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A global model perturbed parameter ensemble of 60 simulations was used to explore how combinations of six parameters related to secondary organic aerosol (SOA) formation affect particle number concentrations and organic aerosol mass. The parameters represent the formation of organic compounds with different volatilities from biogenic and anthropogenic sources. The most plausible parameter combinations were determined by comparing the simulations against observations of the number concentration of particles larger than 3 nm diameter (N3), the number concentration of particles larger than 50 nm diameter (N50), and the organic aerosol (OA) mass concentration. The simulations expose a high degree of model equifinality in which the skill of widely different parameter combinations cannot be distinguished against observations. We therefore conclude that, based on the observations we have used, a six-parameter SOA scheme is under-determined. Nevertheless, the model skill in simulating N3 and N50 is clearly determined by the low-volatility and extremely low-volatility compounds that affect new particle formation and growth, and the skill in simulating OA mass is determined by the low-volatility and semi-volatile compounds. The biogenic low-volatility class of compounds that grow nucleated clusters and condense on all particles is found to have the strongest effect on the model skill in simulating N3, N50, and OA. The simulations also expose potential structural deficiencies in the model: we find that parameter combinations that are best for N3 and N50 are worst for OA mass, and the ensemble exaggerates the observed seasonal cycle of particle concentrations – a deficiency that we conclude requires an additional anthropogenic source of either primary or secondary particles.

Meteoric smoke particles (MSPs) provide a steady source of condensation nuclei to the Arctic lower stratosphere, with heterogeneous nucleation to sulphuric acid aerosol particles. Internally mixed meteoric-sulphuric particles likely also play a significant role in the formation of polar stratospheric clouds and thereby influence stratospheric ozone depletion chemistry, particularly in the quiescent stratosphere.In several Arctic winter field campaigns (EUPLEX 2002/3, RECONCILE 2009/10, ESSenCe 2010/11), in-situ stratospheric aerosol particle concentrations measurements were made from the high-altitude Geophysica aircraft, the COPAS instrument measuring total and refractory (non-volatile) particle concentrations at 20 km altitude (see Curtius et al., 2003; Weigel et al., 2014). These measurements are consistent with there being a substantial seasonal source of meteoric-sulphuric particles to the lower Arctic stratosphere, from each year’s influx of MSPs within the winter-time Arctic polar vortex. In this study we investigate the effect of MSPs on the quiescent Junge layer particle concentration as the polar vortex builds up and after it dissipates. We use the nudged configuration of the UM-UKCA stratosphere-troposphere composition-climate model to reproduce the vertical profile of stratospheric particles measured in-situ during the COPAS 2003 campaign. Our model simulates two types of stratospheric aerosol particles - pure sulphuric acid particles and sulphuric acid particles with a MSP-core. We show that the model is able to reproduce the vertical profile of aerosol particles observed during the COPAS measurements in winter 2003.Our findings illustrate the influx of MSP and SO2 from higher altitudes through the polar vortex, the winter-time build-up of SO2 triggering homogeneous nucleation of pure sulphuric particles, also with the seasonal source of MSP-core sulphuric particles nucleated heterogeneously. We assess the effects of MSPs on the quiescent period particle concentration in the Arctic during winter through to spring.

The widespread presence of meteoric smoke particles (MSPs) within a distinct class of stratospheric aerosol particles has become clear from in-situ measurements in the Arctic, Antarctic and at mid-latitudes. We apply an adapted version of the interactive stratosphere aerosol configuration of the composition-climate model UM-UKCA, to predict the global distribution of meteoric-sulphuric particles nucleated heterogeneously on MSP cores. We compare the UM-UKCA results to new MSP-sulphuric simulations with the European stratosphere-troposphere chemistry-aerosol modelling system IFS-CB05-BASCOE-GLOMAP.The simulations show a strong seasonal cycle in meteoric-sulphuric particle abundance results from the winter-time source of MSPs transported down into the stratosphere in the polar vortex. Coagulation during downward transport sees high latitude MSP concentrations reduce from ~500 per cm3 at 40km to ~20 per cm3 at 25km, the uppermost extent of the stratospheric aerosol particle layer (the Junge layer). Once within the Junge layer's supersaturated environment, meteoric-sulphuric particles form readily on the MSP cores, growing to 50-70nm dry-diameter (Dp) at 20-25km. Further inter-particle coagulation between these non-volatile particles reduces their number to 1-5 per cc at 15-20km, particle sizes there larger, at Dp ~100nm.The model predicts meteoric-sulphurics in high-latitude winter comprise >90% of Dp>10nm particles above 25km, reducing to ~40% at 20km, and ~10% at 15km. These non-volatile particle fractions are slightly less than measured from high-altitude aircraft in the lowermost Arctic stratosphere (Curtius et al., 2005; Weigel et al., 2014), and consistent with mid-latitude aircraft measurements of lower stratospheric aerosol composition (Murphy et al., 1998), total particle concentrations also matching in-situ balloon measurements from Wyoming (Campbell and Deshler, 2014). The MSP-sulphuric interactions also improve agreement with SAGE-II observed stratospheric aerosol extinction in the quiescent 1998-2002 period. Simulations with a factor-8-elevated MSP input form more Dp>10nm meteoric-sulphurics, but the increased number sees fewer growing to Dp ~100nm, the increased MSPs reducing the stratospheric aerosol layer’s light extinction.