Open-path cavity ring-down spectroscopy for trace gas measurements in ambient air.

The present work used a near-infrared methane cavity ring-down spectroscopy (CRDS) sensor to examine performance and limitations of open-path CRDS for atmospheric measurements. A simple purge-enclosure was developed to maintain high mirror reflectivity and allowed >100 hours of operation with mirror reflectivity above 0.99996. We characterized effects of aerosols on ring-down decay signals and found the dominant effect to be fluctuations by large super-micron particles. Simple software filtering approaches were developed to combat these fluctuations allowing noise-equivalent sensitivity of ~6x10-10 cm-1HJ Hz-1/2 within a factor of ~3 of closed-path systems (based on stability of the absorption baseline). Sensor measurements were validated against known methane concentrations in a closed-path configuration, while open-path validation was performed by side-by-side comparison with a commercial closed-path system.