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No description available.

Laser spectroscopic techniques have, during the last decades, demonstrated an extraordinary capability for sensitive detection of molecular constituents in gas phase. Since spectra from such techniques constitute unique and characteristic signatures for each type of species, these techniques enable investigations of molecular structures as well as detection of the presence of species in a gas mixture. They are therefore used for a variety of application, from fundamental studies to the assessment of gas concentrations. In fact, quantitative assessments of gas concentrations by laser-based techniques are constantly gaining in popularity, primarily due to properties such as high sensitivity and selectivity and an ability to perform non-invasive measurement. Moreover, investigations of isolated molecular transitions under different conditions provide excellent means to obtain a comprehensive understanding of spectral broadening mechanisms, which is of importance for, for example, environmental sciences and remote sensing applications. In fundamental studies, spectroscopic parameters are often retrieved from fits of a model function of the technique used, which in turn is based upon a suitable lineshape function. In order to obtain parameter values with highest possible accuracy, it is of importance to use the lineshape model that most correctly can predict the measured spectra. Even though the Voigt function is the most commonly used lineshape model when both Doppler and collision broadenings are present, it is not always suitable when spectroscopic parameters are to be assessed with high precision. This thesis represents a thorough investigation of Dicke narrowing and speed-dependent effects, which are phenomena that are not accounted for by the conventional Voigt profile. For the first time, it is demonstrated that both these effects take place not only in absorption but also in the dispersion mode of detection. Their dispersion lineshape functions are first theoretically presumed and explicitly given before they are validated experimentally by the noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS). By using the models developed, it is also shown that although the two modes of detection, absorption and dispersion, both can provide good quality of fits, they do not always provide identical spectroscopic parameters. A detailed analysis under which conditions they do so, and subsequent recommendations of their use, are presented. It also describes the instrumental implementation of a distributed-feed-back (DFB) laser-based NICE-OHMS instrumentation, which constitutes an important step towards the further development of this technique. Due to the wide tunability of the DFB laser, the setup is capable of extending the working range of NICE-OHMS into the collision broadening region, which, in turn, allows for precise spectroscopic studies. The use of a fiber-coupled DFB laser also provides a compact NICE-OHMS system. The minimum detectable on-resonance absorption was assessed to 2× 10-10 cm-1 for a 70 s integration time.

Using a narrow-band resonant fluorescence spectra from a nano-cell with a thickness of L= [lambda]/2, and VSOP resonances formed at a thickness L =[lambda] ([lambda] is the wavelength of the resonant radiation), for the first time it was experimentally investigated the behaviour of the frequency and intensity (transition probabilities) of the atomic hyperfine structure transitions between the 85Rb, 87Rb, D1 and D2 lines Zeeman sublevels in external magnetic fields in range 5 - 7000G. The behaviour of tens of previously unstudied atomic transitions was analyzed and it is demonstrated that the intensities of these lines can both greatly increase, and decrease (tenfold). For the first time it is demonstrated that, in the case of partial pressure of neon buffer gas up to 6~torr into the nano-cell of thickness L = [lambda] filled with Rb, VSOP resonances are recorded confidently, while the addition of 0.1~torr neon buffer gas in a cell of a centimeter thickness leads to the complete disappearance of VSOP resonances formed with the help of the widely used technique of saturated absorption. It is demonstrated for the first time that the spectral width of the resonant fluorescence spectra of the rubidium nano-cell with thickness L= [lambda]/2, for all values of the neon buffer gas pressures is much narrower (6-8 times) compared with the resonant fluorescence spectra of an ordinary centimeter cell containing rubidium with the same pressures of neon

A l'aide d'un spectre de fluorescence de résonance à bande étroite obtenu avec une nano-cellule d'épaisseur L= [lambda]/2 et des résonances VSOP formées pour une épaisseur L =[lambda] ([lambda] est la longueur d'onde de la radiation résonnante), cette thèse présente pour la première fois une étude expérimentale du comportement en fréquence et en intensité (probabilités de transition) des transitions atomiques de la structure hyperfine entre sous-niveaux Zeeman des raies D1 and D2 pour le 85Rb et le 87Rb en présence de champs magnétiques extérieurs compris entre 5 et 7000 G. Le comportement d'une dizaine de transitions atomiques inétudiées à ce jour a été analysé et nous avons démontré que l'intensité de ces raies peut montrer alternativement de grandes variations : jusqu'à un facteur 10 de taux de croissance ou de décroissance. Pour la première fois, nous avons parfaitement enregistré des résonances VSOP dans le cas où un gaz tampon (néon de pression partielle 6 torr) est introduit dans la nano-cellule d'épaisseur L =[lambda], alors que l'addition d'un gaz tampon (néon) même à une pression partielle de 0,1 torr, dans une cellule d'épaisseur centimétrique conduit à une complète disparition de ces résonances VSOP obtenues par la méthode usuelle d'absorption saturée. Enfin, nous avons montré pour la première fois que la largeur spectrale d'un spectre de fluorescence de résonance d'une nano-cellule de rubidium d'épaisseur L= [lambda]/2, quelques soient les pressions du gaz tampon (néon), est beaucoup plus étroite (6 à 8 fois) que celle obtenue avec une cellule centimétrique de rubidium pour les mêmes valeurs de pressions / Using a narrow-band resonant fluorescence spectra from a nano-cell with a thickness of L= [lambda]/2, and VSOP resonances formed at a thickness L =[lambda] ([lambda] is the wavelength of the resonant radiation), for the first time it was experimentally investigated the behaviour of the frequency and intensity (transition probabilities) of the atomic hyperfine structure transitions between the 85Rb, 87Rb, D1 and D2 lines Zeeman sublevels in external magnetic fields in range 5 - 7000G. The behaviour of tens of previously unstudied atomic transitions was analyzed and it is demonstrated that the intensities of these lines can both greatly increase, and decrease (tenfold). For the first time it is demonstrated that, in the case of partial pressure of neon buffer gas up to 6~torr into the nano-cell of thickness L = [lambda] filled with Rb, VSOP resonances are recorded confidently, while the addition of 0.1~torr neon buffer gas in a cell of a centimeter thickness leads to the complete disappearance of VSOP resonances formed with the help of the widely used technique of saturated absorption. It is demonstrated for the first time that the spectral width of the resonant fluorescence spectra of the rubidium nano-cell with thickness L= [lambda]/2, for all values of the neon buffer gas pressures is much narrower (6-8 times) compared with the resonant fluorescence spectra of an ordinary centimeter cell containing rubidium with the same pressures of neon