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

Ultrasensitive detection of methane, isotopic carbon dioxide, carbon monoxide, formaldehyde, acetylene, and ethylene is performed in the spectral range 2.5–5 μm 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.