This thesis is concerned with various methods for the control and investigation of pulse dynamics in a Photonic Crystal Fibre (PCF) and of the radiation driven by a short pulse. In particular the focus is on pulses in the anomalous dispersion region which would form solitons in the absence of higher order effects. Several different types of radiation can be driven by such pulses if they are perturbed by higher order dispersive and non-linear effects - for example Resonant Radiation (RR) and Negative Resonant Radiation (NRR) two dispersive waves which gain energy at the expense of the pulse. The feature of NRR which is of particular importance is that it is the first observed example of a coupling between positive and negative frequencies in optics. This has only been possible due to recent advances in fields such as PCFs, lasers and analogue systems. As with many scientific discoveries, NRR was found by bringing together ideas and techniques from these different fields. Both the pulse and the driven radiation are investigated using a number of different pulse and PCF parameters. These include power, chirp, polarisation and PCF dispersion. These are used to vary the wavelengths at which the driven radiation occurs as well as its generation efficiency. Furthermore the power and chirp are used to vary where in the PCF the driven radiation is generated by controlling where the driving pulse compresses and spectrally expands. This property is used to investigate different stages in the evolution of the pulse and driven radiation as well as to optimise the generation efficiency of the driven radiation.

La microscopie par diffusion Raman cohérente anti-Stokes (CARS) est une technique de spectro-imagerie qui permet de cartographier les modes vibrationnels intra-moléculaires d'un échantillon biologique, sans nécessité de marquage préalable. La mesure CARS est cependant dégradée par un "fond non-résonant" qui détériore le contraste. Récemment, la microscopie par diffusion Raman stimulée (SRS) fut proposée comme une alternative à la microscopie CARS, permettant d'obtenir une imagerie "sur fond noir". Dans cette thèse, nous décrivons le développement d'un microscope SRS. Nous évaluons le caractère spécifique des contrastes CARS et SRS dans le cadre d'une application biomédicale concrète, à savoir la détection de mélanomes humains. Nous présentons une description exhaustive des phénomènes physiques pouvant conduire à des artéfacts de mesure en SRS. Nous proposons finalement une technique basée sur l'utilisation de trois faisceaux d'excitation à trois couleurs, permettant de supprimer ces artéfacts. Dans une seconde partie, nous nous intéressons à la microscopie CARS en configuration plein champ. Nous proposons une méthode permettant de supprimer le fond non-résonant. Celle-ci est basée sur une analyse de front d'onde du champ anti-Stokes. En guise d'ouverture, nous proposons une technique - toujours basée sur l'analyse de front d'onde - permettant de réaliser la spectroscopie d'absorption quantitative de nano-objets. Nous illustrons le potentiel de cette technique en réalisant des mesures sur des matrices de nanoparticules d'or et sur des nanoparticules uniques. / Coherent Anti-Stokes Raman Scattering (CARS) microscopy is a technique that can map the spatial distribution of intra-molecular vibrational modes of a biological sample. This method thus provides molecular specificity, without staining the sample. However, CARS signal is hampered by a "non-resonant background" which reduces the contrast. Recently, Stimulated Raman Scattering (SRS) microscopy has been proposed as an alternative to CARS microscopy because it is a background free method. In this thesis, we describe the development of a SRS microscope. We evaluate the specificity of CARS and SRS contrasts in a concrete biomedical application, the detection of human melanomas. We present a comprehensive description of the physical phenomena that can lead to artifacts in SRS microscopy. We show that the scattering properties of the sample can lead to artifacts. We propose a technique based on three excitation beams of different color which suppresses these artifacts. In the second part, we focus on CARS microscopy in a wide-field configuration. We implement a technique to remove the non-resonant background. This method is based on wavefront sensing of the anti-Stokes Field by quadriwave lateral sharing interferometry (QWLSI). We demonstrate that the measurement of the intensity and phase of the complex CARS field allows to retrieve the spontaneous Raman scattering spectrum. As a perspective, we propose a technique, still based on wavefront sensing by QWLSI, to achieve quantitative absorption spectroscopy of nano-objects. We illustrate the potential of this technique by performing measurements on arrays of gold nanoparticles and on single nanoparticles.

Neste trabalho estudamos teórica e experimentalmente o efeito de Conjugação de Fase por Mistura Degenerada de Quatro Ondas (CFMD40) e Modulação Transversal de Fase em cristais dopados com Cr+3. Estudamos a CFMD40 em Al2O3:Cr+3 (rubi) e GdAlO3:Cr+3 com um laser de Ar (em λ=514nm) obtendo um bom acordo entre os resultados experimentais e os teóricos (nestes cálculos usamos os valores de n2 de um trabalho anterior [1]). O modelo teórico que fizemos explica muito bem o comportamento de saturação da eficiência da CFMD40 que não era compreendido em trabalhos anteriores [47,48.2]. Usando os mesmos valores de n2 obtivemos um bom acordo entre os resultados experimentais e teóricos para o efeito de Modulação Transversal de Fase. Também fizemos um modelo teórico para o efeito de Modulação Transversal de Fase em CFMD40 que explica nossas observações [2]. A não linearidade destes materiais foi investigada usando-se três técnicas experimentais diferentes [1.2] e por dois outros grupos [61.62] (para o rubi) através de mistura de duas ondas não degeneradas. Todas estas medidas estão em bom acordo. Na alexandrita (BeAl2O 4:Cr+3) estudamos o espectro de χ(3) (ou n2) em ressonância das linhas R. Nos atribuímos a forma assimétrica do espectro como sendo oriunda de duas contribuições para susceptibilidade, onde um termo é devido a interação ressonante com o sistema de dois níveis e o outro devido a mudança de polarizabilidade causada pela população do estado excitado (esta é a primeira vez que este efeito foi observado). / In this work we studied theoretical and experimentally the effects of Phase Conjugation by Degenerate Four Wave Mixing and Transversal Phase (PCD4WM) Modulation in Cr+3 doped crystals. We studied the PDC4WM in Al2O3:Cr+3 (ruby) and GdAlO3:Cr+3 with on Ar laser (at λ= 514 nm) and obtained a good agreement between our experimental and theoretical results (in these ca1culations we used the nonlinear refractive index n 2 values from a previous paper [1]. The theoretical model that we developed explains very well the saturation behaviour of the PDC4WM efficiency that was not understood in previous papers [47.48,2]. These values of n2 are also in good agreement with our results in Transverse Phase Modulation. We also developed a theoretical model for the effect of Transverse Phase Modulation in PCDFWM that explains our observations [2]. The nonlinearity ?n IND.2? from these materials was investigated by us using three different techniques [1.2], by other two groups [61.62] (for the ruby) in nondegenerate two-wave mixing and all those measurements are in good agreement. In alexandrite (BeAl2O4:Cr +3) we studied the χ(3) (or n2) spectrum in resonance with the R lines. We attributed the asymetric shape of the spectrum by the effect of two differents contributions, one term due to the resonant interaction of the two-level system and the other due to the polarizability change caused by excited state population (this is the first observation of this kind of effect.

Esta tese descreve a demonstração experimental de dispositivos baseados em fibras de cristal fotônico (PCFs), que aproveitam a flexibilidade estrutural oferecida pela matriz de capilares que compõe a seção reta da fibra, de forma a preencher estes capilares com líquidos e materiais nanoestruturados. Para o caso de materiais nanoestruturados, uma vez preenchida a fibra, os materiais nela inseridos interagem eficientemente com a luz guiada. Essa arquitetura diferenciada em relação às fibras ópticas convencionais abre novas perspectivas no desenvolvimento de aplicações como óptica não-linear e sensoriamento. PCFs de núcleo líquido, por outro lado, impõe dificuldades para a implementação de dispositivos práticos, devido às altas taxas de evaporação dos líquidos inseridos. Por esta razão, foi desenvolvida uma nova técnica para vedar seletivamente ambas as faces externas do núcleo líquido de uma PCF, utilizando um polímero curável. Estes tampões poliméricos evitam a evaporação, causando um impacto mínimo no guiamento da luz, tornando o dispositivo usável por semanas. Esta nova técnica de vedação foi empregada em um experimento para a geração de supercontínuo em uma PCF com núcleo de água destilada, proporcionando uma estabilidade de pelo menos 1 hora. Combinando líquidos e materiais nanoestruturados, foi também foi desenvolvido um sensor de temperatura baseado no preenchimento do núcleo de uma PCF por uma amostra coloidal de nanopartículas semicondutoras de CdSe/ZnS, dispersas em óleo mineral. O espectro de luminescência destes pontos quânticos coloidais é fortemente dependente da temperatura e os resultados obtidos mostraram que a grande interação entre a luz e o colóide, aliada a geometria da fibra, proporcionando uma sensibilidade ~5,5 vezes maior que a apresentada por uma rede de Bragg escrita em uma fibra óptica padrão, com boa relação sinal-ruído. / This thesis describes the experimental demonstration of devices based on photonic crystal fibers (PCFs). PCFs are optical fibers whose core is surrounded by a regular matrix of holes, which runs longitudinally across its length. This singular configuration allows the insertion of liquids and nanostructured material into the fiber. Nanostructured materials embedded inside the fiber efficiently interact with the guided light, opening up possibilities of novel applications regarding the fields of non-linear optics, as well as optical sensing. On the other hand, liquid-core PCFs suffer from some disadvantages concerning practical device applications, on account of the high evaporation of the inserted liquids. In order to address this issue, we developed a novel technique to selectively seal the external faces of a liquid-core PCF, by using a polymer plug. These polymer plugs avoid evaporation while causing a minimum impact on the light guiding characteristics of the PCF. This novel sealing technique was employed in a supercontinuum generation experiment, by using a PCF whose core was water-filled. A temporal stability of at least one-hour on the resulting spectrum was achieved. Combining the above techniques, we also developed a temperature sensor based on the core-filling of a PCF by a colloidal ensemble of CdSe/ZnS semiconductor nanoparticles dispersed in mineral oil. Those colloidal quantum-dots display a luminescence spectrum which is strongly dependent on temperature and the experimental results indicated that the greater interaction between the guided light and the colloidal sample, provided by the fiber geometry, allowed a sensitivity which is approximately 5.5 times than possible with a conventional Bragg grating, while keeping a satisfactory signal-to-noise ratio.

Investigamos as propriedades quânticas conjuntas dos três feixes intensos de luz produzidos por um oscilador paramétrico ótico (OPO) operando acima do limiar, denominados bombeio, sinal e complementar. Analisamos experimentalmente as flutuações quânticas de intensidade e fase destes feixes, e como se correlacionam. Observamos pela primeira vez a presença de correlações quânticas entre as fases dos três campos. O ruído observado na soma das fases de sinal e complementar, Vq12=1,28(3)>1, passa a apresentar compressão de ruído após ser corrigido pelas flutuações de fase do feixe de bombeio, resultando em (Vq12)\' =0,84(3)<1. Para potências mais altas de bombeio, observamos também a existência de correlações quânticas diretamente entre as amplitudes do feixe de bombeio e um dos feixes convertidos (sinal ou complementar); a máxima compressão de ruído medida correspondeu a Vp02=0,86(3)<1. Estendemos nosso estudo às propriedades de emaranhamento deste sistema tripartite, para tanto utilizando dois critérios distintos. Nossos dados apontam a separabilidade do sistema no regime de operação estudado, em contradição com o modelo teórico. Utilizando o critério de emaranhamento de P. van Loock e A. Furusawa, obtivemos os seguintes valores para as combinação de variâncias que comprovariam a inseparabilidade caso fossem menores que 2: V0=1,29(5)<2, V1=2,04(11)>2 e V2=2,09(7)>2. Com relação ao segundo critério de separabilidade, positividade sob transposição parcial, obtivemos os seguintes autovalores simpléticos a partir da matriz de covariância medida: A0=0,94(8) e A1=0,36(6)<1, em que o emaranhamento seria evidenciado caso A0<1 e A1<1. Esta discordância com a previsão teórica está relacionada a um ruído clássico espúrio observado no sistema, cujas características são levantadas nesta tese. Nossa análise indica os rumos a serem seguidos para a observação do emaranhamento. Mostramos teoricamente que o emaranhamento tripartite previsto pode ser utilizado como recurso para a criação de um sistema emaranhado multipartite. Para tanto, diversos OPOs são utilizados em uma configuração em cadeia, na qual o feixe de bombeio refletido pelo primeiro OPO serve de bombeio para o segundo e assim sucessivamente. Este esquema permite a geração de uma rede quântica multicolor escalável. Por fim, descrevemos a construção de um laser de Ti:safira que representa o primeiro passo na integração entre luz não-clássica e física atômica a ser investigada em nosso laboratório. Este laser pode ser utilizado, ao mesmo tempo, como bombeio do OPO e de uma nuvem de átomos. O emaranhamento tripartite gerado no OPO estabeleceria a conexão destes últimos com os feixes convertidos, cujos comprimentos de onda possibilitariam a transmissão direta destes feixes de luz através de fibras óticas comerciais de telecomunicação. / We have investigated the collective quantum properties of the three bright light beams produced by an optical parametric oscillator (OPO) operating above threshold, named pump, signal, and idler. We have analyzed experimentally their intensity and phase quantum fluctuations, and how they are correlated. For the first time, we have observed the existence of phase quantum correlations among the three beams. The measured phase-sum noise between signal and idler, Vq12=1,28(3)>1, presents squeezing when corrected by the phase fluctuations of the pump beam, resulting in (Vq12)\'=0,84(3)<1. For higher pump powers, we have observed the existence of amplitude quantum correlations directly between pump and one of the downconverted beams (signal or idler); the maximum measured squeezing level corresponded to the noise Vp02=0,86(3)<1. Our investigations included the entanglement properties of this tripartite system, tested by two different criteria. Our data points to the separability of the system in the accessible regime of operation, in contradiction with the theoretical predictions. Applying the criterion by P. van Loock and A. Furusawa, we have obtained the following values of combinations of variances which would attest the inseparability in case values smaller than 2 would be obtained: V0=1,29(5)<2, V1=2,04(11)>2, and V2=2,09(7)>2. For the second criterion, the positivity under partial transpose, we have obtained the following symplectic eigenvalues calculated from the measured covariance matrix: A0=0,94(8) and A1=0,36(6)<1, where entanglement is attested in case A0<1,and A1<1. This discrepancy with the theoretical prediction is caused by a classical spurious noise observed in the system, which characteristics are investigated in this thesis. Our analysis indicates the path to successfully observe tripartite entanglement. We show theoretically that the predicted tripartite entanglement can be employed as a resource for the construction of a multipartite entangled system. This is accomplished by pumping several OPO\'s with the same optical field, such that the pump beam reflected by the first OPO is utilized to pump a second one, and so on. This scheme allows the generation of a multicolor scalable quantum network. Finally, we describe the construction of a Ti:sapphire laser which represents the first step in the integration between non-classical light and atomic physics to be investigated in our laboratory. This laser could be employed at the same time to pump an OPO and to interact with a cloud of atoms. The tripartite entanglement produced by the OPO could then entangle the atoms to the downconverted beams, which wavelength would allow the transmission of these beams through commercial optical fibers for telecom.

Ce manuscrit présente le rayonnement de second harmonique provenant de plusieurs milieux diélectriques allant de la réponse interfaciale à la réponse volumique. Ce travail de thèse constitue une première étape dans le but d'étudier une bulle de savon dans un piège optique par génération de second harmonique. Deux axes de recherche sont ainsi explorés : d'une part l'étude de la génération de second harmonique sur deux tensioactifs le TTAB et le SDS, constituants de base d'une bulle de savon, et de l'autre l'élaboration d'un nouveau dispositif expérimental permettant d'allier un piège optique à une excitation de second harmonique par un laser femtoseconde. Dans un premier temps, on explicite le montage optique reposant sur le principe d'un microscope confocal inversé et les mesures associées de la réponse harmonique d'interface air/verre et air/eau. Dans un second temps, on s'intéresse comme objet modèle, en lieu et place de la bulle, à une microparticule de silice. Ainsi, on commence par analyser sa réponse harmonique en microscopie non linéaire quand celle-ci se trouve déposée sur une matrice de verre. L'étude de cet objet met en avant l'interdépendance entre les aspects d'optique linéaire mesurés à la longueur d'onde fondamentale et l'intensité harmonique mesurée. Par la suite, cette microsphère est placée au sein du piège optique réalisé par un second faisceau. Malgré la faible taille et la symétrie de la particule diélectrique, on parvient à mettre en évidence la réponse harmonique d'une particule unique piégée. Enfin, dans une dernière partie, on s'intéresse à caractériser la génération de second harmonique pour des solutions savonneuses, première étape dans la réalisation d'une bulle. Les mesures de diffusion de second harmonique en volume pour des solutions de TTAB et SDS de diverses concentrations montrent un comportement similaire et une singularité lors du passage de la concentration micellaire critique. Lors de l'étude du signal de second harmonique à l'interface air/eau savonneuse en revanche, on mesure des comportements différents pour des tensioactifs anioniques et cationiques, provenant de la charge de surface et de l'orientation de l'eau sous-jacente / This thesis reports an experimental study of harmonic radiation from various dielectric media. We both study second harmonic generation on interfaces and hyper Rayleigh scattering in solutions. We present the first step for the realization of the following project : the study of the second harmonic generation on an optically trapped soapy bubble. To do so, two main axis of investigation are developped. Firstly, we study the harmonic response of two commonly used surfactants such as TTAB, a cationic one and SDS carrying a negative charge. This study consits of understanding the main component of a soapy bubble. We investigate how harmonic intensity is modified with an increase of soap concentration. These experiements are carried both in volume and at the air/water interface. The harmonic scattered intensity shows similar features for SDS and TTAB, as a sudden drop appearing at the critical micelar concentration. However, on the surface, the two oppositely charged surfactants give a radically different evolution of second harmonic signal versus their concentration. Indeed, the water molecules of the surroundings behaves in an opposite manner with negative or positive charged surfactants. The second axis of research that we work on in this thesis, is on a novel experimental development. We combine an optical tweezer to trap microsized particles with a femtosecond laser probe to generate the second harmonic. This is a first step in order to trap a bubble and study it with second harmonic generation. This non linear inverted confocal microscope is used to study harmonic profil of an silica bead stuck on a sample. This study gives a glance of the complexity of the correlation between linear optics effects on the laser probe beam and the created harmonic intensity. We also perform experiments on a trapped particle and we measure the harmonic response of an unique particle

Dans ce travail de thèse, nous avons étudié des effets d'optique non-linéaire d'ordre trois dans les cavités à cristaux photoniques en silicium. Le premier d'entre eux est un phénomène d'auto-oscillations à haute fréquence (GHz) dans ces cavités, qui a pour origine une modulation de la transmission de la cavité due à l'interaction entre la dispersion due aux porteurs libres et l’absorption à deux photons. Nous avons observé ces auto-oscillations, pour la première fois, dans les nanocavités à cristaux photoniques silicium avec une fréquence de l’ordre de 3 GHz et une grande pureté spectrale. Nous avons développé un modèle pour analyser les mécanismes qui régissent l'apparition de ces auto-oscillations, ainsi que les amplitudes des fréquences fondamentale et harmoniques de ces oscillations. Ce phénomène d'auto-oscillations permettrait de réaliser des sources micro-ondes en silicium très compactes. Le deuxième phénomène étudié est celui de la diffusion Raman, qui est le seul moyen d'obtenir des lasers entièrement en silicium démontré jusqu'à présent. Cette diffusion Raman a été mesurée tout d'abord dans des guides d'onde à cristaux photoniques étroits (W0.63) de longueur 100 microns, où nous avons pu obtenir un nombre de photons Stokes allant jusqu'à 9, montrant ainsi que la diffusion Raman stimulée prédominait dans ces guides d'onde, bien que nous n’ayons pas pu y obtenir un effet laser Raman franc. Nous avons ensuite mesuré la diffusion Raman dans des nanocavités doublement résonantes conçues spécifiquement à partir de ces guides d'ondes pour optimiser l'effet Raman, avec des facteurs de qualités allant jusqu'à 235000 pour la résonance Stokes. Bien que nous n'ayons pu mesurer que de la diffusion Raman spontanée dans ces cavités, avec un facteur de Purcell de 2.9, l'étude théorique que nous avons effectuée sur les lasers Raman, et qui s'accorde parfaitement avec les résultats expérimentaux, montre qu’il serait possible d'obtenir un laser Raman dans ces cavités avec un seuil en dessous du milliwatt à condition de diminuer ces pertes dues à l'absorption par porteurs libres. Ceci pourrait être accompli en diminuant le temps de vie des porteurs libres, par exemple en les retirant du silicium à l’aide d’une jonction MSM. / In this thesis, we studied third order nonlinear optical effects in photonic crystal cavities. The first of those effects is is the phenomenon of high frequency (GHz) self-pulsing in these cavities, which originates from a modulation of the transmission of the cavity due to the interaction between the free-carrier dispersion and the two-photon absorption. We have observed these self-induced oscillations for the first time in silicon photonic crystal nanocavities, with a frequency of about 3 GHz and a high spectral purity. We have developed a model to analyze the mechanisms that govern the onset of these oscillations, as well as the amplitudes of the fundamental and harmonic frequencies of these oscillations. This self-pulsing phenomenon would allow us to realize realize ultra-compact microwave sources made of silicon. The second phenomenon studied is that of Raman scattering, which is the only way to obtain lasers fully in silicon demonstrated so far. The Raman scattering was measured first in narrow photonic crystals waveguides (W0.63) of length 100 microns, where we could obtain a number of Stokes photons up to 9, showing that the stimulated Raman scattering predominated in these waveguides, although we have not been able to obtain a true Raman laser effect in them. We then measured the Raman scattering in doubly resonant nanocavities specifically designed from these waveguides to optimize the Raman effect, with quality factors up to 235000 for the Stokes resonance. Although we could only measure spontaneous Raman scattering in these cavities, with a Purcell factor of 2.9, the theoretical study that we conducted on the Raman lasers, which agrees perfectly with the experimental results, shows that it would be possible to obtain a Raman laser in these cavities with a threshold below the milliwatt, provided we reduce the losses due to the free-carrier absorption. This could be accomplished by decreasing the free-carrier lifetime, for example by removing the free carriers from the silicon using a MSM junction.

Ce travail porte sur l'étude de la cohérence entre champs triplets générés par interaction non linéaire d'ordre trois. Un protocole indirect, basé sur l'étude du champ issu de la somme de fréquences des champs triplets dans un cristal non linéaire a été envisagé. Une modélisation théorique en formalisme quantique de l'évolution des champs, de leur génération à leur recombinaison, a été développée, donnant lieu à une recherche exhaustive des signatures de corrélations susceptibles d'émerger de notre protocole. Les expériences menées, à savoir la génération non linéaire bi-stimulée et la recombinaison des champs ainsi générés, sont en accord avec notre modèle théorique et permettent de mettre en évidence le masquage des corrélations entre les champs dans ce régime fortement injecté, ces corrélations étant contenues dans les fluctuations quantiques, alors négligeables, des opérateurs champs. Le calcul théorique prédit une signature de corrélations fortes entre les photons triplets dans la cas d'un génération par fluorescence paramétrique, et plus faible dans le cas d'une génération mono-stimulée. / This work deals about the study of coherence between triple photon beams generated by a third order non linear interaction. A protocol, based on the study of the field arising from sum-frequency of the triplet fields in a non linear crystal, was proposed. A theoretical model, in the quantum formalism, was developed, leading to an exhaustive research of the potential signature of the correlations. All the possible schemes were studied : triple fields generation from parametric fluorescence or from stimulated interaction, and recombination of two or three of the triple fields. The experiments we led, i.e. the bi-stimulated non linear generation and the recombination of the so-born fields, agree with our theoretical model and put into light the correlations hiding in this highly stimulated regime, since these correlations lie in the quantum fluctuations of the fields operators. The theoretical calculations predicts a strong correlations signature when the fields are generated from parametric fluorescence, and a weaker one in the case of a generation mono-stimulated.

D'importants progrès ont été accomplis dans le domaine des matériaux à transition despin depuis leur première observation par Cambi en 1931. La combinaison de lachiralité avec le magnétisme résulte en de nouvelles propriétés très intéressantes quiouvrent la voie pour de potentielles applications technologiques. Ce manuscrit décritles résultats obtenus par diverses stratégies poursuivies vers des matériauxmoléculaires non-centrosymétriques à transition de spin par combinaison decomplexes à transition de spin avec des anions chiraux à symétries D3 et D2. / Many advancements in the field of spin crossover materials have been carried outsince the first observation by Cambi in 1931. The combination of chirality andmagnetism yields fascinating properties that open the way for potential technologicalapplications. Obtaining new non-centrosymmetric magnetic compounds yieldsinteresting subjects for non-linear optical studies or crystallography. This manuscriptdescribes the results obtained by various strategies pursued toward spin crossovernon-centrosymmetric molecular materials by combining spin crossover complexes withchiral anions based on D3 and D2 symmetric anions.

Diese Arbeit beinhaltet experimentelle und theoretische Untersuchungen der optischen Frequenzverdopplung (second-harmonic generation, kurz SHG) an metallischen Nanopartikeln. Frequenzverdopplung bedeutet, daß ein bei der Frequenz omega angeregtes Nanopartikel Strahlung der Frequenz 2*omega emittiert. Dieser Effekt tritt nicht nur in Materialien mit nichtzentrosymmetrischer Kristallstruktur, sondern auch an der Oberfläche von Metallen auf. Deshalb läßt er sich gut mit plasmonischen Feldüberhöhungen an metallischen Nanoantennen verbinden. Die Frequenzverdopplung wird an verschiedenen Nanostrukturen wie dreieckförmigen, stäbchenförmigen und vor allem kegelförmigen Nanopartikeln experimentell untersucht, welche aufgrund ihrer scharfen Spitzen starke SHG-Signale emittieren. Besonders die Kegel sind interessant: Bei Anregung mit einem fokussierten, radial polarisierten Strahl dominiert je nach Kegelgröße und Umgebungsmedium ein SHG-Signal entweder von der Spitze oder von der Bodenkante des Kegels. Diese an den Kegeln gemessenen Resultate werden durch theoretische Untersuchungen untermauert. In diesen Rechnungen werden die plasmonischen Feldüberhöhungen und die sich daraus ergebende Frequenzverdopplung für einen Kegel mit verschiedenen Parametern modelliert. An einem einzelnen Kegel gewonnene Resultate werden auch mit den Fällen eines kugelförmigen und eines stäbchenförmigen Partikels verglichen. Ein weiterer Gegenstand der theoretischen Untersuchungen ist die Superposition der zweiten Harmonischen von mehreren emittierenden Nanopartikeln zu einem Feldmaximum. Dabei wird eine kreisförmige Anordnung von 8 Nanostäbchen bzw. Nanokegeln von einer radial polarisierten Mode angeregt. Die Superposition der emittierten zweiten Harmonischen ergibt ein Feldmaximum innerhalb der Anordnung der Emitter. Durch eine Verkippung des anregenden Strahls kann dieser Fokus im Raum bewegt werden. Letztere Untersuchung ist insbesondere interessant im Hinblick auf lokalisierte photochemische Reaktionen, die durch das frequenzverdoppelte Licht von Nanopartikeln ausgelöst werden sollen. Mit chemischen Substanzen, die bei omega transparent, bei 2*omega aber photoreaktiv sind, wäre im Nahfeld dieser Nanoantennen eine starke Lokalisierung der Reaktion auf Bereiche kleiner als 100~nm möglich. Anhand von Photolacken und Polymermatrizen mit diesen Eigenschaften wird experimentell untersucht, ob frequenzverdoppeltes Licht überhaupt solche Reaktionen auslösen kann oder ob die photochemische Reaktionen überwiegend durch direkte Zwei-Photonen-Absorption des anregenden Lichts ausgelöst werden. Die Ergebnisse zeigen allerdings, daß die Zwei-Photonen-Absorption dominant ist. Durch die Zwei-Photonen-Absorption im Nahfeld von Partikeln ist aber dennoch eine vergleichbare Lokalisierung der Reaktion möglich. / This work includes experimental and theoretical investigations of second-harmonic generation (SHG) at metallic nanoparticles. SHG means that a nanoparticle that is excited at the frequency omega emits radiation at the frequency 2*omega. SHG does not only occur in materials with noncentrosymmetric structure, but also on metal surfaces. Hence, SHG can be combined well with plasmonic field enhancement at metallic nanoantennae. SHG is investigated experimentally at different nanostructures such as triangle-like, rod-like and especially cone-like nanoparticles. With their sharp tips these structures show a much stronger SHG signal than spherical nanoparticles. Especially the cones are interesting: Excited with a focused radially polarized beam, for different cone sizes and in different surrounding media either the signal from the tip or the signal from the bottom edge dominates. The measurement results from the cones are underpinned by theoretical investigations. In these calculations the plasmonic field enhancements and the resulting SHG are modeled for a cone with different parameters. The single-cone results are also compared with the cases of a spherical or rod-shaped particle. A further subject of the theoretical investigations is the superposition of the SHG radiation from a number of emitting nanoparticles to a field maximum. For that, a circular arrangement of 8 nanorods or nanocones is excited by a radially polarized beam. The superposition of the second-harmonic radiation fields yields a field maximum in the space between the emitters. A tilt of the exciting beam can move this focus in space. The latter item is of special interest concerning localised photochemical reactions induced by the second-harmonic light from nanoparticles. In the near field of these nanoantennae, a strong localisation of the reaction on regions smaller than 100 nm would be possible by using chemical substances being transparent at omega, but photoreactive at 2*omega. With photoresists and polymer matrices, experiments are carried out to investigate whether SHG light can trigger such reactions at all, or if these photochemical reactions are triggered predominantly by direct two-photon absorption of the exciting light. The results show that the two-photon absorption is the dominant process. Yet, through two-photon absorption in the near field of particles, the localisation of the reaction is still similar.