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We report airborne measurements of acetaldehyde (CH(3)CHO) during the first and second deployments of the National Aeronautics and Space Administration (NASA) Atmospheric Tomography Mission (ATom). The budget of CH(3)CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly-developed online air-sea exchange module. The upper limit of the global ocean net emission of CH(3)CHO is estimated to be 34 Tg a(−1) (42 Tg a(−1) if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH(3)CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH(3)CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid (PAA) is an ideal indicator of the rapid CH(3)CHO production in the remote troposphere. The higher-than-expected CH(3)CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

We present new data sets of black carbon (BC) aerosol mass mixing ratio (MMR) obtained from aircraft missions over North America, Europe, the Arctic, and the outflow region of Saharan Africa before and after trans-Atlantic transport. The data, collected from 2011 to 2013 with single-particle soot photometers, provide new insight into the variability and distribution of BC over global scales and refine understanding of AeroCom global model ensemble performance. The results indicate extensive global-scale longitudinal mixing of BC above altitude pressures as low as 400hPa. They also constrain the absolute and temporal variability of upper tropospheric BC MMR and point to opportunities for new tests of global aerosol models in the upper troposphere. A comparison to the AeroCom Phase II results generally reinforces previous estimates of the ensemble performance, except that it also strengthens confidence that the ensemble actually is biased high in the Arctic in all seasons.