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Ο όρος μη-γραμμική οπτική αντιπροσωπεύει τον κλάδο της οπτικής ο οποίος μελετά την αλληλεπίδραση της ύλης με ακτινοβολία πολύ ισχυρής έντασης. Όταν ένα υλικό εκτεθεί σε ακτινοβολία υψηλής έντασης όπως αυτή του laser, οι οπτικές του ιδιότητες αλλάζουν εξαιτίας της πόλωσης που επάγεται στα δομικά υλικά του και το αποτέλεσμα είναι η αλλαγή των οπτικών του ιδιοτήτων. Αυτό με τη σειρά του οδηγεί σε μία πληθώρα φαινομένων τα οποία μας βοηθούν στη κατανόηση της δομής του υλικού άλλα και των φυσικών μηχανισμών που κρύβονται πίσω από αυτά. Υλικά με μεγάλες μη-γραμμικες οπτικές ιδιότητες είναι πολύ χρήσιμα στην έρευνα και την ανάπτυξη πολλών κλάδων της τεχνολογίας. Σαν παράδειγμα μπορεί να αναφερθεί η ανάπτυξη των οπτικών και κβαντικών υπολογιστών, αλλά και τεχνολογιών οι οποίες μπορούν να βρουν εφαρμογή στις τηλεπικοινωνίες. Στη παρούσα εργασία μελετώνται οι μη-γραμμκές οπτικές ιδιότητες υλικών με μορφή διαλυμάτων. Η διάρθρωση της εργασίας είναι ως εξής: Στο πρώτο κεφάλαιο γίνεται μία εισαγωγή και παρουσιάζονται κάποιες βασικές έννοιες της μη-γραμμικής οπτικής. Έπειτα παρουσιάζεται ο τρόπος που μπορούν να εξαχθούν οι σχέσεις οι οποίες περιγράφουν τις μη-γραμμικές οπτικές ιδιότητες των υλικών όπως τη μη-γραμμική επιδεκτικότητα τρίτης τάξης με βάση τη κλασσική Φυσική και τη κβαντομηχανική. Το κεφάλαιο κλείνει παρουσιάζοντας μερικά φαινόμενα τα οποία οφείλονται στη μη-γραμμική επιδεκτικότητα τρίτης τάξης. Στο δεύτερο κεφάλαιο γίνεται η παρουσίαση των πειραματικών τεχνικών που χρησιμοποιήθηκαν για τη διεξαγωγή των πειραμάτων, αλλά και η διαδικασία που ακολουθήθηκε για την εξαγωγή των μη-γραμμικών οπτικών ιδιοτήτων από τα πειραματικά δεδομένα. Στα κεφάλαια που ακολουθούν παρουσιάζονται τα πειραματικά αποτελέσματα των συστημάτων που μελετήθηκαν. Πιο συγκεκριμένα στο τρίτο κεφάλαιο παρουσιάζονται τα πειραματικά αποτελέσματα που προέκυψαν από τη μελέτη νανοσωματιδίων οξειδίων του σιδήρου καλυμμένων με πολυμερή αλλά και ακάλυπτων όταν διεγείρονταν με παλμούς laser χρονικής διάρκειας 35 ps και 4 ns και μήκη κύματος 532 nm και 1064 nm. Στόχος της μελέτης ήταν ο προσδιορισμός αν το πολυμερές που βρίσκεται αγκυροβολημένο στην επιφάνεια του νανοσωματιδίου ή απουσία αυτού έχει κάποια επίδραση στις μη-γραμμικές οπτικές ιδιότητες αυτών. Στο τέταρτο κεφάλαιο παρουσιάζονται τα πειραματικά αποτελέσματα της μελέτης των μικκυλιακών συστημάτων Pd για μήκη κύματος διέγερση 532 nm και 1064 nm. Η μελέτη έγινε για χρονικό εύρος παλμού laser 35 ps και 4 ns. Τα συμπολυμερή τα οποία σχημάτιζαν το μικκύλιο απέτρεπαν τη συσσωμάτωση των νανοσωματιδίων Pd και τη δημιουργία σταθερών κολλοειδών διαλυμάτων. Τα συμπολυμερή που χρησιμοποιήθηκαν επίσης δημιουργούσαν νανοδομές οι οποίες είχαν καλά ορισμένες διαστάσεις και σχήματα. Στόχος της μελέτης ήταν να διαπιστωθεί το κατά πόσο η διάσταση, το σχήμα καθώς και η αλλαγή του συμπολυμερούς επηρεάζουν τις μη-γραμμικές οπτικές των νανοδομών. Στο πέμπτο κεφάλαιο παρουσιάζονται τα αποτελέσματα που προέκυψαν από τη μελέτη οργανομεταλλικών ενώσεων διθειολενικών συμπλόκων. Η επίδραση των υποκαταστών του σκελετού του μορίου καθώς και του κεντρικού ατόμου της ένωσης εξετάστηκαν για παλμούς laser χρονικής διάρκειας 35 ps και μήκους κύματος 532 nm και 1064 nm. Στο έκτο και τελευταίο κεφάλαιο παρουσιάζονται τα πειραματικά αποτελέσματα που προέκυψαν από τη μελέτη δυαδικών συστημάτων φουλλερενίων δότη-αποδέκτη ηλεκτρονίων για παλμούς laser 35 ps και μήκους κύματος 532 nm. Τα αποτελέσματα δείχνουν ότι αυτά τα συστήματα έχουν πολύ αυξημένες μη-γραμμικές οπτικές σε σχέση με τα απλά φουλλερένια καθιστώντας τα υποψήφια για πιθανές εφαρμογές σε διατάξεις οπτικών αισθητήρων και οπτικών πυλών. / The field of optics that examines the interaction of matter with very high intensity radiation is called nonlinear optics. When a material is exposed to radiation with high intensity such as the radiation emitted by a laser, the optical properties of the material change as a result of the induced polarization that occurs in the atoms or the molecules that constitute the material. This in turn can lead to a variety of phenomena that helps us to understand and establish relations between the structure and the physical mechanisms that take place when light interacts with matter. Materials with large nonlinear optical properties are considered possible candidates for applications in a wide range of technology such us optical or quantum computers or even in the field of telecommunications. In this work the nonlinear optical properties of metallic nanoparticles, organometallic molecules and fullerene derivates is examined. The investigated systems were in form of solutions and the nonlinear optical properties were determined with the use of Z-scan and OKE techniques. The laser pulse duration was 35 ps and 4 ns, while the excitation wavelength was 532 nm and 1064 nm respectively. In the first chapter an introduction is presented to some elements of the field of nonlinear optics. Then the derivation of the relations that describe the nonlinear optical parameters like the third order susceptibility (χ(3)) with the use of electromagnetic theory and quantum mechanics is presented. At the end some interesting phenomena that occur as a result of third order susceptibility are described. The second chapter is devoted to the experimental techniques that were used to determine the nonlinear optical properties of the investigated systems that are presented in this work. The Z-scan and OKE techniques are described thoroughly as well and the process of the determination of the nonlinear optical properties from the experimental data. In the next four chapters, experimental results are presented of the nonlinear optical properties for all the systems that were studied during this work. At the third chapter the results for γ-Fe2O3 nanoparticles are presented. Those systems were either covered or uncovered with polymeric brushes, and had different sizes of the nanoparticle core. The results show that the presence or not of the polymeric brushes, as well and the size of the core has an impact on the nonlinear optical properties those systems. In chapter four are presented the results from the investigation of the nonlinear optical properties of Pd nanoparticles encapsulated into amphiphilic block copolymer micelles. The investigation was done under 35 ps and 4 ns laser pulse duration at excitation wavelengths of 532 and 1064 nm. It is concluded that the NLO response of the systems is depending on the size of the micelle, the shape but also from the metallic load of the micelle. In the final two chapters they are presented the results regarding the NLO properties of organometallic and fullerene derivates molecules. In chapter five the investigation of the nonlinear optical properties of various dithiolene complexes is presented, under 35 ps laser pulse duration at 532 and 1064 nm. The results shows that the central atom attached to the molecule is playing crucial role to the NLO response but also and the number and the nature of substituent attached to the molecule. At the final chapter the determined NLO properties of some donor – acceptor fullerene derivatives are presented. The results show that functionalized fullerene derivatives have greater NLO response than the neat fullerene making them promising candidates for applications in optoelectronics and all-optical switching.

Στην εργασία αυτή, μελετάμε, τόσο με αναλυτικό όσο και με υπολογιστικό τρόπο, γραμμικά και μη γραμμικά οπτικά φαινόμενα σε συστήματα ημιαγώγιμων κβαντικών πηγαδιών GaAs/AlGaAs δύο ενεργειακών υποζωνών, όπου επάγονται διαϋποζωνικές μεταβάσεις, υπό την επίδραση ηλεκτρομαγνητικών πεδίων. Στο πρώτο κεφάλαιο, γίνεται μια θεωρητική περιγραφή των ημιαγώγιμων ετεροεπαφών. Ακολουθούν βασικά στοιχεία της στατιστικής και κβαντικής μηχανικής. Στο δεύτερο κεφάλαιο, εξάγονται οι γενικευμένες εξισώσεις Bloch για τις διαϋποζωνικές μεταβάσεις σε ημιαγώγιμα κβαντικά πηγάδια, στις οποίες ενυπάρχουν όροι που υπεισάγουν τις μη αμελητέες, λόγω εμπλουτισμού, αλληλεπιδράσεις μεταξύ των ηλεκτρονίων. Οι εξισώσεις αυτές αποτελούν τη βάση της μελέτης που ακολουθεί. Στα δύο επόμενα κεφάλαια, μελετούμε την αλληλεπίδραση μιας δομής διπλών συζευγμένων ημιαγώγιμων κβαντικών πηγαδιών με ένα ηλεκτρομαγνητικό πεδίο μεταβλητής γωνιακής συχνότητας, καταλήγουμε σε αναλυτικές εκφράσεις για τη οπτική επιδεκτικότητα πρώτης, τρίτης και πέμπτης τάξεως και αναλύουμε τα φάσματα διαφόρων οπτικών φαινομένων, ως προς τη γωνιακή συχνότητα του εξωτερικού πεδίου, για διάφορες τιμές της επιφανειακής ηλεκτρονιακής πυκνότητας της κβαντικής δομής. Επιπλέον, προσδιορίζουμε τις περιοχές όπου λαμβάνουν τιμή οι διάφορες παράμετροι, ούτος ώστε στο σύστημά μας να αναδυθεί η οπτική διστάθεια. Στα τρία τελευταία κεφάλαια, θεωρούμε ότι η ημιαγώγιμη κβαντική δομή αλληλεπιδρά ταυτόχρονα με ένα ισχυρό ηλεκτρομαγνητικό πεδίο (πεδίο άντλησης) καθορισμένης γωνιακής συχνότητας και ένα ασθενές (πεδίο ανίχνευσης) μεταβλητής συχνότητας και μελετούμε τα φάσματα γραμμικών και μη γραμμικών φαινομένων του πεδίου ανίχνευσης (μίξη τεσσάρων κυμάτων, απορρόφηση, διασπορά, μη γραμμικό οπτικό φαινόμενο Kerr), σε στάσιμη κατάσταση, καθώς και τη χρονική εξέλιξη αυτών. Περιγράφουμε τα φαινόμενα τόσο με αναλυτικές εκφράσεις που εξάγουμε, όσο και με την αριθμητική επίλυση των μη-γραμμικών διαφορικών εξισώσεων του πίνακα πυκνότητας που διέπουν τη δυναμική. Στη μελέτη των φαινομένων αυτών, εξετάζεται η επίδραση της επιφανειακής ηλεκτρονιακής πυκνότητας της κβαντικής δομής στις οπτικές ιδιότητες των κβαντικών πηγαδιών. / In this PhD thesis, we study analytically and numerically linear and nonlinear optical phenomena in intersubband transitions of a symmetric GaAs/AlGaAs double quantum well structure, with two energy subbands. In the first chapter, a theoretical description of the semiconductor heterostructures is presented. This is accompanied with a brief analysis of the basic elements of statistical and quantum mechanics follows, as far as this kind of structures is concerned. In the second chapter, we derive the generalised optical Bloch equations in intersubband transitions of semiconductor quantum well structures, which constitute the basis of the analysis that follows. These equations contain terms which owe their presence to the electron-electron interactions, because the quantum structure is doped with electron carriers. In the two following chapters, we consider the interaction of intersubband transitions of a double quantum well structure with an electromagnetic field of varying frequency, we derive analytical expressions for the first, third and fifth order optical susceptibility and, at last, we analyze the corresponding spectra, with respect to the frequency of the external field, for different values of electron sheet density of the structure. Furthermore, we identify the areas of values of the parameters used, in which the phenomenon of optical bistability arises. In the last three chapters, we consider the two quantum well subbands to be coupled to a strong pump electromagnetic field with fixed frequency and a weak probe electromagnetic field of varying frequency and study the spectra of various linear and nonlinear optical phenomena, which are due to the existence of the probe field. More specifically, we examine the spectra of four-wave mixing, absorption, dispersion and the nonlinear optical Kerr effect of the probe field as they evolve in time and in the steady state. Both analytical expressions are derived and numerical results are presented by solving the nonlinear differential density matrix equations that govern the dynamics of the system. In the study of the different kinds of optical phenomena, the influence of the electron sheet density on the spectral shapes is carefully examined.

Made available in DSpace on 2015-05-14T12:14:09Z (GMT). No. of bitstreams: 1 arquivototal.pdf: 5247280 bytes, checksum: a825d4cf1e9d423d3daa9794ddd2962e (MD5) Previous issue date: 2013-07-23 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPES / The response of a material to an incident radiation can be described in terms of the susceptibility of the medium. In an atomic vapor, this susceptibility strongly depends on the frequency of the radiation and can vary over several orders of magnitude near the resonance. When a material is illuminated by light whose electric field is intense, the Kerr effect may become significant, showing a linear variation of the refractive index as a function of the intensity of the laser beam. Several techniques allow the measurement of this nonlinear effect. One of the simplest and most accurate is the z-scan technique. It consists in moving the medium to be probed along the axis of a focused laser beam. The transmittance through an aperture is measured as a function of the cell position and the obtained curve allows one to determine the nonlinear refractive index (n2) of the material. In this work, we investigate the nonlinear refractive index of a vapor of cesium atoms. We used the z-scan technique for various detunings around the Cs D2 transition (wavelength at 852 nm). To monitor the frequency of the laser, we simultaneously used an auxiliary saturated absorption setup and a Fabry-Perot analyzer. Through simple relationships between n2 and the aperture transmittance, we obtained a value for n2 as a function of the laser detuning. A theoretical model was developed to be compared to our experimental results. We used the density matrix formalism to calculate n2, taking into account the velocity distribution of the atoms in the calculation of the matrix elements. We started by treating the atoms as two-level systems, which allows us to test different limits of velocity integration. We then carried out a more realistic model for the D2 line of Cs, considering one fundamental level and three excited levels. We showed that for each hyperfine transition, the third-order fundamental-excited coherence depends on the population of the excited states as well as on the coherence created between the excited levels. To our knowledge, our experimental results are the first measurements of n2 for a cesium vapor, using the z-scan technique. The measured values of n2 are consistent with our theoretical calculations. / A resposta de um meio material à radiação incidente pode ser descrita em termos da susceptibilidade ótica desse meio. Em vapores atômicos, essa susceptibilidade depende fortemente da freqüência da radiação e pode variar, em torno da ressonância, por várias ordens de grandeza. Quando um material é iluminado por um feixe de luz cujo campo elétrico é muito intenso, evidencia-se o efeito Kerr, ou seja, o próprio índice de refração do material varia linearmente com a intensidade do feixe laser. Para medir esse efeito não linear da polarização do material, existem varias técnicas na literatura. Uma das mais simples e precisa é a varredura z (z-scan). O z-scan consiste em deslocar o meio a ser estudado ao longo do eixo de um feixe laser focalizado. Mede-se então a transmitância através de uma abertura, em função da posição da célula. A partir dessa curva de transmitância, é possível determinar o índice de refração não linear do material. Neste trabalho, investigamos a dependência espectral do índice de refração não linear do vapor atômico de césio. Realizamos experimentos com a técnica z-scan para várias dessintonizações na linha D2 (comprimento de onda de 852 nm). O monitoramento da freqüência do laser é feito através de uma montagem auxiliar de absorção saturada e de uma cavidade Fabry-Pérot. Utilizando relações simples entre n2 e a transmitância na abertura, obtivemos um valor de n2 para cada dessintonização. Para interpretar os resultados experimentais, usamos o formalismo de matriz densidade para calcular teoricamente o n2. No cálculo dos elementos da matriz densidade, deve-se levar em consideração a distribuição de velocidades dos átomos. Iniciamos nosso modelo tratando os átomos como sistemas de dois níveis, com o objetivo de compreender os diferentes limites da integração em velocidade. Em seguida passamos para um modelo mais realista para a linha D2 do Cs envolvendo um nível fundamental e três excitados. Mostramos que, para cada transição hiperfina, a coerência fundamental-excitada de terceira ordem depende de efeito de população dos estados excitados e da coerência criada entre eles. Nossos resultados experimentais são, até onde sabemos, as primeiras medidas usando z-scan para a obtenção do indice de refração de vapor de césio. Os valores medidos de n2 são condizentes com os nossos cálculos teóricos.

Topological insulators are materials with their electronic band structure in bulk resembling that of an ordinary insulator, but the surface states are metallic. These surface states are topologically protected, meaning that they are robust against impurities. The topological phenomena of three dimensional topological insulators can be expressed within topological field theories, predicting axion electrodynamics and the topological magnetoelectric effect. An experiment have been suggested to measure the topological phenomena. In this thesis, the underlying theory and details around the experiment are explained and more detailed derivations and expressions are provided.

Para o desenvolvimento da nanociência atual há forte demanda por equipamentos capazes de caracterizar sistemas em escalas da ordem nanométrica. Este contexto impulsionou o desenvolvimento de microscópios ópticos de varredura em campopróximo (Scanning Near-field Optical Microscope SNOM). Diferentemente da microscopia óptica tradicional, os SNOMs detectam a radiação eletromagnética evanescente e, conseqüentemente, a resolução não é limitada pelo critério de Rayleigh. No Laboratório de Materiais Magnéticos IFUSP desenvolvemos um SNOM sensível a efeitos Kerr magnetoópticos (MO-SNOM). Dessa maneira, associamos a alta resolução da técnica à alta sensibilidade dos efeitos magnetoópticos. Trata-se se uma área relativamente pouco explorada e carente de resultados sistemáticos na literatura. Utilizando o MO-SNOM, caracterizamos partículas microestruturadas de Co70.4Fe4.6Si15B10 amorfo com dimensões de 16x16x0.08 microm3 e 4x4x0.08 microm3. Os resultados compreendem dezenas de imagens de susceptibilidade magnetoóptica diferencial com resolução melhor que 200 nm e curvas de histerese local. Em primeira análise, a demonstração de resultados sistemáticos ajuda a estabelecer a técnica. O comportamento magnético das partículas, estudadas sob várias condições de campo aplicado, se mostrou determinado basicamente pela anisotropia de forma. As curvas de histerese local mostraram comportamentos intrinsecamente locais e motivaram uma interessante discussão sobre os parâmetros de caracterização magnética convencionais. As medidas realizadas indicam que o efeito Kerr magnetoótico transversal em campopróximo é similar ao campo-distante. Os resultados são fortemente sustentados por medidas de microscopia magnetoóptica de campo-distante, simulações micromagnéticas e medidas de microscopia de força magnética. Medidas complementares revelam o potencial do MO-SNOM para caracterizações de objetos extensos quanto a potenciais de pinning. Além disso, medidas em filmes finos de NiFe/FeMn acoplados por exchange-bias evidenciam a alta sensibilidade do MO-SNOM, estimada de DM ~ 2 x 10-12 emu. / To support nanosciences evolution, there is a strong demand for developing new instrumentation devoted to nano-scale characterization. In this context, the development of the Scanning Near-field Optical Microscope (SNOM) took place. In contrast to traditional optical microscopes, SNOM deals with evanescent electromagnetic radiation and, consequently, the resolution is no longer limited by the Rayleigh criterion. At Laboratório de Materiais Magnéticos (LMM) IFUSP a SNOM devoted to magneto-optical Kerr effect measurements (MO-SNOM) has been developed. The MOSNOM associates the high resolution of the near-field technique to the high sensibility of the magneto-optical Kerr effect. Near-field magneto-optical microscopy is not yet wellestablished and there is a lack of systematic results in the literature. Using the MO-SNOM, amorphous Co70.4Fe4.6Si15B10 particles with 16x16x0.08 microm3 and 4x4x0.08 microm3 dimensions were studied. With resolution better than 200 nm, several magneto-optical differential susceptibility images and local hysteresis loops were obtained. The systematic results uphold the establishment of this new technique. Under the different applied field conditions, the magnetic behavior of the particles was found to be determined by shape anisotropy. Local hysteresis loops presented shapes intrinsic of local field induced process. The unusual hystesesis loops motivated interesting discussion about the conventional magnetic parameters. The MO-SNOM measurements indicate that the near-field transverse magneto-optical Kerr effect is similar to the far-field case. The results are highly supported by far-field magneto-optical microscopy, micromagnetic simulations and magnetic force microscopy measurements. Complementary measurements indicate the MO-SNOM potential to extensive magnetic surface characterization related to pinning potential distribution. Furthermore, measurements on the exchange-bias coupled NiFe/FeMn thin films make evident the MO-SNOM high sensitivity, estimated to be DeltaM ~ 2 x 10-12 emu.

Observamos o comportamento espectral do efeito Kerr transversal, para filmes amorfos de terra rara - cobalto na região do espectro visível e ultravioleta próximo (comprimento de onda, , entre 325 nm e 670 nm), onde o sinal magnetoóptico apresentou um máximo na região azul do espectro. Concluímos que, para esta região espectral, a variação relativa de refletividade é proporcional à magnetização do cobalto e a constante de proporcionalidade depende da composição da liga e do comprimento de onda da luz. Desenvolvemos uma técnica de modulação de fase, própria para medir o efeito Kerr transversal e a comparamos com a técnica de modulação de amplitude. Montamos um magnetômetro a efeito Kerr que opera com a modulação de fase e utiliza um laser de He-Cd ( = 325 nm e 442 nm) ou um diodo laser vermelho ( = 670 nm). Fazendo uma analogia com a figura de mérito para os efeitos Kerr longitudinal e polar (Fe), nós propusemos uma figura de mérito para o efeito Kerr transversal (FJ. Mostramos que sua dependência do ângulo de incidência é semelhante à da variação relativa de refletividade e, comparando medidas da figura de mérito do efeito Kerr longitudinal com a figura de mérito para o efeito transversal, comprovamos que a grandeza proposta é um bom parâmetro para medida de qualidade magnetoóptica de materiais. Observamos os efeitos do sperimagnetismo de ligas com anisotropia local fraca (Gd-Co) e forte (Ho-Co), através do comportamento térmico dos ciclos de histerese magnética e magnetoóptica. Dentre os fenômenos observados estão os efeitos da compensação, o crescimento hiperbólico do campo coercivo e os efeitos da reorientação de spin. Para a liga de Gd20C080a, transição observada foi uma inversão de spin, cujo o campo magnético aplicado, no qual ocorre a transição, cresce exponencialmente com o aumento da temperatura da amostra. / We have observed the spectral behavior of the transverse magnetooptical Kerr effect (TMOKE) in thin films of rare earth - cobalt amorphous alloys for the visible and the near-ultraviolet ranges of spectrurn (wavelength fiom 325 nm up to 670 nm). The relative change of reflectivity has shown a maximum at the blue wavelength. We have concluded that this magneto-optical signal is proportional to the cobalt magnetization and the proportionality constant depends on the alloy composition and on the wavelength. Besides developing an apparatus and a new phase modulation technique for the TMOKE, we have compared it to the more usual amplitude modulation TMOKE technique. This apparatus operates using either a He-Cd laser ( = 325 nm and 442 nm) for a red diode laser ( = 670nm). We have proposed the figure of merit for the transverse Kerr effect (F,) by analogy with the figure of merit for the longitudinal and polar Kerr effect (Fe). We have measured F, as a function of the angle of incidence and we have shown that F, has the same behavior of the magneto-optical signal. A comparison between F, and Fe has shown that F, is as good parameter as well as Fe for the characterization of the materials magneto-optical quality. We have studied the sperimagnetism of thin films of amorphous alloys with weak (Gd-Co) and strong (Ho-Co) random local anisotropy by the thermal behavior of the magnetic and magneto-optical hysteresis loops. The phenomena of compensation, coercivity and spin-reorientation phase transitions were observed. The comparison between magnetic and magneto-optical hysteresis loops for Gd20C~8h0as shown that the transition occurs from a colinear phase to an opposite collinear phase. In this case, the transition magnetic field grows exponentially when the temperature increases.

Le manuscrit présente une étude de la réponse optique non linéaire quadratique et cubique de nano-structures métalliques d'or déposées sur substrat. Le travail s'inscrit plus généralement dans le domaine de la plasmonique non linéaire et vise à mieux comprendre l'interaction entre les nanostructures et la lumière, dans un régime d'intensités incidentes fortes, lorsque la réponse n'est plus linéaire. Les exaltations des champs électromagnétiques locaux dans ces structures par les résonances de plasmon de surface, excitations collectives des électrons de conduction, favorisent en effet considérablement ces processus. Dans le cadre de la réponse quadratique, l'étude a essentiellement porté sur le processus appelé génération de second harmonique (SHG, acronyme pour Second Harmonic Generation) par lequel deux photons incidents à la fréquence fondamentale sont convertis en un photon à la fréquence harmonique double. Ce processus est fortement dépendant de la morphologie des nanostructures métalliques. Pour la réponse cubique, l'étude a porté sur les effets Kerr optiques qui décrivent la variation de l'indice optique des nanostructures avec l'intensité de l'onde incidente. Une attention toute particulière a été donnée aux conditions géométriques d'éclairement effectué avec une grande ouverture numérique. Le champ électromagnétique incident ne doit en effet plus être considéré dans l'approximation paraxiale / The manuscript reports a study about the quadratic and cubic nonlinear optical response from gold metallic nanostructures which are deposited onto substrates. The field of this work is more commonly known as nonlinear plasmonics and it consists in trying to understand the interaction between nanostructures and light, in a regime of high incident intensities when the response is no longer linear. The local electromagnetic field enhancement in these structures due to the surface plasmon resonance, the latters being collectives excitations of the conduction band electrons, increase drastically the cross-section for these processes. In the context of a quadratic response, the study has been focused on the Second Harmonic Generation (SHG) process whereby two incident photons at the fundamental wavelength are converted into one photon at twice the harmonic frequency. This process is highly dependent to the metallic nanostructures morphology. For the cubic response, the study has been focused on the optical Kerr effect which describes the optical index variation of nanostructure with the intensity of the incident wave.Specifics considerations have been taken into account about the geometrical illumination conditions which are performed with a large numerical aperture. The electromagnetic incident field cannot be anymore considered within the paraxial approximation

In the quest for ultrathin materials compatible with CMOS technology for all-optical signal processing applications in integrated photonics, graphene appears to be a promising candidate, with broadband1 optical properties and a high and broadband optical nonlinearity. However, researchers do not agree on the value of its nonlinear refractive index, and commonly used characterization methods do not provide a clear picture of the optical nonlinearity, in terms of its tensor nature or relaxation time. In the first part of this thesis, apart from the previously used Z-scan method, we have also used the ultrafast Optical Kerr Effect method coupled to Optical Heterodyne Detection (OHD-OKE) for the characterization of the third order optical nonlinearity of monolayer CVD graphene at telecom wavelengths. This method allows to separately measure the real and the imaginary part of the third-order nonlinearity, as well as their dynamics. With respect to the Z-scan method, OHD-OKE presents the major advantage of being robust against inhomogeneities of the sample. As such, we have demonstrated that graphene has a negative nonlinear refractive index, contrary to previously reported results. In addition, we have studied the real and imaginary part of graphene’s nonlinearity, when electrostatic gating is applied to change the chemical potential of graphene. Furthermore, we have proposed an enhanced version of the OHD-OKE method, together with the appropriate theoretical framework, in order to extract the tensor elements of the nonlinearity including the out-of-plane tensor elements. In particular, we have measured separately the time response of the two main tensor elements of the nonlinear susceptibility and we have experimentally verified that the out-of-plane tensor components are negligible. In the second part of this thesis, we have investigated, from an experimental point of view, the use of the nonlinear optical response of graphene for all-optical switching applications in integrated photonics. Namely, we have designed simple silicon nitride waveguide structures that constitute basic building blocks of switching devices, which were then fabricated and covered by graphene patches. Finally, we have experimentally tested the graphene-covered structures at low and high power levels and discussed the results. / Doctorat en Sciences de l'ingénieur et technologie / info:eu-repo/semantics/nonPublished

Dans cette thèse nous étudions les propriétés d'ondes stationnaires dans des structures composées d'une couche diélectrique nonlinéaire de type Kerr et des couches métalliques et diélectriques linéaires. Nous élaborons différents modèles pour étudier les propriétées de plasmons-solitons dans deux types de structures : (i) une région diélectrique nonlinéaire semi-infinie, des couches de métal et de diélectrique linéaires et (ii) une couche de diélectrique nonlinéaire d'épaisseur finie entre deux régions métalliques (guide d'onde métallique à coeur nonlinéaire). Pour le premier type de structures, nous montrons qu'en utilisant une structure à quatre couches, il est possible d'obtenir des plasmons-solitons de basses puissance. Pour des guides d'onde métalliques à coeur nonlinéaire, nous trouvons de modes d'ordres supérieurs. Pour certains des modes symétriques, nous observons une bifurcation par brisure de symétrie donnant naissance à des modes asymétriques dans une structure symétrique. / In this PhD thesis, we study the properties of stationary transverse magnetic polarized waves in structures composed of a Kerr-type nonlinear dielectric layer, metal and linear dielectric layers. We develop several models to study the properties of plasmon-soliton waves in two types of structures: a semi-infinite nonlinear dielectric in contact with metal and linear dielectric layers and a finite-size nonlinear dielectric layer sandwiched between two metal regions (nonlinear slot waveguide). Our models allow us to compute the nonlinear dispersion relations and the corresponding field profiles. For the first type of structure, we prove that using the four-layer structures that we propose, it is possible to obtain plasmon-soliton waves at the power levels. For nonlinear slot waveguide structures, we discover the existence of new, higher order modes. For some of the symmetric modes, we observe a symmetry breaking bifurcation giving birth to asymmetric modes in symmetric structure.