Ammonia in the summer Arctic marine boundary layer: Sources, Sinks and Implications
Abstract:The abundance of NH3 can influence new particle formation rates, aerosol chemical and optical properties, as well as N-sensitive ecosystems via deposition. Sources and sinks of gas-phase ammonia (NH3) are poorly constrained in the High Arctic due to a lack of field observations. In particular, both the magnitude and direction of sea-air NH3 exchange are highly uncertain, although previous studies suggest the open ocean is likely to act as a net sink at high latitudes.
In order to investigate potential NH3 sources, sinks and impacts, hourly gas-phase NH3 and particulate-phase NH4+ and SO42- measurements were taken from 13 July to 7 August 2014 aboard a research cruise throughout Baffin Bay and the eastern Canadian Arctic Archipelago. Simultaneous measurements of total seawater ammonium, pH and sea surface temperature were used to compute the compensation point (χ), which is the ambient NH3 concentration at which sea-air fluxes change direction. Ambient NH3 ranged from 30-650 ng m-3 throughout the cruise and was several orders of magnitude larger than measured χ values (0.4-10 ng m-3). Hence, the summertime Arctic Ocean is a strong net sink of NH3.
GEOS-Chem (a chemical transport model) was employed to examine the impact of seabird guano (feces) on surface NH3 concentrations. A simulation without guano-derived NH3 emissions yielded highly acidic aerosol and underestimated surface NH3 by several orders of magnitude. Including NH3 emission estimates from seabird guano greatly improved model-measurement comparison. The importance of seabird guano as an NH3 source was also investigated using the FLEXible PARTicle dispersion model driven by WRF meteorology (FLEXPART-WRF). FLEXPART-WRF results confirm that air masses with origins co-located with large seabird colonies were enriched in NH3, whereas those originating over the open ocean were depleted in NH3. The influence of NH3 from wildfires, as well as implications for N-deposition and aerosol neutralization are also discussed.