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Troposphere carbon monoxide (CO), as well as other trace species retrieved with advanced ultraspectral remote sensors of Earth observing satellites, is critical in air quality observation, modelling, and forecasting. The retrieval algorithm and the accuracy of the parameters retrieved from passive satellite remote sounders must be validated. The Intercontinental Chemical Transport Experiment - North America (INTEXNA) and the European Aqua Thermodynamic Experiment (EAQUATE) provide important validation of satellite observations with ongoing satellite measurement programmes such as Terra, Aura, and Aqua. One of the experimental objectives is to validate chemical species observed from ultraspectral sounders with aircraft in situ measurements, such as the NPOESS Airborne Sounder Testbed-Interferometer (NAST-I). Detailed intercomparisons between aircraft in situ measured and NAST-I retrieved CO profiles were performed to assess the retrieval capability of a passive infrared spectral remote sounder. Validation results illustrate that the CO vertical structure can be obtained by the NAST-I. The thermal radiances are most sensitive to CO emissions from the free troposphere. However, the profile retrieval accuracy depends on the CO uncertainty in the terrestrial boundary layer. It is shown here that the CO distribution in the terrestrial boundary layer over the sea cannot be obtained with reliable accuracy where there is little contrast between the surface air and surface skin temperature. Copyright Y 2007 Royal Meteorological Society