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The heterogeneous hydrolysis of N2O5 on the surface ofdeliquescent aerosol leads to HNO3 formation and acts as a major sink ofNOx in the atmosphere during night-time. The reaction constant of thisheterogeneous hydrolysis is determined by temperature (T), relative humidity(RH), aerosol particle composition, and the surface area concentration(S). However, these parameters were not comprehensively considered in theparameterization of the heterogeneous hydrolysis of N2O5 in previousmass-based 3-D aerosol modelling studies. In this investigation, we propose asophisticated parameterization (NewN2O5) of N2O5 heterogeneoushydrolysis with respect to T, RH, aerosol particle compositions, and S basedon laboratory experiments. We evaluated closure between NewN2O5 and astate-of-the-art parameterization based on a sectional aerosol treatment. Thecomparison showed a good linear relationship (R =  0.91) between these twoparameterizations. NewN2O5 was incorporated into a 3-D fully online coupledmodel, COSMO–MUSCAT, with the mass-based aerosol treatment. As a case study,we used the data from the HOPE Melpitz campaign (10–25 September 2013) tovalidate model performance. Here, we investigated the improvement of nitrateprediction over western and central Europe. The modelled particulatenitrate mass concentrations ([NO3−]) were validated by filtermeasurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz).The modelled [NO3−] was significantly overestimated for this periodby a factor of 5–19, with the corrected NH3 emissions (reduced by50 %) and the original parameterization of N2O5 heterogeneoushydrolysis. The NewN2O5 significantly reduces the overestimation of[NO3−] by  ∼  35 %. Particularly, the overestimationfactor was reduced to approximately 1.4 in our case study (12,17–18 and 25 September 2013) when [NO3−] was dominated by local chemicalformations. In our case, the suppression of organic coating was negligibleover western and central Europe, with an influence on [NO3−] of lessthan 2 % on average and 20 % at the most significant moment. To obtain asignificant impact of the organic coating effect, N2O5, SOA, andNH3 need to be present when RH is high and T is low. However,those conditions were rarely fulfilled simultaneously over western andcentral Europe. Hence, the organic coating effect on the reaction probability ofN2O5 may not be as significant as expected over western andcentral Europe

atmospheric chemistry and physics

A parameterization of the heterogeneous hydrolysis of N&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;O&amp;lt;sub&amp;gt;5&amp;lt;/sub&amp;gt; for mass-based aerosol models: improvement of particulate nitrate prediction