A comparison of the composition and structure of carbon films deposited by ns and fs laser ablation of graphite is the subject of this thesis. In addition, the effect of irradiation on the surface of graphite has been investigated in detail. Laser-induced phase transitions from graphite to sp-bonded carbon and trans-polyacetylene chains as well as the formation of nano-diamond have been observed after irradiation with fs pulses. An optical orientation mechanism involving both electric and magnetic interactions is proposed to understand the formation of nano-stripes and other structures on irradiated graphite surfaces. These phenomena are not observed after nanosecond laser irradiation. Tetrahedral carbon (ta-C) films deposited at cryogenic temperatures using ns laser radiation consist of sub-micron graphitized grains embedded in a matrix of sp3-hybridized bonded carbon. Nano-buckling is evident in ta-C films deposited by fs ablation where the composition is found to consist of mixed sp, sp2, and sp3 – hybridized carbons species. It is found that the concentration of sp-bonded chains is negligible in ns-C films. Surface enhanced Raman spectroscopy has been used to characterize molecular species in ns and fs carbon films. Time of flight mass spectroscopy has been used to study plume species produced by laser ablation. It is also found that polyyne molecules can be formed by fs laser dissociation of small molecules in organic solvents. This process is accompanied by the deposition of hexagonal nano-diamond films on substrates placed near the laser focus during irradiation. This opens a new path in the synthesis of 1D conducting molecules and nano-diamond materials for nano-science applications. Quantum chemical calculations involving density functional theory (Gaussian '03) have been carried out in support of this work and have been used to study Raman and IR vibrational modes of several novel carbon molecules synthesized in ta-C films and in the liquid phase. These studies have been extended to assist in the identification of astronomical spectra.

A comparison of the composition and structure of carbon films deposited by ns and fs laser ablation of graphite is the subject of this thesis. In addition, the effect of irradiation on the surface of graphite has been investigated in detail. Laser-induced phase transitions from graphite to sp-bonded carbon and trans-polyacetylene chains as well as the formation of nano-diamond have been observed after irradiation with fs pulses. An optical orientation mechanism involving both electric and magnetic interactions is proposed to understand the formation of nano-stripes and other structures on irradiated graphite surfaces. These phenomena are not observed after nanosecond laser irradiation. Tetrahedral carbon (ta-C) films deposited at cryogenic temperatures using ns laser radiation consist of sub-micron graphitized grains embedded in a matrix of sp3-hybridized bonded carbon. Nano-buckling is evident in ta-C films deposited by fs ablation where the composition is found to consist of mixed sp, sp2, and sp3 – hybridized carbons species. It is found that the concentration of sp-bonded chains is negligible in ns-C films. Surface enhanced Raman spectroscopy has been used to characterize molecular species in ns and fs carbon films. Time of flight mass spectroscopy has been used to study plume species produced by laser ablation. It is also found that polyyne molecules can be formed by fs laser dissociation of small molecules in organic solvents. This process is accompanied by the deposition of hexagonal nano-diamond films on substrates placed near the laser focus during irradiation. This opens a new path in the synthesis of 1D conducting molecules and nano-diamond materials for nano-science applications. Quantum chemical calculations involving density functional theory (Gaussian '03) have been carried out in support of this work and have been used to study Raman and IR vibrational modes of several novel carbon molecules synthesized in ta-C films and in the liquid phase. These studies have been extended to assist in the identification of astronomical spectra.

Technological progress in commercializing ultrafast lasers and detectors has allowed realization of cooperative processes on an ultrashort time scale, which demand a re-evaluation of the conventional cooperative phenomena with a new insight. Ultrafast cooperative phenomena in coherently prepared media and various applications of superfluorescence and coherent Raman scattering are studied in this dissertation. In particular, a simple theoretical testimony on analogy between a cooperative emission and coherent Raman scattering is presented by offering an opportunity to perform parallel research on these two processes from a unified point of view. On one hand, the superfluorescent pulse with a time duration of a few tens of picoseconds (ps) from alkali metal vapor is observed for the first time, even though cooperative phenomena in atomic vapor have been extensively studied for more than five decades. A dense rubidium vapor pumped by ultrashort (100 femtosecond, fs) pulses allows a realization of the ultrafast superfluorescence while a time-resolved study of superfluorescence is accomplished by using a streak camera with 2 ps time resolution. Experimental research on quantum nature of cooperative emissions has been “frozen” over the years (three decades) possibly because of the technical difficulties. Quantum fluctuations of superfluorescence development are explored experimentally by taking advantage of the ultra fast streak camera. Presumable applications of the superfluorescent pulse in e.g., a remote sensing, and an ultraviolet upconversion of the input infrared laser pulse are presented. The quantum interference due to different excitation pathways is revealed by the temporal coherent control technique while observing interferometric signals from alkali metal vapors. On the other hand, a new spectroscopic technique based on ultrafast coherent Raman scattering is developed. The key advantage of the presented technique is to suppress the non-resonant background noise which usually obscures possible applications of the other conventional coherent Raman techniques in practice. A reduction of the background noise is achieved by shaping and delaying the third pulse which probes the coherence of the medium (i.e., an enhancement of specific vibrations of the target molecules in unison) firstly prepared by two broadband pulses. We demonstrate a robustness and superiority of signal-to-noise ratio of the developed technique by identifying as few as 10000 bacterial spores at a single laser shot level. Finally, several comparative studies between cooperative and uncooperative processes are presented. A picosecond cooperative phenomenon in a three-photon resonant medium induced by a single as well as two-color ultrashort pulses is investigated. A time-resolved study shows that a picosecond cooperative effect is crucial in the well-established fields of resonant-enhanced multiphoton ionizations and harmonic generations. We also present a quantitative analysis for spontaneous versus broadband coherent Raman scattering on pyridine molecules. The spontaneous Raman signal is enhanced by 5 orders as a result of cooperative phenomena.

Local refractive index changes (RIC) are the building blocks of laser-induced optical functions in bulk transparent materials, where the use of a fused silica as a target material plays a paramount role. Depending on the regime of laser interaction ultra-short pulses can induce positive isotropic refractive index changes (usually denoted as type I) or produce self-arranged nano-scale layered structures resulting in form birefringence (type II). In this thesis we have studied two objectives related to these material transformations. From the one side, we qualitatively determined the effects of the focused ultra-short laser pulses on the fused silica and borosilicate glasses. With the independent control of the energetic dose, pulse duration and focusing conditions, the isotropic type I and birefringent type II traces could be performed with the certain optical properties. Finally, complex polarization sensitive devices were designed and fabricated. From the other side, as these types of RIC have consequences in the functionality and the performances of 3D embedded optical devices, an investigation of the laser-induced structures is particularly useful. We applied photoluminescence and Raman microscopy (RM) to investigate defect formation and glass network reorganization paths. The proposed spectroscopy study distinguishes type I and type II regions by presence and distribution of silicon clusters and non-bridging oxygen hole centers (NBOHC). RM reveals signs of compaction of the glass network in the RIC regions. At the same time, zones with high concentration of NBOHC where no visible RIC and densification signs were detected. Assuming that these zones are precursors of permanent visible modification, we propose a scenario of cold defect-assisted densification realized in type I irradiation regime. This, thereby, revises the densification paths in fused silica

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.

Le développement récent, dans le domaine de la santé, de lasers femtoseconde pompés par diode, délivrant des impulsions de forte énergie et utilisés en chirurgie (en particulier en ophtalmologie), nous amene à chercher de nouveaux domaines d’application dans le secteur de la santé. En effet, la durée très brève de l’interaction laser avec la matière (de l’ordre de 10-15s) et les fortes intensités de radiation délivrées, permettent d’envisager une ablation tissulaire rapide avec des effets thermiques négligeables.Ce travail va un triple objectif:- Etudier la capacité d’ablation de l’émail dentaire et de la dentine avec un laser femto seconde,- Mesurer l’accroissement de température généré par l’interaction laser/tissus avec et sans spray d’air + eau, sachant qu’un accroissement de température au delà de 5.5°C engendre des dommages irréversibles (nécrose) du tissu pulpaire.- Mener une étude comparative de l’adhésion des matériaux de restauration composite sur les surfaces préparées par laser versus l’adhésion sur des surfaces dentinaires préparées de façon conventionnelle avec une fraise et une turbine. / Recent development has led to the commercialization of high power femtosecond lasers, opening a new perspective into the field of laser surgery. Due to the short laser – material interaction time and the very high radiation intensity achieved with this type of laser, the ablation of a wide range of materials can be achieved with negligible thermal effects.The present work aims at- Studying the ablation of dental enamel and dentin by femtosecond laser- Measuring the increase of pulpal temperature generated during the laser treatment without external cooling and with external cooling using an air jet and a combination of the air jet and water irrigation.- Comparing the adhesion of restorative materials to dentin surface treated by the laser and by the conventional drilling method with a burr.

Pour des applications technologiques d’enregistrement magnétique de l’information à haute densité et vitesse d’écriture et de lecture ultra-rapide, les chercheurs se sont penchés vers des méthodes de manipulation de l’aimantation sans application de champ magnétique externe. Il a été découvert qu’il était possible de renverser de manière déterministe l’aimantation de plusieurs matériaux ferri- et ferro-magnétiques à l’aide uniquement d’impulsions laser ultracourtes polarisées circulairement. Ce retournement tout-optique s’est avéré être un processus cumulatif nécessitant plusieurs impulsions ultracourtes dans les matériaux ferromagnétiques. Notamment dans les multicouches (Co/Pt), le retournement tout-optique se fait en deux étapes : une désaimantation indépendamment de l’hélicité suivie d’une ré-aimantation dans une direction ou l’autre selon l’hélicité. Pour autant, le mécanisme à l’origine du rétablissement de l’ordre magnétique n’a pas été étudié jusqu’à présent. Dans cette thèse, nous avons étudié le mécanisme de renversement de l’aimantation dans les couches ferromagnétiques résultant de l’excitation par impulsions laser ultracourtes polarisées circulairement. Pour cela, nous étions intéressé par la réponse d’une paroi de domaine dans les couches minces de Pt/Co/Pt à la suite d’une excitation laser et en fonction de la polarisation de la lumière. Nous avons démontré la possibilité d’induire un déplacement tout-optique et déterministe d’une paroi de domaine. Nous montrons que la propagation de la paroi résulte de la compétition entre trois contributions : le gradient de température dû aux effets de chauffage par le laser, l’effet de l’hélicité de la lumière et les effets de piégeages de la paroi. Par ailleurs, par mesures expérimentales du dichroïsme circulaire, nous excluons un mécanisme purement thermique du déplacement de paroi. Ainsi nous confirmons que le retournement tout-optique des couches ferromagnétiques se fait par une nucléation suivie d’une ré-aimantation par propagation déterministe des parois de domaines selon l’hélicité. De plus, nous avons exploré la possibilité d’utiliser le retournement tout-optique dans des dispositifs spintroniques pour l’enregistrement de l’information à haute densité. Pour se faire, il est nécessaire d’étudier les effets de tailles du retournement lorsque le matériau est structuré en îlots à l’échelle du micro- ou nanomètre. Nous avons montré qu’un plus grand nombre d’impulsions laser est nécessaire afin de renverser l’aimantation de micro-disques comparés à la couche continue ferromagnétique. Il en résulte que le champ dipolaire aide le renversement de l’aimantation dans les couches continues rendant ainsi le retournement tout-optique énergétiquement plus favorable / Over the past decade, the demand for an even higher capacity to store data has been gradually increasing. To achieve ultrafast and ultrahigh density magnetic data storage, low-power methods to manipulate the magnetization without applying an external magnetic field has attracted growing attention. The possibility to deterministically reverse the magnetization with only circularly polarized light was evidenced in multiple ferri- and ferro-magnetic materials. This phenomenon was called helicity-dependent all-optical switching (HD-AOS). In ferromagnets, it was demonstrated that HD-AOS was a cumulative and multishot process with a helicity-independent demagnetization followed by a helicity-dependent magnetization recovery. Yet, the microscopic mechanism of this helicity-dependent remagnetization remained highly debated. In this thesis, we investigated the magnetization reversal mechanism of all-optical switching in ferromagnetic materials. To explore a potential switching process through domain nucleation and domain wall (DW) propagation, we studied the response of a DW upon femto- or pico-second laser irradiation in Co/Pt thin films that exhibit HD-AOS. We reported helicity-dependent all-optical domain wall motion. We demonstrated that it results from the balance of three contributions: the temperature gradient due to the laser heating, the helicity effect and the pinning effects. By measuring the magnetic circular dichroism, a purely thermal mechanism of the laser-induced DW motion appears to be excluded. Furthermore, we examined the size effects in AOS in Co/Pt films patterned into microdots with a diameter between 10 and 3 μm. This allowed us to explore the role of the dipolar field in the switching mechanism. We discovered that a larger number of laser pulses was required to reverse the magnetization of a microdot compared to the continuous film. This indicated that the dipolar field actually eases the magnetization reversal in the full film. Thus, AOS is less energy-efficient in patterned films, hence making Pt/Co/Pt multilayers not an ideal candidate for integrating AOS in spintronic devices

Master of Science / Industrial & Manufacturing Systems Engineering / Shuting Lei / Transparent brittle materials such as glass and silicon dioxide have begun to replace the conventional materials due to the advantageous properties including high strength and hardness, resistance to corrosion, wear, chemicals and heat, high electrical isolation, low optical absorption, large optical transmission range and biocompatibility. However because these materials are extremely hard and brittle, development of an ideal machining process has been a challenge for researchers. Non-traditional machining processes such as abrasive jet and ultrasonic machining have improved machining quality but these processes typically results with issues of poor surface integrity, high tool wear and low productivity. Therefore a machining technique that overcomes the disadvantages of existing methods must be developed. This study focused primarily on improving the machinability and attaining crack-free machined surfaces on transparent brittle materials by inducing micro cracks or seed damages on the subsurface of the materials. The hypothesis was that micro-cracks induced by femtosecond laser would synergistically assist the material removal process by a cutting tool by weakening or softening the material, followed by conventional machining process. Laser induced damages due to varying laser intensities and at different depths in bulk BK7 glass was studied in order to select the optimal laser machining conditions for the experiments. Dimensional and structural profiles of laser cracks are observed using an optical microscope. A comparative study of machined untreated BK7 samples and damage induced BK7 samples was conducted. Due to its simple process kinematics and tool geometry, orthogonal machining is used for the study. Results showed that machining laser-treated samples caused an average 75% force reduction on comparison to machining of untreated samples. Laser treated machined samples were produced without subsurface damages, and reduced tool wear was noted. Overall improved machinability of BK7 glass samples was achieved.

L’avènement des technologies lasers femtoseconde utilisant une fibre optique comme milieu amplificateur incite les industriels à se renseigner sur cette technologie. Dans ce contexte, et dans le cadre du projet Futures et Ruptures, cette thèse se propose de caractériser une nouvelle source femtoseconde, le Tangerine d’Amplitude Systèmes. Utilisant les capacités de ce laser, et avec la collaboration d’IREPA LASER, nous feront une étude comparative avec les lasers femtoseconde déjà existant en s’appuyant sur l’état de l’art, l’optique non-linéaire et quelques simulations d’ablation. L’amélioration des procédés d’usinage pour des applications industrielles nous permettra de modifier et compléter nos connaissances dans l’usinage de différents matériaux tout en montrant les qualités de cette nouvelle technologie. Enfin, une application de miniaturisation de dispositifs électronique pour le domaine du biomédical nous permettra d’utiliser toutes les connaissances acquises et de mener à bien ce projet. / Surgical procedures are moving increasingly toward minimally invasive techniques because these techniques offer great comfort to the patient, a short recovery time and are reasonably-priced. As part of this thesis, it is proposed to study the integration of micrometer-sized sensors directly into needles for example. The PhD student will study the process of laser-matter interaction for new nano and femtosecond sources which should be optimized in order to develop a machining technique of surgical instruments in order to incorporate the sensors. The aim of the thesis is the demonstration of the feasibility of developing the technique of laser etching for the integration of sensors into millimeter-sized needles as well as tests in real conditions. Multiple lasers will be used; The Tangerine laser from ‘Amplitude Systèmes’ with the well know Ti:Sa laser. His work there will be to upgrade the laser up to its best capacity both in terms of fluence or accuracy and in terms of software and its ease of use. The ablation of the silicon from the rear of the electronic chip to the edge of the photodetector in order to carry the light and energy supply all 3D Hall effects micro-magnetors will be the main purpose of the PhD student. He will highlight differences between two femtosecond laser as thermally affected area or ablation rate and will choose which one is able to achieve our goal.

The development and transition of optical fiber sensors from experimental stage to practical applications largely depends on manufacturing cost and simplicity. To date, in-fiber grating sensors are largely manufactured by ultraviolet lasers despite higher fabrication cost and complexity. Besides, ultraviolet radiation can only write gratings in doped fibers. Therefore, reaping the benefits of existing fibers such as pure silica fiber, photonics crystal fibers etc. cannot be achieved using this technique. In contrast, uses of ultra-fast lasers have the potential to eliminate or minimize those drawbacks. However, extensive fabrication and packaging research is required for ultrafast laser technology to mature and offer grating based sensors fabrication in industrial scale. This dissertation presents design and fabrication of fiber optic sensors using femtosecond laser for measurement of ambient refractive index and temperature. The femtosecond laser operating at 780 nm with pulse duration of 172 fs and pulse repetition rate of 1 kHz is used to study bulk index modification and fabricate fiber long period and short period gratings. Effective and reliable fabrication of in-fiber gratings requires spatial control of refractive index written in optical fiber. With an aim to better control spatial index modulation in direct ultrafast writing, primary focus of this work is given to write single-shot submicron periodic voids in bulk glass. Femtosecond pulse filamentation in glass is studied to understand the morphology of bulk index change written by ultrashort pulses. Laser writing parameters (such as beam diameter, pulse energy, scanning speed, depth of focus, etc.) are then further tuned to write pulse filamentation induced refractive index change in optical fibers suitable for fiber grating fabrication. In order to design and tailor grating’s spectrum, measurement of in-fiber index is introduced in this work. We propose fiber Bragg grating based Fabry-Perot cavity structure (cavity length, L= 10 mm) to characterize femtosecond pulse filamentation induced refractive index change in the core of standard SMF. In addition, Mach-Zehnder interferometer (MZI) is proposed as an alternative yet effective and low cost tool to measure in-fiber index change. Comsol simulation is used to validate the quantification of index change. Measured index change is used in Optiwave simulation to design fiber long period gratings in standard telecommunication and pure silica core fibers. To increase fabrication reliability, we introduce inscription of helical long period gratings using a custom made rotary stage. Tapered photonic crystal and microfiber based Mach-Zehnder interferometer is also investigated for ambient refractive index measurement. Miniature fiber Bragg grating written in microfiber Mach-Zehnder interferometer is used in this work for multi-parameter sensing as well as temperature compensated refractive index sensing. Microfiber Bragg gratings buried in materials of higher thermal expansion coefficient is also proposed to significantly enhance temperature sensitivity. / Graduate / 0548, 0794, 0775 / fariduvic@gmail.com