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Black carbon-containing aerosol particles play an important role in the direct and indirect radiative forcing of climate. However, the magnitude and sign of the net radiative effect is strongly dependent on the physical properties of the black carbon (BC) component of the particles, such as mass concentration, number size distribution and mixing state. Here we use a global aerosol model combined with aircraft measurements of BC particle number and size from the Single Particle Soot Photometer (SP2) to assess the realism with which these physical properties are predicted by global models. The comparison reveals a substantial mismatch between the measured and modelled BC size distribution over the size range of the SP2 instrument (90–400 nm BC diameter). The model predicts BC particle number concentrations a factor ~3.5–5.7 higher than measured and a mode diameter that is ~40–65 nm smaller than observed. More than ~90% of the model particles with dry diameters ≳260 nm contain BC, while the observations suggest only 14% on average. These model–observation biases in the BC properties are considerably greater than for the overall particle distribution, suggesting that the discrepancy is associated with model assumptions about the size and mixing state of the emitted carbonaceous particles. We expect the discrepancy in BC size distribution to be common among most global aerosol models, with implications for model estimates of absorption optical depth and direct radiative forcing., Atmospheric Chemistry and Physics, 13 (9), ISSN:1680-7375, ISSN:1680-7367

The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 “year without a summer”, and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, although there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km−2 and on Greenland from 31 to 194 kg km−2, as compared to the mean ice-core-derived estimates of roughly 50 kg km−2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought., Atmospheric Chemistry and Physics, 18 (3), ISSN:1680-7375, ISSN:1680-7367

We perform a model intercomparison of summertime high Arctic ( > 80°N) clouds observed during the 2008 Arctic Summer Cloud Ocean Study (ASCOS) campaign, when observed cloud condensation nuclei (CCN) concentrations fell below 1cm−3. Previous analyses have suggested that at these low CCN concentrations the liquid water content (LWC) and radiative properties of the clouds are determined primarily by the CCN concentrations, conditions that have previously been referred to as the tenuous cloud regime. The intercomparison includes results from three large eddy simulation models (UCLALES-SALSA, COSMO-LES, and MIMICA) and three numerical weather prediction models (COSMO-NWP, WRF, and UM-CASIM). We test the sensitivities of the model results to different treatments of cloud droplet activation, including prescribed cloud droplet number concentrations (CDNCs) and diagnostic CCN activation based on either fixed aerosol concentrations or prognostic aerosol with in-cloud processing. There remains considerable diversity even in experiments with prescribed CDNCs and prescribed ice crystal number concentrations (ICNC). The sensitivity of mixed-phase Arctic cloud properties to changes in CDNC depends on the representation of the cloud droplet size distribution within each model, which impacts autoconversion rates. Our results therefore suggest that properly estimating aerosol–cloud interactions requires an appropriate treatment of the cloud droplet size distribution within models, as well as in situ observations of hydrometeor size distributions to constrain them. The results strongly support the hypothesis that the liquid water content of these clouds is CCN limited. For the observed meteorological conditions, the cloud generally did not collapse when the CCN concentration was held constant at the relatively high CCN concentrations measured during the cloudy period, but the cloud thins or collapses as the CCN concentration is reduced. The CCN concentration at which collapse occurs varies substantially between models. Only one model predicts complete dissipation of the cloud due to glaciation, and this occurs only for the largest prescribed ICNC tested in this study. Global and regional models with either prescribed CDNCs or prescribed aerosol concentrations would not reproduce these dissipation events. Additionally, future increases in Arctic aerosol concentrations would be expected to decrease the frequency of occurrence of such cloud dissipation events, with implications for the radiative balance at the surface. Our results also show that cooling of the sea-ice surface following cloud dissipation increases atmospheric stability near the surface, further suppressing cloud formation. Therefore, this suggests that linkages between aerosol and clouds, as well as linkages between clouds, surface temperatures, and atmospheric stability need to be considered for weather and climate predictions in this region., Atmospheric Chemistry and Physics, 18 (15), ISSN:1680-7375, ISSN:1680-7367

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of −24 % and −35 % for particles with dry diameters >50 and >120 nm, as well as −36 % and −34 % for CCN at supersaturations of 0.2 % and 1.0 %, respectively. However, they seem to behave differently for particles activating at very low supersaturations (, Atmospheric Chemistry and Physics, 19 (13), ISSN:1680-7375, ISSN:1680-7367

Despite the importance of ice-nucleating particles (INPs) for climate and precipitation, our understanding of these particles is far from complete. Here, we investigated INPs at three coastal marine sites in Canada, two at mid-latitude (Amphitrite Point and Labrador Sea) and one in the Arctic (Lancaster Sound). For Amphitrite Point, 23 sets of samples were analyzed, and for Labrador Sea and Lancaster Sound, one set of samples was analyzed for each location. At all three sites, the ice-nucleating ability on a per number basis (expressed as the fraction of aerosol particles acting as an INP) was strongly dependent on the particle size. For example, at diameters of around 0.2µm, approximately 1 in 106 particles acted as an INP at −25°C, while at diameters of around 8µm, approximately 1 in 10 particles acted as an INP at −25°C. The ice-nucleating ability on a per surface-area basis (expressed as the surface active site density, ns) was also dependent on the particle size, with larger particles being more efficient at nucleating ice. The ns values of supermicron particles at Amphitrite Point and Labrador Sea were larger than previously measured ns values of sea spray aerosols, suggesting that sea spray aerosols were not a major contributor to the supermicron INP population at these two sites. Consistent with this observation, a global model of INP concentrations under-predicted the INP concentrations when assuming only marine organics as INPs. On the other hand, assuming only K-feldspar as INPs, the same model was able to reproduce the measurements at a freezing temperature of −25°C, but under-predicted INP concentrations at −15°C, suggesting that the model is missing a source of INPs active at a freezing temperature of −15°C., Atmospheric Chemistry and Physics, 18 (21), ISSN:1680-7375, ISSN:1680-7367