[1] The processes driving current changes in Arctic atmospheric composition and climate are still uncertain. In particular the relative contributions of major source regions from the midlatitudes remain a matter of debate in the literature. The objectives of this study are to better quantify the relative contributions of different processes governing the transport of pollution from the midlatitudes to the Arctic and the relative contributions of different geopolitical source regions. We use a suite of observational data sets (including the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaigns and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument) to constrain a global aerosol simulation from the ECHAM5-HAMMOZ model. Preliminary comparison of model results with vertical profiles of sulfate and black carbon (BC) collected during the ARCTAS campaigns and with aerosol extinction time series retrieved from CALIOP indicates that the model underestimates export of aerosols from the planetary boundary layer to the free troposphere in the midlatitudes and long-range transport of aerosols from the midlatitudes toward the Arctic. In contrast, observed CO profiles are relatively well simulated, which points to a possible problem with wet scavenging. Decreasing the prescribed aerosol scavenging coefficients within the range of experimental data available in the literature significantly improves the agreement with observations.

Stratospheric aerosols play a significant role in stratospheric chemistry. In the past, it was assumed that only liquid droplets are present in the stratosphere. Nevertheless, a few lidar measurements have shown that sudden enhancement of aerosol content in the middle stratosphere could be due to meteoritic debris. Aircraft measurements have shown that solid particles can be found in the lower stratosphere; these particles are mainly soot, but also include some interplanetary material. In order to better document the various characteristics of aerosols in the unperturbed stratosphere (i.e., free of volcanic aerosols), we have performed observations using different balloon-borne instruments (Stratospheric and Tropospheric Aerosol Counter (STAC), Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON), and Micro Radiometre Ballon (MicroRADIBAL)) and also some satellite data (Global ozone monitoring by occultation of stars Envisat (GOMOS-Envisat)). These instruments allow us to obtain the number of particles in different size classes, the wavelength dependence of aerosol extinction, and the radiance of the light scattered by aerosols. Combining all the data together, it appears that significant amounts of particles are ubiquitous in the middle stratosphere, above the canonical sulfate aerosol layer. "Background'' interplanetary dusts in low concentration are likely present in the stratosphere. Above 30 km, interplanetary dust and largest grains from meteoroid disintegration dominate. Although the disintegration of meteoroids occurs in the upper stratosphere or in the mesosphere at all latitudes, these solid aerosols can be transported to the polar regions by the general circulation and can descend into the middle and lower stratosphere during winter mesospheric descents. Between about 22 km and 30 km, soot particles contribute to the population of aerosols at all latitudes. These soot, likely originating from biomass burning at all latitudes, could be injected into the lower stratosphere by the pyroconvective effect and can then reach the middle stratosphere perhaps owing to the gravitophotophoresis effect as was theoretically proposed. In the lower unperturbed stratosphere, liquid sulfate aerosols dominate, although soot particles are still present. Local horizontal and vertical enhancements of solid aerosols have sometimes been detected, although their origin is not yet determined. The presence of these solid particles can strongly bias the interpretation of in situ and remote sensing measurements when only the presence of liquid aerosols is assumed. Therefore, a new strategy of measurement will be necessary in the future to better characterize the stratospheric aerosol content free of volcanic particles

Abstract. Mineral dust from arid areas is a major component of global aerosol and has strong interactions with climate and biogeochemistry.

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO₂ injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the upper troposphere and lower stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected from satellites by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and from the surface by the Network for the Detection of Atmospheric Composition Changes (NDACC) lidar deployed at OHP (Observatoire de Haute-Provence, France). By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro Radiomètre Ballon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the surface area density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15–0.21 μm, 5.5–14.7 μm² cm⁻³, 5.5–29.5 × 10⁻⁴ km⁻¹, and 4.9–12.6 × 10⁻¹⁰ kg[S] kg⁻¹[air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70–80 days, a value much shorter than the 12–14 months calculated for aerosols from the 1991 eruption of Mt Pinatubo. The OSIRIS stratospheric aerosol optical depth (AOD) at 750 nm is enhanced by a factor of 6, with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14–15 km are largely modulated by stratosphere–troposphere exchange processes. The spatial extent of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18–20 km, in agreement with lidar observations. Good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations, with a maximum located about 1 km above the tropopause ranging from 1 to 2 × 10⁻⁹ kg[S] kg⁻¹[air], which is one order of magnitude higher than the background level