Uncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of −0.07 W m−2, and regional changes of −2 W m−2 (Africa) and −0.5 W m−2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.

Abstract. In this paper, we present the implementation and evaluation of the aerosol microphysics module SALSA2.0 in the framework of the aerosol–chemistry–climate model ECHAM-HAMMOZ. It is an alternative microphysics module to the default modal microphysics scheme M7 in ECHAM-HAMMOZ. The SALSA2.0 implementation within ECHAM-HAMMOZ is evaluated against observations of aerosol optical properties, aerosol mass, and size distributions, comparing also to the skill of the M7 implementation. The largest differences between the implementation of SALSA2.0 and M7 are in the methods used for calculating microphysical processes, i.e., nucleation, condensation, coagulation, and hydration. These differences in the microphysics are reflected in the results so that the largest differences between SALSA2.0 and M7 are evident over regions where the aerosol size distribution is heavily modified by the microphysical processing of aerosol particles. Such regions are, for example, highly polluted regions and regions strongly affected by biomass burning. In addition, in a simulation of the 1991 Mt. Pinatubo eruption in which a stratospheric sulfate plume was formed, the global burden and the effective radii of the stratospheric aerosol are very different in SALSA2.0 and M7. While SALSA2.0 was able to reproduce the observed time evolution of the global burden of sulfate and the effective radii of stratospheric aerosol, M7 strongly overestimates the removal of coarse stratospheric particles and thus underestimates the effective radius of stratospheric aerosol. As the mode widths of M7 have been optimized for the troposphere and were not designed to represent stratospheric aerosol, the ability of M7 to simulate the volcano plume was improved by modifying the mode widths, decreasing the standard deviations of the accumulation and coarse modes from 1.59 and 2.0, respectively, to 1.2 similar to what was observed after the Mt. Pinatubo eruption. Overall, SALSA2.0 shows promise in improving the aerosol description of ECHAM-HAMMOZ and can be further improved by implementing methods for aerosol processes that are more suitable for the sectional method, e.g., size-dependent emissions for aerosol species and size-resolved wet deposition.

Identification of aerosol types is important, because different aerosol types have different effects on health, visibility and climate change. The space‐borne lidar CALIOP on‐board the CALIPSO satellite provides information on the types of aerosols in the separate layers that can be detected with this instrument. In this study, the aerosol subtypes of CALIOP measurements are compared with daily aerosol types derived from AERONET level 2.0 inversion data. AERONET aerosol types are categorized by single scattering albedo and Ångström exponent values. The comparison shows that 70% of the CALIOP and AERONET aerosol types are in agreement. Best agreement is achieved for dust and polluted dust types.

Abstract. Chemistry transport models (CTMs) are an indispensable tool for studying and predicting atmospheric and climate effects associated with carbonaceous aerosol from open biomass burning (BB); this type of aerosol is known to contribute significantly to both global radiative forcing and to episodes of air pollution in regions affected by wildfires. Improving model performance requires systematic comparison of simulation results with measurements of BB aerosol and elucidation of possible reasons for discrepancies between them, which, by default, are frequently attributed in the literature to uncertainties in emission data. Based on published laboratory data on the atmospheric evolution of BB aerosol and using the volatility basis set (VBS) framework for organic aerosol modeling, we examined the importance of taking gas-particle partitioning and oxidation of semivolatile organic compounds (SVOCs) into account in simulations of the mesoscale evolution of smoke plumes from intense wildfires that occurred in western Russia in 2010. Biomass burning emissions of primary aerosol components were constrained with PM 10 and CO data from the air pollution monitoring network in the Moscow region. The results of the simulations performed with the CHIMERE CTM were evaluated by considering, in particular, the ratio of smoke-related enhancements in PM 10 and CO concentrations ( PM 10 and CO) measured in Finland (in the city of Kuopio), nearly 1000 km downstream of the fire emission sources. It is found that while the simulations based on a "conventional" approach to BB aerosol modeling (disregarding oxidation of SVOCs and assuming organic aerosol material to be non-volatile) strongly underestimated values of PM 10 / CO observed in Kuopio (by a factor of 2), employing the "advanced" representation of atmospheric processing of organic aerosol material resulted in bringing the simulations to a much closer agreement with the ground measurements. Furthermore, taking gas-particle partitioning and oxidation of SVOCs into account is found to result in a major improvement of the agreement of simulations and satellite measurements of aerosol optical depth, as well as in considerable changes in predicted aerosol composition and top-down BB aerosol emission estimates derived from AOD measurements.

Optically thick smoke aerosol plumes originating from biomass burning (BB) in the southwestern African Savanna during the austral spring are transported westward by the free tropospheric winds to primarily overlie vast stretches of stratocumulus cloud decks in the southeast Atlantic. We evaluated the simulations of long‐range transport of BB aerosol by the Goddard Earth Observing System (GEOS‐5) and four other global aerosol models over the complete South African‐Atlantic region using Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) observations to find any distinguishing or common model biases. Models, in general, captured the vertical distribution of aerosol over land but exhibited some common features after long‐range transport of smoke plumes that were distinct from that of CALIOP. Most importantly, the model‐simulated BB aerosol plumes quickly descend to lower levels just off the western coast of the continent, while CALIOP data suggest that smoke plumes continue their horizontal transport at elevated levels above the marine boundary layer. This is crucial because the sign of simulated aerosol semidirect effect can change depending on whether the bulk of the absorbing aerosols is present within or above the cloud levels in a model. The levels to which the aerosol plumes get subsided and the steepness of their descent vary amongst the models and amongst the different subregions of the domain. Investigations into possible causes of differences between GEOS‐5 and CALIOP aerosol transport over the ocean revealed a minimal role of aerosol removal process representation in the model as opposed to model dynamics.