Optically pumped chirped grating for tunable chromatic dispersion compensation

We demonstrate a novel optically tunable dispersion compensator based on pumping a chirped grating made in Er/Yb co-doped fiber. The dispersion was tuned from 900 to 1900ps/nm and also from-600 to-950ps/nm in the experiment. © 2010 Optical Society of America.

Different generation regimes of mode-locked all-positive-dispersion all-fiber Yb laser

Different generation modes of all-positive-dispersion all-fibre Yb laser mode-locked due to effect of non-linear polarization evolution are investigated. For the first time we realized in the same laser both generation of single picoseconds pulse train and a newly observed lasing regime where generated are picosecond wave-packets, each being a train of femtosecond sub-pulses. Using both experimental results and numerical modeling we discuss in detail the mechanisms of laser mode-locking and switching of generation regimes and show a strong dependence of output laser characteristics on configuration of polarization controllers. A good qualitative agreement between experimental results and numerical modeling is demonstrated. © 2010 Copyright SPIE - The International Society for Optical Engineering.

Modeling 2R regenerator based on High Nonlinear Dispersion Imbalanced Loop Mirror (HN-DILM)

The model of Reshaping and Re-amplification (2R) regenerator based on High Nonlinear Dispersion Imbalanced Loop Mirror (HN-DILM) has been designed to examine its capability to reduce the necessary of fiber loop length and input peak power by deploying High Non linear Fiber (HNLF) compared to Dispersion Shifted Fiber (DSF). The simulation results show by deployed a HNLF as a nonlinear element in Dispersion Imbalanced Loop Mirror (DILM) requires only 400mW peak powers to obtain a peak of transmission compared to DSF which requires a higher peak power at 2000mW to obtain a certain transmissivity. It also shows that HNLF required shorter fiber length to achieve the highest transmission. The 2R regenerator also increases the extinction ratio (ER) of the entire system. © 2010 IEEE.

Enzymatic Polymerization of High Molecular Weight DNA

The use of DNA as a polymeric building material transcends its function in biology and is exciting in bionanotechnology for applications ranging from biosensing, to diagnostics, and to targeted drug delivery. These applications are enabled by DNA’s unique structural and chemical properties, embodied as a directional polyanion that exhibits molecular recognition capabilities. Hence, the efficient and precise synthesis of high molecular weight DNA materials has become key to advance DNA bionanotechnology. Current synthesis methods largely rely on either solid phase chemical synthesis or template-dependent polymerase amplification. The inherent step-by-step fashion of solid phase synthesis limits the length of the resulting DNA to typically less than 150 nucleotides. In contrast, polymerase based enzymatic synthesis methods (e.g., polymerase chain reaction) are not limited by product length, but require a DNA template to guide the synthesis. Furthermore, advanced DNA bionanotechnology requires tailorable structural and self-assembly properties. Current synthesis methods, however, often involve multiple conjugating reactions and extensive purification steps.

The research described in this dissertation aims to develop a facile method to synthesize high molecular weight, single stranded DNA (or polynucleotide) with versatile functionalities. We exploit the ability of a template-independent DNA polymerase−terminal deoxynucleotidyl transferase (TdT) to catalyze the polymerization of 2’-deoxyribonucleoside 5’-triphosphates (dNTP, monomer) from the 3’-hydroxyl group of an oligodeoxyribonucleotide (initiator). We termed this enzymatic synthesis method: TdT catalyzed enzymatic polymerization, or TcEP.

Specifically, this dissertation is structured to address three specific research aims. With the objective to generate high molecular weight polynucleotides, Specific Aim 1 studies the reaction kinetics of TcEP by investigating the polymerization of 2’-deoxythymidine 5’-triphosphates (monomer) from the 3’-hydroxyl group of oligodeoxyribothymidine (initiator) using in situ 1H NMR and fluorescent gel electrophoresis. We found that TcEP kinetics follows the “living” chain-growth polycondensation mechanism, and like in “living” polymerizations, the molecular weight of the final product is determined by the starting molar ratio of monomer to initiator. The distribution of the molecular weight is crucially influenced by the molar ratio of initiator to TdT. We developed a reaction kinetics model that allows us to quantitatively describe the reaction and predict the molecular weight of the reaction products.

Specific Aim 2 further explores TcEP’s ability to transcend homo-polynucleotide synthesis by varying the choices of initiators and monomers. We investigated the effects of initiator length and sequence on TcEP, and found that the minimum length of an effective initiator should be 10 nucleotides and that the formation of secondary structures close to the 3’-hydroxyl group can impede the polymerization reaction. We also demonstrated TcEP’s capacity to incorporate a wide range of unnatural dNTPs into the growing chain, such as, hydrophobic fluorescent dNTP and fluoro modified dNTP. By harnessing the encoded nucleotide sequence of an initiator and the chemical diversity of monomers, TcEP enables us to introduce molecular recognition capabilities and chemical functionalities on the 5’-terminus and 3’-terminus, respectively.

Building on TcEP’s synthesis capacities, in Specific Aim 3 we invented a two-step strategy to synthesize diblock amphiphilic polynucleotides, in which the first, hydrophilic block serves as a macro-initiator for the growth of the second block, comprised of natural and/or unnatural nucleotides. By tuning the hydrophilic length, we synthesized the amphiphilic diblock polynucleotides that can self-assemble into micellar structures ranging from star-like to crew-cut morphologies. The observed self-assembly behaviors agree with predictions from dissipative particle dynamics simulations as well as scaling law for polyelectrolyte block copolymers.

In summary, we developed an enzymatic synthesis method (i.e., TcEP) that enables the facile synthesis of high molecular weight polynucleotides with low polydispersity. Although we can control the nucleotide sequence only to a limited extent, TcEP offers a method to integrate an oligodeoxyribonucleotide with specific sequence at the 5’-terminus and to incorporate functional groups along the growing chains simultaneously. Additionally, we used TcEP to synthesize amphiphilic polynucleotides that display self-assemble ability. We anticipate that our facile synthesis method will not only advance molecular biology, but also invigorate materials science and bionanotechnology.

Évolution de la dispersion des durées de vie au Québec au cours du XXe siècle

Mémoire numérisé par la Direction des bibliothèques de l'Université de Montréal.

Preparation of Polymer Nanoparticles by Ring Opening Metathesis Polymerization in Aqueous Dispersed Systems with Water-Soluble Ruthenium-based Catalyst

Ring opening metathesis polymerization (ROMP) is a variant of olefin metathesis used to polymerize strained cyclic olefins. Ruthenium-based Grubbs’ catalysts are widely used in ROMP to produce industrially important products. While highly efficient in organic solvents such as dichloromethane and toluene, these hydrophobic catalysts are not typically applied in aqueous systems. With the advancements in emulsion and miniemulsion polymerization, it is promising to conduct ROMP in an aqueous dispersed phase to generate well-defined latex nanoparticles while improving heat transfer and reducing the use of volatile organic solvents (VOCs). Herein I report the efforts made using a PEGylated ruthenium alkylidene as the catalyst to initiate ROMP in an oil-in-water miniemulsion. 1H NMR revealed that the synthesized PEGylated catalyst was stable and reactive in water. Using 1,5-cyclooctadiene (COD) as monomer, we showed the highly efficient catalyst yielded colloidally stable polymer latexes with ~ 100% conversion at room temperature. Kinetic studies demonstrated first-order kinetics with good livingness as confirmed by the shift of gel permeation chromatography (GPC) traces. Depending on the surfactants used, the particle sizes ranged from 100 to 300 nm with monomodal distributions. The more strained cyclic olefin norbornene (NB) could also be efficiently polymerized with a PEGylated ruthenium alkylidene in miniemulsion to full conversion and with minimal coagulum formation.

Evaluation of Gaseous Fluid Dispersion Through Packed Bed Using Radiotracers Technique

In this study, it was developed a methodology for the determination of the dispersion of a gaseous tracer in porous media using the radiotracer technique. In order to evaluate several porous media, a cylindrical filter was constructed in PVC and connected to a system with constant flow. Inside this unit silica crystals (16-20) mesh was used as porous media and CH3Br (Methyl Bromide) marked with 82Br was used as radiotracer. An instantaneous pulse of tracer was applied in the system entrance and registered by two NaI (3x3)” scintillation detectors located one before and the other after the filter. The curves produced by the radioactive cloud and recorded by the detector were analyzed statistically using the weighted moment method. The mathematical model one considered as great dispersion of tracer was used to evaluate the flow conditions inside the filter system. The results show us that the weight moment method associated with radiotracer techniques is useful to evaluated an industrial filter and allows to measure the residence time distribution, τ, and the axial dispersion, DAB, gas in a porous medium.

Modélisation de la dispersion chromatique et de l’atténuation dans les fibres microstructurées à coeur suspendu

D’abord, nous présentons les principes physiques nous permettant de modéliser et comprendre le phénomène de propagation linéaire des impulsions lumineuses dans un milieu homogène, dans les guides d’ondes planaires et enfin dans les fibres optiques microstructurées. Ensuite, nous faisons une analyse mathématique rigoureuse des équations linéaires de propagation et posons le problème comme celui de la recherche de valeurs propres d’opérateurs auto-adjoints dans un espace de Hilbert. On verra que ces résultats théoriques s’appliquent aux équations simulées dans le logiciel Comsol Multiphysics. Enfin, nous recensons et proposons différentes façons de prédire les valeurs de dispersion chromatique et d’atténuation dans les fibres microstructurées à coeur suspendu en utilisant les notions et équations discutés dans les deux premiers chapitres. Le choix de la géométrie, du matériau et de la longueur d’onde de la lumière transmise sont parmi les variables étudiées numériquement. Nous ferons également un exemple détaillé d’utilisation du logiciel Comsol Multiphysics pour construire un modèle de fibre optique microstructurée.

Formulation and analysis of a diffusion-velocity particle model for transport-dispersion equations

The modelling of diffusive terms in particle methods is a delicate matter and several models were proposed in the literature to take such terms into account. The diffusion velocity method (DVM), originally designed for the diffusion of passive scalars, turns diffusive terms into convective ones by expressing them as a divergence involving a so-called diffusion velocity. In this paper, DVM is extended to the diffusion of vectorial quantities in the three-dimensional Navier–Stokes equations, in their incompressible, velocity–vorticity formulation. The integration of a large eddy simulation (LES) turbulence model is investigated and a DVM general formulation is proposed. Either with or without LES, a novel expression of the diffusion velocity is derived, which makes it easier to approximate and which highlights the analogy with the original formulation for scalar transport. From this statement, DVM is then analysed in one dimension, both analytically and numerically on test cases to point out its good behaviour.

Simulations of droplet dispersion in the wakes of cylinders and icing tunnel spray bars

Simulations of droplet dispersion behind cylinder wakes and downstream of icing tunnel spray bars were conducted. In both cases, a range of droplet sizes were investigated numerically with a Lagrangian particle trajectory approach while the turbulent air flow was investigated with a hybrid Reynolds-Averaged Navier-Stokes/Large-Eddy Simulations approach scheme. In the first study, droplets were injected downstream of a cylinder at sub-critical conditions (i.e. with laminar boundary layer separation). A stochastic continuous random walk (CRW) turbulence model was used to capture the effects of sub-grid turbulence. Small inertia droplets (characterized by small Stokes numbers) were affected by both the large-scale and small-scale vortex structures and closely followed the air flow, while exhibiting a dispersion consistent with that of a scalar flow field. Droplets with intermediate Stokes numbers were centrifuged by the vortices to the outer edges of the wake, yielding an increased dispersion. Large Stokes number droplets were found to be less responsive to the vortex structures and exhibited the least dispersion. Particle concentration was also correlated with vorticity distribution which yielded preferential bias effects as a function of different particle sizes. This trend was qualitatively similar to results seen in homogenous isotropic turbulence, though the influence of particle inertia was less pronounced for the cylinder wake case. A similar study was completed for droplet dispersion within the Icing Research Tunnel (IRT) at the NASA Glenn Research Center, where it is important to obtain a nearly uniform liquid water content (LWC) distribution in the test section (to recreate atmospheric icing conditions).. For this goal, droplets are diffused by the mean and turbulent flow generated from the nozzle air jets, from the upstream spray bars, and from the vertical strut wakes. To understand the influence of these three components, a set of simulations was conducted with a sequential inclusion of these components. Firstly, a jet in an otherwise quiescent airflow was simulated to capture the impact of the air jet on flow turbulence and droplet distribution, and the predictions compared well with experimental results. The effects of the spray bar wake and vertical strut wake were then included with two more simulation conditions, for which it was found that the air jets were the primary driving force for droplet dispersion, i.e. that the spray bar and vertical strut wake effects were secondary.

Interference lithography for optical devices and coatings

Interference lithography can create large-area, defect-free nanostructures with unique optical properties. In this thesis, interference lithography will be utilized to create photonic crystals for functional devices or coatings. For instance, typical lithographic processing techniques were used to create 1, 2 and 3 dimensional photonic crystals in SU8 photoresist. These structures were in-filled with birefringent liquid crystal to make active devices, and the orientation of the liquid crystal directors within the SU8 matrix was studied. Most of this thesis will be focused on utilizing polymerization induced phase separation as a single-step method for fabrication by interference lithography. For example, layered polymer/nanoparticle composites have been created through the one-step two-beam interference lithographic exposure of a dispersion of 25 and 50 nm silica particles within a photopolymerizable mixture at a wavelength of 532 nm. In the areas of constructive interference, the monomer begins to polymerize via a free-radical process and concurrently the nanoparticles move into the regions of destructive interference. The holographic exposure of the particles within the monomer resin offers a single-step method to anisotropically structure the nanoconstituents within a composite. A one-step holographic exposure was also used to fabricate self- healing coatings that use water from the environment to catalyze polymerization. Polymerization induced phase separation was used to sequester an isocyanate monomer within an acrylate matrix. Due to the periodic modulation of the index of refraction between the monomer and polymer, the coating can reflect a desired wavelength, allowing for tunable coloration. When the coating is scratched, polymerization of the liquid isocyanate is catalyzed by moisture in air; if the indices of the two polymers are matched, the coatings turn transparent after healing. Interference lithography offers a method of creating multifunctional self-healing coatings that readout when damage has occurred.