The influence of clouds on radical concentrations: observations and modelling studies of HOx during the Hill Cap Cloud Thuringia (HCCT) campaign in 2010
- 1National Centre for Atmospheric Science, University of Leeds, Leeds, LS2 9JT, UK
- 2School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
- 3Leibniz-Institut für Troposphärenforschung (TROPOS), Permoserstr. 15, 04318 Leipzig, Germany
- 4National Centre for Atmospheric Science, University of York, York, YO10 5DD, UK
- 5Department of Chemistry, University of York, York, YO10 5DD, UK
- *now at: National Risk Management Research Laboratory, US Environmental Protection Agency, Research Triangle Park, North Carolina 27711, USA
Abstract. The potential for chemistry occurring in cloud droplets to impact atmospheric composition has been known for some time. However, the lack of direct observations and uncertainty in the magnitude of these reactions led to this area being overlooked in most chemistry transport models. Here we present observations from Mt Schmücke, Germany, of the HO2 radical made alongside a suite of cloud measurements. HO2 concentrations were depleted in-cloud by up to 90% with the rate of heterogeneous loss of HO2 to clouds necessary to bring model and measurements into agreement, demonstrating a dependence on droplet surface area and pH. This provides the first observationally derived assessment for the uptake coefficient of HO2 to cloud droplets and was found to be in good agreement with theoretically derived parameterisations. Global model simulations, including this cloud uptake, showed impacts on the oxidising capacity of the troposphere that depended critically on whether the HO2 uptake leads to production of H2O2 or H2O.