This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a⁻¹ (range 34–144 Tg a⁻¹) and the median SOA source strength (natural and anthropogenic) is 19 Tg a⁻¹ (range 13–121 Tg a⁻¹). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a⁻¹ (range 16–121 Tg a⁻¹), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a⁻¹; range 13–20 Tg a⁻¹, with one model at 37 Tg a⁻¹). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a⁻¹ (range 28–209 Tg a⁻¹), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63° N to 52° S and 72° W to 124° E has been achieved within the Raman and polarization lidar network Polly^NET. This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. Polly^NET is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at http://polly.tropos.de/. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Ångström exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the Polly^NET locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of Polly^NET to support the establishment of a global aerosol climatology that covers the entire troposphere.

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

Primary and secondary aerosol particles originating from biomass burning contribute significantly to the atmospheric aerosol budget and thereby to both direct and indirect radiative forcing. Based on detailed measurements of a large number of biomass burning plumes of variable age in southern Africa, we show that the size distribution, chemical composition, single-scattering albedo, and hygroscopicity of biomass burning particles change considerably during the first 2–4 h of their atmospheric transport. These changes, driven by atmospheric oxidation and subsequent secondary aerosol formation, may reach a factor of 6 for the aerosol scattering coefficient and a factor >10 for the cloud condensation nuclei concentration. Since the observed changes take place over the spatial and temporal scales that are neither covered by emission inventories nor captured by large-scale model simulations, the findings reported here point out a significant gap in our understanding on the climatic effects of biomass burning aerosols.

Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM_2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM_2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m⁻², with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO₂ emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m⁻², which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM_2.5 concentrations.

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (N_tot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on N_tot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 10² cm⁻³) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 10³–10⁴ cm⁻³) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate N_tot (∼ 10²–10³ cm⁻³). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of N_tot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of N_tot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm⁻³, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for N_tot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.