Aerosol measurements during COPE: composition, size and sources of CCN and IN at the interface between marine and terrestrial influences

Abstract

<p><strong>Abstract.</strong> We present measurements of boundary layer aerosol concentration, size and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation mode mass loadings were typically 2–3 μg m<sup>−3</sup>, the majority of which was sulphuric acid over the sea, or ammonium sulphate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ~150–280 cm<sup>−3</sup> at 0.1 % and 400–500 cm<sup>−3</sup> at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100–500 cm<sup>−3</sup>. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulphate, meaning marine sulphate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to sea spray, and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulphate, and black carbon. The CCN concentrations here were around six times higher than in the clean cases, and the cloud drop number concentrations were 3–4 times higher. Sources of ice nuclei (IN) were assessed by comparing different parameterisations of the nucleation of ice, using measured aerosol concentrations as input. The parameterisations based on total aerosol produced IN concentrations that agreed within an order of magnitude with measured first ice concentrations at cloud temperatures as low as −12 °C. Composition-specific parameterisations for mineral dust, fluorescent particles and sea spray OA were 3–4 orders of magnitude lower, meaning either a source of IN was present that was not characterised by our measurements, and/or one or more of the compositionspecific parameterisations greatly underestimated IN in this environment.</p>

An Approach to Removing Large Quantities of Atmospheric Greenhouse Gases

“…Alternatively, the Marshall-Palmer approximation accurately estimates droplet radii spectra for drizzle, rain, or storm events, and can be applied to perform more detailed droplet surface area estimates [18], [19]. The parameters and measurement methods used to characterize precipitation inside clouds and atmosphere volumes are described in [20]- [22].…”