Direct Comb Vernier Spectroscopy for Fractional Isotopic Ratio Determinations.

Accurate isotopic composition analysis of the greenhouse-gasses emitted in the atmosphere is an important step to mitigate global climate warnings. Optical frequency comb-based spectroscopic techniques have shown ideal performance to accomplish the simultaneous monitoring of the different isotope substituted species of such gases. The capabilities of one such technique, namely, direct comb Vernier spectroscopy, to determine the fractional isotopic ratio composition are discussed. This technique combines interferometric filtering of the comb source in a Fabry-Perot that contains the sample gas, with a high resolution dispersion spectrometer to resolve the spectral content of each interacting frequency inside of the Fabry-Perot. Following this methodology, simultaneous spectra of ro-vibrational transitions of 12C16O2 and 13C16O2 molecules are recorded and analyzed with an accurate fitting procedure. Fractional isotopic ratio 13C/12C at 3% of precision is measured for a sample of CO2 gas, showing the potentialities of the technique for all isotopic-related applications of this important pollutant.

Tunable Microcavity-Stabilized Quantum Cascade Laser for Mid-IR High-Resolution Spectroscopy and Sensing.

The need for highly performing and stable methods for mid-IR molecular sensing and metrology pushes towards the development of more and more compact and robust systems. Among the innovative solutions aimed at answering the need for stable mid-IR references are crystalline microresonators, which have recently shown excellent capabilities for frequency stabilization and linewidth narrowing of quantum cascade lasers with compact setups. In this work, we report on the first system for mid-IR high-resolution spectroscopy based on a quantum cascade laser locked to a CaF2 microresonator. Electronic locking narrows the laser linewidth by one order of magnitude and guarantees good stability over long timescales, allowing, at the same time, an easy way for finely tuning the laser frequency over the molecular absorption line. Improvements in terms of resolution and frequency stability of the source are demonstrated by direct sub-Doppler recording of a molecular line.