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Owing to its centrosymmetric structure, the critical optical component of a silica fiber cannot to possess a second-order nonlinear optical susceptibility, Χ(²), preventing a silica fiber from many potential applications. Here, we theoretically and experimentally demonstrate a new technique to generate large and thermodynamically stable second-order nonlinearity into silica optical tapered fibers without breaking the centrosymmetry of the silica glass. The nonlinearity is introduced by surface layers with high polar-ordering fabricated by a novel hybrid covalent/ionic self-assembly multilayer technique. Despite the overall rotational symmetry of the nonlinear fiber, we observe significant second harmonic generation with ~ 400–500 fold enhancement of the SHG power compared to the traditional tapers. Phase matching for a SHG process in second-order nonlinear tapered fibers is also realized by the compensation of waveguide modal dispersion with material chromatic dispersion, which occurs only for submicron tapers where the modal dispersion is large. In addition, quasi-phase-matching for a nonlinear taper can be accomplished by introducing a periodic pattern into the nonlinear film coating. We use UV laser ablation for the controlled removal of particular nonlinear film segments on a taper surface in order to produce a Χ(²) grating structure. A resulting SHG enhancement from quasi-phase-matching is observed over a broadband spectrum of the pump light mainly due to the non-uniform shape of a taper waveguide. The laser ablation is a clean and fast technique able to produce well-define patterns of polymer films on either flat or curved substrate geometry. With surface layers containing reactive functional groups e.g. primary amines, we demonstrate that the resulting patterned film obtained from the laser ablation can be used as a template for further self-assembly of nanoparticles with high selectivity. A pattern feature size down to ~ 2μm or smaller can be fabricated using this approach. We also discuss preliminary results on a novel technique to further improve spatial accuracy for selective self-assembly of nanoparticles at an unprecedented level. Different types of nanoparticles are joined in order to form well-defined, molecular-like superstructures with nanoscale accuracy and precision. The technique is based on a selective surface functionalization of photosensitive molecules coated on metallic nanoparticles utilizing enhanced two-photon photocleavage at the plasmonically-active sites (hot spots) of the nanoparticles in resonance with an applied electromagnetic wave. As a result, the surface functional groups at the nanoparticle hot spots are different from the the other areas, allowing other kinds of nanoparticles to self-assemble at the hot spots with high degree of selectivity. / Ph. D.

L’optique non linéaire qui convertit la gamme de fréquences des sources lasers vers l’ultraviolet, le visible, l’infrarouge ou le térahertz par exemple, joue un rôle crucial pour la médicine, l’industrie, les applications militaires, la recherche etc. L’accord de phase par biréfringence (BPM) ou le quasi-accord de phase (QPM) à partir de processus non linéaires quadratiques, peuvent être utilisés pour la conversion de fréquence dans le domaine de transparence de cristaux non linéaires. Dans ce travail de thèse, un cristal uniaxe de La3Ga5.5Nb0.5O14 (LGN) a été élaboré en utilisant une méthode de Czochralski, puis il a été étudié pour le BPM. Nous avons aussi validé la théorie du QPM angulaire (AQPM), qui correspond à la généralisation du QPM à n’importe quel angle par rapport au vecteur du réseau. Pour cela, nous avons étudié un cristal biaxe de Rb: KTiOPO4 à domaines ferroélectriques alternés périodiquement (PPRKTP) usiné en forme de sphère. Tous ces résultats constituent une base fiable for les études avenir consacrées à la conception de dispositifs pour la conversion de fréquence. / Nonlinear optics converting the frequency range of laser sources to ultraviolet, visible, infrared or terahertz ranges for example, plays a crucial role in medicine, industry, military applications, research and so on. Birefringence phase-matching (BPM) or quasi-phase-matching (QPM) from quadratic nonlinear processes, can be used for frequency conversion in the transparency range of nonlinear crystals. In this PhD work, a La3Ga5.5Nb0.5O14 (LGN) uniaxial crystal was grown using a Czochralski method and then studied for BPM. We also validated the theory of angular-QPM (AQPM), corresponding to a generalization of QPM achieved at any angle with respect to the grating vector. For that purpose, we studied a periodically-poled large-aperture Rb:KTiOPO4 (PPRKTP) biaxial crystal cut a sphere. All the results provide a reliable basis for further studies devoted to the design of frequency conversion devices.

<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>

Fine-pitch ferroelectric domain gratings are extensively used for generation of light in the visible and near-infrared spectral regions through quasi-phase matched (QPM) frequency conversion. Sub-μm QPM devices enables demonstration of nonlinear optics with counterpropagating waves, a field of nonlinear optics which remains sparsely explored due to the difficulty of fabricatinghigh quality gratings. In recent years, bulk Rb-doped KTiOPO4 (RKTP) has emerged as a highly promising nonlinear materials for fabrication of fine-pitch QPM devices through periodic electric-field poling. RKTP possesses large optical nonlinearity and high resistance to optical damage, while demonstrating improved material homogeneity and lower ionic conductivity than its isomorphs, which are important features for poling. Although fine-pitch QPM gratings, as well as large aperture QPM devices, have been demonstrated, fabrication of sub-μm high quality QPM devices remains a challenge. The primary aim of this research was to develop a reliable method to fabricate high-quality sub-μm periodically poled RKTP crystals (PPRKTP) and exploit them in novel optical applications. For this purpose, a novel poling method was developed. It was based on periodic modulation of the coercive field through ion exchange, where K+ ions are exchanged with Rb+ in the crystal, to modulate the coercive field and the ionic conductivity. This enables periodic poling of higher quality and with shorter period than ever before. High quality PPRKTP with a period of 755 nm were fabricated and used to demonstrate the first cascaded mirrorless optical parametric oscillator (MOPO), as well as the first MOPO pumped by a Q-switched laser. PPRKTP samples for blue light generation were fabricated, and second harmonic generation (SHG) was investigated with a high power 946 nm fiber laser. Up to 2 W of blue power was demonstrated for bulk samples, where the output power was limited by absorption of the SHG, leading to thermal dephasing of the devices. Laser-written waveguides were fabricated in PPRKTP for the first time, and a record high SHG power of 76 mW was obtained. Finally, the high-temperature stability of ferroelectric domain gratings was investigated. This is of utmost importance when a PPRKTP crystal is used as a seed for crystal growth. It was found that for charged domains walls, the domain-wall motion was highly anisotropic with rapid movement in y-direction while only small movements were observed in the x-direction of the crystal. / Ickelinjära ferroelektriska kristaller med artificiella domängitter med perioder av några mikrometer används idag för generering av ljus i de synliga och nära-infraröda våglängdsområdena, genom kvasifasmatchad (QPM) frekvenskonvertering. Med sub-μm QPM domängitter kan man åstadkomma ickelinjära optiska effekter med motpropagerande parametriska ljusvågor. Detta är ett område av den ickelinjära optiken som fortfarande är tämligen outforskat på grund av svårigheten med att tillverka högkvalitativa domängitter.  Under de senaste åren har Rb-dopat KTiOPO4 (RKTP) blivit ett mycket lovande ickelinjärt material för tillverkning av QPM-gitter med mycket korta perioder genom periodisk elektrisk fält polning. RKTP kristallen har en hög optisk ickelinejäritet och den tål höga optiska intensiteter, samtidigt som materialet har bättre materialhomogenitet och lägre jonledningsförmåga än vad dess isomorfa kristaller har. De två senare egenskaperna har visat sig viktiga för att få en lyckad polning. Fastän QPM-gitter med kort periodicitet, liksom QPM-gitter med stor apertur, har demonstrerats, är tillverkningen av högkvalitativa QPM-kristaller med sub-µm perioder fortfarande en utmaning. Det primära syftet med denna avhandling var att utveckla en pålitlig metod för att tillverka högkvalitativa sub-μm periodiskt polade RKTP kristaller (PPRKTP) och utnyttja dem i nya optiska tillämpningar. I detta syfte utvecklades en ny polningsmetod. Den baseras på periodiskt jonutbyte, där K+ joner byts mot Rb+ i kristallen, vilket resulterar i en samtidig modulation av materialets koerciva fält och jonledningsförmåga. Detta möjliggör i sin tur periodisk polning av högre kvalitet och med kortare perioder än någonsin tidigare har uppnåtts. Högkvalitativa PPRKTP kristaller med en period på 755 nm tillverkades och användes för att demonstrera den första kaskaderade spegelfria optiska parametriska oscillatorn (MOPO), liksom den första MOPO processen pumpad av en Q-switchad laser. Vidare utvecklades PPRKTP-kristaller för generering av blått ljus via frekvensdubbling. Dessa utvärderades med hjälp av en högeffekts-fiberlaser vid 946 nm. Upp till 2 W av blått ljus erhölls för bulkkristallerna. Uteffekten begränsades av absorption av det blåa frekvensdubblade ljuset, vilket ledde till urfasning i QPM-gittret p.g.a. termiska effekter. Laserskrivna vågledare tillverkades sedan i PPRKTP för första gången, och en rekordhög effekt på 76 mW erhölls via frekvensdubbling. Slutligen undersöktes stabiliteten hos de periodiskt polade domängitterna vid höga temperaturer. Det är viktigt att domängittrena är stabila när PPRKTP kristallerna används som ympämne för kristalltillväxt. Det visade sig att instabila domänväggar flyttade sig mycket anisotropt, med en snabb rörelse i kristallens y-riktning och en långsam rörelse i kristallens x-riktning. / <p>QC 20170519</p>

This thesis describes the experimental implementation of novel intersecting cavity terahertz optical parametric oscillators based on bulk and periodically-poled magnesium oxide-doped lithium niobate. Both collinear and non-collinear phase-matching geometries have been demonstrated and injection-seeding has been implemented in devices using periodically-poled material to reduce threshold and increase the down-conversion efficiency. A comprehensive characterisation of the original intracavity terahertz OPO was undertaken, which revealed the parameters having the greatest impact on OPO efficiency (idler mirror reflectivity and cavity length) and led to a better understanding of the losses in the system. During the characterisation process, generation of further terahertz radiation at the same frequency as that generated by the parametric process was observed and identified as being a result of difference frequency generation (DFG) between the parametrically-generated idler and terahertz waves. This phenomenon had previously only been observed when periodically-poled materials were employed in the system. The effect of this additional DFG process has been analysed in terms of the enhancement of the terahertz field on the basis of the coupled wave equations and physically measured quantities. The use of periodically-poled lithium niobate has been a major part of the research presented in this thesis. A comprehensive study of the modified phase-matching conditions was carried out and both collinear and novel hybrid non-collinear phase-matching geometries were identified. Several computer models were developed to assess the performance of any given grating design in these different geometries and the effects of temperature tuning and pump wavelength variation were also investigated using the models. Experimental studies confirmed the viability of the modelling approach but material limitations (particularly the early onset of crystal damage) limited the outcomes of the experiments. A detailed comparison of the poled and bulk materials was made to highlight the present drawbacks of the poled material. Finally, injection seeding was used to improve the efficiency of the collinear phase-matched PPLN OPOs. When seeding was used the depletion of the pump pulse was increased to the point of being measurable, reaching an upper level of 10%. Coupling constraints placed on the seed laser limited the amount of depletion attained. The potential for injection seeding to be used in the hybrid non-collinear phase-matching scheme was also identified but not realised during the course of this work. Were this technique successful, the tuning range of the intersecting cavity terahertz OPO could be extended to encompass the sub-1THz region, something that has previously been limited by the available idler cavity angles.

De nos jours, la génération paramétrique optique (OPG) avec la plus grande largeur spectrale possible, est une bonne alternative pour couvrir les bandes II (2–5 µm) ou band III (8–12 µm) de transmission de l’atmosphère. Une telle émission à partir de processus non linéaires quadratiques en conditions d’accord de phase par biréfringence (BPM), nous a intéressés. Elle est réalisée sur le domaine de transparence de cristaux non linéaires déjà identifiés, mais ils ne sont pas satisfaisants. C’est pourquoi ce travail de thèse est consacré d’abord à l’étude du cristal biaxe GdCa4O(BO3)3 (GdCOB), et des cristaux uniaxes La3Ga5.5Nb0.5O14 (LGN) et NaI3O8. Nous avons enregistré leurs courbes d’accord de phase et les rendements de conversion associés en conditions de BPM. Nous avons sélectionné la génération de second harmonique et la différence de fréquence dans des lames, des sphères ou cylindres. Nous avons affiné les équations de Sellmeier. Nous avons déterminé la valeur absolue des coefficients non linéaires des cristaux uniaxes. Nous avons aussi déterminé la valeur absolue et le signe de tous les coefficients du cristal biaxe BaGa4Se7. Tous ces résultats constituent une base fiable pour les évaluations expérimentales à venir de la plus grande largeur spectrale des OPG qui utilisent ces cristaux.Key words: optique non linéaire, génération paramétrique, accord de phase, cristaux non linéaires / Nowadays, the optical parametric generators (OPG) with the broadest spectral bandwidth is a good alternative cover band II (2–5 µm) or band III (8–12 µm) of transmission range of the atmosphere. We were interested in such an emission from quadratic nonlinear processes under birefringence phase-matching conditions (BPM). It is performed in the transparency range of already identified nonlinear crystals, but they are not satisfying. Then this PhD work is devoted first to the study of GdCa4O(BO3)3 (GdCOB) biaxial crystal, and La3Ga5.5Nb0.5O14 (LGN) and NaI3O8 uniaxial crystals. We recorded their tuning curves and conversion efficiencies for BPM. We selected second harmonic generation and difference frequency generation in slabs, spheres or cylinders. We refined the Sellmeier equations. We determined the magnitude of the nonlinear coefficients, spectral and angular acceptances in uniaxial crystals. We also determined the magnitude and sign of all the nonlinear coefficients of BaGa4Se7 biaxial crystal. All these results provide reliable data for further experimental evaluations of OPG broadest spectral bandwidth covering band II or III using these crystals.Key words: nonlinear optics, parametric generation, phase-matching, nonlinear crystals

Material and structure engineering are increasingly employed in active optical media,in this context defined as media capable of providing laser or/and optical parametric gain. For laser materials, the main aim of the engineering is to tailor the absorption and emission cross sections in order to optimise the laser performance. At the same time, the engineering also results in a collateral modification of the material’s nonlinear response. In the first part of this work, the nonlinear index of refraction is characterised for two crystallographic forms of laser-ion doped and undoped double-tungstate crystals. These laser crystals have broad gain bandwidths, in particular when doped with Yb3+. As shown in this work, the crystals also have large Kerr nonlinearities, where the values vary significantly for different chemical compositions of the crystals. The combination of a broad gain bandwidthand a high Kerr nonlinearity makes the laser-ion doped double tungstates excellent candidates to employ for the generation of ultrashort laser pulses by Kerr-lens modelocking. The second part of the work relates to the applications of engineered second-order nonlinear media, which here in particular are periodically-poled KTiOPO4 crystals. Periodic structure engineering of second-order nonlinear crystals on a submicrometre scale opens up for the realisation of novel nonlinear devices. By the use of quasi-phase matching in these structures, it is possible to efficiently downconvert a pump wave into two counterpropagating parametric waves, which leads to a device called a mirrorless optical parametric oscillator. The nonlinear response in these engineered submicrometre structures is such that the parametric wave that propagates in the opposite direction of the pump automatically has a narrow bandwidth, whereas the parametric wave that propagates with the pump essentially is a frequency-shifted replica of the pump wave. The unusual spectral properties andthe tunabilities of mirrorless optical parametric oscillators are investigated. / QC 20120330

<p>This thesis discusses a new scheme for generating radiation in the mid infrared spectral region, especially the 3.5-5 µm range. The scheme uses established Nd³⁺-lasers at 1.06 µm and down conversion in nonlinear optical crystals. The down conversion is made by two optical parametric oscillators (OPO) in series. The second OPO is a classical OPO using a zink germanium phosphide (ZGP) crystal. ZGP is the best nonlinear material available for the 4-8 µm spectral range, but it is absorbing below 2 µm. The new development presented in this thesis is the OPO used to convert the 1.06 µm laser radiation to a suitable OPO pump near 2 µm.</p><p>The OPO uses a type I quasi phase-matched crystal, which accesses high nonlinearities and avoids walk-off. The problem with type I OPOs close to degeneracy is the broad bandwidth of the generated radiation, which reduces the efficiency of a second OPO. This has been solved with a spectrally selective cavity using a volume Bragg grating output coupler. Unlike other bandwidth limiting schemes this introduces no intracavity losses and thus efficient OPO operation is achievable.</p><p>Narrow linewidth (~0.5 nm) OPO operation has been achieved with periodically poled LiNbO₃ (PPLN) and periodically poled KTiOPO4 (PPKTP) while locking the signal wavelength at 2008 nm and simultaneously generating an idler at 2264 nm. A high average power PPLN OPO with 36 % conversion efficiency and 47 % slope efficiency is reported. Operation very close to degeneracy at 2128 nm with the narrowband signal and idler peaks separated by 0.6 nm was demonstrated in a PPKTP OPO. Both the signal at 2008 nm and the combined signal and idler around 2128 nm from the PPKTP OPOs have been used to show efficient pumping of a ZGP OPO. The maximum conversion efficiency from 1 µm to the mid-IR demonstrated is 7 % with a slope efficiency of 10 %. This is not quite as high as what has been presented by other authors, but the experiments reported here have not shown the optimum efficiency of the new scheme. Relatively simple improvements are expected to give a significant increase in conversion efficiency.</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. 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