| 1. |
- Khodabakhsh, Amir, 1983-
(författare)
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Fourier transform and Vernier spectroscopy using optical frequency combs
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Optical frequency comb spectroscopy (OFCS) combines two previously exclusive features, i.e., wide optical bandwidth and high spectral resolution, enabling precise measurements of entire molecular bands and simultaneous monitoring of multiple gas species in a short measurement time. Moreover, the equidistant mode structure of frequency combs enables efficient coupling of the comb power to enhancement resonant cavities, yielding high detection sensitivities. Different broadband detection methods have been developed to exploit the full potential of frequency combs in spectroscopy, based either on Fourier transform spectroscopy or on dispersive elements.There have been two main aims of the research presented in this thesis. The first has been to improve the performance of mechanical Fourier transform spectrometers (FTS) based on frequency combs in terms of sensitivity, resolution and spectral coverage. In pursuit of this aim, we have developed a new spectroscopic technique, so-called noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), and achieved a shot-noise-limited sensitivity and low ppb (parts-per-billion, 10−9) CO2 concentration detection limit in the near-infrared range using commercially available components. We have also realized a novel method for acquisition and analysis of comb-based FTS spectra, a so-called sub-nominal resolution method, which provides ultra-high spectral resolution and frequency accuracy (both in kHz range, limited only by the stability of the comb) over the broadband spectral range of the frequency comb. Finally, we have developed an optical parametric oscillator generating a frequency comb in the mid-infrared range, where the strongest ro-vibrational molecular absorption lines reside. Using this mid-infrared comb and an FTS, we have demonstrated, for the first time, comb spectroscopy above 5 μm, measured broadband spectra of several species and reached low ppb detection limits for CH4, NO and CO in 1 s.The second aim has been more application-oriented, focused on frequency comb spectroscopy in combustion environments and under atmospheric conditions for fast and sensitive multispecies detection. We have demonstrated, for the first time, cavity-enhanced optical frequency comb spectroscopy in a flame, detected broadband high temperature H2O and OH spectra using the FTS in the near-infrared range and showed the potential of the technique for flame thermometry. For applications demanding a short measurement time and high sensitivity under atmospheric pressure conditions, we have implemented continuous-filtering Vernier spectroscopy, a dispersion-based spectroscopic technique, for the first time in the mid-infrared range. The spectrometer was sensitive, fast, robust, and capable of multispecies detection with 2 ppb detection limit for CH4 in 25 ms.
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| 2. |
- Johansson, Alexandra C., 1987-
(författare)
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Optical Frequency Comb Fourier Transform Spectroscopy
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Fourier transform spectroscopy (FTS) based on optical frequency combs is an excellent spectroscopic tool as it provides broadband molecular spectra with high spectral resolution and an absolutely calibrated frequency scale. Moreover, the equidistant comb mode structure enables efficient coupling of the comb to enhancement cavities, yielding high detection sensitivity. This thesis focuses on further advances in comb-based FTS to improve its performance and extend its capabilities for broadband precision spectroscopy, particularly in terms of i) spectral resolution, ii) accuracy and precision of molecular parameters as well as concentrations retrieved from fitting models to spectra, and iii) species selectivity.To improve the spectral resolution we developed a new methodology to acquire and analyze comb-based FTS signals that yields spectra with a resolution limited by the comb linewidth rather than the optical path difference of the FTS, referred to as the sub-nominal resolution method. This method enables measurements of narrow features, e.g. low-pressure absorption spectra and modes of enhancement cavities, with frequency scale accuracy and precision provided by the comb. Using the technique we measured low-pressure spectra of the entire 3ν1+ν3 carbon dioxide (CO2) band at 1575 nm with sufficient signal-to-noise ratio and precision to observe collision narrowing of the absorption lineshape, which was for the first time with a comb-based spectroscopic technique. This allowed retrieval of spectral line parameters for this CO2 band using the speed-dependent Voigt profile.Using the sub-nominal resolution method, we measured the transmission modes of a Fabry-Perot cavity over 15 THz of bandwidth with kHz resolution and characterized the cavity modes in terms of their center frequency, linewidth, and amplitude. From the mode center frequencies, we retrieved the group delay dispersion of cavity mirror coatings and intracavity gas with an unprecedented combination of spectral bandwidth and resolution. By measuring both the mode broadening and frequency shift simultaneously we performed broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), which allows for simultaneous and calibration-free assessment of the absorption and dispersion spectra of intracavity gas. In this first demonstration we measured the absorption and dispersion spectra of three combination bands of CO2 in the 1525 to 1620 nm range.Another comb-based FTS technique is noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), which combines phase modulation and cavity-enhancement to obtain broadband and highly sensitive absorption spectra. In this thesis we improved the NICE-OFCS technique in terms of stability, sensitivity and modeling of the NICE-OFCS signal. We implemented a model of the NICE-OFCS signal with multiline fitting for assessment of gas concentration. We also identified the optimum operating conditions of the NICE-OFCS systems for accurate gas concentration assessment.Finally, to improve the species selectivity we combined comb-based FTS with the Faraday rotation spectroscopy (FRS) technique. In this first demonstration of optical frequency comb Faraday rotation spectroscopy (OFC-FRS), we measured background and interference-free spectra of the entire Q- and R-branches of the fundamental vibrational band of nitric oxide at 5.3 μm showing good agreement with the theoretical model.
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| 3. |
- Hausmaninger, Thomas, 1987-
(författare)
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Mid- and near-infrared NICE-OHMS : techniques for ultra-sensitive detection of molecules in gas phase
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) is a technique for ultra-sensitive detection of molecular absorption and dispersion. For highest performance, the technique combines cavity enhancement (CE) with frequency modulation (FM); while the former increases the effective interaction length between the light and the analyte by several orders of magnitudes, the latter removes the in-coupling of 1/f noise and makes the signals background free. The combination of CE and FM also gives the technique an immunity to amplitude noise caused by the jitter of the laser frequency relative to the cavity resonance frequencies. All these properties make the technique suitable for ultra sensitive trace gas detection in the sub-parts-per-trillion (ppt) range. The aim of this thesis is to improve the performance of the NICE-OHMS technique and to increase its range of applications.The work in this thesis can be divided into three areas:Firstly, a mid-infrared (MIR)-NICE-OHMS instrumentation was developed. In a first realization an unprecedented white-noise equivalent absorption limit for Doppler broadened (Db) detection in the MIR of 3×10-9 cm-1Hz-1/2was demonstrated. This was subsequently improved to 2.4×10-10 cm-1Hz-1/2allowing for detection methane and its two main isotopologues (CH3D and 13CH4) at their natural abundance.Secondly, further development of an existing near-infrared NICE-OHMS system was performed. This resulted in an improved longtime stability and the first shot-noise limited NICE-OHMS system for Db detection with a noise equivalent absorption limit of 2.3×10-14 cm-1detected over 200 s. Thirdly, models and theoretical descriptions of NICE-OHMS signals under strong absorption conditions and from methane under high laser power were developed. It was experimentally verified that the models allow for a more accurate evaluation of NICE-OHMS signals under a wide range of conditions.
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| 4. |
- Silander, Isak, 1980-
(författare)
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Cavity enhanced optical sensing
- 2015
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- 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.
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