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This dataset provides (1) the results of in situ aerosol particle property measurements collected over remote tropical areas of both Pacific and Atlantic Oceans during the NASA airborne Atmospheric Tomography (ATom) campaigns for ATom-1 and ATom-2 and (2) modeled outputs of comparable aerosol properties, atmospheric chemistry and meteorology at 70 m resolution from four chemical-transport models matched to the location and time of the aircraft measurements.