Photomasks are the backbone of microfabrication industries. Currently they are fabricated by lithographic process, which is very expensive and time consuming since it is a several step process. These issues can be addressed by fabricating photomask by direct femtosecond laser writing, which is a single step process and comparatively cheaper and faster than lithography. In this paper we discuss about our investigations on the effect of two types of laser writing techniques, namely, front and rear side laser writing with regard to the feature size and the edge quality of the feature. It is proved conclusively that for the patterning of mask, front side laser writing is a better technique than rear side laser writing with regard to smaller feature size and better edge quality. Moreover the energy required for front side laser writing is considerably lower than that for rear side laser writing. / Singapore-MIT Alliance (SMA)

For the past decade, the epoxy based photoresist SU-8 has been used commercially and in the lab for fabricating micro- and nano-structures. Investigators have studied how processing parameters such as pre- and post-exposure bake temperatures affect the resolution and quality of SU-8 structures patterned using ultraviolet or x-ray lithography. Despite the advances in understanding the phenomena, not all of them have been explored, especially those that are specific to multi-photon direct laser writing (mpDLW). Unlike conventional exposure techniques, mpDLW is an inherently three-dimensional (3D) process that is activated by nonlinear absorption of light. This dissertation reports how several key processing parameters affect mpDLW using SU-8 including pre-exposure bake duration, focal depth, incident laser power, focal-point scan speed, and excitation wavelength. An examination of solvent content of films at various stages in the mpDLW by 1H-NMR shows that even moderate solvent content (over 1 wt-%) affects film viscosity and photoacid diffusion lengths, and can greatly affect the overall fidelity of small features. A study of micro-fabricated feature size versus writing depth in the material shows that even slight refractive index mismatch between SU-8 and the medium between it and the focusing objective introduces spherical aberration that distorts the focus, causing feature size to decrease or even increase in size with writing depth, depending on the average exposure power used. Proper adjustment of the average exposure power was demonstrated as a means to fabricate more uniform features with writing depth. Third, when varying the power and scan speed, it was observed that the feature-size scales with these two parameters in a manner that is consistent with a three-photon absorption mechanism at an excitation wavelength of 800 nm. When an iii excitation wavelength of 725 nm is used, the feature-size scaling becomes consistent with that of two photon absorption. This shows that the photoinitiators in the SU-8 can be activated by either two- or three-photon absorption over this wavelength range. Using an irradiance of ~2 TW cm-2 and elongated femtosecond pulses resulted in an observed fourth order power dependence. This observation is in agreement with the literature and suggests that the effective absorptive nonlinearity is also sensitive to pulse duration. These findings will be useful for creating accurate models of the process of mpDLW in SU-8. These models could be used to optimize the processing parameters and develop new processing methods and materials for high-resolution fabrication of robust 3D microstructures. Some of the findings were used to develop a method for fabricating functional microlenses on the tip of optical fibers. This approach opens a new route to functional integrated photonic devices.

L’inscription par laser femtoseconde directe dans les cristaux laser offre une nouvelle opportunité de conception et développement de sources laser intégrées. Elle conduit à un prototypage rapide et à un bon rapport coût-efficacité, conformément aux futures feuilles de route de la photonique. Cependant, les défis liés au dépôt d’énergie d’un laser intense dans des milieux transparents et les modifications qui s’ensuivent restent encore des questions ouvertes. Ces défis ont été relevés en partie grâce à une étude minutieuse et systématique des zones modifiées par laser femtoseconde dans les matériaux transparents. Le fluorure de calcium (CaF2), en raison de sa symétrie cubique et de ses excellentes propriétés de luminescence en tant que cristal laser, a été choisi comme matériaux de référence dans cette thèse. L’inscription laser en régime femtoseconde de guides d’ondes à l’intérieur de ce cristal a été réalisée pour une conception future de source laser intégrée. Pour la première fois, des écritures laser « lisses » et non réciproques ont été observées à l’intérieur de certains échantillons « coupés spécialement » de cristaux de CaF2. De plus, un guidage de la lumière dépendant de la polarisation a été identifié et est présenté. Un modèle et une méthode ont été développés pour caractériser quantitativement et qualitativement ces guides d’ondes, en particulier pour les mesures de perte de transmission, ainsi que les cartographies tridimensionnelles de l’indice de réfraction des zones modifiées. / Femtosecond laser micromachining inside laser crystals offers a new platform to miniaturize highly compact laser sources. It leads to rapid prototyping and cost-effectiveness in line with the future photonics roadmaps. However, the challenges in relation to an intense laser pulse energy deposition within transparent media and the modifications that follow still remain open-ended questions. These challenges have been addressed with a careful and systematic study of femtosecond modified zones inside transparent materials. Due to its cubic symmetry and excellent luminescence properties as laser crystal, Calcium Fluoride (CaF2) was selected, and ultrafast laser inscription of waveguides inside this crystal was realized. Smooth and non-reciprocal writings were observed inside certain “specially cut” samples of the CaF2 crystals for the first time. Additionally, polarization dependent guiding is identified and presented. Furthermore, an authentic model and concept was engaged for the quantitative and qualitative characterization of the waveguides, particularly for the transmission loss measurements and the three-dimensional refractive index mappings of the modified zones.

This dissertation describes methodology that significantly improves the state of femtosecond laser writing of metals. The developments address two major shortcomings: poor material quality, and limited 3D patterning capabilities. In two dimensions, we grow monocrystalline silver prisms through femtosecond laser irradiation. We thus demonstrate the ability to create high quality material (with limited number of domains), unlike published reports of 2D structures composed of nanoparticle aggregates. This development has broader implications beyond metal writing, as it demonstrates a one-step fabrication process to localize bottom-up growth of high quality monocrystalline material on a substrate. In three dimensions, we direct laser write fully disconnected 3D silver structures in a polymer matrix. Since the silver structures are embedded in a stable matrix, they are not required to be self-supported, enabling the one-step fabrication of 3D patterns of 3D metal structures that need-not be connected. We demonstrate sub-100-nm silver structures. This latter development addresses a broader limitation in fabrication technologies, where 3D patterning of metal structures is difficult. We demonstrate several 3D silver patterns that cannot be obtained through any other fabrication technique known to us. We expect these advances to contribute to the development of new devices in optics, plasmonics, and metamaterials. With further improvements in the fabrication methods, the list of potential applications broadens to include electronics (e.g. 3D microelectronic circuits), chemistry (e.g. catalysis), and biology (e.g. plasmonic biosensing). / Engineering and Applied Sciences

This thesis explores a novel methodology to fabricate three dimensional (3D) metal-dielectric structures, and two dimensional (2D) graphite layers for emerging metamaterials and graphene applications. The investigations we report here go beyond the limitations of conventional fabrication techniques that require multiple post-processing steps and/or are restricted to fabrication in two dimensions. Our method combines photoreduction mechanism with an ultrafast laser direct writing process in innovative ways. This study aims to open the doors to new ways of manufacturing nanoelectronic and nanophotonic devices. With an introductory analysis on how the various laser and chemical components affect the fabrication mechanism, this dissertation is divided into three sections. / Engineering and Applied Sciences

Ce travail porte sur l’étude d’une nouvelle technique de microscopie basée sur le phénomène d’absorption linéaire ultra-faible (LOPA) de matériaux photosensibles pour la fabrication de structures submicrométriques à deux et à trois dimensions (2D, 3D). Premièrement, nous avons étudié théoriquement la distribution de l'intensité lumineuse dans la région focale d’un objectif de microscope de grande ouverture numérique en fonction des différentes conditions de travail, telles que la propagation de la lumière dans un milieu absorbant avec variation d'indice de refraction. Nous avons démontré que lorsque l'on travaille avec un matériau quasi homogène ayant de très faible absorption à la longueur d’onde du faisceau d’excitation, le faisceau laser peut être focalisé en profondeur à l'intérieur du matériau, ce qui permet de manipuler optiquement des objets en 3D. Nous avons ensuite démontré expérimentalement l'utilisation de cette technique pour fabriquer des structures à la demande. Différentes structures 2D et 3D submicrométriques ont été crées en résine SU-8, en utilisant un laser continue de faible puissance à 532 nm. Ces résultats sont similaires à ceux obtenus par la méthode d’absorption à deux photons, mais le coût de fabrication a été énormément réduit. De plus, nous avons démontré qu'il est possible de fabriquer des structures photoniques à base de polymère contenant une seule nanoparticule (NP), en utilisant un procédé à deux étapes. En effet, nous avons d'abord déterminé avec précision la position d'une seule NP d’or, en utilisant une puissance d’excitation très faible, puis nous l'avons insérée dans une structure photonique par une puissance d’excitation plus élevée. Le couplage d'une NP d’or et d'une structure photonique à base de polymère a été ensuite étudié théoriquement et expérimentalement, montrant une amélioration importante de la collection des photons émis par la NP. / This work deals with a novel microscopy technique based on the ultra-low one-photon absorption (LOPA) mechanism of photosensitive materials for fabrication of arbitrary two- and three-dimensional (2D, 3D) submicrometer structures. First, we theoretically investigated the intensity distribution at focusing region of a high numerical aperture objective lens as a function of various working conditions, such as propagation of light mismatched refractive index and/or absorbing media. We demonstrated that when working with refractive index mismatch-free and very low absorption conditions, the light could be focused deeply inside the material, allowing a 3D optical manipulation. We then demonstrated experimentally the use of this simple technique for fabrication of desired structures. Different 2D and 3D structures, with a feature as small as 150 nm, have been created in SU-8 photoresist by using a low power and continuous-wave laser emitting at 532 nm. Furthermore, we demonstrated that it is possible to fabricate a polymer-based photonic structure containing a single nanoparticle (NP), by using a double-step method. Indeed, the LOPA microscopy allowed us first to accurately determine the location of a single gold NP and then to embed it as desired into an arbitrary SU-8 photonic structure. The coupling of a gold NP and a polymer-based photonic structure was theoretically and experimentally investigated showing a six-fold photons collection enhancement as compared to that of a NP in unpatterned film.

Topological states in photonic systems are described by qualitative discrete quantum numbers and feature unique combinations of properties such as robustness to perturbations and dissipationless surface transport of energy and information. Due to the many easily accessible platforms in photonics, topological photonics is one of the spearheads of topological physics that has offered exciting possibilities for investigations of novel topological phenomena and numerous promising technological uses. This master thesis aims at investigating from a theoretical and experimental perspective the properties of topological states of interacting light modes in arrays of coupled waveguides. First, we present a review of recent advances in the recently emerged field of topological physics. Then we review recent work on lattice models that feature topological edge states, and subsequently, we identify the existence of robust corner states on the edge of honeycomb lattices. These states display, similarly to the corner states known in 1D SSH and 2D Kagome lattices, exponential localisation with naturally occurring total destructive interference. Additionally, the corner states share properties with the dynamic transport modes of photonic Floquet topological insulators. However, the origin of the corner localisation is different from the previously studied examples: instead of dimerised coupling strength, the asymmetric and dimerised number of neighbours in the direction of the corner generates the intensity gradient. Motivated by our numerical study, we outline an experimental realisation of the novel honeycomb corner states, by means of waveguide lattices written in glass. The waveguides are 3D written in the bulk of a glass sample, with the lattice pattern orthogonal to the main direction of propagation which acts as a time coordinate in the experiments. Femtosecond direct laser writing enables fabricating truly 3D waveguides. Our experimental preparations cover a study of the effects of fabrication parameters for the relevant structures. We discuss how the localisation and robustness properties of the honeycomb corner states would next be investigated in the prepared experimental setting. / Topologiska tillstånd i fotoniska system beskrivs av särskilda topologiska diskreta kvanttal och har unika kombinationer av egenskaper såsom robusthet mot fluktuationer och förlustfri yttransport av energi och information. Tack vare de många lättillgängliga plattformarna inom fotonik är topologisk fotonik en av spjutspetsarna inom topologisk fysik och har erbjudit unika möjligheter för undersökningar av nya topologiska fenomen och med många lovande tekniska användningsområden. Denna masteruppsats syftar till att undersöka, ur ett teoretiskt och experimentellt perspektiv, egenskaperna hos topologiska tillstånd av interagerande ljusmoder i gitter av kopplade vågledare. Först presenterar vi en översikt av de senaste framstegen inom det nyligen uppkomna området topologisk fysik. Sedan sammanfattar vi det senaste arbetet med gittermodeller som har topologiska kanttillstånd, och därefter identifierar vi förekomsten av robusta hörntillstånd på kanten av bikakegitter. Dessa tillstånd uppvisar, på samma sätt som hörntillstånden som är kända i 1D SSH- och 2D Kagome-gitter, hög kantlokalisering med naturligt förekommande total destruktiv interferens. Dessutom delar hörntillstånden egenskaper med de kända fotoniska Floquet-topologiska isolatorerna som uppvisar topologisk transport. Ursprunget till hörnlokaliseringen skiljer sig dock från de tidigare studerade exemplen: istället för en dimeriserad kopplingsstyrka genererar det asymmetriska och dimeriserade antalet grannar i hörnets riktning intensitetsgradienten. Med motivering i den numeriska studien inleder vi en experimentell realisering av de nya bikakehörntillstånden, med hjälp av vågledargitter skrivna i glas. Vågledarna är 3D-skrivna på insidan av ett glasprov, med gittermönstret ortogonalt mot huvudutbredningsriktningen som fungerar som en tidskoordinat i experimenten. Direkt laserskrivning med femtosekundlaser gör det möjligt att tillverka vågledare i tre dimensioner. Våra experimentella förberedelser omfattar en studie av effekterna av tillverkningsparametrar för de relevanta strukturerna. Vi diskuterar hur lokaliserings- och robusthetsegenskaperna för bikakehörntillstånden sedan skulle undersökas med den experimentella metoden.

A la suite de la première démonstration de l'écriture de guide d'onde au sein de verres en 1996 par laser femtoseconde, l'écriture direct par Laser Femtoseconde (Femtoseconde Direct Laser Writing - FLDW) est apparu comme une technique souple pour la fabrication de structure photonique en trois dimensions au sein de matériaux pour l'optique. La thèse a porté sur l'inscription par laser femtoseconde de fonctionnalités optiques au sein de verres. Des éléments diffractifs par modification de l'indice de réfraction et des structures présentant des propriétés de luminescence ou d'optique non linéaire d'ordre deux ont pu être obtenus au sein de matériaux vitreux et étudiés. / Since the first demonstration of femtosecond laser written waveguides in 1996, femtosecond laser direct writing (FLDW) has been providing a versatile means to fabricate embedded 3-D microstructures in transparent materials. The key mechanisms are nonlinear absorption processes that occur when a laser beam is tightly focused into a material and the intensity of the focused beam reaches the range creating enough free electrons to induce structural modification. This dissertation was an attempt to make an improvement on the existing FLDW technique to achieve a reliable fabrication protocol for integrated optical devices involving micro diffractive optical elements and laser-structures exhibiting second order nonlinear optical properties. Relaxation processes of directly-written structures in chalcogenide glasses have been also investigated.

Printing of 3-dimensional nanostructures with high-resolution by two-photon polymerization has gained significant attention recently. Isopropyl thioxanthone (ITX) has been studied and used as a photoinitiator because of its unique property in initiating and depleting polymerization, but to further improve the resolution of 3D structures, new photoinitiating materials are necessary to decrease the power requirements especially in industrial world. In this dissertation, different new types of thioxanthone-based photoinitiators were synthesized and our new initiators possessed a clear enhancement in terms of excitation over ITX. To clearly reveal the writing mechanism behind it, the behavior of the initiators was evaluated by several methods such as low temperature phosphorescence spectroscopy and density functional theory (DFT) calculations. The first type of new molecules with alkyne bridge will be discussed in chapter 2 and the further developed initiators with electron donating and withdrawing groups will be discussed in chapter 3. By modifying the structure of ITX, we have revealed and proposed an important pathway to guide future development of photoinitiators in direct laser writing.

L'inscription laser directe est un domaine de recherche en croissance depuis ces deux dernières décennies, fournissant un moyen efficace et robuste pour inscrire directement des structures en trois dimensions (3D) dans des matériaux transparents tels que des verres en utilisant des impulsions laser femtosecondes. Cette technique présente de nombreux avantages par rapport à la technique de lithographie, qui se limite à la structuration en deux dimensions (2D) et implique de nombreuses étapes de fabrication. Cela rend la technique d’inscription laser direct bien adaptée aux nouveaux procédés de fabrication. Généralement, l’inscription laser dans les verres induit des changements physiques tels qu'un changement permanent de l'indice de réfraction localisé. Ces modifications ont été classés en trois types distincts : (Type I, Type II et Type III). Dans ce travail, nous présentons un nouveau type de changement d'indice de réfraction, appelé type A qui est basé sur la création d’agrégats d'argent photo-induit. En effet, dans des verres dans lesquels sont incorporés des ions argent Ag+, lors de leurs synthèses, l’inscription laser directe induit la création d’agrégats d’argent fluorescents Agmx+ au voisinage du voxel d’interaction. Ces agrégats modifient localement les propriétés optiques comme : la fluorescence, la non-linéarité et la réponse plasmonique du verre. Ainsi, différents guides d'ondes, un séparateur de faisceau 50-50, ainsi que des coupleurs optiques ont été inscrits en se basant sur ce nouveau Type A et complétement caractérisés. D'autre part, une étude comparative entre les deux types de guides d'ondes (type A et type I) est présentée, tout en montrant qu’en ajustant les paramètres laser, il est possible de déclencher soit le Type I soit le Type A. Enfin, en se basant sur des guides d’ondes de type A inscrits proche de la surface du verre, un capteur d'indice de réfraction hautement sensible a été inscrit dans une lame de verre de 1 cm de long. Ce capteur miniaturisé peut présenter deux fenêtres de détection d’indice, ce qui constitue une première mondiale. Les propriétés des guides d'ondes inscrits dans ces verres massifs ont été transposées à des fibres en forme de ruban, du même matériau contenant de l'argent. Les résultats obtenus dans ce travail de thèse ouvrent la voie à la fabrication de circuits intégrés en 3D et de capteurs à fibre basés sur des propriétés optiques originales inaccessibles avec des guides d’onde de Type I standard. / Direct Laser Writing (DLW) has been an exponentially growing research field during the last two decades, by providing an efficient and robust way to directly address three dimensional (3D) structures in transparent materials such as glasses using femtosecond laser pulses. It exhibits many advantages over lithography technique which is mostly limited to two dimensional (2D) structuring and involves many fabrication steps. This competitive aspect makes the DLW technique suitable for future technological transfer to advanced industrial manufacturing. Generally, DLW in glasses induces physical changes such as permanent local refractive index modifications that have been classified under three distinct types: (Type I, Type II & Type III). In silver containing glasses with embedded silver ions Ag+, DLW induces the creation of fluorescent silver clusters Agmx+ at the vicinity of the interaction voxel. In this work, we present a new type of refractive index change, called type A that is based on the creation of the photo-induced silver clusters allowing the creation of new linear and nonlinear optical waveguides in silver containing glasses. Various waveguides, a 50-50 Y beam splitter, as well as optical couplers, were written based on type A modification inside bulk glasses and further characterized. On the other hand, a comparison study between type A and type I waveguides is presented, showing that finely tuning the laser parameters allows the creation of either type A or type I modification inside silver containing glasses. Finally, based on type A near-surface waveguides, a highly sensitive refractive index sensor is created in a 1 cm glass chip, which could exhibit a pioneer demonstration of double sensing refractive ranges. The waveguiding properties observed and reported in the bulk of such silver containing glasses were transposed to ribbon shaped fibers of the same material. Those results pave the way towards the fabrication of 3D integrated circuits and fiber sensors with original fluorescent, nonlinear and plasmonic properties that are not accessible using the standard type I modification