The resonance fluorescence instrument for the measurement of atmospheric CO described by Volz and Kley <1985> was characterized in the laboratory and adapted for use on aircraft. A major finding was that the background signal is largely due to continuum resonance Raman scattering by molecular oxygen and thus cannot be reduced by better design. The instrument was deployed on the United Kingdom Meteorological Office (UKMO) C-130 Hercules during August 1993 and in subsequent missions. The instrument achieved a detection limit (3&sgr;) of 5 ppb at a time resolution of 30 s. For a typical CO concentration of 100 ppb, the signal-to-noise ratio (1&sgr;) was 15 for an integration time of 2 s, which was the minimum time resolution that could be obtained during the flights because of limited pump capacity. Data collected over the North Atlantic show distinct layers of CO above the atmospheric boundary layer (ABL) that are well correlated with enhanced NOy mixing ratios and indicate transport of pollution from the American continent. Such layers, albeit much less pronounced, were encountered in westerly flow in the midtroposphere west of the coast of Portugal. Fairly high mixing ratios were observed in the lower troposphere associated with transport from southern Europe. ¿ American Geophysical Union 1996