In this thesis, resonance enhanced multiphoton ionisation (REMPI) in combination with time-of-flight mass spectrometry (TOF-MS) has been used to detect nascent photofragments resulting from the UV dissociation of a variety of small molecules. The translational anisotropy and angular momentum polarisation of these photofragments has been measured and used to elucidate the underlying photodissociation dynamics. Firstly, the photodissociation of NO₂ at 320nm has been investigated and the vector correlations of the nascent NO photofragments have been measured in terms of a set of semi-classical bipolar moments. The measured angular momentum alignment is found to be consistent with an impulsive model for the dissociation, with <b>&mu;</b> and <b>&nu;</b> in the same molecular plane and both preferentially perpendicular to <b>J</b>, whilst angular momentum orientation measurements provide evidence for an additional torque due to the O-N-O bond opening during dissociation. These measurements were taken using a rotationally cooled, skimmed molecular beam and significant deviations were found between the bipolar moments measured using this source and previous measurements using a rotationally hotter source. The effect of parent molecular rotations on the measured bipolar moments has been quantified and successfully used to explain these deviations. The photodissociation of Cl₂ has been studied in the wavelength region (320-350)nm. UV absorption in this wavelength region may result in two dissociation channels, (Cl+Cl) and (Cl+Cl*), and the angular momentum polarisation of both the Cl(²P_3/2) and Cl*(²P_1/2) photofragments has been measured. This angular momentum polarisation has been reported in terms of a polarisation parameter formalism which, together with the measured translational anisotropies, has been used to determine the different potential energy surfaces contributing to the dissociation process. Translational anisotropy measurements of the Cl(²P_3/2) fragments have shown that, for the ground-state channel, dissociation results from a pure perpendicular transition to the C state, whilst alignment measurements show that non-adiabatic transitions to the A state are significant at large internuclear separations. The measured alignment parameters are found to be relatively constant for all dissociation wavelengths and are consistent with theoretical predictions. Translational anisotropy measurements of the Cl(2P_1/2) photofragments show that, for the excited-state channel, dissociation occurs following a mixed parallel and perpendicular excitation to the B and C states respectively and the interference between these two dissociation pathways has been shown to result in angular momentum orientation. The predissociation dynamics of the C ³&Pi;_g (&nu;=0) and (&nu;=1) Rydberg states of O₂ has been extensively studied. The translational anisotropy and angular momentum alignment of the O(³P) and O(¹D) photofragments resulting from this predissociation has been measured in terms of a polarisation parameter formalism, which has been extended for a two-photon dissociation process. Measurements have been taken at various fixed wavelengths within the two bands in order to investigate the differences in the predissociation dynamics of intermediate levels with different values of |&Omega;|(=0,1,2 in this case). The translational anisotropy is found to be dependent on the dissociation wavelength with the variations found to be consistent with rotational depolarisation due to the long lifetime of the excited C state. All photofragments have been found to be aligned, with the relationship between the measured O(³P) and O(¹D) alignment being found to be consistent with a diabatic model of the dissociation. In addition, all photofragments are found to display coherent orientation resulting from interference between two possible two-photon absorption pathways. The measured orientation is affected by rotational depolarisation due to the long lifetime of the excited C state; once this effect is accounted for the orientation is found to be nearly constant over all dissociation wavelengths. The origin of the coherent orientation is attributed to two-photon absorption to different spin-orbit components of the C state.

We investigate two medium-facilitated interactions between properties of light upon propagation through optical fiber. The first is interaction between the spin and intrinsic orbital angular momentum in a linear optical medium. This interaction gives rise to fine structure in the longitudinal momenta of fiber modes and manifests in rotational beating effects. We probe those beating effects experimentally in cutback experiments, where small segments are cut from the output of a fiber to probe the evolution of both output polarization and spatial orientation, and find agreement between theoretical predictions and measured behavior. The second is nonlinear optical interaction due to cross- and self-phase modulation between the complex-valued temporal amplitude profile of pump pulses and the amplitude profiles of generated signal and idler pulses in optical fiber photon-pair sources utilizing the four-wave mixing process named modulation instability. We develop a model including the effects of these nonlinear phase modulations (NPM) describing the time-domain wave function of the output biphoton in the low-gain regime. Assuming Gaussian temporal amplitude profiles for the pump pulse, we numerically simulate the structure of the biphoton wave function, in symmetric and asymmetric group velocity matching configurations. Comparing the overlap of the joint temporal amplitudes with and without NPM indicates how good of an approximation neglecting NPM is, and we investigate the effects of NPM on the Schmidt modes. We find that effects of NPM are small on temporally separable sources utilizing symmetric group velocity matching, but appreciably change the state of temporally entangled sources with the same group velocity matching scheme. For sources designed to produce entangled biphotons, our simulations suggest that NPM increases the Schmidt number, which may increase entanglement resource availability with utilization of a phase-sensitive detection scheme. We find that NPM effects on temporally separable sources designed with asymmetric group velocity matching produce non-negligible changes in the state structure. The purity is unaffected at perfect asymmetric group velocity matching, but if the pump is detuned from the correct wavelength, the purity degrades. The largest changes to the state due to NPM occur in long fibers with long pulse durations and low repetition rates.

Objetiva-se discutir e explorar as consequências da conservação do momento angular em situações físicas que apresentem dissipação de energia. Frequentemente, sistemas mecânicos dissipativos são omitidos nas formulações matemáticas da mecânica clássica. No entanto, a conservação da energia mecânica é uma idealização drasticamente incompatível, a longos períodos de tempo, com a maioria das situações reais. Apesar de parecer controversa, esta abordagem é compreensível desde que é incluída na dissipação toda a complexidade dos sistemas mecânicos, os quais não podemos modelar completamente. Espera-se assim que os resultados obtidos sejam parcialmente comprovados em experimentos, sendo que a discrepância é atribuída à parte desconhecida do fenômeno, que muitas vezes é considerada irrelevante para fins práticos. Devido à mencionada complexidade de fenômenos dissipativos, a postura adotada nesta dissertação foi analisar específicos exemplos, de natureza distinta, simplificados, que apresentem as duas propriedades em questão. Concentrou-se especialmente no problema de dissipação de energia em corpos deformáveis na ausência de estímulos externos. / The goal of this work is to study physical systems where angular momentum is a conserved quantity while energy is dissipated. It is a common practice among people working on classical mechanics to neglect energy dissipation. While this hypothesis leads to beautiful mathematical theories, it is strongly violated by the majority of real world systems. The physical complexity of the many ways in which energy is dissipated turns the mathematical modelling of dissipative forces troublesome. There is essentially no general mathematical model for dissipative forces in good agreement with a wide range of experiments. This is in contrast to the very few accepted conservative force models: gravity, elasticity and magneto-electricity. The dissipative force model usually varies among the various physical situations. So, in this work several systems where energy is dissipated while angular momentum is conserved will be considered. The main example will be the motion of a deformable body free from external forces and torques.

Recent advances in the chemical vapor deposition method of growing graphene sheets suggest that graphene rings can grow. We may anticipate that chemical methods can be developed to construct twisted nano-ribbons to form Möbius structures in the very near future. I investigated the quantum mechanics of an electron constrained to motion on a nanoscale Möbius ring by solving the Schrdinger equation on the curved surface. The close analogy between ordinary cylindrical rings and Möbius rings is displayed by the closeness of their energy spectra. The expectation values for the angular momentum component L_z are shown to be close, but not exactly equal, to integral or half-integral multiples of hbar. The half-integer angular momentum states are present only for the nontrivial topology of Möbius rings. The effect of the curvature of the Möbius rings manifests itself in the level splitting. This can be understood in terms of representations of the discrete rotational groups C_nv. The nonzero variance of L_z will allow weak transitions between integral and half-integral angular momentum states, while preserving the unit angular momentum for photons. Again, since the topology of the system is critical for the Aharonov-Bohm effect, I investigated the AB effect on Möbius rings and found a remarkable pattern in transmission through finite-width 2D ring structures with finite-width input and output contacts attached at the periphery. The periodicity in the magnetic flux, in units of h/e, is weakly broken on 2D rings of finite width. The unusual states with half-integer values of observed on Möbius rings, investigated earlier, display a different characteristic in transmission. In view of the fascinating properties displayed by the non-trivial topology in terms of its novel two-dimensional physics, we expect that the properties of carriers on the Möbius ring that we have presented here will be relevant for practical applications.

Three-dimensional (3D) displays project 3D images that give 3D perceptions and mimic real-world objects. Among the rich varieties of 3D displays, multiview displays take advantage of light’s various degrees of freedom and provide some of the 3D perceptions by projecting 2D subsampling of a 3D object. More 2D subsampling is required to project images with smoother parallax and more realistic sensation. As an additional degree of freedom with theoretically unlimited state space, orbital angular momentum (OAM) modes may be an alternative to the conventional multiview approaches and potentially project more images. This research involves exploring the possibility of encoding/decoding off-axis points in 2D images with OAM modes, development of the optical system, and design and development of a multiview colour display architecture. The first part of the research is exploring encoding/decoding off-axis points with OAM modes. Conventionally OAM modes are used to encode/decode the on-axis information only. Analysis of on-axis OAM beams referenced to off-axis points suggests representation of off-axis displacements as a set of expanded OAM components. At current stage off-axis points within an effective coding area are possible to be encoded/decoded with chosen OAM modes for multiplexing. Experimentally a 2D image is encoded/decoded with an OAM modes. When the encoding/decoding OAM modes match, the image is reconstructed. On the other hand, a dark region with zero intensity is shown. The dark region suggests the effective coding area for multiplexing. The final part of the research develops a multiview colour display. Based on understandings of off-axis representation of a set of different OAM components and experimental test of the optical system, three 1 mm monochromatic images are encoded, multiplexed and projected. Having studied wavelength effects on OAM coding, the initial architecture is updated to a scalable colour display consisting of four wavelengths.

Imaging at the nanoscale and/or at remote locations holds great promise for studies in fields as disparate as the life sciences and materials sciences. One such microscopy technique, stimulated emission depletion (STED) microscopy, is one of several fluorescence based imaging techniques that offers resolution beyond the diffraction-limit. All current implementations of STED microscopy, however, involve the use of free-space beam shaping devices to achieve the Gaussian- and donut-shaped Orbital Angular Momentum (OAM) carrying beams at the desired colors –-- a challenging prospect from the standpoint of device assembly and mechanical stability during operation. A fiber-based solution could address these engineering challenges, and perhaps more interestingly, it may facilitate endoscopic implementation of in vivo STED imaging, a prospect that has thus far not been realized because optical fibers were previously considered to be incapable of transmitting the OAM beams that are necessary for STED. In this thesis, we investigate fiber-based STED systems to enable endoscopic nanoscale imaging. We discuss the design and characteristics of a novel class of fibers supporting and stably propagating Gaussian and OAM modes. Optimization of the design parameters leads to stable excitation and depletion beams propagating in the same fiber in the visible spectral range, for the first time, with high efficiency (>99%) and mode purity (>98%). Using the fabricated vortex fiber, we demonstrate an all-fiber STED system with modes that are tolerant to perturbations, and we obtain naturally self-aligned PSFs for the excitation and depletion beams. Initial experiments of STED imaging using our device yields a 4-fold improvement in lateral resolution compared to confocal imaging. In an experiment in parallel, we show the means of using q-plates as free-space mode converters that yield alignment tolerant STED microscopy systems at wavelengths covering the entire visible spectrum, and hence dyes of interest in such imaging schematics. Our study indicates that the vortex fiber is capable of providing an all-fiber platform for STED systems, and for other imaging systems where the exploitation of spatio-spectral beam shaping is required.

This thesis encompasses a body of experimental work on the use of structured light in quantum cryptographic protocols. In particular, we investigate the ability to perform quantum key distribution through various quantum channels (fibre, free-space, underwater) in laboratory and realistic conditions. We first demonstrate that a special type of optical fibre (vortex fibre) capable of coherently transmitting vector vortex modes is a viable quantum channel. Next, we describe the first demonstration of high-dimensional quantum cryptography using structured photons in an urban setting. In particular, the prevalence of atmospheric turbulence can introduce many errors to a transmitted key; however, we are still able to transmit more information per carrier using a 4-dimensional scheme in comparison to a 2-dimensional one. Lastly, we investigate the possibility of performing secure quantum communication with twisted photons in an uncontrolled underwater channel. We find that though it is possible for low-dimensional schemes, high-dimensional schemes suffer from underwater turbulence without the use of corrective wavefront techniques.

No description available.

Although a tropical cyclone may conceptually be regarded as an axisymmetric vortex, there is substantial evidence that asymmetric dynamics play an important role. In this thesis, dynamical impacts of rotating convective asymmetries are examined in this thesis. Two types of rotating convective asymmetries are considered: rotating eyewall convective maximum which is located in the core region of the storm and spiral bands which are located outside the core. Both of them can be characterized as rotating asymmetric convective heat sources, and they are superimposed on a balanced, axisymmetric vortex to approximate the effect of rotating eyewall convective maximum and spiral bands on tropical cyclone by using a simple nonhydrostatic three-dimensional, but linear model that is based on vortex anelastic equations. The evolution of rotating convective asymmetric heat sources on a balanced, axisymmetric vortex, which is modeled after tropical cyclones, is investigated to examine angular momentum transport by gravity waves that radiate away from the core region. Results show that gravity waves can transport angular momentum away from a tropical cyclone, but a very small amount, which is several orders of magnitude smaller than the estimate by recent studies. The significantly large difference may largely be due to the difference between two-dimensional and three-dimensional adjustment processes. Assuming that the effects of spiral bands on tropical cyclone wind field are caused by the response to diabatic heating in their convection, rotating asymmetric heat sources are constructed to reflect observations of spiral bands. These heat sources are rotated around a realistic but idealized balanced axisymmetric vortex. Simulation results show that the response of tropical cyclone wind field to idealized spiral band heat sources can successfully capture a number of observed well-known features of spiral band circulation, such as overturning secondary circulation, descending mid-level inflow, and cyclonic tangential acceleration. Comparison to full-physics numerical simulations confirms the validity of this method which provides a simple dynamical framework to better understand the impact of spiral bands in tropical cyclone.

High angular momentum Rydberg wave packets are studied. Application of carefully tailored electric fields to low angular momentum, high- n ( n ∼ 300) Rydberg atoms creates coherent superpositions of Stark states with near extreme values of angular momentum, [cursive l]. Wave packet components orbit the parent nucleus at rates that depend on their energy, leading to periods of localization and delocalization as the components come into and go out of phase with each other. Monitoring survival probability signals in the presence of position dependent probing leads to observation of characteristic oscillations based on the composition of the wave packet. The discrete nature of electron energy levels is observed through the measurement of quantum revivals in the wave packet localization signal. Time-domain spectroscopy of these signals allows determination of both the population and phase of individual superposition components. Precise manipulation of wave packets is achieved through further application of pulsed electric fields. Decoherence effects due to background gas collisions and electrical noise are also detailed. Quantized classical trajectory Monte-Carlo simulations are introduced and agree remarkably well with experimental results.