Cette thèse étudie l'interaction de nanopointes avec des impulsions laser ultracourtes pour observer l'émission photo-assistée d'électrons. Plusieurs mécanismes physiques entrent en jeu, chacun ayant une signature unique identifiable dans le spectre d'énergie des électrons. Nous avons développé une nouvelle expérience pour observer et identifier ces mécanismes d'émission. Ceci inclut le développement complet d'un système laser flexible (notamment un amplificateur optique non colinéaire (NOPA) haute cadence), une chambre ultra-vide avec détecteur d'électrons (mesure de spectre d'électrons et carte 2D de l'émission) et un dispositif de nanopositionnement de la pointe dans le foyer du laser, et enfin la fabrication et caractérisation de pointes diverses (en collaboration avec les laboratoires CEMES (Toulouse) et GPM (Rouen)). Nous avons observé l'émission photo-induite d'électrons à partir de nanopointes de différents matériaux (tungstène, argent, et une nouvelle pointe formée autour d'un nanotube de carbone unique). Nous avons confirmé l'observation de pics ATP (signature de la photoémission au dessus du seuil) sur une pointe de tungstène. Nous avons détecté la première émission induite par laser à partir de nanocône de carbone unique. Enfin, nous avons observé un plateau dans le spectre d'énergie des électrons d'une pointe d'argent, signature de la recollision et rediffusion des électrons sur la pointe. Pour identifier et caractériser ces mécanismes, des études variées ont été faites en fonction de la tension appliquée sur la pointe, du taux de répétition du laser, de sa polarisation, de sa puissance et de sa longueur d'onde. En étudiant la forme du spectre des photoélectrons, nous avons pu extraire des informations sur l'interaction: le facteur d'amplification du champ laser proche de la nanopointe et la probabilité d'absorption d'un photon au dessus du seuil. / This thesis concerns the interaction of a sharp nanotip with an ultrashort laser pulse for the observation of emission of photoelectrons. An electron can be emitted from a sharp nanotip system by many different mechanisms. Each mechanism gives a unique signature that can be identified by the photoelectron energy spectrum. We developed a new experiment to observe and identify these emission mechanisms. This consists of a flexible laser system (including the development of a high repetition rate, variable repetition rate noncollinear optical parametric amplifier (NOPA)), ultra high vacuum chamber, electron detector (electron spectrometer with 2D resolution), nanopositioning of a sharp nanotip in the focus of the laser, and fabrication of these nanotip samples in a variety of materials (in collaboration with CEMES (Toulouse) and GPM (Rouen)). We observed the emission of photoelectrons from various nanotips based on different materials: tungsten, silver, and a new type of carbon-based nanotip formed around a single carbon nanotube. We confirm the observation of above threshold photoemission (ATP) peaks from a tungsten nanotip. We detected the first laser induced electron emission from a carbon cone based on a single carbon nanotube. We observed a plateau in the electron spectra from a silver nanotip, the signature of electron recollision and rescattering in the tip. Various studies were performed in function of the voltage applied, repetition rate of the laser, laser polarization, energy and wavelength of the laser in order to understand these phenomena. From spectral features we were able to extract information about the system such as the enhancement factor of the laser electric field near the nanotip and the probability of above threshold photon absorption. Comparisons of the various spectra observed allowed us to spectrally identify the mechanisms for photoemission for tip based systems.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21569号 / 理博第4476号 / 新制||理||1642(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)准教授 橋田 昌樹, 教授 阪部 周二, 教授 鶴 剛 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

No description available.

京都大学 / 新制・課程博士 / 博士(工学) / 甲第23388号 / 工博第4880号 / 新制||工||1763(附属図書館) / 京都大学大学院工学研究科材料化学専攻 / (主査)教授 三浦 清貴, 教授 田中 勝久, 教授 藤田 晃司 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第20706号 / 工博第4403号 / 新制||工||1684(附属図書館) / 京都大学大学院工学研究科材料化学専攻 / (主査)教授 三浦 清貴, 教授 田中 勝久, 教授 作花 哲夫 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM

Femtosecond lasers deliver a high peak concentration of optical power while maintaining low average power. With an accompanying optical setup, this power can be focused and used for high-precision fabrication of metallized polymers via ablation, creating conductive structures on a thin film. These lasers can also be harnessed in tandem with hydrofluoric acid and the two-photon absorption principle to selectively etch silicon carbide, a very durable and machining-resistant semiconductor with desirable properties. This thesis presents improvements made to the Laser-Assisted Chemical Etching (LACE) technique and the ablation system. ��, the two- photon absorption coefficient of silicon carbide, is measured and characterized for each wafer using an optical system. The LACE etch rate of silicon carbide is found to be on average a quarter of a micrometer per 120 seconds. A new destructive imaging technique for characterizing high- aspect-ratio through-wafer non-line-of-sight features in silicon carbide is discussed, with the result of an SEM image of a LACE feature that was impossible to achieve previously. The photolithography process necessary to make use of those through-wafer features is explored. A method of leveraging image processing to maintain the focus of the laser close to the machined sample is explained, resulting in the creation of terahertz metal- mesh filters with a near one-hundred-percent success rate. It is recommended that future work explore the use of an installed confocal microscopy as a method of surface-tracking and result characterization.

No description available.

This dissertation expounds growing insight of the electrospray droplet ionization mechanism following ablation of dried hydrophobic and hydrophilic molecules using femtosecond laser pulses and mass analysis of the gas phase ions. Both hydrophobic and hydrophilic molecules were laser vaporized into an electrospray solvent opposite in polarity revealing appreciable ion intensity for all samples in contrast to ESI-MS and DESI measurements were solubility of the analyte in the spray solvent is a prerequisite. Quantitative analysis of equimolar protein solutions was established using LEMS reporting over three decades of quantitave response with little evidence of ion suppression. In contrast, ESI-MS measurements of similar equimolar protein solutions revealed severe ion suppression eliminating ion current from one of the protein analytes. Finally, the nature of an analyte following nonresonant laser vaporization has been the subject of debate. Aqueous trypsin was laser vaporized into an electrospray solvent containing either buffer or acid with substrate. LEMS measurements using buffer revealed enzyme-substrate intermediate charge states and continued enzymatic activity while the lack of enzyme-substrate intermediates and stymied enzymatic activity observed using acid suggests nonresonant laser vaporization preserves solution phase structure. This dissertation also extends considerably the use of LEMS for identification and characterization of energetic materials in their pre- and post-blast forms without sample preparation. The use of mulivarate analysis for the classification of large sample sets was also demonstrated showing high fidelity assignment of commercial formulations to their manufacturer. Five unburnt smokeless powders investigated using LEMS revealed unique combinations of organic molecules such as stabilizers and plasticizers using a simple electrospray solvent. Principal component analysis (PCA) provided exact classification of the mass spectra with respect to the manufacturer of the ordinance. LEMS measurements were then obtained from five commercial gunshot residue samples, or post-blast smokeless powder, revealing trace amounts of organics such as the stabilizers and large quantities of inorganic barium originating from the primer. Principal component analysis (PCA) again provided exact classification of the gunshot residue mass spectra with respect to the manufacturer of the ordinance. The use of a common transition metal complexation agent enabled full characterization of eight gunshot residue samples to include the heavy metals contained in the primer and the organics such as the stabilizers and plasticizers without any sample preparation or pre-concentration procedures. Principal component analysis (PCA) again provided high fidelity classification of the gunshot residue mass spectra with respect to the manufacturer of the ordinance after mass analysis with LEMS. Finally, highly energetic formulations such as composition 4 (C-4) and detonation cord subjected to nonresonant femtosecond laser vaporization enabled full characterization of these complex compositions identifying binders, stabilizers, the explosive ingredient and age-related decomposition derivative signature molecules with appreciable ion current detected using both positive and negative ion modes. / Chemistry

<p> Lithium niobate is an important photonic material that has potential applications in MEMS. Unfortunately, it is difficult to process using conventional methods. This thesis is an exploratory study to determine the viability of using a femtosecond laser as a fabrication tool for lithium niobate. Unexpectedly, a rich range of behaviour, likely arising from the complex material structure and composition, was discovered. Depending on the processing conditions, it was demonstrated that machining can either result in deep, high-aspect ratio grooves with minimal surrounding damage or dramatic modification of the lithium niobate to great depths with very little material removal.</p> <p> When machining grooves, increasing the effective number of pulses Neff (i.e. decreasing cutting speed) gave rapidly increasing ablation depths until a threshold was reached, after which the grooves were nearly filled with amorphous material. The depth of these amorphous channels rapidly saturates and becomes nearly independent of Neff. The ablation depth dependence on fluence showed gentle and strong ablation regimes. The amorphous channel depth depended almost linearly on fluence. Subsequent laser passes over amorphous channels eventually removed the amorphous material from the groove, indicating a dependence on the time between laser pulses. Crystal orientation was not a factor.</p> <p> The results are understood in terms of incubation and wave guiding. The first pulses ablate some material and incubate a channel of material below the surface. With further pulses, increasing incubation accelerates ablation. At the threshold Neff, the absorption coefficient has increased enough that the next pulse is able to melt a significant amount of material, which expands to fill the groove. It is suggested that, initially, the amorphous material is able to guide subsequent pulses to the bottom of the channel, resulting in a very slowly increasing depth with Neff. Subsequent passes cause ablation once again since compositional changes in the amorphous material have relaxed. Irradiated samples appear thermally reduced, which would create colour centres leading to increased absorption and thus incubation.</p> <p> Femtosecond lasers are indeed able to create MEMS structures. Multiple passes in the ablation regime yielded deep grooves, with laser polarization perpendicular to the groove giving the best results. Fabrication of micro-cantilevers and bridges was demonstrated.<p> / Thesis / Master of Applied Science (MASc)

Thesis (MSc)--Stellenbosch University, 2012. / ENGLISH ABSTRACT: Terahertz radiation is currently used in security, information and communication technology (ICT), and biomedical sciences among others. The usability of terahertz (THz) radiation, in many of its applications depends on characteristics of the materials being investigated in the THz range. At the heart of THz usage is a THz spectroscopy system necessary for the generation and detection of the THz radiation. In this thesis, we characterise such a THz spectroscopy system. In our typical THz spectrometric system, we make use of femtosecond (fs) laser technology and pump-probe principles for emission and detection of THz radiation. Background about the principles of generation THz radiation using fs triggered antennas and the principles of the spectroscopy technique and appropriate literature references are presented. Using an assembled commercially available kit, we reproduce known spectra in order to confirm correct functionality (for calibration) of the assembled spectroscopy system and to gain experience in interpreting these spectra. By introducing a suitable x - y scanning device we construct a crude THz imaging device to illustrate the principle. / AFRIKAANSE OPSOMMING: Terahertsstraling word deesdae wyd in die sekuriteits, inligting-en-kommunikasie en biomediese sektore aangewend. Die gepastheid van terahertsstraling (THz) vir ’n spesifieke toepassings hang af van die eienskappe van die materiale wat ondersoek word. Vir die uitvoer van sulke eksperimente word ’n THz-spektroskopie sisteem benodig vir die opwekking en meting van THz-straling. In hierdie tesis word so ’n THz-spektroskopie sisteem beskou en gekarakteriseer. In die sisteem word van ’n femtosekondelaser (fs) gebruik gemaak in ’nn pomp-en-proef opstelling vir die uitstraling en meting van THz-straling. Die beginsels rakende die opwekking van THz-straling, deur gebruik te maak van ’n antenna wat deur ’n fs-laser geskakel word, asook die beginsels van die spektroskopiese tegniek, met toepaslike verwysings, word in die tesis aangebied. Deur gebruik te maak van’n kommersiële THz opstelling is bekende spektra gemeet om die korrekte funksionering (vir kalibrasie doeleindes) na te gaan en om ondervinding op te doen in die interpretasie van hierdie spektra. ’n X-Y-translasie toestel is tot die opstelling bygevoeg om THz-afbeelding moontlik te maak en sodoende hierdie beginsel te illustreer.