Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere

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.