We demonstrate the use of compact solar-tracking Fourier transform spectrometers (Bruker EM27/SUN) for differential measurements of the column-averaged dry-air mole fractions of CH₄ and CO₂ within urban areas. Using Allan variance analysis, we show that the differential column measurement has a precision of 0.01 % for X_CO2 and X_CH4 with an optimum integration time of 10 min, corresponding to Allan deviations of 0.04 ppm and 0.2 ppb, respectively. The sensor system is very stable over time and after relocation across the continent. We report tests of the differential column measurement, and its sensitivity to emission sources, by measuring the downwind-minus-upwind column difference ΔX_CH4 across dairy farms in the Chino area, California, and using the data to verify emissions reported in the literature. Ratios of spatial column differences ΔX_CH4∕ΔX_CO2 were observed across Pasadena within the Los Angeles basin, indicating values consistent with regional emission ratios from the literature. Our precise, rapid measurements allow us to determine significant short-term variations (5–10 min) of X_CO2 and X_CH4 and to show that they represent atmospheric phenomena.

Overall, this study helps establish a range of new applications for compact solar-viewing Fourier transform spectrometers. By accurately measuring the small differences in integrated column amounts across local and regional sources, we directly observe the mass loading of the atmosphere due to the influence of emissions in the intervening locale. The inference of the source strength is much more direct than inversion modeling using only surface concentrations and less subject to errors associated with small-scale transport phenomena.