An all-solid-state continuous-wave (cw) laser system for mid-infrared absorption measurements of the carbon monoxide (CO) molecule has been developed and demonstrated. The single-mode, tunable output of an external-cavity diode laser (ECDL) is difference-frequency mixed (DFM) with the output of a 550-mW diode-pumped cw Nd:YAG laser in a periodically-poled lithium niobate (PPLN) crystal to produce tunable cw radiation in the mid-infrared. The wavelength of the 860-nm ECDL can be coarse tuned between 860.78 to 872.82 nm allowing the sensor to be operated in the 4.4 – 4.8 µm region. Results from single-pass mid-IR direct absorption experiments for CO concentration measurements are discussed. CO measurements were performed in CO/CO2/N2 mixtures in a room temperature gas cell that allowed the evaluation of the sensor operation and data reduction procedures. Field testing was performed at two locations: in the exhaust of a well-stirred reactor (WSR) at Wright-Patterson Air Force Base and the exhaust of a gas turbine at Honeywell Engines and Systems. Field tests demonstrated the feasibility of the sensor for operation in harsh combustion environments but much improvement in the sensor design and operation was required. Experiments in near-adiabatic hydrogen/air CO2-doped flames were performed featuring two-line thermometry in the 4.8 µm spectral region. The sensor concentration measurement uncertainty was estimated at 2% for gas cell testing. CO concentration measurements agreed within 15% of conventional extractive sampling at WSR, and for the flame experiments the repeatability of the peak absorption gives a system uncertainty of 10%. The noise equivalent CO detection limit for these experiments was estimated at 2 ppm per meter, for combustion gas at 1000 K assuming a SNR ratio of 1.

Entanglement is the hallmark of quantum mechanics. Quantum entanglement -- putting two or more identical particles into a non-factorable state -- has been leveraged for applications ranging from quantum computation and encryption to high-precision metrology. Entanglement is a practical engineering resource and a tool for sidestepping certain limitations of classical measurement and communication. Engineered nonlinear optical waveguides are an enabling technology for generating entangled photon pairs and manipulating the state of single photons. This dissertation reports on: i) frequency conversion of single photons from the mid-infrared to 843nm as a tool for incorporating quantum memories in quantum networks, ii) the design, fabrication, and test of a prototype broadband source of polarization and frequency entangled photons; and iii) a roadmap for further investigations of this source, including applications in quantum interferometry and high-precision optical metrology. The devices presented herein are quasi-phase-matched lithium niobate waveguides. Lithium niobate is a second-order nonlinear optical material and can mediate optical energy conversion to different wavelengths. This nonlinear effect is the basis of both quantum frequency conversion and entangled photon generation, and is enhanced by i) confining light in waveguides to increase conversion efficiency, and ii) quasi-phase matching, a technique for engineering the second-order nonlinear response by locally altering the direction of a material's polarization vector. Waveguides are formed by diffusing titanium into a lithium niobate wafer. Quasi-phase matching is achieved by electric field poling, with multiple stages of process development and optimization to fabricate the delicate structures necessary for broadband entangled photon generation. The results presented herein update and optimize past fabrication techniques, demonstrate novel optical devices, and propose future avenues for device development. Quantum frequency conversion from 1848nm to 843nm is demonstrated for the first time, with >75% single-photon conversion efficiency. A new electric field poling methodology is presented, combining elements from multiple historical techniques with a new fast-feedback control system. This poling technique is used to fabricate the first chirped-and-apodized Type-II quasi-phase-matched structures in titanium-diffused lithium niobate waveguides, culminating in a measured phasematching spectrum that is predominantly Gaussian (R^2 = 0.80), nearly eight times broader than the unchirped spectrum, and agrees well with simulations.

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<p>The topic of this thesis is development ofdevices fortelecom applications based on poled optical fibers. The focusis on two different specific functions, wavelength conversionand optical switching.</p><p>Optical switching is demonstrated in a poled optical fiberat telecom wavelengths (~1.55 mm). The fiber has two holesrunning along the core in which electrodes are inserted. Thefiber device is made electro-optically active with a polingprocess in which a strong electric field is recorded in thefiber at a temperature of 270 o C. The fiber is then put in onearm of a Mach-Zehnder interferometer and by applying a voltageacross the two electrodes in the fiber the refractive index ismodulated and the optical signal switched from one output portto the other. So far the lowest switching voltage achieved is~1600 V which is too high for a commercial device, but byoptimizing the design of the fiber and the poling process aswitching voltage as low as 50 V is aimed for.</p><p>A method to deposit a thin silver electrode inside the holesof an optical fiber is also demonstrated. A new way of creatingperiodic electrodes by periodically ablating the silver filmelectrode inside the holes of an optical fiber is also shown.The periodic electrodes can be used to create a quasi-phasematched (QPM) nonlinearity in the fiber which is useful forincreasing the efficiency of a nonlinear process such aswavelength conversion. Poling of a fiber with silver electrodesshowed a huge increase in the nonlinearity. This could be dueto a resonant enhancement caused by silver nanoclusters.</p><p><b>Keywords:</b>Poling, twinhole fiber, fiber electrodes,silver film electrodes, silver diffusion, quasi-phase matching,optical switching, frequency conversion, optical modulation</p>

Globally increasing levels of bandwidth and capacity requirements force the optical communications industry to produce new products that are faster, more powerful, and more efficient. In particular, optical-electronic-optical (O-E-O) conversions in Wavelength Division Multiplexing (WDM) mechanisms prevent higher data transfer speeds and create a serious bottleneck for optical communications. These O-E-O transitions are mostly encountered in the Wavelength converters of WDMs, and as a result, all-optical wavelength conversion methods have become extremely important. The main discussion in this thesis will concentrate on a specific all-optical wavelength conversion mechanism. In this mechanism, photonic crystal structures are integrated with moving MEMS/NEMS structures to create a state-of-the-art all-optical wavelength converter prototype. A wavelength conversion of 20% is achieved using this structure. Since the interaction of light with moving MEMS/NEMS structures plays an important role in the proposed wavelength conversion mechanism, modeling and simulation of electromagnetic waves becomes a very crucial step in the design process. Consequently, a subsection of this thesis will focus on a proposed enhancement to the finite-difference time-domain (FDTD) to model moving structures more efficiently and more realistically. This technique is named "Linear Dielectric Interpolation" and will be applied to more realistically and efficiently model the proposed photonic crystal MEMS/NEMS wavelength conversion mechanism.

In the field of second harmonic (SH) generation most studies have been concerned with maximizing conversion efficiencies, generally achievable at the phase matching (PM) condition. Outside of the PM the conversion efficiency drastically decreases. This has caused that the possible working conditions out of PM to remain largely unexplored. In this thesis work we initiated a systematic study of the SH behavior in under conditions of large phase mismatch. When a pump pulse crosses an interface between a linear and a nonlinear medium there are always two generated SH components. These components may be understood on the basis of the mathematical solution of the inhomogeneous wave equations at the SH frequency. The homogeneous (HOM) solution is a component with wave-vector k(2¿) as expected from the dispersion relation and exchanges energy with the pump until the inevitable walk-off. The inhomogeneous (INH) solution is a component with a wave-vector 2k(¿), twice the pump wave-vector, and travels locked to the pump pulse. We divide our work in two parts, one for each generated component. Inhomogeneous component. We start a systematic study of the behavior of the generated INH component, phase locked to the pump. The consequences of phase locking (PL) can guide us towards new scenarios by allowing working conditions hitherto assumed inaccessible for absorbing materials. We show that while the HOM component travels with the group velocity given by material dispersion, the IHN component is captured by the pump pulse and experiences the same effective dispersion of the pump. It does not follow the PM condition. It naturally follows that the suppression of absorption at the SH wavelengths will occur if the pump is tuned to a region of transparency. We extended the same theory for the generated third harmonic (TH). We then studied the surprising behavior of SH and TH INH components with frequencies above the absorption edge when the material is placed inside a cavity resonant only at the fundamental frequency. We have shown that the PL mechanism not only inhibits absorption but also fosters the enhancement of harmonic generation by several orders of magnitude compared to the no-cavity case. Finally, we tested the INH SH and TH behaviors in metallic frequency regime of material. Homogeneous component. The techniques used to PM the nonlinear interaction enable efficient nonlinear interactions but drastically limit the spectral bandwidth of the nonlinear optical process, making the designed frequency converter only suitable for a fixed input wavelength and single interaction only. It has been shown that the use of disordered nonlinear media relaxes the PM condition thus allowing one to achieve relatively efficient broad bandwidth regime of the frequency conversion. An example of a quadratic nonlinear medium with a disordered domain structure is an un-poled Strontium Barium Niobate (SBN) crystal. It is composed of a system of random size anti parallel ferroelectric domains that allow to phase-match any second-order parametric process over a broad range of wavelengths without any poling. We have initiated an experimental and theoretical investigation of the properties of the SH waves generated in SBN crystals, with an extension to the generated TH. This study covers the coherence and polarization properties of the generated signal, as well as its spatial distribution. In addition, we have made an experimental study of the noncollinear interaction of short optical pulses in a SBN crystal by using two fundamental waves intersecting inside the crystal. We have shown that this effect may be employed as a simple tool for monitoring both the pulse duration and initial chirp. This method offers a simple and economic alternative to the existing methods for pulse characterization.

Ce travail porte sur l’étude des mécanismes de conversion de fréquences dans les cristaux photoniques non linéaires bidimensionnels. En particulier, nous avons étudié la génération paramétrique optique (GPO) dans les cristaux de LiTaO3 (PPLT- 2D) à réseau carré. Nous nous sommes d’abord intéressés à l’étude théorique et numérique de structures PPLT- 2D. Une étude numérique, nous a permis de comprendre la contribution des vecteurs de réseau réciproque (kmn) pour différents types de réseaux, en particulier les réseaux carrés et rectangulaires. Par simulations numériques, nous avons également étudié l’influence de l’angle incidence du faisceau de pompe sur l’efficacité de conversion paramétrique dans ses structures. Les mesures expérimentales nous ont permis de mettre en évidence, pour la première fois, l’existence de plusieurs singularités où le signal est partagé pour générer deux idlers et vice versa. En effet, en analysant les propriétés spectrales et angulaires des faisceaux à la sortie du cristal, nous avons, expérimentalement et numériquement, identifié les contributions impliquées dans ces processus communs de GPO. De plus, nous avons étudié le management du gain paramétrique optique dans un réseau carré de PPLT-2D. Les résultats montrent que l’exploitation de la direction non colinéaire permet d’augmenter le gain suivant deux angles d’incidences de la pompe : 0.8° et 1.6°. Cela implique, une meilleure efficacité de conversion en minimisant le walk-off entre la pompe et l’idler. Dans ces conditions, le gain pourrait être proche de celui de la direction colinéaire. Un bon accord a été constaté entre les résultats expérimentaux et ceux de la simulation. / This work deals with the study of the mechanisms of frequency conversion in two-dimensional nonlinear photonic crystals. In particular, we have studied optical parametric (OPG) generation in square-lattice LiTaO3 crystals (PPLT-2D). We first focused on the theoretical and numerical study of PPLT-2D structures. A numerical study allowed us to understand the contribution of the reciprocal lattice vectors (kmn) for different types of gratting, in particular square and rectangular lattices. By numerical simulations, we also studied the influence of the incidence angle of the pump beam on the efficiency of the parametric conversion in these structures. Experimental measurements have allowed us to demonstrate, for the first time, the existence of several singularities where the signal is shared to generate two idlers and vice versa. Indeed, by analyzing the spectral and angular properties of the beams at the output of the crystal, we have experimentally and numerically identified the contributions involved in these common OPG processes. In addition, we studied the management of the optical parametric gain in a square lattice of PPLT-2D. The results show that the use of the non-collinear direction makes it possible to increase the gain according to two angles of incidence of the pump: 0.8 ° and 1.6 °. This implies, better conversion efficiency by minimizing the walk-off between the pump and the idler. Under these conditions, the gain could be close to that of the collinear direction. A good agreement was found between the experimental results and those of the simulation.

Le fluoroborate de calcium Ca5(BO3)3F (CBF) et l'aluminoborate d'yttrium YAl3(BO3)4 (YAB) ont été étudiés pour respectivement la génération de 3ème et 4ème harmonique de laser proche infrarouge tel que YAG :Nd émettant à 1064 nm. Dans l'optique d'améliorer la qualité cristalline du CBF, nous avons étudié les paramètres de sa synthèse par réaction à l'état solide et ceux de sa cristallogénèse par la méthode Czochralski. Les acceptances thermiques pour la génération de 2nde harmonique à 1064 nm en type I et II ont également été déterminés. Et un cristal de CBF a permis de générer une énergie de 131,4 µJ à 355 nm par génération de 3ème harmonique, soit un rendement de conversion de 6,1%. Concernant le YAB, le flux à base de LaB3O6 a été étudié pour sa croissance cristalline par la méthode TSSG : des cristaux de tailles centimétriques sans fracture, ni inclusion ont été obtenus. Les défauts structuraux des cristaux (stries de croissance, macles etc.) ont été analysés. Par ailleurs, des investigations sur la réduction carbothermique ont été menées pour limiter la pollution en fer des cristaux. Une énergie laser de 163 µJ a été obtenue par doublage de fréquence de 532 nm à 266 nm, soit un rendement de conversion de 14,7%. / Calcium fluoroborate Ca5(BO3)3F (CBF) and yttrium aluminum borate YAl3(BO3)4 were studied respectively for 3rd and 4th harmonic generation of near infrared laser as Nd:YAG laser emitting at 1064 nm. In order to improve the crystalline quality of CBF, solid state reaction parameters and crystal growth conditions by using Czochralski furnace were investigated. Thermal acceptances for second harmonic generation at 1064 nm for type I and II were determined. 131,4 µJ energy at 355 nm was obtained by 3rd harmonic generation, corresponding to a conversion efficiency of 6,1%. When it came to YAB, LaB3O6 based flux was investigated for its crystal growth by TSSG method: centimeter size, inclusion and crack free crystals were obtained. Structural defects of crystals (striations, twins etc.) were analyzed. Furthermore, carbothermal reduction investigation was carried out to limit iron pollution in crystals. Eventually 163 µJ at 266 nm were obtained by frequency doubling from 532 nm to 266 nm, corresponding to a conversion efficiency of 14,7%.

The topic of this thesis is development ofdevices fortelecom applications based on poled optical fibers. The focusis on two different specific functions, wavelength conversionand optical switching. Optical switching is demonstrated in a poled optical fiberat telecom wavelengths (~1.55 mm). The fiber has two holesrunning along the core in which electrodes are inserted. Thefiber device is made electro-optically active with a polingprocess in which a strong electric field is recorded in thefiber at a temperature of 270 o C. The fiber is then put in onearm of a Mach-Zehnder interferometer and by applying a voltageacross the two electrodes in the fiber the refractive index ismodulated and the optical signal switched from one output portto the other. So far the lowest switching voltage achieved is~1600 V which is too high for a commercial device, but byoptimizing the design of the fiber and the poling process aswitching voltage as low as 50 V is aimed for. A method to deposit a thin silver electrode inside the holesof an optical fiber is also demonstrated. A new way of creatingperiodic electrodes by periodically ablating the silver filmelectrode inside the holes of an optical fiber is also shown.The periodic electrodes can be used to create a quasi-phasematched (QPM) nonlinearity in the fiber which is useful forincreasing the efficiency of a nonlinear process such aswavelength conversion. Poling of a fiber with silver electrodesshowed a huge increase in the nonlinearity. This could be dueto a resonant enhancement caused by silver nanoclusters. <b>Keywords:</b>Poling, twinhole fiber, fiber electrodes,silver film electrodes, silver diffusion, quasi-phase matching,optical switching, frequency conversion, optical modulation / NR 20140805

Semiconductor based micro- and nano-structures grown in a systematic and controlled way using selective area growth are emerging as a promising route toward devices for integrated optical circuitry in optoelectronics and photonics field. This dissertation focuses on the experimental investigation of the nonlinear optical effects in selectively grown gallium nitride micro-pyramids that act as optical cavities, zinc oxide submicron rods and indium gallium nitride multiple quantum well core shell submicron tubes on the apex of GaN micro pyramids that act as optical antennae. Localized spatial excitation of these low dimensional semiconductor structures was optimized for nonlinear optical light (NLO) generation due to second harmonic generation (SHG) and multi-photon luminescence (MPL). The evolution of both processes are mapped along the symmetric axis of the individual structures for multiple fundamental input frequencies of light. Effects such as cavity formation of generated light, electron-hole plasma generation and coherent emission are observed. The efficiency and tunability of the frequency conversion that can be achieved in the individual structures of various geometries are estimated. By controlling the local excitation cross-section within the structures along with modulation of optical excitation intensity, the nonlinear optical process generated in these structures can be manipulated to generate coherent light in the UV-Blue region via SHG process or green emission via MPL process. The results show that these unique structures hold the potential to convert red input pulsed light into blue output pulsed light which is highly directional.