D. J. Mondeel

Oceanic distributions and emissions of short‐lived halocarbons

[1] Using data from seven cruises over a 10-year span, we report marine boundary layer mixing ratios (i.e., dry mole fractions as pmol mol 1 or ppt), degrees of surface seawater saturation, and air-sea fluxes of three short-lived halocarbons that are significant in tropospheric and potentially stratospheric chemistry. CHBr3 ,C H2Br2, and CH3I were all highly supersaturated almost everywhere, all the time. Highest saturations of the two polybrominated gases were observed in coastal waters and areas of upwelling, such as those near the equator and along ocean fronts. CH3I distributions reflected the different chemistry and cycling of this gas in both the water and the atmosphere. Seasonal variations in fluxes were apparent where cruises overlapped and were consistent among oceans. Undersaturations of these gases were noted at some locations in the Southern Ocean, owing to mixing of surface and subsurface waters, not necessarily biological or chemical sinks. The Pacific Ocean appears to be a much stronger source of CHBr3 to the marine boundary layer than the Atlantic. The high supersaturations, fluxes, and marine boundary layer mixing ratios in the tropics are consistent with the suggestion that tropical convection could deliver some portion of these gases and their breakdown products to the upper troposphere and lower stratosphere.

Considerable contribution of the Montreal Protocol to declining greenhouse gas emissions from the United States

Ozone depleting substances (ODSs) controlled by the Montreal Protocol are potent greenhouse gases (GHGs), as are their substitutes, the hydrofluorocarbons (HFCs). Here we provide for the first time a comprehensive estimate of U.S. emissions of ODSs and HFCs based on precise measurements in discrete air samples from across North America and in the remote atmosphere. Derived emissions show spatial and seasonal variations qualitatively consistent with known uses and largely confirm U.S. Environmental Protection Agency (EPA) national emissions inventories for most gases. The measurement-based results further indicate a substantial decline of ODS emissions from 2008 to 2014, equivalent to ~50% of the CO2-equivalent decline in combined emissions of CO2 and all other long-lived GHGs inventoried by the EPA for the same period. Total estimated CO2-equivalent emissions of HFCs were comparable to the sum of ODS emissions in 2014, but can be expected to decline in the future in response to recent policy measures.