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Discussion papers | Copyright
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 11 Jul 2018

Research article | 11 Jul 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Surface–atmosphere exchange of water-soluble gases and aerosols above agricultural grassland pre- and post-fertilisation

Robbie Ramsay1,2, Chiara F. Di Marco1, Mathew R. Heal2, Marsailidh M. Twigg1, Nicholas Cowan1, Matthew R. Jones1, Sarah R. Leeson1, William J. Bloss3, Louisa J. Kramer3, Leigh Crilley3, Matthias Sörgel4, Meinrat Andreae4,5, and Eiko Nemitz1 Robbie Ramsay et al.
  • 1Centre for Ecology & Hydrology (CEH), Edinburgh, EH26 0QB, UK
  • 2School of Chemistry, University of Edinburgh, West Mains Road, EH9 3JJ, UK
  • 3School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham, B15 2TT, UK
  • 4Max Plank Institute for Chemistry, Biogeochemistry Department, Mainz, P.O. Box 3060, Germany
  • 5Scripps Institution of Oceanography, University of California San Diego, La Jolla, CA 92093, USA

Abstract. The increasing use of intensive agricultural practices can lead to damaging consequences for the atmosphere through enhanced emissions of air pollutants. However, there are few direct measurements of the surface–atmosphere exchange of trace gases and water-soluble aerosols over agricultural grassland, particularly of reactive nitrogen compounds. In this study, we present measurements of the concentrations, fluxes and deposition velocities of the trace gases HCl, HONO, HNO3, SO2 and NH3, and their associated water-soluble aerosol counterparts Cl, NO2, NO3, SO42−, NH4+ as determined hourly for one month in May–June 2016 over agricultural grassland pre- and post-fertilisation. Measurements were made using the Gradient of Aerosols and Gases Online Registration (GRAEGOR) wet–chemical two–point gradient instrument. Emissions of NH3 peaked at 1460ngm−2s−1 three hours after fertilisation, with an emission of HONO peaking at 4.92ngm−2s−1 occurring five hours after fertilisation. Apparent emissions of NO3 aerosol were observed after fertilisation which, coupled with a divergence of HNO3 deposition velocity (Vd) from its theoretical maximum value, suggested the reaction of emitted NH3 with atmospheric HNO3 to form ammonium nitrate aerosol. The use of the conservative exchange fluxes of tot-NH4+ and tot-NO3 indicated net emission of tot-NO3, implying a ground source of HNO3 after fertilisation. Daytime concentrations of HONO remained above the detection limit (30ngm−3) throughout the campaign, suggesting a daytime source for HONO at the site. Whilst the mean Vd of NH4+ was with 0.93mm/s in the range expected for the accumulation mode, the larger average Vd for Cl (3.65mm/s), NO3 (1.97mm/s), SO42− (1.89mm/s) reflected the contribution of a super-micron fraction and decreased with increasing PM2.5/PM10 ratio (a proxy measurement for aerosol size), providing direct evidence of a size-dependence of aerosol deposition velocity for aerosol chemical compounds.

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Robbie Ramsay et al.
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Short summary
The affect of agricultural activities on the atmosphere requires more measurements of trace gases and water–soluble aerosols to better understand. This research presents one month of such measurements above agricultural grassland during a period of fertiliser application. It was found that emissions of the important trace gases ammonia and nitrous acid peaked after fertiliser use, and that the velocity at which the measured aerosols were deposited was dependent upon their size.
The affect of agricultural activities on the atmosphere requires more measurements of trace...