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This dataset provides concentrations of volatile organic compounds (VOCs) measured by the Trace Organic Gas Analyzer (TOGA) during airborne campaigns conducted by NASA's Atmospheric Tomography (ATom) mission. Specific data were obtained for radical precursors, tracers of anthropogenic and biogenic activities, tracers of urban and biomass combustion emissions, products of oxidative processing, precursors to aerosol formation, and compounds important for aerosol modification and transformation. TOGA measures a wide range of VOCs with high sensitivity (ppt or lower), frequency (2.0 min.), accuracy (15% or better), and precision (<3%). ATom deployed an extensive gas and aerosol payload on the NASA DC-8 aircraft for systematic, global-scale sampling of the atmosphere, profiling continuously from 0.2 to 12 km altitude. Flights occurred in each of 4 seasons from 2016 to 2018.