Improvements in the treatment of breast cancer have resulted in better survival rates and less breast cancer related morbidity. Nevertheless, a significant group of patients still experience a diminished quality of life as a result of lymphedema. In the early, often reversible, stage of lymphedema patients can experience subjective changes in the affected area. However, with the traditionally available tools the lymphedema often remains clinically undetectable and patients are denied essential care that can prevent worsening. Furthermore, most lymphedema assessment tools fail to support a clear unambiguous definition of lymphedema. This underlines the need for a sensitive objective measurement method that can assess lymphedema in a subclinical stage. In this study we demonstrated that measuring tissue dielectric constant (TDC) using the MoistureMeter-D is an effective method to detect tissue water changes and could potentially provide a cost-effective adequate tool to measure the early onset of breast cancer related lymphedema (BCRL). Secondarily, we established the correlation between the novel TDC method and the frequently used arm volume measurements and self-assessment questionnaires. A group of 20 female patients with clinically BCRL were included. TDC measurements in both arms and all quadrant of both breast were recorded along with volumetric measurements of both arms. All patients were asked to complete a self-report questionnaire. The novel TDC method detected significantly higher tissue water levels in the affected arm and breast compared to the control side. The TDC ratio between control and affected side showed significant correlation with self-reported pain and discomfort in both arm and breast. In the arm, the TDC method also showed correlation with the volume measurement method. The TDC value of the arm was correlated to age, but not to BMI. This study demonstrates that measuring TDC using the MMD is an effective method for quantifying lymphedema in arm and breast and is an important tool in detecting early TWC changes.

This thesis presents an investigation of the dynamic properties of wide range of interfacial systems, from colloidal particles in solution, through the realm of aerosols and onto studies of molecular adsorption at an interface. The primary experimental technique utilized is optical tweezers. An exploration of the history of the use of radiation pressure to manipulate matter is presented, followed by an introduction to how optical tweezers work. Some of the more advanced methods of tweezing are discussed, with an emphasis on the use of spatial light modulators (SLMs) to realise dynamic holographic optical tweezers (DHOTs), an example of which has been constructed within our laboratory using off-the-shelf optical components, and combined with a spectrometer to facilitate high resolution spectroscopic studies of microscopic systems. The spectroscopic analysis of microparticles is greatly enhanced by optical feedback generated when the wavelength of light utilized is an integer number of wavelengths around the circumference of the microsphere. Enhanced signal occurs at these wavelengths, termed whispering gallery modes (WGMs). The absolute position of these resonances depends strongly upon the shape, size and refractive index of the particle, and is predicted by Mie theory. A discussion of the concepts behind Mie theory, as well as how to use an experimental WGM spectrum to deduce the size and composition of a microparticle, is provided. This technique is then put to use in a detailed study on the properties of single aerosols, comprised of sodium chloride solution, and generated using a handheld medical nebulizer. Studies have been carried out on both evaporating and growing droplets trapped with a Gaussian beam; in the latter case, periods of size stability are observed, owing to resonant absorption of radiation at the trapping laser wavelength. The SLM can be used to change the trapping laser to a Laguerre-Gaussian (LG) mode, and an investigation of how this affects the dynamics of the droplet is presented. It is found that the use of LG modes with $ellgeq10$ produced Raman spectra with significantly more intense WGMs, and also suppressed droplet evaporation. Through observations made with fluorescent polystyrene microspheres, it is argued that the LG modes are more efficient at coupling into WGMs of the droplets. Leading on from these experiments on salt water droplets, experiments have been conducted using ionic liquids (ILs). These fluids have many fascinating properties and potential applications. The optical trapping of droplets comprised of aqueous solutions of the ionic liquid ethylammonium nitrate (EAN) and water has been demonstrated for the first time. These droplets are analysed spectroscopically by illuminating them with the output from a broadband LED; WGMs that are observed in the backscattered light are used to determine their size and composition. The response of the droplets to conditions of varying relative humidity has also been investigated. In order to characterise the relative humidity experienced by both the salt water and IL droplets, the concentration of water vapour within the trapping cells has been measured using diode laser absorption spectroscopy. The spatially modulated laser beam is then utilized in a different fashion; instead of optically tweezing a sample, a low numerical aperture objective lens is utilized to focus the laser onto the surface of a gold coated microscope slide. When a colloidal sample is placed on this surface, the thermal gradients cause the particles to form two dimensional crystals. The SLM is utilized to form multiple nucleation sites, and the dynamics of the crystals are directly observed in real time using video microscopy. It is found that grain rotation-induced grain coalescence (GRIGC) occurs, with the rotation of both crystals before coalescence. Control over the grain size is achieved by altering the separation of the laser spots, and shows that the time scale for grain boundary annealing in our system is in good agreement with theoretical expressions formulated for nanocrystal growth. Finally, as a complimentary technique to the microparticle spectroscopy previously discussed, a bulk interface is probed by using evanescent wave broadband cavity enhanced absorption spectroscopy (EW-BBCEAS) specifically to study the adsorption of cytochrome c (cyt c) to a fused silica surface. Visible radiation from a supercontinuum source is coupled into an optical cavity consisting of a pair of broadband high reflectivity mirrors, and a total internal reflection (TIR) event at the prism/water interface. Aqueous solutions of cyt c are placed onto the TIR footprint on the prism surface and the subsequent protein adsorption is probed by the resulting evanescent wave. The time integrated cavity output is directed into a spectrometer, where it is dispersed and analysed. The broadband nature of the source allows observation of a wide spectral range (ca 250 nm in the visible). The system is calibrated by measuring the absorption spectra of dyes of a known absorbance. Absorption spectra of cyt c are obtained for both S and P polarized radiation, allowing information about the orientation of the adsorbed protein to be extracted.

Experimental investigations of the optical properties of GaN nanostructured light emitting diode (LED) arrays are presented. Microphotoluminescence spectroscopy with pulsed and continuous wave lasers was used to probe the carrier dynamics and emission mechanisms of nanorod LED arrays fabricated by a top down etching method. Results show a possible reduction in internal electric field as nanorod diameter decreases. Localisation effects were also observed, affecting the spectral shape of the nanorod emission. Under two-photon excitation, quantum dot-like sharp spectral peaks in the PL spectra are found to exist in abundance amongst all the nanorod samples. The optical properties of these localised states, which are shown to be associated with the nanorod free-surfaces, are characterised using non-linear and time resolved spectroscopy. An investigation into spatially resolved single nanorods was also carried out. Single nanorods were isolated, and characterised using pulsed lasers. The etching is shown to increase the carrier decay life-time at extended intervals over several hundred ns. The temporal evolution and excitation power density dependence of the quantum dot-like states are also presented for the first time. The long lived localised states are thought to arise from surface effects, in particular Fermi-surface pinning, causing localisation and spatial separation of carriers. Additional work on nano-pyramid array LEDs, with quantum wells on semi-polar surfaces is also presented. Optical properties using micro-photoluminescence are compared to cathodoluminescence studies. An uneven distribution of emission wavelengths across the pyramid facet is thought to lead to an emission mechanism involving carriers transferring between multiple spatially localised states. Finally, experimental techniques and fabrication methods for future work are documented in detail.

The effect of uncertainty in gas composition on the accuracy of gas-phase thermometry using Laser-Induced Thermal Grating Spectroscopy, LITGS, is studied. Temperatures are obtained from measurements of the sound speed derived from the frequency of oscillations ƒ_OSC imposed upon the LITGS signal arising from the transit of acoustic waves across the density modulation feature. The dependence of the sound speed, c_s on √γ/m, where γ is the ratio of specific heats and m is the mean molecular mass leads to a dependence upon gas composition. LITGS signals were generated in acetone vapour in a variety of gas mixtures in a temperature controlled cell at 4 bar total pressure using pump pulses from a frequency quadrupled Q-switched Nd:YAG laser at 266 nm and a cw diode pumped solid state probe laser at 671 nm. Studies were undertaken of the variation in ƒ_OSC with gas composition using gas mixtures of O₂ and N₂ with component concentrations in the range 0-100 %, and was found to agree with theoretical predictions. Measurement precision of the data (one standard deviation in 50 measurements) was found to be typically ± 1.7 % for measurements at 4 bar total pressure. The effect of varying concentrations in exhaust gas residuals (EGR) typical of pre-ignition gases in a spark ignition internal combustion engine were studied using synthetic air (N₂/ O₂ mixtures) containing variable amounts of simulated EGR components, CO₂ and H₂O. The effect of variation in CO₂ concentration in dry synthetic air was measured at 4 bar and 30°C and found to agree with theoretical predictions. Experiments conducted at 30°C, with the addition of a saturated vapour pressure of water indicate that the effect of a saturated vapour pressure of water on the oscillation frequency in synthetic EGR is on the borderline of resolution. The effect of variable amounts of typical hydrocarbon fuel vapour on ƒ_OSC was studied using 2,2,4-trimethyl-pentane in gas mixtures composed of synthetic air and variable amounts of EGR and water vapour at 80°C. Kinetic theory was used in order to model the dependence of the oscillation frequency ƒ_OSC on various gas compositions containing fuel and EGR, in order to construct an error surface for comparison with experimental measurements. Experimental data were found to agree with the model predictions to within experimental error for a representative data set within the range of calculated values. The results indicate that uncertainties in temperature values derived from LITGS thermometry can be estimated with confidence within reasonable estimates of composition variations in an internal combustion engine, and should lead to absolute temperature accuracy of within 2-3 %.

This thesis describes the development of a new experimental technique for studying tunable-collision-energy, quantum state-selected, low-temperature ion-molecule reactions. This has been achieved through the combination of a Stark decelerator for neutral dipolar molecules, and a linear Paul ion trap. The Stark deceleration process for ND₃ was examined in detail, through the analysis of experimental data in combination with newly written molecular dynamics simulation programs. In order to prepare a sample of molecules appropriate for collision studies, additional beamline components were introduced after the decelerator. These components were: two hexapoles, to provide transverse focussing, maximising the molecular density; a molecular buncher, providing increased longitudinal velocity resolution; and a fast-opening shutter, to separate decelerated molecules from undecelerated molecules. The sympathetic-cooling of Xe⁺ ions and ND⁺₃ ions by laser-cooled, Coulomb crystallised ⁴⁰Ca⁺ ions with the ion trap was also studied. In particular, the stable trapping of Xe⁺ was demonstrated for the first time, and the experimental developments that led to this are discussed. The work in this thesis represents significant progress towards studying the reaction of tunable-energy ND₃ in the |j,mk> = |1,−1> quantum state with cold Xe⁺ ions. Ion-molecule reactions utilising ND₃ molecules electrostatically guided through the Stark decelerator were performed. It was observed that the main source of error in these experiments was in the calculation of the initial number of Xe⁺ ions that had been sympathetically cooled into the Coulomb crystal. The sensitivity of the crystal morphology to the number of Xe⁺ ions was evaluated using molecular dynamics simulations. Strategies have been developed to reduce this uncertainty in future studies. In addition to experimental work, the theory of low temperature ion-molecule reactions has been developed further. The temperature at which classical and quantum mechanical calculations diverge due to purely statistical effects has been investigated using different model intermolecular potentials, for closed-shell and open-shell species, and in the ground and rotationally excited states. From the results of these calculations, several promising candidate reactions have been suggested that might exhibit statistical quantum behaviour at experimentally achievable temperatures.

Cette thèse reporte une horloge atomique à cellule de césium de haute-performance basée sur le phénomène de piégeage cohérent de population (CPT). Cette horloge associe une diode laser DFB (à 895 nm, raie D1 du Cs), un modulateur électro-optique fibré, un modulateur acousto-optique, un système Michelson, une électronique bas bruit contrôlée par une carte FPGA et une cellule à vapeur de césium contenant un mélange de gaz tampon azote-argon. L’horloge exploite un schéma de pompage CPT optimisé nommé push-pull optical pumping (PPOP) permettant la détection de résonances CPT à fort contraste.L’horloge repose sur l’exploitation d’un nouveau protocole d’interrogation pulsé nommé Auto-Balanced Ramsey (ABR). Ce dernier repose sur l’utilisation de deux séquences Ramsey avec des temps noirs de durées différentes. Ce dernier repose sur l’utilisation de deux séquences Ramsey avec des temps noirs de durées différentes. La mise en place de ce protocole ABR-CPT, amélioré par la suite avec symétrisation (SABR-CPT), conduit à une réduction drastique des effets de déplacement lumineux, avec en particulier une diminution de la sensibilité de la fréquence d’horloge aux variations de puissance laser par un facteur 80 comparativement à une interrogation Ramsey-CPT conventionnelle. Cette horloge CPT démontre à ce jour une stabilité relative de fréquence de 2 10-13 τ -1/2, atteignant le niveau record (pour ce type d’horloge) de 2,5 10-15 à 10 000 s. Des travaux annexes de spectroscopie laser en microcellules à vapeur de césium sont aussi reportés dans ce manuscrit. On notera en particulier la démonstration d’un laser stabilisé par spectroscopie sub-Doppler bi-fréquence dans une microcellule Cs avec une stabilité de fréquence préliminaire meilleure que 2 10-12 à 1 s. Ces performances sont 10 fois meilleures que celles de micro-horloges atomiques micro-ondes CPT. / This thesis reports a high-performance Cs vapor cell atomic based on coherent population trapping (CPT). This clock combines a DFB diode laser (895 nm, Cs D1 line), a fibred electro-optical modulator, an acousto-optical modulator, a Michelson system, FPGA-based low noise electronics and a N2-Ar buffer gas filled Cs vapor cell. The clock is based on an optimized CPT pumping scheme, named push-pull optical pumping (PPOP), allowing the detection of high-contrast CPT resonances.The clock uses a novel pulsed interrogation protocol named Auto-Balanced Ramsey (ABR). This method is based on the extraction of two error signals derived from two successive Ramsey sequences with different dark periods. The ABR-CPT protocol, improved further with symmetrization (SABR-CPT), allows a drastic reduction of light-shifts effects, yielding in particular to reduce the sensitivity of the clock frequency to laser power variations by a factor 80, in comparison with a standard Ramsey-CPT interrogation. This clock CPT demonstrates a fractional frequency stability of 2 10-13 τ -1/2, reaching the record level (for this kind of clock) of 2.5 10-15 at 10 000 s. Annex laser spectroscopy studies in Cs microfabricated cells were performed in this thesis. We shall note the preliminary demonstration of a laser frequency-stabilized using dual-frequency sub-Doppler spectroscopy in a Cs microcell, exhibiting a fractional frequency stability better than 2 10-12 at 1 s. These performances are 10 times better than those of microwave CPT-based chip-scale atomic clocks.

In dieser Arbeit wurde eine einfache laserspektroskopische Messmethode für lokale elektrische Feldstärken im Hinblick auf ihre Messmöglichkeiten und -grenzen untersucht. Als empfindliche optische Feldsensoren dienen dabei Wasserstoffatome, für die die Stark-Aufspaltung der Spektrallinien im elektrischen Feld wohl bekannt und exakt berechenbar ist. Die experimentellen Untersuchungen wurden an einer Niederdruck-Gaszelle durchgeführt, in der ein elektrisch geheizter Wolframdraht für thermische Dissoziation von Wasserstoffmolekülen sorgte. Die Wasserstoffatome wurden durch zwei gegenläufige Laserstrahlen Doppler-frei angeregt. Die Durchstimmung der schmalbandigen Laserstrahlung über den Wellenlängenbereich der Zwei-Photonen-Resonanz lieferte direkt das vom elektrischen Feld hervorgerufene Stark-Spektrum des angeregten Zustands. Weil die Methode im Gegensatz zu ähnlichen, erheblich aufwendigeren Verfahren nur die niedrigsten Wasserstoff-Energieniveaus benutzt, die mit Zwei-Photonen-Anregung direkt aus dem Grundzustand erreichbar sind, kommt sie mit einem einzigen Laser aus. Für das erste angeregte Niveau mit n = 2 wird Strahlung bei 243 nm benötigt, das nächsthöhere Niveau mit n = 3 erfordert 205 nm. Für n = 2 wurden Untersuchungen an Wasserstoff und Deuterium durchgeführt und Stark-Spektren mittels optogalvanischer Detektion gemessen. Schwerpunkt der Arbeit waren aber die Messungen an Wasserstoff für n = 3, bei denen zusätzlich Balmer-alpha-Fluoreszenz im Sichtbaren zur Detektion eingesetzt werden konnte. Bei elektrischen Feldern bis 200 V/cm wurden Stark-Spektren für drei verschiedene Polarisationszustände der Laserstrahlung aufgenommen. Als Ergebnis konnte jeweils ein Paar isolierter Stark-Komponenten in den Spektren identifiziert werden, dessen gut messbarer Frequenzabstand durch Vergleich mit theoretischen Werten die Bestimmung der elektrischen Feldstärke ermöglicht. / A method for electric field measurements that observes the Stark spectra of the low excited levels n = 2 and n = 3 of atomic hydrogen has been explored in this work. As advantage these levels can be excited Doppler-free from the ground state by a single laser and the highly resolved Stark spectra are easy to understand and to be calculated. Good sensitivity of electric field measurements is achieved with specially designed solid state laser systems, which provide tuneable pulsed UV radiation with a high pulse peak-power and a narrow bandwidth needed for Doppler-free two-photon excitation. Using hydrogen and deuterium the Stark spectra of the n = 2 level are detected as optogalvanic signal. For three different cases of laser polarization the n = 3 spectra of hydrogen are measured simultaneously with optogalvanic and laser induced Balmer alpha fluorescence detection. Electric fields down to 200 V/cm can be determined from the Stark spectra of n = 2 level, while the spectra of n = 3 level enable measurements of electric fields as small as 50 V/cm in each of the three cases of laser polarization.

Optical frequency standards with the reference to a narrow electronic transition of a laser-cooled collection of neutral atomic particles are becoming essential tools of research in modern precision physics experiments. In the core of a building block of an optical frequency standard is the optical continuous wave laser that has a good spectral purity of the emitted light. Such a stable optical oscillator is highly desirable in high resolution spectroscopy, if it emits in a good quality beam at a short visible wavelength. This Master thesis explores efficient techniques for building such an optical frequency source intended for use in the cooling and trapping of Calcium atoms scheme. The strong dipole transition at the blue wavelength in the atomic Calcium is needed to reduce the kinetic energy of atoms by nearly six orders of magnitude. A further reduction in the thermal energy of the laser cooled atoms is required to locate with ultra-high precision the 400 Hz narrow clock transition of the stable 40Ca isotope. The experimental methods that achieve this and approach sub-microkelvin temperature of the laser cooled bosonic isotopes of alkaline earths are inspected. The blue laser with a uniform intensity distribution in the beam is useful to maintain the trapped number of cold atoms during these experiments. The spectroscopic properties of the relative transitions in Calcium atom are also reviewed following relevant publications in the area. The constructed blue laser can be used as a primary wavelength source in the lasers network for cooling and trapping of Calcium atoms. These experiments will constitute part of the project to build an optical atom clock referenced to 40Ca narrow linewidth transition. The blue laser is constructed by generating second harmonic in a Potassium Niobate crystal, which is temperature controlled to use a type-I noncritical phase-matching of the optical nonlinear process. The power of the intracavity-generated second harmonic depends on the resonance properties of the optical resonator where this nonlinear crystal is placed. The study is aimed at characterising the designed optical resonator and the experimental parameters that describe it. The formula is derived that relates the resonance power enhancement coefficient with finesse and the power coupling contrast of a passive optical cavity. The obtained relationship is verfied during the experiments. The produced efficiency of the intracavity second harmonic generation is approx. 0.0023 mWblue/(mWred)2. The research work also examines the noise characteristics of the infrared diode laser that is used as a pump source for the intracavity generated second harmonic and determines the spectroscopic precision of the produced blue light. The frequency locking experiment is analysed using the unbalanced scheme of the polarisation stabilisation technique. The designed optical buildup cavity became a part of the unbalanced frequency discriminator in such a scheme. The results demonstrate high gain of frequency noise suppression of the stabilised laser. The unbalanced arrangement of the H}ansch-Couillaud technique has been possible due to a very low amplitude noise of semiconductor lasers.

Thesis (M.S.)--Mississippi State University. Department of Physics and Astronomy. / Title from title screen. Includes bibliographical references.

This thesis describes experimental work towards developing a trapped ion quantum information processor. An existing ion trap apparatus was capable of trapping and laser-cooling single ions or small ion strings of 40 Ca+, and had been used for studies of quantum jumps and natural lifetime measurements in Ca. This thesis describes improvements in this apparatus, which have allowed the stability and the flexibility of experimental control of the ions to be greatly increased. This enabled experiments to read out the spin state of a single trapped ion, and to load ions with isotope selectivity through photoionization. The optical systems were improved by installation of new lasers, optical reference cavities, and a system of acousto-optic modulators for laser intensity switching and frequency control. The photon counting for fluorescence detection was improved, and a new photon time-of-arrival correlation circuit developed. This has permitted rapid and more sensitive detection of micromotion, and hence cancellation of stray fields in the trap. A study of resonant circuits in the low RF, high voltage (10 MHz, 1 kV) regime was carried out with a view to developing a new RF supply for the Paul trap with reduced noise and increased power. A new supply based on a helical resonator was built and used to trap ions. This technique has reduced noise and will permit higher secular frequencies to be attained in the future. A magnetic field B in the ion trap is used to define a quantization axis, and in one series of experiments was required to be of order 100 G to provide a substantial Zeeman splitting. A set of magnetic field coils to control the size and direction of B is described. The design of these posed some problems owing to an unforseen issue with the vacuum chamber. In short, it is magnetizable and acts to first approximation like a magnetic shield. The field coils had to be sufficiently substantial to produce the desired field at the ion even in the presence of this shielding effect, and dark resonance (and other) spectra with Zeeman splitting were obtained to calibrate the field using the ion as a probe. Finally, the thesis describes the successful loading of the ion trap by laser photoionization from a weak atomic beam. This involved two new lasers at 423 nm and 389 nm. Saturated absorption spectroscopy of neutral calcium is first described, then transverse excitation of an atomic beam in our vacuum chamber is used to identify all the main isotopes of calcium and confirm their abundances in our source (a heated sample of natural calcium). Finally, photoionization is used to load the trap. This has three advantages over electron-impact ionization. By avoiding an electron gun, we avoid charging of insulating patches and subsequent electric field drift as they discharge; the flux in the atomic beam and hence calcium (and other) deposits on the electrodes can be greatly reduced; and most importantly, the photoionization is isotope selective. Evidence is presented which suggests that even with an non-enriched source, the rare isotope 43 Ca can be loaded with reasonable efficiency. This isotope is advantageous for quantum information experiments for several reasons, but chiefly because its ground state hyperfine structure can act as a stable qubit.