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Thermal infrared spectra can provide unique information on atmospheric ammonia enhancements, including those produced by agricultural, industrial, and biomass burning sources. In this work, we develop and test a quantitative ammonia retrieval algorithm using data from the airborne hyperspectral thermal emission spectrometer (HyTES) instrument over diverse targets, including persistent ammonia sources, such as cattle feedlots and a power plant, as well as a small, smoldering wildfire. Although no formal validation was possible due to lack of collocated observations, the HyTES ammonia values over feedlots in the California San Joaquin Valley are shown to be consistent within the estimated retrieval uncertainty of ∼20%–50% with in situ ammonia values collected over the same facilities during the 2013 DISCOVER-AQ field campaign. HyTES also observed meter-scale thermal hot spots associated with a small wildfire in Northern Arizona, which was determined to coincide with the emission of free ammonia, presumed to originate from the fire. This very localized emission source, not visible from satellite sensors, could be resolved in HyTES imagery. The ammonia enhancement immediately downwind from the smoldering fire, before the free ammonia reacted to form aerosols, was found to be distinguishable from the background with values three to ten times smaller than ammonia enhancements from the power plant and cattle feedlots, respectively. High-resolution detection and quantification of ammonia over nonpersistent sources like wildfires from HyTES shows that it is a powerful tool that can be used to improve regional scale fire emission inventories by accounting for the presence of temporally short ammonia processes.