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Master of Science / Department of Physics / Brian R. Washburn / This thesis reports our attempt towards achieving a phase stabilized free-space nonlinear polarization rotation (NPR) mode locked erbium doped fiber laser frequency comb system. Optical frequency combs generated by mode-locked femtosecond fiber lasers are vital tools for ultra-precision frequency metrology and molecular spectroscopy. However, the comb bandwidth and average output power become the two main limiting elements in the application of femtosecond optical frequency combs. We have specifically investigated the free-space mode locking dynamics of erbium-doped fiber (EDF) mode-locked ultrafast lasers via nonlinear polarization rotation (NPR) in the normal dispersion regime. To do so, we built a passively mode-locked fiber laser based on NPR with a repetition rate of 89 MHz producing an octave-spanning spectrum due to supercontinuum (SC) generation in highly nonlinear fiber (HNLF). Most significantly, we have achieved highly stable self-starting NPR mode-locked femtosecond fiber laser based frequency comb which has been running mode locked for the past one year without any need to redo the mode locking. By using the free-space NPR comb scheme, we have not only shortened the cavity length, but also have obtained 5 to 10 times higher output power (more than 30 mW at central wavelength of 1570 nm) and much broader spectral comb bandwidth (about 54 nm) compared to conventional all-fiber cavity structure with less than 1 mW average output power and only 10 nm spectral bandwidth. The pulse output from the NPR comb is amplified through a 1 m long EDF, then compressed by a length of anomalous dispersion fiber to a near transform limited pulse duration. The amplified transform limited pulse, with an average power of 180 mW and pulse duration of 70 fs, is used to generate a supercontinuum of 140 mW. SC generation via propagation in HNLF is optimized for specific polling period and heating temperature of PPLN crystal for SHG around 1030 nm. At last, we will also discuss the attempt of second harmonic generation (SHG) by quasi phase matching in the periodically polled lithium niobate (PPLN) crystal due to nonlinear effect corresponding to different polling period and heating temperature.

Un nombre croissant d’applications telles que le micro-usinage ou le diagnostique de composants électroniques nécessitent de fortes puissances moyennes dans différentes gammes de longueurs d’onde (infra-rouge à 1030 nm, vert à 515 nm ou ultra-violet à 343 nm). Ces fortes puissances moyennes lasers ne sont généralement atteignables qu’à l’aide d’architecture laser de type MOPA (Master Oscillator Power Amplifier). C’est dans cette optique que la société Eolite Systems veut développer ses propres oscillateurs car elle maitrise déjà l’amplification à l’aide de fibres de type barreau à large aire modale. Le développement d’oscillateurs picosecondes de fortes puissances moyennes est ainsi une brique essentielle dans la chaîne d’amplification globale. Dans le cadre d’un contrat CIFRE entre Eolite Systems et le Laboratoire Onde et Matière d’Aquitaine de l’Universitéde Bordeaux 1, nous avons développé différents laser dont la puissance moyenne est supérieure à 10W, à une cadence de 74 MHz. La durée des impulsions générées s’étend de 20 ps à 130 fs. Le fonctionnement de ces différents lasers repose sur l’utilisation de la rotation non-linéaire de polarisation dans la fibre optique qui, dans le régime de fonctionnement à dispersion normale, permet d’atteindre le verrouillage en phase des modes et ainsi la génération d’impulsions d’énergie de l’ordre de 150nJ. Nous avons développé un code de simulation numérique afin de rendre compte de la dynamique des impulsions dans la cavité. Les résultats obtenus à l’aide de ce code sont en bon accord avec ceux obtenus lors des différentes expériences. / A growing number of applications such as micro-machining of electronical components need high average power in a various range of wavelengths (infrared at 1030 nm, green at 515 nm and ultravioletat 343 nm). These high average power lasers are generally design using a MOPA (MasterOscillator Power Amplifier) scheme. Following this idea, Eolite systems wants to develop its own oscillators since it already masters the different difficulties when trying to reach high average power,especially by using rod-type fibers with a large mode area. The development of high power picosecondfiber oscillators is a essential piece in the global amplification scheme. In the frame of a CIFRE contract between Eolite Systems and the Laboratoire Onde et Matière d’Aquitaine of the Universitéde Bordeaux 1 we have developed different laser oscillators with an average power of more than10 W at a repetition rate of 74 MHz. The pulse duration generated is ranging from 20 ps down to130 fs. The pulsed regime was initiated using non-linear polarization evolution in the fiber and in anormal dispersion laser cavity. This lead to the generation of pulse energies in the range of 150 nJ for the different architectures. We also developed a numerical code in ordre to fully understand the influence of the different elements in the laser cavity. The results are in good agreement with those obtained with the experimental setup.

RésuméLa diffraction et la diffusion de rayons X sont utilisées dans de nombreux domaines de la physique, de la médecine et de la technologie. Des faisceaux de haute brillance sont néanmoins requis pour améliorer les performances de ces techniques. L’utilisation de la diffusion Compton d’un laser sur un faisceau d’électrons présente un grand intérêt pour la production de rayons X. Ce processus permet l’emploi d’un anneau de stockage d’électrons compacts et d’un résonateur optique pour accroître la puissance laser. Avec un tel système, un taux de collision laser-électron supérieur au méga Hertz est envisageable permettant d’atteindre un flux de rayons X de l’ordre de 10¹³ photons/s. Dans le premier chapitre, je décris les motivations pour le développement d’une source de rayons X basée sur la diffusion Compton et utilisant un résonateur optique. Je détermine aussi les performances que l’on peut attendre de ce type de sources ainsi que l’état de l’art actuel dans ce domaine. Dans le deuxième chapitre, je décris le comportement et les propriétés des résonateurs optiques en régime impulsionnel. J’introduis la notion de phase CEP (‘carrier envelope phase’) et je montre la nécessité de contrôler à la fois la fréquence de répétition de l’oscillateur laser et cette phase CEP. Le chapitre 3 est consacré aux oscillateurs fibrés à blocage de mode. Je montre les performances du laser que j’ai construit en utilisant le phénomène de rotation de polarisation non-linéaire.La méthode d’asservissement laser-résonateur optique ‘tilt locking’ est introduite au chapitre 4. Je décris tout d’abord les études de simulations et le montage expérimental qui ont permis de tester la méthode en régime impulsionnel. Je donne ensuite les résultats expérimentaux qui démontrent la faisabilité de la méthode ‘tilt locking’ en régime impulsionnel. J’effectue aussi une comparaison expérimentale des performances de la méthode ‘tilt locking’ avec la méthode classique ‘Pound-Drever-Hall’. Je termine le chapitre en indiquant une difficulté expérimentale de la méthode pour générer plusieurs signaux d’erreurs.Je décris la conception du système optique de la machine Compton TTX de l’université Tsinghua dans le chapitre 5. Les performances attendues pour cette machine sont des flux de rayons X compris entre 10¹º et 10¹³ photons/s. / 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.

Les effets non-linéaires dépendant essentiellement de l’intensité du champ électrique de l’onde et du guide, sont indispensables à la génération des régimes impulsionnels dans les lasers à fibre dopée. L’effet Kerr, qui se manifeste quel que soit l’énergie de propagation et de pompage, va engendrer le phénomène de l’auto modulation de phase (SPM) qui se traduira par un élargissement spectral. La SPM peut se voir aussi dans l’interaction entre les deux ondes qui se propagent le long des axes lents et rapides du guide (XPM). Dans un guide uniforme passif, cette auto modulation de phase en se conjuguant avec la dispersion chromatique du guide peut conduire à l’impulsion soliton, mais ce cadre doit être largement dépassé pour aborder la mise en forme d’impulsions dans un système dissipatif, tel qu’une cavité laser. Ce cadre élargi est celui du soliton dissipatif. Dans ce travail, nous avons passé en revue la fibre optique dopée en tant que milieu actif. Nous avons présenté le principe physique du blocage de modes, en introduisant l’absorbant saturable virtuel reposant sur l’évolution non linéaire de la polarisation (ENLP). Dans la partie expérimentale, on s’est penché plus particulièrement sur de nouvelles dynamiques à haute cadence (multi-GHz) d’un laser à fibre dopée, à modes bloqués. Avant de présenter et positionner notre travail, on s’est intéressé dans un premier temps à ce qui a été publié sur la génération des trains d’impulsions ultracourtes à haute cadence. Nous avons étudié chaque configuration, allant de la génération de régime harmonique à haute cadence par le blocage de modes habituel jusqu’aux techniques utilisant l’instabilité de modulation avec un filtrage interférométrique (µcavité, F.P, SFBG). En évaluant les opportunités de réalisation de chacune, nous avons été attirés par la configuration de Mao, publiée dans Sci. Reports, toute fibrée, qui sera le premier volet de notre contribution expérimentale. Effectivement, dans un premier temps nous avons repris les travaux de Mao et al. où le MZI est pris en série dans la cavité fondamentale. Dans le souci d’apporter plus de stabilité, nous avons proposé une autre configuration où le MZI est pris dans une boucle de recirculation qui permettra plus de filtrage des modes cavité en phase. Cette stabilité du régime impulsionnel, à haute cadence, a été observée en temps réel. / Non-linear effects, which depend essentially on the intensity of the electric field of the wave and the guide, are essential for the generation of pulse regimes in doped fiber lasers. The Kerr effect, which occurs regardless of the propagation and pumping energy, will generate the phenomenon of phase auto modulation (SPM), which will result in a spectral expansion. The SPM can also be seen in the interaction between the two waves that propagate along the slow and fast axes of the guide (XPM). In a passive uniform guide, this self-phase modulation in combination with the chromatic dispersion of the guide can lead to the soliton pulse, but this framework must be largely overcome to address pulse shaping in a dissipative system, such as a laser cavity. This extended framework is that of the dissipative soliton. In this work, we reviewed doped optical fiber as an active medium. We presented the physical principle of mode blocking, introducing the virtual saturable absorber based on the non-linear evolution of polarization (ENLP). In the experimental part, we focused more particularly on new high rate dynamics (multi-GHz) of a doped fiber laser with blocked modes. Before presenting and positioning our work, we first focused on what was published on the generation of ultra-short high speed pulse trains. We studied each configuration, ranging from the generation of high-rate harmonic regime by blocking the usual modes to techniques using modulation instability with interferometric filtering (µcavity, F.P, SFBG). In assessing the opportunities for each, we were attracted by the configuration of Mao, published in Sci. Reports, all fiber, which will be the first part of our experimental contribution. Indeed, initially we resumed the work of Mao et al. where the MZI is taken in series in the fundamental cavity. In order to provide more stability, we have proposed another configuration where the MZI is caught in a recirculation loop that will allow more filtering of the cavity modes in phase. This stability of the impulse regime, at high repetition rate, was observed in real time.

Les travaux de cette thèse s'efforcent d'apporter une solution au problème persistant de grande pauvreté des lasers à fibre à modes bloqués, en termes de fonctionnalités et de flexibilité. La thèse propose une cavité laser fibrée ayant comme spécificité d'être multifonctionnelle. La cavité est dotée de composants accordables, qui apportent la flexibilité nécessaire pour réaliser des fonctions allant de la génération d’impulsions aux profils complexes (solitons, bi-solitons, tri-solitons, etc) jusqu’à la sculpture des profils d’impulsion, en passant par la régulation des puissances crête, et la régénération de profils d’intensités sévèrement dégradés. La cavité laser que nous proposons a comme spécificité d'être pilotée par un composant clé, qui est un miroir à boucle optique non-linéaire (NOLM : Nonlinear Optical Loop Mirror) multifonction. Nous avons conçu ce NOLM en apportant des modifications structurelles dans l'architecture usuelle de ce dispositif, et en lui adjoignant : une fibre compensatrice de dispersion, un filtre passe bande à bande passante accordable, et un amplificateur (précédé d'un filtre égaliseur de gain, selon le besoin). Le NOLM ainsi conçu est doté de deux paramètres manuellement accordables, à savoir: la bande passante du filtre passe bande et la puissance de pompage de l'amplificateur. Ces deux paramètres permettent de régler sa fonction de transfert, et à accroître ainsi ses fonctionnalités et sa flexibilité. Ainsi, en plus de son rôle comme élément déclencheur du blocage de modes, ce NOLM réalise des fonctions optiques essentielles telles que la régénération des profils d'intensité fortement dégradés par des phénomènes de propagation ; ce qui contribue au renforcement de la stabilité du laser. Nous démontrons également la possibilité de réguler la puissance crête des impulsions, en la verrouillant à une valeur prédéfinie. Nous montrons enfin que le laser multifonction offre la possibilité de réaliser la sculpture des profils d'impulsion, c'est-à-dire, de générer des impulsions dotées d'une puissance crête et une largeur temporelle fixés à l'avance via un réglage approprié des paramètres de contrôle du NOLM.Les applications visées par ce laser multifonction, concernent toutes les activités qui requièrent des sources d'impulsions finement accordables, tant au niveau de puissance crête des impulsions que de leur largeur temporelle. Ces activités, nombreuses dans le domaine Télécom, incluent les opérations de remise en forme des porteuses d'information, les opérations de compression ou étirement de profil d'impulsion, les diagnostics de composants optiques et contrôles non destructifs des lignes de transmission par réflectométrie. / The work of this thesis strives to provide a solution to the persistent problem of poverty of mode-locked fiber lasers, in terms of functionality and flexibility. The thesis proposes a fiber-laser cavity having the specificity of being multifunctional. The cavity is equipped with tunable components, which provide the flexibility to realize functions ranging from the generation of pulses with complex profiles (solitons, bi-solitons, tri-solitons, etc.) up to the carving of pulse profiles, passing through the regulation of peak powers, and the regeneration of severely degraded intensity profiles. The laser cavity that we propose has the specificity of being controlled by a key component, which is a multifunctional nonlinear optical loop mirror (NOLM). We have designed this NOLM by making structural modifications in the usual architecture of this device, and by adding to it: a dispersion compensating fiber, a bandpass filter with tunable bandwidth, and an amplifier (preceded by a gain flattening filter, as needed) with tunable gain. These two parameters make it possible to adjust its transfer function, and thus to increase its functionalities and its flexibility. Thus, in addition to its role as a trigger for mode locking, this NOLM performs essential optical functions such as the regeneration of strongly degraded intensity profiles; which contributes to strengthening the stability of the laser.We also show the possibility of regulating the pulse peak power by locking it around a predefined value. Finally, we show that the multifunction laser offers the possibility to carve pulse profiles, that is, to generate pulses endowed with a peak power and a temporal width set in advance through an appropriate adjustment of the NOLM control parameters. The applications targeted by this multifunction laser are those requiring pulses with finely tunable peak power and temporal width. These activities, include the pulse reshaping in Telecoms, operations of compression or stretching of pulse profiles, optical component diagnostics, and non-destructive control of transmission lines

<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.