<p>Laser-based absorption spectroscopy (AS) is a powerful technique for qualitative and quantitative studies of atoms and molecules. An important field of use of AS is the detection of species in trace concentrations, which has applications not only in physics and chemistry but also in biology and medicine, encompassing environmental monitoring, regulation of industrial processes and breath analysis. Although a large number of molecular species can successfully be detected with established AS techniques, there are some applications that require higher sensitivity, selectivity and accuracy, yet robust and compact instrumentation.</p><p>Various approaches have been made during the years to improve on the performance of AS, usually based on modulation spectrometry or external cavities. The most sensitive absorption technique of today is, however, noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS). This technique elegantly combines several approaches: external cavities (for optical path length enhancement), modulation techniques (for noise reduction) and saturation spectroscopy (for enhanced selectivity). However, due to its complexity, the technique has so far not been applied to practical trace species detection.</p><p>This thesis provides the background for an understanding of NICE-OHMS and describes the construction of a first compact NICE-OHMS spectrometer based on a narrowband fiber laser. Moreover, it gives theoretical expressions for NICE-OHMS signal lineshapes, measured in various modes of detection, which can be fitted to the experimental data and thereby facilitate the assessment of species concentration. The sensitivity of the instrumentation is demonstrated by detection of acetylene (C₂H₂) and carbon dioxide (CO₂) in the 1.5 μm region. A fractional absorption sensitivity of 3*10^-9 (integrated absorption of 5*10^-11 cm^-1), could be achieved using a cavity with a finesse of 4800 and an acquisition time of 0.7 s. This results in a detection limit for C₂H₂ of 4.5 ppt (4.5*10^-12 atm).</p><p>In addition, the thesis revives the idea of using an accurate (frequency) measurement of the free-spectral-range (FSR) of an external cavity for sensitive and calibration-free concentration assessment. A theoretical description of the expected signal lineshapes is given, and in a first experimental demonstration the FSR could be measured with a resolution of 5 Hz, resulting in a fractional absorption sensitivity of 1*10^-7, and subsequently in a detection limit for C₂H₂ of 180 ppt (12.5 s acquisition time).</p><p>The thesis, finally, also contributes to the continuously ongoing development of conventional AS and wavelength modulated AS by addressing concepts related to when the light optically saturates the transition.</p>

Laser-based absorption spectroscopy (AS) is a powerful technique for qualitative and quantitative studies of atoms and molecules. An important field of use of AS is the detection of species in trace concentrations, which has applications not only in physics and chemistry but also in biology and medicine, encompassing environmental monitoring, regulation of industrial processes and breath analysis. Although a large number of molecular species can successfully be detected with established AS techniques, there are some applications that require higher sensitivity, selectivity and accuracy, yet robust and compact instrumentation. Various approaches have been made during the years to improve on the performance of AS, usually based on modulation spectrometry or external cavities. The most sensitive absorption technique of today is, however, noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS). This technique elegantly combines several approaches: external cavities (for optical path length enhancement), modulation techniques (for noise reduction) and saturation spectroscopy (for enhanced selectivity). However, due to its complexity, the technique has so far not been applied to practical trace species detection. This thesis provides the background for an understanding of NICE-OHMS and describes the construction of a first compact NICE-OHMS spectrometer based on a narrowband fiber laser. Moreover, it gives theoretical expressions for NICE-OHMS signal lineshapes, measured in various modes of detection, which can be fitted to the experimental data and thereby facilitate the assessment of species concentration. The sensitivity of the instrumentation is demonstrated by detection of acetylene (C2H2) and carbon dioxide (CO2) in the 1.5 μm region. A fractional absorption sensitivity of 3*10-9 (integrated absorption of 5*10-11 cm-1), could be achieved using a cavity with a finesse of 4800 and an acquisition time of 0.7 s. This results in a detection limit for C2H2 of 4.5 ppt (4.5*10-12 atm). In addition, the thesis revives the idea of using an accurate (frequency) measurement of the free-spectral-range (FSR) of an external cavity for sensitive and calibration-free concentration assessment. A theoretical description of the expected signal lineshapes is given, and in a first experimental demonstration the FSR could be measured with a resolution of 5 Hz, resulting in a fractional absorption sensitivity of 1*10-7, and subsequently in a detection limit for C2H2 of 180 ppt (12.5 s acquisition time). The thesis, finally, also contributes to the continuously ongoing development of conventional AS and wavelength modulated AS by addressing concepts related to when the light optically saturates the transition.

Noise-immune cavity-enhanced optical heterodyne molecular spectro-metry (NICE-OHMS) is one of the most sensitive laser-based absorption techniques. The high sensitivity of NICE-OHMS is obtained by a unique combination of cavity enhancement (for increased interaction length with a sample) with frequency modulation spectrometry (for reduction of noise). Moreover, sub-Doppler detection is possible due to the presence of high intensity counter-propagating waves inside an external resonator, which provides an excellent spectral selectivity. The high sensitivity and selectivity make NICE-OHMS particularly suitable for trace gas detection. Despite this, the technique has so far not been often used for practical applications due to its technical complexity, originating primarily from the requirement of an active stabilization of the laser frequency to a cavity mode. The main aim of the work presented in this thesis has been to develop a simpler and more robust NICE-OHMS instrumentation without compro-mising the high sensitivity and selectivity of the technique. A compact NICE-OHMS setup based on a fiber laser and a fiber-coupled electro-optic modulator has been constructed. The main advantage of the fiber laser is its narrow free-running linewidth, which significantly simplifies the frequency stabilization procedure. It has been demonstrated, using acetylene and carbon dioxide as pilot species, that the system is capable of detecting relative absorption down to 3 × 10-9 on a Doppler-broadened transition, and sub-Doppler optical phase shift down to 1.6 × 10-10, the latter corresponding to a detection limit of 1 × 10-12 atm of C2H2. Moreover, the potential of dual frequency modulation dispersion spectrometry (DFM-DS), an integral part of NICE-OHMS, for concentration measurements has been assessed. This thesis contributes also to the theoretical description of Doppler-broadened and sub-Doppler NICE-OHMS signals, as well as DFM-DS signals. It has been shown that the concentration of an analyte can be deduced from a Doppler-broadened NICE-OHMS signal detected at an arbitrary and unknown detection phase, provided that a fit of the theoretical lineshape to the experimental data is performed. The influence of optical saturation on Doppler-broadened NICE-OHMS signals has been described theoretically and demonstrated experimentally. In particular, it has been shown that the Doppler-broadened dispersion signal is unaffected by optical saturation in the Doppler limit. An expression for the sub-Doppler optical phase shift, valid for high degrees of saturation, has been derived and verified experimentally up to degrees of saturation of 100.

An optical cavity comprises a set of mirrors between which light can be reflected a number of times. The selectivity and stability of optical cavities make them extremely useful as frequency references or discri­mi­nators. With light coupled into the cavity, a sample placed inside a cavity will experience a significantly increased interaction length. Hence, they can be used also as amplifiers for sensing purposes. In the field of laser spectroscopy, some of the most sensitive techniques are therefore built upon optical cavities. In this work optical cavities are used to measure properties of gas samples, i.e. absorption, dispersion, and refractivity, with unprecedented precision. The most sensitive detection technique of all, Doppler-broadened noise-immune cavity enhanced optical heterodyne molecular spectrometry (Db NICE-OHMS), has in this work been developed to an ultra-sensitive spectroscopic technique with unprecedented detection sensitivity. By identifying limiting factors, realizing new experimental setups, and deter­mining optimal detection conditions, the sensitivity of the technique has been improved several orders of magnitude, from 8 × 10-11 to 9 × 10-14 cm-1. The pressure interval in which NICE-OHMS can be applied has been extended by deri­vation and verification of dispersions equations for so-called Dicke narrowing and speed dependent broadening effects. The theoretical description of NICE-OHMS has been expanded through the development of a formalism that can be applied to the situations when the cavity absorption cannot be considered to be small, which has expanded the dynamic range of the technique. In order to enable analysis of a large number of molecules at their most sensitive transitions (mainly their funda­mental CH vibrational transitions) NICE-OHMS instrumentation has also been developed for measurements in the mid-infrared (MIR) region. While it has been difficult to realize this in the past due to a lack of optical modulators in the MIR range, the system has been based on an optical para­metric oscillator, which can be modulated in the near-infrared (NIR) range. As the index of refraction can be related to density, it is possible to retrieve gas density from measurements of the index of refraction. Two such instru­men­tations have been realized. The first one is based on a laser locked to a measure­ment cavity whose frequency is measured by compassion with an optical frequency comb. The second one is based on two lasers locked to a dual-cavity (i.e. one reference and one measurement cavity). By these methods changes in gas density down to 1 × 10-9 kg/m3 can be detected. All instrumentations presented in this work have pushed forward the limits of what previously has been considered measurable. The knowledge acquired will be of great use for future ultrasensitive cavity-based detection methods.

X-ray diffraction and scattering, X-ray spectroscopy, and X-ray crystallography are widely used in the life sciences, material science, and medical diagnosis. High-quality and high-brightness X-rays are a strong requirement to improve applications. Inverse Compton scattering (ICS) X-ray source has attracted great interests worldwide lately. To significantly enhance the average X-ray photon flux, a compact electron storage-ring combined with a high finesse optical enhancement cavity (OEC) can be utilized. In such a system, the collision rate between the electron beam and the laser pulse is greatly increased to the MHz range, enabling a photon flux up to 10¹³ph/s.In the first chapter, I describe the motivation behind the development of OEC based on ICS X-ray source. The characteristics of this kind of X-ray source are summarized, compared to those of the conventional low-repetition-rate Terawatt laser system based on ICS X-ray source. The latest progress and research status of OEC based on ICS X-ray source are presented. Pulsed-laser injected high-finesse OEC stacking theory and properties are discussed in Chapter 2. Not only does the OEC based on ICS X-ray source require the laser pulse repetition rate to be matched to the free spectral range (FSR) of the cavity, where both also have to match the electron storage-ring circulation frequency. In addition, we have to match the phase shift of the laser repetition rate to the phase offset introduced by the dispersion of the cavity mirrors, since our cavity finesse design value is quite high. The stacking theory is analyzed in the frequency domain. Cavity properties, including cavity mirror dispersion, finesse, and FSR, are discussed in detail. A laser frequency comb and OEC coupling is analyzed also. The laser source development is presented in Chapter 3. We constructed a mode-locked fiber laser based on nonlinear polarization rotation. The locking model, locking techniques, and the theory, simulations and experimental tests of tilt locking (TL) in the pulsed laser injected high-finesse OEC are discussed in Chapter 4. We succeeded in locking a pulsed laser to a high-finesse cavity with the TL technique. The experimental results show that the TL and the Pound-Drever-Hall techniques have the same performance: stable locking, high sensitivity, and the same power coupling rate for picosecond laser pulse case, while the test results for full spectrum TL locking show that it is uneasy to align the split-photodiode to the beam waist.Based on the above experimental study and tests, we design the OEC system for Tsinghua University X-ray project in Chapter 5. The expected X-ray flux is 10¹º to 10¹³ ph/s. We detail every subsystem requirement.

X-ray diffraction and scattering, X-ray spectroscopy, and X-ray crystallography are widely used in the life sciences, material science, and medical diagnosis. High-quality and high-brightness X-rays are a strong requirement to improve applications. Inverse Compton scattering (ICS) X-ray source has attracted great interests worldwide lately. To significantly enhance the average X-ray photon flux, a compact electron storage-ring combined with a high finesse optical enhancement cavity (OEC) can be utilized. In such a system, the collision rate between the electron beam and the laser pulse is greatly increased to the MHz range, enabling a photon flux up to 10¹³ph/s.In the first chapter, I describe the motivation behind the development of OEC based on ICS X-ray source. The characteristics of this kind of X-ray source are summarized, compared to those of the conventional low-repetition-rate Terawatt laser system based on ICS X-ray source. The latest progress and research status of OEC based on ICS X-ray source are presented. Pulsed-laser injected high-finesse OEC stacking theory and properties are discussed in Chapter 2. Not only does the OEC based on ICS X-ray source require the laser pulse repetition rate to be matched to the free spectral range (FSR) of the cavity, where both also have to match the electron storage-ring circulation frequency. In addition, we have to match the phase shift of the laser repetition rate to the phase offset introduced by the dispersion of the cavity mirrors, since our cavity finesse design value is quite high. The stacking theory is analyzed in the frequency domain. Cavity properties, including cavity mirror dispersion, finesse, and FSR, are discussed in detail. A laser frequency comb and OEC coupling is analyzed also. The laser source development is presented in Chapter 3. We constructed a mode-locked fiber laser based on nonlinear polarization rotation. The locking model, locking techniques, and the theory, simulations and experimental tests of tilt locking (TL) in the pulsed laser injected high-finesse OEC are discussed in Chapter 4. We succeeded in locking a pulsed laser to a high-finesse cavity with the TL technique. The experimental results show that the TL and the Pound-Drever-Hall techniques have the same performance: stable locking, high sensitivity, and the same power coupling rate for picosecond laser pulse case, while the test results for full spectrum TL locking show that it is uneasy to align the split-photodiode to the beam waist.Based on the above experimental study and tests, we design the OEC system for Tsinghua University X-ray project in Chapter 5. The expected X-ray flux is 10¹º to 10¹³ ph/s. We detail every subsystem requirement.

Made available in DSpace on 2016-03-15T19:37:34Z (GMT). No. of bitstreams: 1 Claudia Barros dos Santos.pdf: 3294972 bytes, checksum: b848d69d9c6a8c824e5142a4e3659d37 (MD5) Previous issue date: 2011-01-21 / In this work, we inserted two Arrayed Waveguide Gratings (AWGs), in an Erbium doped fiber ring cavity laser, where a single gain medium at room temperature can emit laser in multiples wavelengths, simultaneous and individualy controlled. The setup allowed us to check different functions in the ring cavity. Here we show emission in CW regime, Passive Mode-Locking, using Carbon Nanotubes as saturable absorbers and finally Active mode-locking at 7GHz, simultaneously. / Neste trabalho, fez-se a inserção de duas grades de difração matriciais com guias de onda, ou AWGs (Arrayed Waveguide Gratings) em uma cavidade laser de fibra dopada com Érbio, onde um único meio de ganho em temperatura ambiente pode gerar ação laser em múltiplos comprimentos de onda, com emissões simultâneas e controladas individualmente. A configuração utilizada permitiu o teste com diferentes regimes de operação simultâneos dentro da cavidade. Mostramos a possibilidade de emissão laser em regime CW, em regime de mode-locking passivo, com o uso de nanotubos de carbono como absorvedor saturável e, por último, em regime de modelocking ativo com uma freqüência de modulação de 7 GHz.

Made available in DSpace on 2016-03-15T19:37:35Z (GMT). No. of bitstreams: 1 Claudia Barros dos Santos.pdf: 3294972 bytes, checksum: b848d69d9c6a8c824e5142a4e3659d37 (MD5) Previous issue date: 2011-01-21 / In this work, we inserted two Arrayed Waveguide Gratings (AWGs), in an Erbium doped fiber ring cavity laser, where a single gain medium at room temperature can emit laser in multiples wavelengths, simultaneous and individualy controlled. The setup allowed us to check different functions in the ring cavity. Here we show emission in CW regime, Passive Mode-Locking, using Carbon Nanotubes as saturable absorbers and finally Active mode-locking at 7GHz, simultaneously. / Neste trabalho, fez-se a inserção de duas grades de difração matriciais com guias de onda, ou AWGs (Arrayed Waveguide Gratings) em uma cavidade laser de fibra dopada com Érbio, onde um único meio de ganho em temperatura ambiente pode gerar ação laser em múltiplos comprimentos de onda, com emissões simultâneas e controladas individualmente. A configuração utilizada permitiu o teste com diferentes regimes de operação simultâneos dentro da cavidade. Mostramos a possibilidade de emissão laser em regime CW, em regime de mode-locking passivo, com o uso de nanotubos de carbono como absorvedor saturável e, por último, em regime de modelocking ativo com uma freqüência de modulação de 7 GHz.

Made available in DSpace on 2016-03-15T19:38:55Z (GMT). No. of bitstreams: 1 DAVID STEINBERG.pdf: 3031041 bytes, checksum: e320f0c21b75ca5bdd5a63f93fa6dd1d (MD5) Previous issue date: 2015-08-27 / Fundo Mackenzie de Pesquisa / In this thesis, for the first time we present results of passively-mode-locking O-band Raman fiber laser operating at 1310 nm by using carbon nanotubes as saturable absorber. The first results were obtained for an experimental setup based on single mode fiber (SMF) with laser operating near zero fiber dispersion at 1310 nm at anomalous regime. In this same configuration, a study of pulse duration shortening in terms of intracavity dispersion management with dispersion shifted fiber lengths (DSF) was performed. Replacing the SMF by a highly doped germanium fiber as gain medium of Raman fiber laser, operation was shifted to normal dispersion regime and passive mode-locking was also generated. In this laser, a study of pulse duration shortening in terms of gain medium length reduction was performed and the picosecond pulse regime of the laser could be estimated. We also present a brief comparison between the two dispersion regimes of the Raman fiber laser and passive mode-locking results obtained with different diameters of carbon nanotubes as saturable absorbers. / Nesta tese, apresentamos pela primeira vez resultados do acoplamento passivo de modos em um laser Raman à fibra operando em 1310 nm na banda O, utilizando nanotubos de carbono como absorvedor saturável. Os primeiros resultados foram obtidos de uma configuração experimental baseada totalmente em fibra monomodo padrão (SMF) com o laser operando próximo ao zero de dispersão da fibra em 1310 nm, porém em regime anômalo. Nesta mesma configuração, um estudo do encurtamento da duração do pulso em função do gerenciamento da dispersão intracavidade com comprimentos de fibra de dispersão deslocada (DSF) foi realizado. Substituindo a SMF por uma fibra altamente dopada com germânio como meio do ganho do laser Raman, a operação do laser foi deslocada para o regime de dispersão normal e o regime de acoplamento passivo de modos também foi gerado. Neste laser, um estudo do encurtamento da duração do pulso em função da redução do comprimento do meio de ganho foi realizado e a operação do acoplamento passivo de modos do laser em regime de picossegundos pôde ser estimada. Também apresentamos uma breve comparação entre os dois regimes de dispersão do laser Raman à fibra e resultados do acoplamento passivo de modos obtidos com diferentes diâmetros de nanotubos de carbono como absorvedores saturáveis.

Cette thèse décrit le développement de deux outils originaux pour l’interférométrie atomique. Le premier est une cavité optique à haute finesse pour la manipulation d’atomes ultra-froids de 87Rb. Cette cavité est d’abord utilisée pour augmenter l’intensité d’un piège dipolaire optique qui permet de piéger et refroidir les atomes. Ainsi, en procédant à un refroidissement par évaporation de l’échantillon atomique, nous avons atteint le régime de condensation de Bose-Einstein. La cavité étant non dégénérée, elle permet également l’injection de différents modes transverses électromagnétiques. Nous avons alors démontré la création et la manipulation de réseau d’ensembles atomiques en utilisant ces modes. La mesure successive de ces ensembles atomiques au cours d’une séquence d’interférométrie atomique permettrait d’augmenter le temps de mesure et ainsi d‘améliorer la sensibilité de l’instrument. Deuxièmement, l’utilisation d’une mesure faible non destructive sur les atomes permet de soutirer de l’information du système sans le perturber. En appliquant une rétroaction après ces mesures, l’état quantique peut être contrôlé. Par l’utilisation d’une séquence de Ramsey adaptée avec des mesures faibles et des corrections de phase, nous avons ainsi démontré la réalisation d’une boucle à verrouillage de phase entre un oscillateur local et l’état atomique. Nous avons ensuite démontré que ce protocole améliore la stabilité d’une horloge atomique en surpassant la limite de stabilité de l’oscillateur local. Nous avons également validé l’utilisation de la plate-forme laser commercial EYLSA de Quantel sur deux expériences de refroidissement d’atomes par laser. / This thesis reports the development of two original tools for atom interferometry.The first is a high finesse optical cavity for the manipulation of 87Rb cold atoms. This cavity isfirstly used to enhance the intensity of an optical dipole trap. Thus, by realizing an evaporativecooling on the atomic sample, we reached Bose-Einstein condensation. Furthermore, the nondegeneratecavity allows the injection of different transverse electromagnetic modes. In thisway, we have demonstrated the generation and the manipulation of arrays of atomic ensemblesusing these modes. Successive measurements of these atomic ensembles in an atominterferometric sequence would increase the interrogation time and thus the sensitivity of thesensor.Secondly, the use of weak nondestructive measurements on the atoms allows to extractinformation from the system with negligible perturbation of the ensemble. Applying feedbackafter the measurement, we were able to control the quantum state of the system. Using amodified Ramsey sequence with weak nondestructive measurements and phase corrections, werealized a phase lock loop between a local oscillator and the atomic state. We have thendemonstrated that this protocol leads to a stability enhancement of an atomic clock byovercoming the limit set by the local oscillator.We also contributed to the development of the commercial laser platform EYLSA fromQuantel, testing its performances on two laser cooling experiments.