The electrical double layer (EDL) is formed due to the accumulation of charge at the interface of a metal surface in contact with an electrolyte. The total charge in the EDL compensates the charge on the metal surface. As EDL is the layer that "connects" the electrode to the "bulk", all electrode mediated transport and redox reaction depends on the structure and dynamics of the ions in the EDL. Thus the ion dynamics in the EDL are critical to a wide range of physical and biological phenomena such as electrochemical reaction, flow in channels of nanofluidic devices, wetting of fluids; to biology, for example, folding and function of proteins, conformation change of DNA and ionic flow through cell membranes. EDL polarization is the ion accumulation or depletion in the EDL due to the potential of the metal surface. The conventional method of measuring the EDL polarization is by monitoring the current flowing through the electrochemical system. Thus, the electrical characteristics of the EDL are inferred indirectly from the total current that is implicitly related to effects such as the impedance of the bulk solution. We have developed a sensitive optical interferometric technique to directly measure the polarization of the metal-electrolyte interface. The key advantage of our method is high sensitivity, and the measurement is specific only to the changes at the metal-electrolyte interface. The ion accumulation in the EDL of a simple salt like NaCl is studied as a function of the frequency and the amplitude of the applied potential on the metal electrode. The amplitude of modulation of the ions is linearly proportional to the amplitude of the applied AC potential. The linearity is observed up to high amplitude (up to 2V) and salt concentration as high as 0.5M. Furthermore, the local segmental dynamics of polyelectrolytes such as polystyrene sulfonate have been measured. Next we extend this novel technique to study electrochemical redox reactions. The oxidation of the widely used redox ion [Fe(CN)6]4- is followed by measuring the response to an AC potential (amplitude ~100mV) as a function of a superimposed saw-tooth potential ramp, at a time period 106 fold slower and amplitude 5-10 fold larger than the AC potential. The sensitivity of the optical method is significantly better than the measurement of the AC current. For a redox process on the electrode, the change in the optical signal is over two orders of magnitude larger than the electrical signal. Using the optical technique, we can separate the kinetic events in redox processes: transport of charged species to the electrode surface and charge transfer across the electrode-electrolyte interface. Because we measure the local electrochemical process, the method can be used to probe redox reaction at multiple spots on the same electrode (i.e., combinatorial electrochemistry). / Ph. D.

The measurement and monitoring of glacial surface velocity is important for many aspects of glaciology, such as determining the mass balance, for characterising the stability or instability of glaciers, or the identification of potential hazards from surging glaciers or Jökulhlaups, a type of glacial outburst flood. Predominately measurements of glacial surface velocity have been produced using either differential interferometry (DInSAR) applied to radar data, or offset-tracking applied to either optical or radar data. Both of these methods have their own set of limitations, notably the one-dimensional nature of DInSAR measurements, and the relatively low accuracy of offset-tracking. Instead using DInSAR and multiple-aperture interferometry (MAI) applied to ERS-1/2 Tandem SAR data, measurements of glacial surface displacements were obtained in the line-of-sight (LOS) and along-track directions respectively. Then using a weighted-least squares adjustment, the method for producing the full three-dimensional surface velocity field is presented and applied to the Svartisen glacial system, Norway and the Petermann Glacier, Greenland. The advantages and disadvantages of applying such a method were explored, of which interferometric coherence is found to be the largest factor in retrieving accurate measurements using MAI. Low interferometric coherence due to temporal decorrelation resulted in the inability to extract the full three-dimensional surface velocity field over the Bagley Icefield, Alaska, and the Mýrdalsjökull & Eýjafjallajökull ice caps, Iceland. A feasibility analysis into the use of Sentinel-1 data, revealed that the current revisit period is too large to maintain interferometric coherence between acquisitions, preventing the application of either DInSAR or offset-tracking in order to measure the surface velocity of the Blåmannsisen Glacier, Norway. Despite the limitations encountered, in part due to the selection of source data, MAI in tandem with DInSAR has been shown to be capable of measuring the three-dimensional surface velocity to a higher accuracy than offset-tracking when coherence is high. The methods used within have been developed to work with pre-processed single look complex (SLC) SAR data rather than raw unfocused SAR data, in an effort to improve their adoption and enable more accurate estimates of glacial surface velocity.

This research focuses on measurements of a convective shear-layer instability seen naturally in quiet hypersonic flow. Experiments were carried out in the Boeing/AFOSR Mach 6 Quiet Tunnel (BAM6QT) at Purdue University. The BAM6QT provides low-disturbance hypersonic flow with freestream noise levels similar to what would be experienced by a flight vehicle. To obtain high-speed, off-the-surface measurements of the instability, a modified focused laser differential interferometer (FLDI) was first designed to work with the contoured Plexiglas windows available in the tunnel.<div><br>A cone-cylinder-flare geometry was then selected to study the instabilities related to an axisymmetric separation bubble at Mach 6. The sharp cone had a 5-degree half-angle, while flare angles of 10 degrees and 3.5 degrees were tested to compare axisymmetric compression with and without separation, respectively. Under quiet flow, laminar separation and reattachment was confirmed by schlieren and surface pressure-fluctuation measurements. Coherent traveling waves were observed. These were attributed to both the second-mode instability, as well as a shear-generated instability from the separation bubble. The symmetry of the bubble was found to be highly sensitive to angle of attack. Additionally, by introducing controlled disturbances on the cone upstream of the separation, larger-amplitude shear-generated waves were measured while the second-mode amplitudes remained unchanged. Therefore, the shear-generated waves were amplified moving through the shear layer, while the second mode remained neutrally stable. These appear to be the first measurements of traveling waves that are generated in the shear layer of a separation bubble in hypersonic flow. <br></div>

La présente thèse traite de méthodes en microscopie holographique numérique (MHN) en couleurs, avec un éclairage de cohérence spatiale partielle. Le principal inconvénient de la microscopie optique classique est sa faible profondeur de champ, rendant difficile l’observation de phénomènes dynamiques dans des échantillons épais. Au contraire, la MHN offre une reconstruction en profondeur grâce à la propagation numérique de l’hologramme. La MHN interférométrique donne aussi le contraste quantitatif de la phase, utile pour analyser des objets transparents. Un éclairage à plusieurs longueurs d’onde dans une configuration appropriée permet la MHN en couleurs. L’imagerie en flux et en couleurs de particules en MHN est ici développée, avec une méthode pour la correction automatique de la balance des couleurs et des défauts permanents. Elle est appliquée pour l’analyse du plancton dans des échantillons d’eau de surface et fournit des images de haute qualité pour les intensité et phase optiques. En outre, la réduction du bruit obtenue en diminuant la cohérence spatiale de l’éclairage en MHN est également étudiée, avec deux modèles évaluant quantitativement ce phénomène en fonction de la cohérence spatiale de la lumière et de la distance entre la source de bruit et le plan d’enregistrement. De plus, la MHN différentielle est aussi abordée. Celle-ci fournit les phases différentielles, la phase étant calculée par intégration. Cependant, les défauts présents conduisent à des aberrations lors du calcul de la phase, qui affectent sa qualité et empêchent la reconstruction holographique. Un traitement spécifique est développé, permettant la reconstruction numérique en profondeur. Enfin, en MHN, un critère est essentiel pour déterminer automatiquement la distance de netteté de l’objet. Deux critères de netteté sont ici mis au point, fonctionnant indépendamment de la nature de l’objet observé (amplitude, phase ou mixte). L’un, monochromatique, est basé sur l’analyse de l’amplitude et sur un filtrage passe-haut ;l’autre, qui détecte rapidement le plan de netteté en MHN en couleurs, compare la phase dans le domaine de Fourier entre les couleurs. Les méthodes développées dans la thèse montrent le potentiel élevé de la MHN en couleurs avec un éclairage partiellement cohérent spatialement, suggérant un avenir prometteur pour cette technique. / The thesis deals with methods and developments in color digital holographic microscopy (DHM), with a partial spatial coherence illumination. The principal drawback of classical optical microscopy is its poor depth of field, which makes difficult the observation of dynamic phenomena in thick samples. On the contrary, DHM provides reconstruction in depth thanks to numeric propagation of the recorded hologram. Another feature of interferometric DHM is the quantitative phase contrast imaging, useful for analyzing transparent objects. Usual DHM is limited to monochromatic case, but multispectral illumination in an appropriate setup leads to color DHM. Color in-flow imaging of particles in DHM is developed in the thesis, with a method for the automatic correction of color balance and permanent defects. It is applied to analyze plankton microorganisms in untreated pond water samples, and provides high quality images, for both optical phase and intensity. Moreover, noise reduction obtained when decreasing the spatial coherence of the illumination in DHM is also investigated in the thesis, with the development of two models that quantitatively assess the noise reduction as a function of both the spatial coherence of the illumination, and the defocus distance of the noise source. Furthermore, differential DHM (DDHM) is also studied in the thesis. As DHM gives the optical phase, DDHM provides differential phases, from which phase is retrieved by integration. However, misalignments and defects give some aberrations, which affect phase quality and hinder refocusing. A specific hologram processing is developed, giving an accurate phase image and enabling holographic reconstruction in depth. Finally, in DHM, a criterion is essential to automatically achieve the refocusing distance of the object. Two refocusing criteria are developed in the thesis, both working independently of the nature of the observed object (amplitude, phase, or both mixed). The first one, monochromatic, is based on amplitude analysis and on a high-pass filtering process. The second one, which gives fast refocusing in multispectral DHM, compares the phase in the Fourier domain among wavelengths. Methods developed in the thesis show the high potential of color DHM with a partial spatial coherence illumination, suggesting a promising future for this technique. / Doctorat en Sciences de l'ingénieur et technologie / info:eu-repo/semantics/nonPublished