Fourier transform and Vernier spectroscopy using optical frequency combs

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.