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During the Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS), the National Polar-orbiting Operational Environmental Satellite System (NPOESS) Airborne Sounder TestbedInterferometer (NAST-I), flying aboard the high-altitude Proteus aircraft, observed the spatial distribution of infrared radiance across the 650–2700 cm⫺1 (3.7–15.4 μm) spectral region with a spectral resolution of 0.25 cm⫺1. NAST-I scans cross track with a moderate spatial resolution (a linear ground resolution equal to 13% of the aircraft altitude at nadir). The broad spectral coverage and high spectral resolution of this instrument provides abundant information about the surface and three-dimensional state of the atmosphere. In this paper, the NAST-I measurements and geophysical product retrieval methodology employed for CLAMS are described. Example results of surface properties and atmospheric temperature, water vapor, ozone, and carbon monoxide distributions are provided. The CLAMS NAST-I geophysical dataset is available for use by the scientific community.