In our modern society, we are surrounded by numerous sensors, constantly feeding us information about our physical environment. From small, wearable sensors that monitor our physiological status to large satellites orbiting around the earth, detecting global changes. Although, the performance of these sensors have been significantly improved during the last decades there is still a demand for faster and more reliable sensing systems with improved sensitivity and selectivity. The rapid progress in nanofabrication techniques has made a profound impact for the development of small, novel sensors that enables miniaturization and integration. A specific area where nanostructures are especially attractive is biochemical sensing, where the exceptional properties of nanomaterials can be utilized in order to detect and analyze biomolecular interactions.  The focus of this thesis is to investigate plasmonic nanoparticles composed of gold or silver and optimize their performance as signal transducers in optical biosensors. Metal nanoparticles exhibit unique optical properties due to excitation of localized surface plasmons, which makes them highly sensitive probes for detecting small, local changes in their surrounding environment, for instance the binding of a biomolecule to the nanoparticle surface. This is the basic principle behind nanoplasmonic sensing based on refractometric detection, a sensing scheme that offers real-time and label-free detection of molecular interactions.  This thesis shows that the sensitivity for detecting local refractive index changes is highly dependent on the geometry of the metal nanoparticles, their interaction with neighboring particles and their chemical composition and functionalization. An increased knowledge about how these parameters affects the sensitivity is essential when developing nanoplasmonic sensing devices with high performance based on metal nanoparticles.

Cavity enhanced spectroscopies (CES) are currently amongst the most sensitive spectroscopic techniques available for probing gas-phase samples, however their application to the liquid-phase has been more limited. Sensitive analysis of submicrolitre liquid samples is highly desirable, as miniaturisation allows for the reaction and analysis of scarce or expensive reagents, produces less waste, and can increase the speed of separations and reactions, whilst having a small footprint and high throughput. Absorption spectroscopy is a particularly desirable technique due to its universal, label-free nature, however its application to small volume liquid samples is hampered by the associated short absorption pathlengths, which limit sensitivity. CES improve sensitivity by trapping light within a confined region, increasing the effective pathlength through the sample. Three distinct types of optical cavity were constructed and evaluated for the purposes of making optical absorption measurements on liquid samples. The first incorporated a high optical quality flow cell into a "macrocavity" formed from two dielectric mirrors separated by 51.3 cm. Cavity losses were minimised by positioning the flow cell at Brewster's angle to the optical axis, and the setup was used to perform a single-wavelength cavity ringdown spectroscopy experiment to detect and quantify nitrite within aqueous samples. The detection limit was determined to be 8.83 nM nitrite in an illuminated volume of only 74.6 nL. Scattering and reflective losses from the flow cell surfaces were found to be the largest barrier to increased sensitivity, leading us to focus on the integration of cavity mirrors within a microfluidic flow system in the work that followed. In the second set of experiments, cavity enhanced absorption spectroscopy (CEAS) measurements were performed on Thymol Blue using custom-made microfluidic chips with integrated cavity mirrors. Unfortunately, due to the plane-parallel configuration of the mirrors and the corresponding difficulty in sustaining stable cavity modes, the results were underwhelming, with a maximum cavity enhancement factor (CEF) of only 2.68. At this point, attention was focussed toward a more well-defined cavity geometry: open-access plano-concave microcavities. The microcavities consist of an array of micron-scale concave mirrors opposed by a planar mirror, with a pathlength that is tunable to sub-nanometer precision using piezoelectric actuators. In contrast to the other experimental setups described, themicrocavities allow for optical measurements to be performed in which we monitor the change of wavelength and/or amplitude of a single well-defined cavity mode in response to a liquid sample introduced between the mirrors. In the first microcavity experiment, we used 10 μm diameter mirrors with cavity lengths from 2.238 μm to 10.318 μm to demonstrate refractive index sensing in glucose solutions with a limit of detection of 3.5 x 10^-4 RIU. The total volume of detection in our setup was 54 fL. Thus, at the limit of detection, the setup can detect the change of refractive index that results from the introduction of 900 zeptomoles (500,000 molecules) of glucose into the device. The microcavity sensor was then adapted to enable broadband absorption measurements of methylene blue via CEAS. By recording data simultaneously from multiple cavities of differing lengths, absorption data is obtained at a number of wavelengths. Using 10 μm diameter mirrors with cavity pathlengths from 476 nm to 728 nm, a limit of detection, expressed as minimum detectable absorption per unit pathlength, of 1.71 cm^-1 was achieved within a volume of 580 attolitres, corresponding to less than 2000 molecules within the mode volume of the cavity. Finally, a new prototype was developed with improved cavity finesse, a much more intense and stable light source, and improved flow design. Using a single plano-concave microcavity within the array with a cavity pathlength of 839.7 nm, and 4 μm radius of curvature mirror, absorption measurements were performed on Methylene Blue. Analysis of this data indicated a CEF of around 9270, and a limit of detection based on the measured signal-to-noise ratio of 0.0146 cm^-1. This corresponds to a minimum detectable concentration of 104 nM Methylene Blue, which given the mode volume of 219 aL, suggests a theoretical minimum detectable number of molecules of 14.

In this thesis devices for controlling the flow of surface plasmon polaritons are described. Dielectric and metallic nanostructures were designed for this purpose, and characterized by leakage radiation microscopy in real and in reciprocal spaces. Manipulation of surface plasmons by dielectric lenses and gradient index elements is presented, and negative refraction, steering and self-collimation of surface plasmons in one- and two-dimensional plasmonic crystals is demonstrated. The achieved degree of control was applied for routing of nanoparticles by optical forces, as well as for two methods of enhancing the figures of merit of plasmonic refractive index sensors, based on the one hand on Fano resonances natural to leakage radiation microscopy, and on the other hand on anisotropie plasmonic bandstructures.

Cette thèse est une contribution à la modélisation et à l'étude expérimentale de cavités à cristaux photoniques à fente développées en vue d’un intégration hybride de matériaux actifs sur silicium. Parmi les travaux de conception, nous avons d'abord utilisé la méthodes des ondes planes et la méthode des différences finies (FDTD) pour concevoir une série de cavités SOI à hétérostructures, mécaniquement robustes, infiltrées par des liquides d’indices (n environ 1,5), présentant des longueurs d'onde de résonance dans la gamme des télécommunications (1,3 μm - 1,6 μm), des facteurs de qualité de plusieurs dizaines de milliers, et des volumes modaux proches de 0,03 (lambda/n)3. Nous avons ensuite étudié analytiquement et numériquement le couplage entre une cavité à cristaux photoniques à fente et un guide d'onde à fente par la théorie des modes couplés, complétée par des simulations FDTD, qui ont permis de confirmer la possibilité d'exciter efficacement les modes de fente des cavités à partir d'un guide externe. Enfin, nous avons étudié numériquement et semi-analytiquement des géométries de molécules photoniques constituées de deux cavités à cristaux photoniques à fentes couplées, dont l’écart fréquentiel entre les supermodes a pu être ajusté en amplitude et en signe. Nous avons utilisé une méthode perturbative (« Tight binding ») pour estimer les distributions spatiales des modes des molécules photoniques et prédire leurs fréquences dans plusieurs configurations de cavités à cristaux photoniques à fentes couplées.Ce travail exploratoire a été complété par une partie expérimentale qui a porté sur l'étude d'une famille de cavités de hétérostructure à cristaux photoniques à fente. Les cavités à cœur creux fabriquées ont montré des facteurs de qualité (Q) de plusieurs dizaines de milliers, associés à des volumes modaux de l’ordre de V=0,03 (λ/n)^3 après infiltration de la fente et des trous des structures par des liquides d'indice de réfraction proches de 1,46. Des facteurs Q/V supérieurs à 600 000 et atteignant 1 000 000 dans le meilleur des cas (vers lambda=1,3µm) ont ainsi été observés. Cette phase expérimentale préliminaire a donné ensuite lieu à deux types de développements.Tout d'abord, les propriétés des cavités à cristaux photoniques à fentes ont été étudiées pour des applications en détection d'indice en volume, et testées en utilisant différents liquides d'indice de réfraction compris entre 1,345 à 1,545. Les résonateurs étudiés ont présenté des sensibilités de ~ 235 nm / RIU et des facteur de mérite de détection d'indice de l’ordre de 3700, à l’état de l’art pour des résonateurs silicium intégrés à cœur creux.Dans une autre direction, le potentiel des résonateurs diélectriques à fente a été exploré en vue d’une intégration des matériaux actifs sur silicium. Un polymère dopé aux nanotubes de carbone semiconducteurs a été déposé comme matériau de couverture en vue d’étudier le renforcement de la photoluminescence (PL) des nano-émetteurs sous pompage optique vertical à lambda=740nm. Les expériences conduites ont permis de corréler le renforcement de la PL des nanotubes avec les modes de résonance des cavités et de démontrer le couplage partiel de cette PL vers des guides SOI longs de plusieurs millimètres (collection par la tranche vers lambda=1.3µm), apportant une preuve de principe d’une possible intégration des nanotubes émetteurs en photonique sur silicium. / This Ph.D. work is a contribution to the modeling and the experimental study of slot photonic crystal cavities for hybrid on-silicon integration. Among the design works, we first have used plane the wave expansion and finite-difference time-domain methods to design a series of mechanically robust (non-free membrane) SOI slot photonic crystal heterostructure cavities with resonance wavelengths in the telecommunication range, i.e. from 1.3 µm – 1.6 µm, with Q-factors of around several tens of thousands and mode volumes around 0.03(lambda/n)^3 after being infiltrated by cladding materials with typical index values around 1.5. We have then analytically and numerically studied the coupling between a slot photonic crystal cavity and a slot photonic crystal waveguide by using the coupled mode theory and FDTD simulation. Then we confirmed the ability to excite the cavity slot modes from a waveguide by using FDTD simulation. Finally, as a preliminary step towards the use of several coupled slotted cavities for future hybrid integration schemes, we have numerically and semi-analytically investigated photonic molecules made of two coupled slot photonic crystal cavities providing two different supermodes (bonding and antibonding ones) with controllable wavelength splitting. We successfully employed the tight-binding (TB) approach, which relies on the overlap of the two tightly confined cavity electric fields, to predict the supermodes frequencies and spatial distributions in several coupled slot photonic crystal cavity configurations.This exploratory work was supplemented by an experimental part, which focused on the investigation of a family of slot photonic crystal heterostructure cavities. The fabricated silicon on insulator hollow core cavities showed quality factors of several tens of thousands, i.e. from 18,000 to 31,000 and mode volume V of ~0.03(λ/n)3 after being infiltrated with liquids of ~1.46 refractive index, yielding Q/V ratio larger than 600,000, and reaching 1,000,000 in the best case (at λ ≈ 1.3 μm).This preliminary experimental stage gave rise to two types of additional developments.Firstly, the properties of the studied slot photonic crystal cavities have been investigated for index sensing applications by using different liquids with refractive index values ranging from 1.345 to 1.545. The considered photonic crystal resonators have demonstrated quality factors of several tens of thousands with sensitivities of ~235 nm/RIU and index sensing FOMs around 3,700, i.e. at the state of the art considering hollow core silicon integrated resonators.Secondly, in the view of the integration of active materials on silicon, the potential of these hollow core nanoresonators has been considered to enhance the photo-luminescence (PL) of semiconductor single-walled carbon nanotubes (SWNTs) integrated in thin films deposited on top of silicon. We have brought the first experimental demonstration of SWNTs PL collection (around lambda=1.28 µm) under vertical pumping at short wavelength (lambda=740 nm) from a slotted resonator into millimeter long integrated silicon waveguides, providing a first proof-of-concept step towards nanotube/Si-PhC integration as an active photonic platform. The reported works demonstrate the feasibility of integrating telecommunication wavelength nanotube emitters in silicon photonics as well as emphasize the role of slot photonic crystal cavities for on-chip hybrid integration.

Ce manuscrit s'inscrit dans le contexte du contrôle de la propagation des plasmons de surface. A cet effet, des nanostructures diélectriques et métalliques ont été conçues et caractérisées par microscopie à champ de fuite dans les espaces réels et réciproques. La manipulation des plasmons de surface à l'aide de lentilles diélectriques et d' éléments à gradient d'indice est présentée, et la réfraction négative, la direction et l'auto-collimation des plasmons de surface dans des cristaux plasmoniques à une ou deux dimensions sont démontrées. Ces résultats ont été utilisés pour le guidage de nanoparticules à l'aide de forces optiques, ainsi que pour deux méthodes permettant de renforcer le facteur de mérite de sondes plasmoniques de variation d'indice de réfraction, basées l' une sur les résonances de Fano naturelles de la microscopie à champ de fuite, et pour la seconde sur les structures des bandes plasmoniques anisotropes. / In this thesis devices for controlling the flow of surface plasmon polaritons are described. Dielectric and metallic nanostructures were designed for this purpose, and characterized by leakage radiation microscopy in real and in reciprocal spaces. Manipulation of surface plasmons by dielectric lenses and gradient index elements is presented, and negative refraction, steering and self-collimation of surface plasmons in one- and two-dimensional plasmonic crystals is demonstrated. The achieved degree of control was applied for routing of nanoparticles by optical forces, as well as for two methods of enhancing the figures of merit of plasmonic refractive index sensors, based on the one hand on Fano resonances natural to leakage radiation microscopy, and on the other hand on anisotropie plasmonic bandstructures.