Frequency-comb-based remote sensing of greenhouse gases over kilometer air paths

Increasing our understanding of regional greenhouse gas transport, sources, and sinks requires accurate, precise, continuous measurements of small gas enhancements over long ranges. We demonstrate a coherent dual frequency-comb spectroscopy technique capable of achieving these goals. Spectra are acquired spanning 5990 to 6260  cm−1 (1600–1670 nm) covering ∼700 absorption features from CO2, CH4, H2O, HDO, and CO213, across a 2 km path. The spectra have sub-1-kHz frequency accuracy, no instrument lineshape, and a 0.0033  cm−1 point spacing. They are fit with different absorption models to yield dry-air mole fractions of greenhouse gases. These results are compared with a point sensor under well-mixed conditions to evaluate the accuracy of models critical to global satellite-based trace gas monitoring. Under heterogeneous conditions, time-resolved data demonstrate tracking of small variations in mole fractions, with a precision <1  ppm for CO2 and <3  ppb for CH4 in 5 min. Portable systems could enable regional monitoring.