modes corroborating the earlier studies. There was a clear difference in the spectra of the polymorphs, indicating that powder BLS can be used for mechanical screening of polymorphs. In Chapter 7, we examined the effects of crystal structure and coformer functionality on the compaction performance of theophylline (THY). The coformers employed include 4-fluoro-3-nitrobenzoic acid (FNBA), acetaminophen (APAP), and p-aminobenzoic acid (PABA). While THY-APAP and THY-FNBA exhibited layered structures, the THY-PABA displayed a interdigitated columnar structure. Powder BLS spectra showed the presence of low frequency shear modes relative to THY for all the three cocrystals. However, the order of frequencies followed: THY-FNBA < THY-APAP < THY-PABA. The shear modulus calculated followed the order THY-APAP≈ THY-FNBA < THY < THY-PABA which is in agreement with the crystal structures discussed. The Young’s modulus followed the order THY-FNBA < THY-APAP < THY < THY-PABA. The two layered structures (THY-APAP, THY-FNBA) showed distinct compaction performance (similar compressibility but different compactability and tabletability). The layered structures were more compressible than THY which is hypothesized to undergo deformation through multiple mechanisms. THY-PABA showed poor compaction properties. This highlights the fact that although the coformer (PABA) is molecularly similar to FNBA, the resultant cocrystals are structurally and mechanically distinct. These observations were well supported by the moduli calculated from powder BLS studies. The order of yield pressures obtained from Heckel analysis followed the same order as shear modulus. The tensile strength of the compacts of the cocrystals level off at around 150 MPa but the tensile strength of THY compacts continues to increase. From a manufacturing perspective the cocrystals can prove to be a better option as they as more compactable at higher porosities or they possess greater tabletability at low compaction pressures. Overall, we have used model systems to demonstrate that the redistribution of intermolecular forces upon point substitution or cocrystallization have a dramatic effect on the material properties. It is also worth noting that elasticity along with plasticity can provide important information about the strength of interactions which would help in understanding the role of weak intermolecular forces in the performance of organic materials. To gain a better perspective of the compaction process and move towards a QbD approach, it is also imperative to understand the link between crystal structures, intermolecular interactions which is possible with the help of novel characterization techniques (BLS, AFM).

La diffusion Brillouin stimulée (DBS) constitue un des effets non-linéaires observés dans les fibres optiques monomodes et est d'une grande importance dans diverses applications. Elle résulte de la diffusion des ondes lasers par interaction avec les ondes acoustiques présentes dans le milieu et se manifeste essentiellement par la génération d'une onde Stokes rétrodiffusée, limitant la puissance maximale d'une onde laser transmise dans une fibre optique et impliquant une sévère contrainte pour les transmissions optiques longue distance. Le décalage fréquentiel de cette onde par rapport à l'onde laser est appelé fréquence Brillouin et est proche de 11 GHz à une longueur d'onde 1550 nm. L'analyse de l'onde Stokes permet également l'étude des effets modifiant les caractéristiques acoustiques, telles que la température et la contrainte. C'est pourquoi la DBS est largement utilisée pour la réalisation de capteurs à fibres optiques. Dans ce présent travail de thèse, une étude générale des propriétés de la DBS dans les fibres est proposée, incluant notamment l'établissement d'une nouvelle expression de la puissance de seuil et une solution approchée aux équations Brillouin traditionnelles. A partir de la technique pompe-sonde utilisant une seule source laser grâce à un modulateur électro-optique et qui consiste en l'introduction artificielle d'une onde Stokes contre-propagative que l'on balaye en fréquence, la courbe de gain Brillouin est analysée pour des températures allant de 1K à la température ambiante. La potentialité unique de capteur Brillouin fibré des très basses températures est démontrée et ce avec une sensibilité inférieure à 1°C. Les résultats en pression hydrostatique montrent pour la première fois une relation parfaitement linéaire avec la fréquence Brillouin, ce qui fait de la DBS un nouvel outil de mesure de la pression dans les fibres optiques.

Fiber optic sensors are designed to measure various parameters. The distributed fiber optics sensor has been a very promising candidate for the structural health monitoring. In this thesis, we characterized LEAF (Large Effective Area Fiber) fiber’s Brillouin scattering spectrum and investigated its potentiality for the distributed Brillouin temperature and strain sensor. Optical fibers with complex refractive index profiles are applied to improve the Brillouin threshold by varying the Brillouin linewidth. As LEAF fiber has a modified refractive index profile, we investigated its Brillouin linewidth’s dependence on the square of the pump light’s frequency. We verified the Brillouin frequency’s variation with input SOP experimentally for LEAF fiber in the spontaneous regime. This sets a limitation for the frequency resolution of distributed Brillouin sensors. We also realized a simultaneous temperature and strain sensor with LEAF fiber applying the Brillouin optical time domain analysis. Based on the direct detection of LEAF beat frequencies, a simultaneous strain and temperature sensor was demonstrated.

Fiber optic sensors are designed to measure various parameters. The distributed fiber optics sensor has been a very promising candidate for the structural health monitoring. In this thesis, we characterized LEAF (Large Effective Area Fiber) fiber’s Brillouin scattering spectrum and investigated its potentiality for the distributed Brillouin temperature and strain sensor. Optical fibers with complex refractive index profiles are applied to improve the Brillouin threshold by varying the Brillouin linewidth. As LEAF fiber has a modified refractive index profile, we investigated its Brillouin linewidth’s dependence on the square of the pump light’s frequency. We verified the Brillouin frequency’s variation with input SOP experimentally for LEAF fiber in the spontaneous regime. This sets a limitation for the frequency resolution of distributed Brillouin sensors. We also realized a simultaneous temperature and strain sensor with LEAF fiber applying the Brillouin optical time domain analysis. Based on the direct detection of LEAF beat frequencies, a simultaneous strain and temperature sensor was demonstrated.

Abstract The polymer electrolytes (ion conducting polymers) consist of macromolecules (usually in the form of polyethereal units) that are doped with alkali mental salts. The polymer electrolytes are being used in Li-polymer buttery. It is suggested that conductivity in these systems takes place through two distinct events. The first is associated with the charge migration of ions between coordination sites in the host material, and the second is that the conductivity is generally observed to rise with increasing flexibility of the polymer chains. Rayleigh-Brillouin scattering spectra of molecular liquids will provide mechanical relaxation information in the frequency range from 10^8 to 10^11 Hz. We have carried out the Brillouin scattering study of PEG400/LiCl mixtures to probe its elastic properties. The change in the flexibility of polymer chains at different temperatures, the fraction of free ion, and their interactions with polymer all effect the Brillouin spectrum and the present work suggests the usefulness of this technique as an useful tool to probe the various interactions in polymer electrolytes.

As features on integrated circuits continue to shrink, currently at 22 nm and predicted to approach 10 nm by 2020, the semiconductor industry is rapidly brushing up against the fundamental limits of electric charge and current based devices. These limits are due to the fact that charges are being pushed around in tiny areas and they repel one another with significant force. Fortunately, there are many other degrees of freedom in solids that do not suffer from these limitations and are just waiting to be harnessed in useful devices. This idea is behind all of the fields that have lately been proliferating ending in -onics, photonics, plasmonics, phononics, and of most relevance to this dissertation spintronics. Spintronics refers to a field of research wherein ways are sought to utilize the spin property of the electron in devices. One of the most attractive aspects of electron spin is that it can be used to store (transiently or permanently), process, and transmit information. The main challenge in spintronics is accessing the spin degree of freedom. Until the discovery of the giant magnetoresistance effect in the late 1980's, the only way to manipulate the electron spin was through a magnetic field. Recent developments have shown that electron spins can be controlled with direct currents of both heat and electrons, which have the benefit of being easy to generate and direct without interfering over a large area. The purpose of this dissertation is to study methods of controlling the dynamics of magnetization in thin films for spintronic applications by imaging the spin wave intensity in devices. To this end we have constructed a micro-focus Brillouin Light Scattering system to map the intensity of spin waves propagating in thin ferromagnetic films on the sub-micron scale. We have studied issues relating to fundamental issues of spin wave propagation in thin films. We have investigated the possibility of spin wave amplification with direct charge currents and spin currents generated by the spin Hall effect. Furthermore, we have demonstrated the ability to measure the magnon and phonon temperatures, which is important for studies of thermal transport. / text