Intracavity trace molecular detection with a broadband mid-IR frequency comb source

Abstract: Ultrasensitive detection of methane, isotopic carbon dioxide, carbon monoxide, formaldehyde, acetylene and ethylene is performed in the spectral range 2.5 - 5 \mu m using intracavity spectroscopy in broadband optical parametric oscillators (OPOs). The OPOs were operated near degeneracy and synchronously pumped either by a mode-locked erbium (1560 nm) or thulium (2050 nm) fiber laser. A large instantaneous bandwidth of up to 800 cm$^{-1}$ allows for simultaneous detection of several gases. We observe an effective path length enhancement due to coherent interaction inside the OPO cavity and achieve part-per-billion sensitivity levels. The measured spectral shapes are in good agreement with a model that takes into account group delay dispersion across the broad OPO frequency band.