The doctoral thesis "Low frequency modes from small nanoparticles (metal nanocrystals) to large nanospheres (viruses): an inelastic light scattering study" is dedicated to investigations of the acoustic properties of different nano-objects : small metal nanoparticles and nanocrystals (D < 30 nm) and large colloid/viral particles (D _ 200 nm). Inelastic light Raman/Brillouin scattering is used as the main research tool to probe the nanoparticle vibrations and to determine their elastic and mechanical parameters. In the first chapter, the well developed theory of elasticity is used to perform a qualitative and nomenclatural analysis of solid sphere vibrations ; several theoretical models allowing to describe the nanoparticle vibrational behavior within a surrounding medium and how the eigenvibrations are modified due to inner crystalline elastic anisotropy are discussed. The second chapter is dedicated to the description of the physics of inelastic light scattering which derives from the fluctuations of the polarizability induced by vibrations. Two types of inelastic light scattering are described : Brillouin scattering which results from the coupling of incident light (photon) with acoustic propagative waves (phonon) in a bulk substance and Raman scattering which is a result of the interaction between an incident photon and localized vibrations, hence nanoparticle vibrations in the present study. As essential in our study, the detailed description and principles of operation of the spectroscopic tools (tandem Fabry-Perot) used to perform these very low frequency inelastic light scattering spectroscopies (between 3 and 300 GHz typically) are given. The third chapter focuses on the study of low frequency modes from small metallic nanoparticles. Three systems are investigated : AuAg and Cu nanoparticles embedded in a vitreous matrix and Au nanocrystals deposited on a surface. The AuAg system allowed to study a notably rich Raman spectrum featuring contributions from fundamental modes and high order harmonics. The experimental data were found to compare rather well with theoretical predictions, thereby providing more insight into the essential ingredients of Raman scattering from nanoparticle modes. The study of deposited Au nanocrystals allowed characterizing the effect of nanocrystalline quality which results in a partial lifting of degeneracy of the nanoparticle modes due to elastic anisotropy. Investigating the wavelength dependence of the Raman spectrum allows a differentiation between single nanocrystals and multiply twinned nanoparticles. Both embedment effects and nanocrystallinity effects are integrated in the study of Cu nanoparticles grown in a glass matrix, where the influence of annealing conditions on the produced nanoparticles was investigated. It was shown that different annealing temperatures [...] result in very different low frequency Raman profiles. [...] The forth chapter reports on the exploration of the possible use of the low frequency inelastic light scattering probe in the characterization of large viruses, as illustrated in the third chapter for small nanoparticles. In order to address the change of the light selection rules as the wavelength of the exciting light becomes comparable to the size of the nanoparticles, the behaviors of the viruses are compared to those of polymer colloids. Ultra Small Angle X-ray Scattering and Atomic Force Microscopy are used to first ensure the comparableness of viruses and polystyrene colloids in terms morphologies. On the basis of the inelastic light scattering data obtained for PS colloids [...], we discuss the difficult interpretation in termsof eigenmodes of the virus counterparts.

Techniques to control dispersion in a medium have attracted much attention due to potential applications to devices such as ring laser gyroscopes, interferometric gravitational wave detectors, data buffers, phased array radars and quantum information processors. Of particular interest is an optical resonator containing a medium with an anomalous dispersion corresponding to fast-light, which behaves as a White Light Cavity (WLC). A WLC can be tailored to improve the sensitivity of sensing devices as well as to realize an optical data buffering system that overcomes the delay-bandwidth product of a conventional cavity. This dissertation describes techniques to tailor the dispersion for fast-light in intracavity media. We present first a demonstration of fast-light in a photorefractive crystal. When placed inside a cavity, such a medium could be used to enhance the bandwidth of a gravitational wave detector. We then describe how a superluminal laser can be realized by adding anomalously dispersive medium inside a ring laser. We identify theoretical conditions under which the sensitivity of the resonance frequency to a change in the cavity length is enhanced by as much as seven orders of magnitude. This paves the way for realizing a fast-light enhanced ring laser gyroscope, for example. This is followed by the development of a novel data buffering system which employs two WLC systems in series. In this system, a data pulse can be delayed an arbitrary amount of time, without significant distortion. The delay time is independent of the data bandwidth, and is limited only by the attenuation experienced by the data pulse as it bounces between two high-reflectivity mirrors. Such a device would represent a significant breakthrough in overcoming the delay-time bandwidth product limitation inherent in conventional data buffers. We then describe our experimental effort to create a fiber-based WLC by using stimulated Brillouin scattering (SBS). Experimental results, in agreement with our theoretical model presented here, show that the WLC effect is small under the conditions supported by current fiber optic technology. We conclude that future efforts to induce a large WLC effect would require fibers with high Brillouin coefficient and low transmission loss, as well as optical elements with very low insertion loss and high power damage thresholds.

The atomic dynamics in liquids is still a challenging subject. The objective of this thesis was to study how the dynamics depends on the TYPE of the atomic interaction. Dynamic properties extracted from inelastic neutron scattering experiments on three binary systems clearly show a discontinous behaviour in the transition from a pure metallic to an ionic and partly covalent bonding regime. Further, results of Monte-Carlo simulations of a new type of spectrometer, a Neutron-Brillouin-Spectrometer, that is currently under construction, are presented. / In dieser Arbeit wurde der Einfluss der Art der zwischenatomaren Wechselwirkung auf die atomare Dynamik in Fluessigkeiten untersucht. Dafuer wurden geeignete binaere Systeme ausgewaehlt und deren Dichtefluktuationen mittels unelastischer Neutronenstreuung gemessen. Neben den teilweise bekannten strukturellen Veraenderungen, die beim Uebergang von rein metallischen zu ionischen und teilweise kovalenten Bindungen auftreten, konnten vor allem die Auswirkungen wechselnder Bindungsverhaeltnisse auf eine Reihe dynamischer Eigenschaften nachgewiesen werden. Besonders hervorzuheben sind dabei der Nachweis eines Hochfrequenzbandes im Frequenzspektrum des fluessigen RbSb sowie in den fluessigen Na-Sn Legierungen die Aufspaltung der aus der longitudinalen Stromkorrelationsfunktion abgeleiteten Dispersion in zwei Baender, die die verschiedenartige Dynamik der unterschiedlich schweren Komponenten widerspiegeln. Desweiteren werden in dieser Arbeit Ergebnisse umfangreicher Monte-Carlo Simulationen fuer ein im Bau befindliches neuartiges Neutronen-Brillouin-Spektrometer vorgestellt.

High-speed optical networks will require all-optical signalprocessing to avoid bottleneck due to optical-to-electrical (O/E)and electrical-to-optical (E/O) conversion. Enabling of opticalprocessing tasks such as optical buffering and data synchronizationwill require large tunable delay. Recently, slow-light physics gotwide attention to generate tunable delay. However, for a slow-lightsystem large delay comes at the expense of increased distortion.This dissertation presents a study of the slow-light systems andquantifies the limitations imposed on delay due to distortion andsystem resource constraints. Optimal designs for two- and three-lineBrillouin slow-light systems showed fractional pulse delay of up to1.7 compared to a single-line gain system. Optimal designs forbroadband Brillouin gain system showed upto 100\% delay improvementcompared to the Gaussian pump. Wavelength conversion and dispersionbased tunable delay systems showed bit delay of 15 bits. An opticalbuffer based on photorefractive medium for real-time data storagewas demonstrated by storing and retrieving a 7-bit data sequence.

<p>All-optical devices have attracted many research interests due to their ultimately low heat dissipation compared to conventional devices based on electric-optical conversion. With recent advances in nonlinear optics, it is now possible to design the optical properties of a medium via all-optical nonlinear effects in a table-top device or even on a chip.</p><p>In this thesis, I realize all-optical control of the optical group velocity using the nonlinear process of stimulated Brillouin scattering (SBS) in optical fibers. The SBS-based techniques generally require very low pump power and offer a wide transparent window and a large tunable range. Moreover, my invention of the arbitrary SBS resonance tailoring technique enables engineering of the optical properties to optimize desired function performance,</p><p>which has made the SBS techniques particularly widely adapted for</p><p>various applications.</p><p>I demonstrate theoretically and experimentally how the all-optical</p><p>control of group velocity is achieved using SBS in optical fibers.</p><p>Particularly, I demonstrate that the frequency dependence of the</p><p>wavevector experienced by the signal beam can be tailored using</p><p>multi-line and broadband pump beams in the SBS process. Based on the theoretical framework, I engineer the spectral profile</p><p> to achieve two different application goals: a uniform low group velocity (slow light) within a broadband spectrum, and a group velocity with a linear dependence on the frequency detuning (group velocity dispersion or GVD).</p><p>In the broadband SBS slow light experiment, I develop a novel noise current modulation method that arbitrarily tailors the spectrum of a diode laser. Applying this method, I obtain a 5-GHz broadband SBS gain with optimized flat-topped profile, in comparison to the ~40 MHz natural linewidth of the SBS resonance. Based on the broadband SBS resonance, I build a 5-GHz optical buffer and use this optical buffer to delay a return-to-zero data sequence of rate 2.5 GHz (pulse width 200 ps). The fast noise modulation method significantly stabilizes the SBS gain and improves the signal fidelity. I obtain a tunable delay up to one pulse-width with a peak signal-to-noise ratio of 7. I also find that SBS slow light performance can be improved by avoiding competing nonlinear effects. A gain-bandwidth product of 344 dB.GHz is obtained in our system with a highly-nonlinear optical fiber.</p><p>Besides the slow light applications, I realize that group velocity dispersion is also optically controlled via the SBS process. In the very recent GVD experiment, I use a dual-line SBS resonance and obtain a tunable GVD parameter of 7.5 ns$^2$/m, which is 10$^9$ times larger than the value found in a single-mode fiber. The large GVD system is used to disperse an optical pulse with a pulse width of 28 ns, which is beyond the capability for current dispersion techniques working in the picosecond and sub picosecond region. The SBS-based all-optical control of GVD is also widely tunable and can</p><p>be applied to any wavelength within the transparent window of the</p><p>optical fiber. I expect many future extensions following this work</p><p>on the SBS-based all-optical GVD control using the readily developed SBS tailoring techniques.</p><p>Finally, I extend the basic theory of backwards SBS to describe the forward SBS observed in a highly nonlinear fiber, where asymmetric forward SBS resonances are observed at the gigahertz range. An especially large gain coefficient of 34.7 W$^{-1}$ is observed at the resonance frequency of 933.8 MHz. This is due to good overlap between the optical wave and the high order guided radial acoustic wave. The interplay from the competing process known as the Kerr effect is also accounted for in the theory.</p> / Dissertation

No description available.

The object of this thesis is the study of nanostructured thin films using inelastic fight scattering and elastic x-ray scattering techniques. Their use in combination with other techniques is a powerful tool for the investigation of nanostructured materials. X-ray, Raman and Brillouin characterisation of cluster-assembled carbon films, promising for applications in the field of catalysis, hydrogen storage and field emission, is here presented. X-ray reflectivity (XRR) provided a measure of the density. Raman spectroscopy showed that the local bonding in these amorphous films depends on the size distribution of the clusters and that it is possible to select the cluster size in order to grow films with tailored properties. Brillouin scattering provided a characterisation at the mesoscopic scale and an estimate of the elastic constants, revealing a very soft material. XRR was employed to study density, layering and roughness of a wide range of amorphous carbon films grown with different techniques. Some films possess an internal layering due to plasma instabilities in the deposition apparatus. By comparing XRR with Electron Energy Loss Spectroscopy, a unique value for the electron "effective mass" was deduced and a general relationship between sp(^3)-content and density was found. XRR and H effusion were used to determine the hydrogen content. A study of the size-dependent melting temperature in tin nanoparticle thin films was undertaken with a combined use of X-Ray Diffraction (XRD) and light scattering. A redshift in the position of a Rayleigh peak in the temperature-dependent Brillouin measurements was shown to be related to the melting of the nanoparticles and explained by an effective medium model. XRD also provided information on the low-level of stress in the particles. Low-frequency Raman scattering was used to study the behaviour of the acoustic modes of a single particle as a function of temperature.

Made available in DSpace on 2014-12-17T15:14:58Z (GMT). No. of bitstreams: 1 FilipeASB_DISSERT.pdf: 919582 bytes, checksum: 74ab71c48467a95bd20314187ea48c0d (MD5) Previous issue date: 2012-07-06 / We studied the spin waves modes that can propagate in magnetic multilayers composed of ferromagnetic metallic films in the nanometer scale. The ferromagnetic films (iron) are separated and coupled through the nonmagnetic spacer films (chromium). The films that make up the multilayer are stacked in a quasiperiodic pattern, following the Fibonacci and double period sequences. We used a phenomenological theory taking into account: the Zeeman energy (between the ferromagnetic films and the external magnetic field), the energy of the magneto-crystalline anisotropy (present in the ferromagnetic films), the energy of the bilinear and biquadratic couplings (between the ferromagnetic films) and the energy of the dipole-dipole interaction (between the ferromagnetic films), to describe the system. The total magnetic energy of the system is numerically minimized and the equilibrium angles of the magnetization of each ferromagnetic film are determined. We solved the equation of motion of the multilayer to find the dispersion relation for the system and, as a consequence, the spin waves modes frequencies. Our theoretical results show that, in the case of trilayers (Fe/Cr/Fe), our model reproduces with excellent agreement experimental results of Brillouin light scattering, known from the literature, by adjusting the physical parameters of the nanofilms. Furthermore, we generalize the model to N ferromagnetic layers which allowed us to determine how complex these systems become when we increase the number of components. It is worth noting that our theoretical calculations generalize all the results known from the literature / Neste trabalho, estudamos os modos de ondas de spin que podem se propagar em multicamadas magn?ticas compostas por filmes met?licos ferromagn?ticos em escala nanom?trica. Os filmes ferromagn?ticos (ferro) s?o intercalados e acoplados atrav?s de filmes espa?adores n?o-magn?ticos (cromo). Os filmes que comp?em a multicamada s?o empilhados de uma forma quasiperi?dica, seguindo as sequ?ncias de Fibonacci e per?odo duplo. Utilizamos uma teoria fenomenol?gica levando em conta: a energia Zeeman (entre os filmes ferromagn?ticos e o campo magn?tico externo), a energia de anisotropia magneto-cristalina (presente nos filmes ferromagn?ticos), a energia dos acoplamentos bilinear e biquadr?tico (entre os filmes ferromagn?ticos) e a energia da intera??o tipo dipolo-dipolo (entre os filmes ferromagn?ticos), para descrever o sistema. A energia magn?tica total do sistema ? minimizada numericamente e os ?ngulos de equil?brio das magnetiza??es de cada filme ferromagn?tico s?o determinados. Em seguida, resolvemos a equa??o de movimento da multicamada para encontrarmos a rela??o de dispers?o para o sistema e consequentemente as frequ?ncias dos modos de ondas de spin. Nossos resultados te?ricos mostram que, no caso de tricamadas (Fe/Cr/Fe), nosso modelo consegue reproduzir com excelente concord?ncia resultados experimentais de espalhamento de luz Brillouin, conhecidos da literatura, atrav?s do ajuste dos par?metros f?sicos dos nanofilmes. Al?m disso, generalizamos o modelo para N camadas ferromagn?ticas, o que nos permitiu verificar o qu?o complexo esses sistemas se tornam quando aumentamos o n?mero de componentes. Vale a pena salientar que nossos c?lculos te?ricos generalizam todos os resultados conhecidos da literatura

In this dissertation, high-power ytterbium-doped fiber amplifiers designed with advanced waveguide concepts are characterized and power scaled. Fiber waveguides utilizing cladding microstructures to achieve wave guidance via the photonic bandgap (PBG) effect and a combination of PBG and modified total internal reflection (MTIR) have been proposed as viable single-mode waveguides. Such novel structures allow larger core diameters (>35 μm diameters) than conventional step-index fibers while still maintaining near-diffraction limited beam quality. These microstructured fibers are demonstrated as robust single-mode waveguides at low powers and are power scaled to realize the thermal power limits of the structure. Here above a certain power threshold, these coiled few-mode fibers have been shown to be limited by modal instability (MI); where energy is dynamically transferred between the fundamental mode and higher-order modes. Nonlinear effects such as stimulated Brillouin scattering (SBS) are also studied in these fiber waveguides as part of this dissertation. Suppressing SBS is critical towards achieving narrow optical bandwidths (linewidths) necessary for efficient fiber amplifier beam combining. Towards that end, new effects that favorably reduce acoustic wave dispersion to increase the SBS threshold are discovered and reported. The first advanced waveguide examined is a Yb-doped 50/400 µm diameter core/clad PBGF. The PBGF is power scaled with a single-frequency 1064 nm seed to an MI-limited 410 W with 79% optical-to-optical efficiency and near-diffraction limited beam quality (M-Squared < 1.25) before MI onset. To this author's knowledge, this represents 2.4x improvement in power output from a PBGF amplifier without consideration for linewidth and a 16x improvement in single-frequency power output from a PBGF amplifier. During power scaling of the PBGF, a remarkably low Brillouin response was elicited from the fiber even when the ultra large diameter 50 µm core is accounted for in the SBS threshold equation. Subsequent interrogation of the Brillouin response in a pump probe Brillouin gain spectrum diagnostic estimated a Brillouin gain coefficient, gB, of 0.62E-11 m/W; which is 4x reduced from standard silica-based fiber. A finite element numerical model that solves the inhomogenous Helmholtz equation that governs the acoustic and optical coupling in SBS is utilized to verify experimental results with an estimated gB = 0.68E-11 m/W. Consequently, a novel SBS-suppression mechanism based on inclusion of sub-optical wavelength acoustic features in the core is proposed. The second advanced waveguide analyzed is a 35/350 µm diameter core/clad fiber that achieved wave guidance via both PBG and MTIR, and is referred to as a hybrid fiber. The waveguide benefits mutually from the amenable properties of PBG and MTIR wave guidance because robust single-mode propagation with minimal confinement loss is assured due to MTIR effects, and the waveguide spectrally filters unwanted wavelengths via the PBG effect. The waveguide employs annular Yb-doped gain tailoring to reduce thermal effects and mitigate MI. Moreover, it is designed to suppress Raman processes for a 1064 nm signal by attenuating wavelengths > 1110 nm via the PBG effect. When seeded with a 1064 nm signal deterministically broadened to ~1 GHz, the hybrid fiber was power scaled to a MI-limited 820 W with 78% optical-to-optical efficiency and near diffraction limited beam quality of M_Squared ~1.2 before MI onset. This represents a 14x improvement in power output from a hybrid fiber, and demonstrates that this type of fiber amplifier is a quality candidate for further power scaling for beam combining.

Hybrid microstructured fibers, utilizing both air holes and high index cladding structures, provide important advantages over conventional fiber including robust fundamental mode operation with large core diameters (>30 mu m) and spectral filtering (i.e. amplified spontaneous emission and Raman suppression). This work investigates the capabilities of a hybrid fiber designed to suppress stimulated Brillouin scattering (SBS) and modal instability (MI) by characterizing these effects in a counter-pumped amplifier configuration as well as interrogating SBS using a pump-probe Brillouin gain spectrum (BGS) diagnostic suite. The fiber has a 35 mu m annularly gain tailored core, the center doped with Yb and the second annulus comprised of un-doped fused silica, designed to optimize gain in the fundamental mode while limiting gain to higher order modes. A narrow-linewidth seed was amplified to an MI-limited 820 W, with near-diffraction-limited beam quality, an effective linewidth similar to 1 GHz, and a pump conversion efficiency of 78%. Via a BGS pump-probe measurement system a high resolution spectra and corresponding gain coefficient were obtained. The primary gain peak, corresponding to the Yb doped region of the core, occurred at 15.9 GHz and had a gain coefficient of 1.92x10(-11) m/W. A much weaker BGS response, due to the pure silica annulus, occurred at 16.3 GHz. This result demonstrates the feasibility of power scaling hybrid microstructured fiber amplifiers