Working with nanoscale optics requires methods and equipment designed for the purpose. This thesis describes the development of techniques and a system for performing highly localised spectroscopy. The system consists of a nanonics multiview 2000 scanning near-field optical microscope, a grating spectrometer and a photonic crystal fibre supercontinuum light source. Discussion of the microscope includes its modes of operation and development of software to collect and analyse data. In order to demonstrate the setup, an example of localised spectroscopy is presented in the form of an investigation of hollow core photonic crystal fibre. Taking spectra of the components of the cladding of these fibres makes it possible to investigate the origins of bandgap guidance. A core focus of nanoscale optics is the interaction of light with metal structures. This field is called plasmonics. Fabrication of structures is presented and requires special facilities and processes. These processes are both time consuming and expensive, both factors that emphasise the need for prior modelling. Forward difference time domain modelling of a proposed structure comprising of a concentrically arranged ring and disk is explored using home written code and a commercial package called CST Microwave Studio. The investigation of this concentric design through modelling shows a very highly localised field enhancement which can be engineered to have a narrow spectral resonance in the near infrared. The interaction of the two components which govern this resonance is explained using a theory called plasmon hybridization. Once the optical behaviour of small metal objects is understood they can be used in other ways. An example of this is shown in Porous Silicon. As a material it provides an excellent template for formation of metal nano-particles. Embedded in a high surface area network of silicon these particles can be used as very effcient catalysts.

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Next generation photonics-based technologies will ultimately rely on novel materials and devices. For this purpose, phenomena at subwavelength scales are being studied to advance both fundamental knowledge and experimental capabilities. In this dissertation, concepts specific to near-field optics and experimental capabilities specific to near-field microscopy are used to investigate various aspects of the statistical properties of random electromagnetic fields in the vicinity of optically inhomogeneous media which emit or scatter radiation. The properties of such fields are being characterized within the frame of the coherence theory. While successful in describing the far-field properties of optical fields, the fundamental results of the conventional coherence theory disregard the contribution of short-range evanescent waves. Nonetheless, the specific features of random fields at subwavelength distances from interfaces of real media are influenced by the presence of evanescent waves because, in this case, both propagating and nonpropagating components contribute to the detectable properties of the radiation. In our studies, we have fully accounted for both contributions and, as a result, different surface and subsurface characteristics of inhomogeneous media could be explored. We investigated different properties of random optical near-fields which exhibit either Gaussian or non-Gaussian statistics. We have demonstrated that characteristics of optical radiation such as first- and second-order statistics of intensity and the spectral density in the vicinity of random media are all determined by both evanescent waves contribution and the statistical properties of the physical interface. For instance, we quantified the subtle differences which exist between the near- and far-field spectra of radiation and we brought the first experimental evidence that, contrary to the predictions of the conventional coherence theory, the values of coherence length in the near field depend on the distance from the interface and, moreover, they can be smaller than the wavelength of light. The results included in this dissertation demonstrate that the statistical properties of the electromagnetic fields which exist in the close proximity of inhomogeneous media can be used to extract structural information. They also suggest the possibility to adjust the coherence properties of the emitted radiation by modifying the statistical properties of the interfaces. Understanding the random interference phenomena in the near-field could also lead to new possibilities for surface and subsurface diagnostics of inhomogeneous media. In addition, controlling the statistical properties of radiation at subwavelength scales should be of paramount importance in the design of miniaturized optical sources, detectors and sensors.

The propagation symmetry of electromagnetic fields is affected by encounters with material systems. The effects of such interactions, for example, modifications of intensity, phase, polarization, angular spectrum, frequency, etc. can be used to obtain information about the material system. However, the propagation of electromagnetic waves imposes a fundamental limit to the length scales over which the material properties can be observed. In the realm of near-field optics, this limitation is overcome only through a secondary interaction that couples the high-spatial-frequency (but non-propagating) field components to propagating waves that can be detected. The available information depends intrinsically on this secondary interaction, which constitutes the topic of this study. Quantitative measurements of material properties can be performed only by controlling the subtle characteristics of these processes. This dissertation discusses situations where the effects of near-field interactions can be (i) neglected in certain passive testing techniques, (ii) exploited for active probing of static or dynamic systems, or (iii) statistically isolated when considering optically inhomogeneous materials. This dissertation presents novel theoretical developments, experimental measurements, and numerical results that elucidate the vectorial aspects of the interaction between light and nano-structured material for use in sensing applications.

Diese Arbeit beschreibt eine ausfŸhrliche Untersuchung der physikalischen Eigenschaften von Mikrokugelresonatoren aus Quarzglas. Diese Resonatoren unterstŸtzen sogennante whispering-gallery Moden (WGM), die GŸten so hoch bis 109 bieten. Als experimentelle Hilfsmittel wurden ein Nahfeld- und ein Konfokalmikroskop benutzt, um die Struktur der Moden bezŸglich der Topographie des Resonators eindeutig zu identifizieren, oder um einzelne Quantenemitter zu detektieren und anzuregen. Die resonante †berhšhung des elektromagnetischen Feldes in den Moden des Resonators wurde ausgenutzt, um stimulierte Raman-Streuung mit extrem niedrigem Schwellenwert im Quarzglas zu beobachten. Ein Rekordschwellenwert von 4.5 Mikrowatts wurde gemessen. Mittels einer Nahfeldsonde wurde die Modenstruktur des Mikro-Ramanlasers gemessen. Mikroresonatoren stellen einen Grundbaustein der Resonator-Quantenelektrodynamik dar. In dieser Arbeit wurde die Kopplung von einem einzelnen strahlenden Dipol an die WGM sowohl theoretisch als auch experimentell untersucht. Die kontrollierte Kopplung von einem einzelnen Nanoteilchen an die WGM eines Mikrokugelresonators wurde nachgewiesen. Erste Ergebnisse in der Kopplung eines einzelnen Emitters an die Moden des Resonators wurden erzielt. Die resonante Wechselwirkung mit Resonatormoden wurde ausgenutzt, um den Photonentransfer zwischen zwei Nanoteilchen dramatisch zu verstŠrken. Schlie§lich wurde die bislang unbeachtete Analogie zwischen dem Quantensystem eines einzelnen Emitters in Wechselwirkung mit einer einzelnen Resonatormode und dem klassischen System zweier gekoppelten Moden experimentell untersucht. Es wurde bewiesen, wie die aus der Resonatorquantenelektrodynamik bekannten Kopplungsregime der starken und schwachen Kopplung in Analogie auch an einem klassischen System beobachtet werden kšnnen. Der †bergang von schwacher zu starker Kopplung wurde beobachtet, und bislang gemessene unerwartet hohe Kopplungsraten konnten einfach erklŠrt werden. / This work presents an extensive study of the physical properties of silica microsphere resonators, which support whispering-gallery modes (WGMs). These modes feature Q-factors as high as 109 corresponding to a finesse of 3 millions for spheres with a diameter of about 80 micrometers. These are to date among the highest available Q-factors, leading to cavity lifetimes of up to few microseconds. A near-field microscope and a confocal microscope are used as tools to unequivocally identify the mode structure related to the sphere topography, and for excitation and detection of single quantum emitters. The high field enhancement of the cavity modes is exploited to observe ultra-low threshold stimulated Raman scattering in silica glass. A record ultra-low threshold of 4.5 microwatts was recorded. The mode structure of the laser is investigated by means of a near-field probe, and the interaction of the probe itself with the lasing properties is investigated in a systematic way. Microcavities also one of the building blocks of Cavity QED. Here, the coupling of a radiative dipole to the whispering-gallery modes has been studied both theoretically and experimentally. The controlled coupling of a single nanoparticle to the WGMs is demonstrated, and first results in coupling a single quantum emitter to the modes of a microsphere are reported. The resonant interaction with these modes is exploited to enhance photon exchange between two nanoparticles. Finally a novel analogy between a system composed of a single atom interacting with one cavity mode on one side and intramodal coupling in microsphere resonators induced by a near-field probe on the other side is presented and experimentally explored. The induced coupling regimes reflect the different regimes of weak and strong coupling typical of Cavity QED. The transition between the two coupling regimes is observed, and a previously observed unexpectedly large coupling rate is explained.

Diese Arbeit leistet einen Beitrag zum Verständnis optischer Anregungen in metallischen Nanostrukturen. Am Beispiel ausgewählter Strukturen werden experimentell die Dynamik dieser Anregungen mit Femtosekunden-Zeitauflösung und ihre elektromagnetischen Moden auf der Nanometer-Längenskala untersucht. Anhand winkel- und zeitaufgelöster Transmissionsexperimente an metallischen Dünnfilmgittern wird gezeigt, dass resonante Oberflächenplasmon-Polaritonen (OPPen) wesentlich die optischen Eigenschaften dieser Strukturen beeinflussen. Die Lebensdauer solcher Anregungen wird ermittelt und damit nachgewiesen, dass Kopplungen zwischen OPP-Resonanzen drastische Lebensdauer-Modifikationen zur Folge haben. In einem eigens konstruierten, spektral auflösenden optischen Nahfeldmikroskop werden die elektromagnetischen Feldverteilungen der OPPen direkt abgebildet. Derartige Experimente erlauben erstmals eine Zuordnung der räumlichen Moden zur zeitlichen Dynamik verschiedener OPP-Resonanzen. Diese Erkenntnisse ermöglichen zudem eine Interpretation des nahfeldmikroskopischen Bildkontrasts bezüglich der Beiträge verschiedener vektorieller Komponenten des optischen Nahfeldes. Die selektive Abbildung unterschiedlicher elektrischer und magnetischer Feldkomponenten in Abhängigkeit vom Sondentyp wird demonstriert. Darüberhinaus wird die OPP-Erzeugung in einem Gitter auf dem Schaft einer Nahfeldspitze ausgenutzt, um propagierende OPPen im Apex zu konzentrieren. Ein weiterer Teil der Arbeit nutzt elektrische Feldüberhöhungen an scharfen Metallspitzen für die lokalisierte Erzeugung nichtlinearer optischer Signale. Die Beobachtung intensiver Multiphoton-Elektronenemission nach Femtosekundenanregung stellt ein zentrales Ergebnis dar. Dieser Prozess wird umfangreich charakterisiert und findet seine erste Anwendung in einer neuartigen Rastersondentechnik, in der die örtlich variierende Elektronenemission der Bildgebung dient. / This thesis contributes to the understanding of optical excitations in metallic nanostructures. In experiments on selected model structures, the dynamics of these excitations and their electromagnetic spatial modes are investigated with femtosecond temporal and nanometer spatial resolution, respectively. Angle- and time-resolved transmission experiments on metallic thin film gratings demonstrate the dominant role resonant surface plasmon polaritons (SPPs) play in the optical properties of such structures. The lifetimes of these excitations are determined, and it is shown that coherent couplings among SPP-resonances result in drastic lifetime modifications. The spatial SPP mode profiles are imaged using a custom-built near-field optical microscope. The experiments reveal a direct correlation between the spatial mode structure and the dynamics of different SPP resonances. These findings allow for an interpretation of the near-field optical image contrast in terms of the contributions of different vectorial components of the electromagnetic near-field. A selective imaging of different electric and magnetic field components is demonstrated for various types of near-field probes. Furthermore, the excitation of SPPs in periodic structures is employed in a novel type of near-field tip. The resonant excitation of SPPs in a nanofabricated grating on the shaft of a sharp metallic tip results in their concentration at the tip apex. The final part of the thesis highlights the importance of optical field enhancements for the local generation of nonlinear optical signals at the apex of sharp metallic tips. Specifically, the observation of intense multiphoton electron emission after femtosecond excitation is a major result. This process is thoroughly characterized, and a novel scanning microscopy application based on this effect is presented. In this technique, an image contrast with nanometer resolution arises from spatially varying electron emission rates.

This dissertation presents subwavelength optics with focus on the theory and applications of subwavelength apertures in a metal film. Two main issues regarding the optics with subwavelength apertures are investigated. As the first issue, the extraordinary optical transmission (EOT) through a single hole in a metallic waveguide is presented. A total transmission through a single subwavelength aperture is theoretically predicted for a perfect electric conductor regardless of the aperture size, without relying on aperture arrays and surface corrugations as presented in previous works. The waveguide EOT is then applied to boost the optical throughput of an apertured near-field scanning optical microscope (NSOM) probe. Using a new structure for the apertured NSOM probe which allows for waveguide EOT, the optical throughput and the damage threshold are boosted by 100× and 40× as compared to a conventional structure, and the experimental findings are backed-up by comprehensive finite-difference time-domain (FDTD) simulations. Single fluorescent molecules are scanned using the EOT apertured NSOM probe, and a spatial resolution of 62 nm is achieved. As the second issue, subwavelength apertures are found useful for optical trapping. A small dielectric particle can significantly change the optical transmission through an aperture by dielectric loading, and subsequently, a large optical force is induced which favors trapping. A self-induced back-action (SIBA) optical trap is designed using a circular nanohole in a gold film. Trapping of 50 nm polystyrene particle is experimentally achieved, which is not possible using a conventional single beam optical tweezers. The circular nanohole SIBA trap works beyond the perturbative regime, as proven by FDTD simulations and a Maxwell stress tensor analysis. We further improve the nanohole trapping using a double-nanohole, which is more sensitive for small dielectric changes due to the intense local field enhancement between its two sharp tips. A single 12 nm silica sphere is experimentally trapped using the double-nanohole, as the smallest trapped dielectric particle reported. We also achieve the trapping of a single protein – a bovine serum albumin (BSA) protein with a hydrodynamic radius of 3.4 nm in the folded form. The trapped BSA is also unfolded by the large optical force, as confirmed by experiments with changing optical power and changing pH. The high signal-to-noise ratio of 33 in monitoring single protein trapping and unfolding shows a tremendous potential for using the double-nanohole as a sensor for protein binding events at a single molecule level. / Graduate

Les nanocavités optiques sur puces sont devenues aujourd'hui des objets de base pour le piégeage et la manipulation d'objets colloïdaux. Nous étudions dans cette thèse des nanocavités comme briques de bases du piégeage et de la manipulation par forces optiques. La preuve de concept du piégeage de microsphères diélectriques apparaît comme le point de départ de l'élaboration d'un laboratoire sur puce. Dans le premier chapitre nous parcourons la bibliographie de l'utilisation des forces optiques en espace libre et en milieu confiné pour le piégeage de particules. Le second chapitre présente les dispositifs expérimentaux pour la caractérisation des nanocavités et les outils mis en place pour les mesures optiques en présence de particules colloïdales. Le troisième chapitre explique la preuve de concept du piégeage de particules de polystyrène de 500 nm, 1 et 2 µm. Dans le chapitre qui suit nous analysons le piégeage de particules en fonction de la puissance injectée dans la cavité. Le chapitre cinq décrit quelques exemples des possibilités de fonctions de manipulation de particules grâce à des cavités couplées. Enfin, dans le dernier chapitre nous montrons les assemblages de particules sur les différents types de cavités étudiées dans cette thèse. / On chips optical nanocavities have become useful tools for trapping and manipulation of colloidal objects. In this thesis we study the nanocavities as building blocks for optical forces, trapping and handling of particles. Proof of concept of trapping dielectric microspheres appears as the starting point of the development of lab on chip. In the first chapter we go through the literature of optical forces in free space and integrated optics. The second chapter presents the experimental tools for the characterization of nanocavities and the set-up developed to perform optical measurements with the colloidal particles. The third chapter describes the proof-of-concept trapping of polystyrene particles of 500 nm, 1 and 2 µm. In the following chapter we analyze the particle trapping as function of the injected power into the cavities. The chapter five gives some examples of the possibilities of particles handling functions with coupled cavities. Eventually, in the last chapter we show assemblies of particles on different geometry of cavities studied in this thesis.

La microscopie en champ proche optique permet d'analyser les phénomènes optiques avec une résolution spatiale sublongueur d'onde comme par exemple la localisation et la propagation de la lumière dans des cristaux photoniques. D'une manière générale, les méthodes de microscopie en champ proche optique reposent sur le positionnement à l'échelle nanométrique d'une sonde locale à proximité de l'échantillon à analyser, puis sur la détection du signal diffusé et collecté lors du balayage de la sonde. En fonction du type de détection optique mise en oeuvre ou du type de sonde utilisée, les grandeurs physiques communément accessibles par ces méthodes sont les distributions spatiales de l'amplitude et de la phase ou de l'intensité des composantes électriques ou magnétiques du champ sondé.Ce travail de thèse est consacré à la mise en place d'une détection hyperstectrale en champ proche optique dans le but de comprendre et de caractériser, à des échelles sublongueurs d'onde, les propriétés spectrales et spatiales de systèmes optiques miniaturisés. L'imagerie hyperstectrale fournit en une seule acquisition, une série d'image à chaque longueur d'onde dans les gammes spectrales visibles, infrarouges et aux longueurs d'onde des télécommunications optiques. Cette nouvelle technique d'imagerie a permis l'observation, sur une large bande spectrale, de phénomènes électromagnétiques dépendant de la longueur d'onde tels que les effets superprisme et mirage dans les cristaux photoniques et la mise en forme de faisceaux de Bessel plasmoniques / The scanning near-field optical microscopy (SNOM) is used to analyze optical phenomena at the sub-wavelength scale such as light localization and propagation in photonic crystals or plasmonic devices. In any case, SNOM experiments rely on the positioning of a local probe in the optical near field of a given structure and on the detection of the surrounding evanescent waves. Depending on the nature of the probe or on the optical detection method, the detected physical properties are the spatial distributions of the amplitude and phase or the intensity of the electric and magnetic components of the probed field. We present here the implementation of an innovative hyperspectral near-field imaging method which aims to detect both spectral and spatial properties of an optical nanosystem at the subwavelength scale. The presented method provides a batch of images over a broad spectral range at visible; near-infrared and telecommunication wavelengths. Using this technique, we report here the near-field observations through the spectrum of the emblematic electromagnetic phenomena involved in photonic crystals and plasmonics such as light waveguiding, trapping or beam shaping

La plasmonique hybride est un sujet d’actualité qui exploite des interactions physiques entre nano-objets métalliques et d’autres nanomatériaux. En bénéficiant des propriétés de chacun de leurs constituants, les nanostructures hybrides sont utilisées dans de nombreuses applications comme la détection d’espèces bio-chimiques. Dans cette thèse, nous présentons une nouvelle nanostructure hybride polymère/metal qui est non seulement utilisée comme nano-émetteur anisotrope qui s’avère aussi être un outil puissant de caractérisation du champ proche optique.La fabrication de cette nouvelle nanostructure est basée sur une approche de par photopolymérisation à l’échelle nanométrique. Cette technique, en comparaison aux méthodes traditionnelles de caractérisation, ne fournit pas seulement l’image de la distribution du champ, mais permet aussi des mesures quantitatives des plasmons de surface avec une résolution sub -5nm, incluant une description fine de la décroissance exponentielle des ondes évanescentes impliquées.A l’aide du mode plasmon dipolaire, une distribution anisotrope de matériau organique est intégrée dans le voisinage de la nanoparticule métallique. Avec une haute concentration de molécules de colorant dans le polymère, l’intensité des signaux de fluorescence et Raman du nano-émetteur hybride dépend de la polarisation incidente. À notre connaissance, il s’agit de la première réalisation d’un nano-émetteur dont le milieu à gain présente une distribution spatiale complexe le rendant sensible à la polarisation / Hybrid plasmonics has given rise to increasing interest in the context of the interaction between metal nano-objects and other materials. By benefiting from each of its constituents, hybrid nanostructures are commonly adopted in studies and optimization of biological and chemical sensors, nanoparticle with high plasmon resonance tunability, and nano-emitters. This PhD thesis presents a hybrid nanostructure of photopolymer/metal nanoparticle that is used as a near-field characterizing tool and as an anisotropic nano-emitter.The fabrication of this hybrid nanostructure is a near-field imprinting process based on nanoscale photopolymerization. This technique, compared with traditional near-field characterization methods, provides not only the image of the field distribution, but also enables quantification of the surface plasmon properties with sub-5nm resolution and reproduction of the exponential decay of the near-field.Under dipolar mode plasmon, the photopolymer was created anisotropically in the vicinity of the metal nanoparticle. With high concentration of dye molecules trapped in the polymer, the hybrid nano-emitter displays surface enhanced fluorescence and Raman signal that is dependent on the incident polarization. To our knowledge, this is the first achievement of the anisotropic nano-emitter based on the inhomogeneous distribution of the active molecule