Bragg reflection waveguides (BRW) or one-dimensional photonic bandgap structures have been demonstrated for phase-matching chi(2) nonlinearities in AlxGa1-xAs. The method exploits strong modal dispersion of a Bragg mode and total internal reflection modes co-propagating inside the waveguide. It is shown that phase-matching is attained among the lowest order modes of interacting harmonics, which allows maximizing the utilization of harmonics powers for nonlinear interactions. As our first demonstration, we report second-harmonic generation (SHG) of a 2-ps telecommunication pump in a 2.4 mm long slab BRW. The conversion efficiency is estimated as 2.0 %/W.cm^2 with a generated SH power of 729 nW. This efficiency has been considerably improved by introducing lateral confinement of optical modes in ridge structures. Characterizations denote that efficiency of SHG in ridge BRWs can increase by over an order of magnitude in comparison to that of the slab device. Also, we report continuous-wave SHG in BRWs. Using a telecommunication pump with a power of 98 mW, the continuous-wave SH power of 23 nW is measured in a 2.0 mm long device. Significant enhancements of chi(2) interactions is obtained in the modified design of matching-layer enhanced BRW (ML-BRW). For the first time, we report type-II SHG in ML-BRW, where the second-harmonic power of 60 µW is measured for a pump power of 3.3 mW in a 2.2 mm long sample. Also, we demonstrate the existence of type-0 SHG, where both pump and SH signal have an identical TM polarization state. It is shown that the efficiency of the type-0 process is comparable to type-I and type-II processes with the phase-matching wavelengths of all three interactions lying within a spectral window as small as 17 nm. ML-BRW is further reported for sum-frequency and difference-frequency generations. For applications requiring high pump power, a generalized ML-BRW design is proposed and demonstrated. The proposed structure offsets the destructive effects of third-order nonlinearities on chi(2) processes when high power harmonics are involved. This is carried out through incorporation of larger bandgap materials by using high aluminum content AlxGa1-xAs layers without undermining the nonlinear conversion efficiency. Theoretical investigations of BRWs as integrated sources of photon-pairs with frequency correlation properties are discussed. It is shown that the versatile dispersion properties in BRWs enables generation of telecommunication anti-correlated photon-pairs with bandwidth tunablity between 1 nm and 450 nm.

Bragg reflection waveguides (BRW) or one-dimensional photonic bandgap structures have been demonstrated for phase-matching chi(2) nonlinearities in AlxGa1-xAs. The method exploits strong modal dispersion of a Bragg mode and total internal reflection modes co-propagating inside the waveguide. It is shown that phase-matching is attained among the lowest order modes of interacting harmonics, which allows maximizing the utilization of harmonics powers for nonlinear interactions. As our first demonstration, we report second-harmonic generation (SHG) of a 2-ps telecommunication pump in a 2.4 mm long slab BRW. The conversion efficiency is estimated as 2.0 %/W.cm^2 with a generated SH power of 729 nW. This efficiency has been considerably improved by introducing lateral confinement of optical modes in ridge structures. Characterizations denote that efficiency of SHG in ridge BRWs can increase by over an order of magnitude in comparison to that of the slab device. Also, we report continuous-wave SHG in BRWs. Using a telecommunication pump with a power of 98 mW, the continuous-wave SH power of 23 nW is measured in a 2.0 mm long device. Significant enhancements of chi(2) interactions is obtained in the modified design of matching-layer enhanced BRW (ML-BRW). For the first time, we report type-II SHG in ML-BRW, where the second-harmonic power of 60 µW is measured for a pump power of 3.3 mW in a 2.2 mm long sample. Also, we demonstrate the existence of type-0 SHG, where both pump and SH signal have an identical TM polarization state. It is shown that the efficiency of the type-0 process is comparable to type-I and type-II processes with the phase-matching wavelengths of all three interactions lying within a spectral window as small as 17 nm. ML-BRW is further reported for sum-frequency and difference-frequency generations. For applications requiring high pump power, a generalized ML-BRW design is proposed and demonstrated. The proposed structure offsets the destructive effects of third-order nonlinearities on chi(2) processes when high power harmonics are involved. This is carried out through incorporation of larger bandgap materials by using high aluminum content AlxGa1-xAs layers without undermining the nonlinear conversion efficiency. Theoretical investigations of BRWs as integrated sources of photon-pairs with frequency correlation properties are discussed. It is shown that the versatile dispersion properties in BRWs enables generation of telecommunication anti-correlated photon-pairs with bandwidth tunablity between 1 nm and 450 nm.

Estudos em interfaces são importantes para o completo entendimento de muitos processos em química, física e biologia. Esses sistemas são governados principalmente pelas propriedades interfaciais dos materiais. Nas duas últimas décadas, o desenvolvimento de novos métodos experimentais melhorou o nosso entendimento das propriedades interfaciais. O advento de uma série de técnicas de espectroscopia a laser baseadas em óptica não linear e o desenvolvimento das técnicas de microscopia por ponta de prova, possibilitaram estudos antes inimagináveis em superfícies e interfaces. Entre as técnicas de espectroscopia não linear, destacamos a espectroscopia por Geração de Soma de Frequências (espectroscopia SFG). Essa técnica foi desenvolvida por Shen et al. em 1987 e, desde então, é aplicada a muitos estudos em superfícies e interfaces. A espectroscopia SFG pode fornecer informações sobre a natureza química por meio do espectro vibracional e sobre o ordenamento médio das moléculas em uma única monocamada. O sinal SFG só pode ser gerado em meios não centrossimétricos, isso inclui superfícies ou interfaces entre meios centrossimétricos, onde há quebra da simetria de inversão. A combinação da espectroscopia SFG com a microscopia óptica tem sido proposta como uma nova técnica experimental para obter imagens em interfaces com sensibilidade química pelo espectro vibracional e contraste pela orientação e ordenamento das moléculas. Neste trabalho, apresentamos o desenvolvimento, construção e caracterização de um Microscópio SFG (MSFG). Esse MSFG foi especialmente projetado para estudos em superfícies ou interfaces tanto líquidas quanto sólidas. Testes iniciais de desempenho do MSFG foram realizados na interface líquido/ar da solução binária água/acetonitrila (H2O⁄CH3CN). Foram obtidas imagens do sinal SFG ressonante com o estiramento simétrico do grupo metil (CH3) da acetonitrila na interface líquido⁄ar da solução binária. Variando a fração molar da acetonitrila na solução entre 4% e 20% observamos a dependência da intensidade do sinal SFG na interface em função da fração molar de acetonitrila no volume do líquido. Testes também foram feitos em filmes Langmuir-Blodgett multicamada de ácido esteárico (CH3(CH2)16COOH). Obtivemos a espectromicroscopia SFG na ressonância dos grupos CH2 e CH3 do ácido graxo. Pelas diferenças entre os espectros SFG das regiões ordenadas e desordenadas, a espectromicroscopia revelou distribuições microscópicas do ordenamento das cadeias alquila que formam o filme. A sensibilidade da detecção do sinal SFG foi caracterizada e revelou a possibilidade de obter imagens na superfície da água em menos de um minuto. A caracterização óptica e os testes nas interfaces líquido⁄ar e sólido⁄ar demonstraram a completa capacidade do MSFG como ferramenta para investigar qualquer superfície ou interface, seja essa líquida ou sólida. / Interface studies are important for the complete understanding of many processes in chemistry, physics and biology. These systems are mainly governed by the interfacial properties of the materials. In the last two decades, the development of new experimental methods improved our understanding of interfacial properties. The advent of a host of laser spectroscopy techniques based on nonlinear optics and the development of the scanning probe microscopy techniques, opened up unimaginable possibilities of studies at surfaces and interfaces. Among these nonlinear spectroscopies we turned our attention to Sum Frequency Generation spectroscopy (SFG spectroscopy). This technique was developed by Shen et al. in 1987 and, since then, it has been applied to many studies of surfaces and interfaces. SFG spectroscopy can provide information about the chemical nature by the vibrational spectra and about the average of molecular ordering in a single monolayer. The SFG signal only can be generated in a noncentrossymetric media, this includes surfaces or interfaces between centrossymetric media, where there is a broken in the inversion symmetry. The combination of SFG spectroscopy with optical microscopy has been proposed as a novel experimental technique to obtain images at interfaces with chemical sensitivity by the vibrational spectra as well as contrast by the ordering and orientation of the molecules. In this work we present the development, construction and characterization of an SFG Microscope (SFGM). This SFGM was specially designed to perform studies on surfaces or interfaces of liquids and solids. Initial SFGM performance tests were performed at the liquid/air interface of the water/acetonitrile (H2O/CH3CN) binary solution. The images of the SFG signal were acquired on the resonance of the methyl group (CH3) of acetonitrile present at the liquid⁄air interface of the binary solution. By varying the molar fraction of acetonitrile in the solution between 4% and 20% we observed the dependency of the SFG signal intensity as a function the acetonitrile bulk mole fraction. We also performed tests in multi-layered Langmuir-Blodgett films of stearic acid (CH3(CH2)16COOH). We obtained the SFG spectromicroscopy in the resonance of CH2 and CH3 groups of the fatty acid. By the differences between the SFG spectra of ordered and disordered regions, the spectromicroscopy revealed microscopic distribution of the conformational ordering in the alkyl chains that composes the film. The sensitivity of the SFG microscope was characterized and it was shown that images could be acquired at the water surface in less than one minute. The optical characterization and the performed tests at the liquid/air and solid/air interfaces demonstrated the full capabilities of the SFGM as a tool for investigations in any liquid or solid interface.

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La détection faible flux dans le moyen infrarouge (MIR) est fortement pénalisée par le rayonnement thermique de l’environnement. La principale solution à ce problème consiste à cryogéniser la plus grande partie possible de la chaîne de détection. Cette méthode atteint ses limites pour certaines applications,notamment l’imagerie haute résolution en astronomie par méthode interférométrique. Une solution alternative consiste à utiliser le processus non linéaire de somme de fréquences pour convertir ce rayonnement moyen infrarouge vers des domaines de longueur d’onde où les détecteurs ne sont plus limités par le rayonnement de l’environnement et fonctionnent efficacement en régime de comptage de photons. Les travaux effectués au cours ces trois années sont le prolongement direct de plus d’une décennie de recherche pour la détection et l’interférométrie par conversion de fréquence. Ils s’inscrivent dans la continuité des travaux de thèses de L. Szemendera et de P. Darré, ayant, pour l’un, posé les premières pierres de l’interférométrie par conversion de fréquence dans le MIR et, pour l’autre, démontré la possibilité d’utiliser cette technique sur le ciel à1550 nmen tirant parti de la technologie de guidage ridge. Cette thèse constitue donc la jonction fructueuse de ces travaux antérieurs, rendue possible par une collaboration avec l’institut Femto-ST. L’utilisation de leurs guides PPLN ridge nous a permis de nous placer au niveau de l’état de l’art pour la détection par conversion de fréquence dans le MIR (3,5 μm)avec des démonstrations expérimentales à la fois en laboratoire et sur le ciel (C2PU). Intégrée à un interféromètre à conversion de fréquence à ces mêmes longueurs d’onde, elle a également permis d’en améliorer significativement les performances et la répétabilité de cette technique, principalement dans le cas d’une source spectralement large bande. Parallèlement, notre collaboration avec le réseau de télescopes CHARA, nous a offert l’opportunité d’étudier les problématiques soulevées par une future mise en œuvre de l’instrument sur ce site. / Low flux detection in the mid infrared (MIR) is strongly penalized by thermal radiation from the environment. The main solution to this problem is to cryogenize as much of the detection chain as possible.This method is reaching its limits for some applications, including high-resolution imaging in astronomy using interferometric methods. An alternative solution is to use the non-linear process of sum frequency generation to convert this mid infrared radiation to wave length domains where detectors are no longer limited by the radiation from environment and operate efficiently in photon counting regime.The work over these three years is part of more than a decade of research into up-conversion detection and interferometry. It is the expansion of the these works of L. Szemendera and P. Darré. The first one laid the fondation of the up-conversion interferometry in the MIR and the second one demonstrated the possibility of using this technique on the sky at 1550 nm by benefiting from the ridge waveguide technology.Thus, this thesis constitutes the fruitful junction of these earlier works, made possible by a collaboration with the Femto-ST Institute. The use of their PPLN ridge waveguides has enabled us to place ourselves at the state of the art for up-conversion detection in the MIR (3,5 μm) with experimental demonstrations both in the laboratory and on the sky (C2PU). Integrated into a up-conversion interferometer at these same wave lengths, it has also significantly improved the performance and repeatability of this technique,in particular in the case of a spectrally broadband source. At the same time, our collaboration with the CHARA telescope array gave us the opportunity to study the problems raised by a future implementation of the instrument on this site.

La technique de l'interférométrie en astronomie permet d'observer des objets avec une haute résolution angulaire comparativement à l'utilisation d'un unique télescope. L'observation dans l'infrarouge moyen représente aujourd'hui un enjeu en interférométrie notamment pour l'étude des noyaux actifs de galaxie ou de la formation des planètes. Cependant ce domaine spectral est particulièrement contraignant puisqu'il est soumis à l'émission propre des éléments optiques de l'instrument mais également de l'atmosphère. Ce manuscrit développe les travaux effectués sur un nouvel instrument utilisant un processus de conversion de fréquence pour transposer le rayonnement infrarouge vers un domaine spectral permettant de s'affranchir de l'émission propres des optiques. Un prototype fonctionnant dans le proche infrarouge à 1,55 µm et convertissant, via une processus de somme de fréquences, le rayonnement dans le domaine visible autour de 630 nm grâce à une pompe intense à 1064 nm, a été mis en place pour démontrer, en laboratoire, le principe de cette solution innovante notamment dans le cadre de l'analyse de la cohérence spatiale d'un corps noir. L'objectif est maintenant de démontrer la capacité de l'instrument à détecter un objet réel. J'introduis dans cette thèse les notions théoriques essentielles à la compréhension des travaux présentés pour ensuite détailler le fonctionnement de l'instrument et les éléments d'amélioration apportés, notamment en terme de transmission, au cours de ma thèse. Les études préliminaires en laboratoire du comportement de l'instrument ont permis d'aboutir aux premières franges sur le ciel en utilisant la plus petite base (34 m) du réseau interférométrique CHARA et de rechercher la magnitude limite de l'instrument. L'utilisation du processus de conversion de fréquence a pour conséquence de filtrer le spectre converti. Ainsi dans la configuration actuelle de l'interféromètre, seul 0,6 nm du spectre infrarouge en entrée du cristal est converti à travers le processus de SFG. Afin d'augmenter la sensibilité, une solution est de créer plusieurs processus de SFG simultanément dans chaque étage de conversion afin d'échantillonner le spectre infrarouge converti. Cette solution requiert d'utiliser plusieurs sources de pompe indépendantes qui vont créer des systèmes de franges incohérents. Je présente l'analyse de la cohérence temporelle d'une source infrarouge large bande convertie via l'utilisation de deux sources de pompe et un moyen de synchroniser les différents systèmes de franges afin de maximiser le contraste. / Interferometry is an instrumental technique suitable to perform astronomical observations at high angular resolution. Currently, the mid-infrared spectral domain is a real issue for the astronomical interferometry to characterize astronomical objects such as proto-planetary discs or active galactic nuclei. However, this spectral domain is subject to a large thermal background emission from the instrument and from the sky. This manuscript describes an innovative instrument using a nonlinear process of sum frequency generation to convert the mid-infrared radiation to a shorter wavelength domain where the thermal emission from the instrument is negligible. A prototype operating in the near-infrared at 1.55 µm and converting the radiation in the visible domain at 630 nm thanks to a strong pump at 1064 nm has already demonstrated its ability to analyse spatial coherence of a blackbody source. The present goal is to demonstrate its ability to detect an object on the sky. In this manuscript I introduce theoritical concepts necessary for an understanding of the overall operation of the instrument. Then, I describe the main improvements provided in this thesis, in particular concerning the instrumental transmission. The preliminary studies of the instrument operation resulted in the first on-sky fringes on the CHARA array and enabled to determine its limiting magnitude. The upconversion process acts as a filter on the converted spectrum. In the current instrumental configuration, only 0.6 nm of the input infrared spectrum is converted through the SFG process. For the purpose of increasing the instrumental sensitivity, we propose to sample the infrared spectrum by using several independent pump laser lines thus creating different incoherent fringe patterns. I present the temporal coherence analysis of a broadband infrared source converted by a dual-line pump laser and a method to synchronize the different fringe patterns to insure a maximum value of the contrast.

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Laddningsbeteendet hos amingruppen vid ytgränsskiktet mellan vatten och luft har studerats under ändring av vattenfasens pH och NaCl-koncentration via den ickelinjära laserspektroskopiska tekniken, vibrationssumfrekvensspektroskopi (VSFS). Modellen som användes för ytan bestod av ett Langmuirmonolager av 1-docosanamin, en icke-löslig fettkedjeamin med NH2-gruppen riktad mot vattenfasen. En av de huvudsakliga syftena med projektet var att bestämma det skenbara samt yt-pKa:t för amingruppen, såväl som att testa gränserna för de klassiska Poisson-Boltzmann-formuleringarna av teorin för det elektriska dubbellagret. Molekylär information av laddningsbeteendet hos aminen erhölls från VSFS-spektra genom att följa NH-, OH- och CH-sträckningsvibrationsmoderna. Specifikt så identifierades de spektrala dragen från den neutrala formen (R-NH2) och den laddade formen (R-NH3+) av aminen, vilka direkt korrelerades med monolagrets ytladdning. Intensiteten hos OH-banden från vattenmolekylerna i det diffusa dubbellagret kunde länkas till ytpotentialen och CH-vibrationerna från alkylkedjan av amino-tensiden kopplades slutligen till packningstätheten hos monolagret. Ytterligare experiment utfördes med en deutererad vattenfas (D2O) för att bekräfta sträckningsvibrationsmoderna hos NH3+, vilka aldrig tidigare har rapporterats. Resultaten visar på att fettkedjeaminen får ett avsevärt lägre yt- och skenbart pKa jämfört med bulken (∼ 4 jämfört med 10,5). Detta är i enlighet med vad Gouy-Chapmann-modellen av det elektriska dubbellagret förutser. Dessutom så indikerar datat att det inneboende pKa:t hos aminen också blir lägre vid ytan än för bulken (9,7±0,7 jämfört med 10,5), vilket kan beskrivas som en effekt av begränsningen i frihetsgrader hos den ytbundna aminen. Dock, så hindrades en mer utförlig kvantitativ jämförelse mot teorin av ett sämre val av det experimentella referensvärdet som användes för att jämföra data mellan olika dagar. Dessutom så var anpassningsrutinen för datat begränsad på grund av spektrala vibrationsöverlapp mellan de relativt svaga aminbanden och de mycket starkare vatten- och alkylsträckningssignalerna. Intressant nog, för högre pH-värden, då aminen är helt oladdad, bevisade sumfrekvensspektra att hydroxidjonen föredrar att adsorbera till ytan genom att monolagret fick en negativ nettoladdning. Överlag så förbättrar studierna som presenteras i denna master-projektuppsats vår molekylära förståelse kring hur den biofysiskt betydande amingruppen beter sig vid ytgränsskikt. / The charging behaviour of the amine moiety at the water-air interface upon changes in the aqueous subphase pH and NaCl concentration has been studied using  the non-linear laser spectroscopy technique, Vibrational Sum Frequency Spectroscopy (VSFS).  The model surface consisted of a Langmuir monolayer of 1-docosaneamine, an insoluble fatty amine that exposes its NH2  group to solution. One of the main purposes of the project is to determine the surface, and the apparent pKa of the amine moiety, as well as testing the limits of validity of classical formulations of the electrical double layer theory within the Poisson-Boltzmann formalism. Molecular information of the charging behaviour was obtained from the VSFS spectra by targeting the NH, OH and CH stretching modes. Specifically, spectral features from the neutral amine (i.e. R-NH2) and charged (R-NH3+) groups could be identified and directly correlated to the surface charge of the monolayer. The intensity of the  OH bands from water molecules in the diffuse double layer, were linked to the surface potential, and finally, the CH modes from the surfactant alkyl chain gave information of the packing density in the monolayer. Additional experiments were also carried out in D2O to help confirm the assignment of the NH3+ stretching modes that had not been previously reported. The results show that as predicted from the Gouy-Chapman electric double layer model, the apparent pKa of the fatty amine monolayer is significantly lower than in the bulk  (∼ 4 compared with 10.5) . However, the data show indication that the intrinsic pKa at the surface is also lower than in the bulk (9.7+/- 0.7, compared to 10.5), an effect that is ascribed to the 2D molecular confinement in the monolayer. A more quantitative comparison with the theoretical predictions was nonetheless hampered by a poor selection of the experimental reference for comparing data collected in different days, and the limitations in the fitting routines due spectral overlap of the relatively weak amine bands with the OH and CH stretching modes. Interestingly, at high pH when the fatty amine is fully uncharged, the sum frequency spectra show evidence that OH- ion preferentially adsorbed to the surface, making it effectively net negatively charged. Overall, the studies presented in this master thesis, improve our molecular understanding of the behaviour of the biophysically relevant amine-functionality at interfaces.