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Aerosol indirect effects continue to constitute one of the most important uncertainties for anthropogenic climate perturbations. Within the international AEROCOM initiative, the representation of aerosol-cloud-radiation interactions in ten different general circulation models (GCMs) is evaluated using three satellite datasets. The focus is on stratiform liquid water clouds since most GCMs do not include ice nucleation effects, and none of the model explicitly parameterises aerosol effects on convective clouds. We compute statistical relationships between aerosol optical depth (andtau; a) and various cloud and radiation quantities in a manner that is consistent between the models and the satellite data. It is found that the model-simulated influence of aerosols on cloud droplet number concentration (Nd) compares relatively well to the satellite data at least over the ocean. The relationship between andtau;a and liquid water path is simulated much too strongly by the models. This suggests that the implementation of the second aerosol indirect effect mainly in terms of an autoconversion parameterisation has to be revisited in the GCMs. A positive relationship between total cloud fraction (fcld) and andtau; a as found in the satellite data is simulated by the majority of the models, albeit less strongly than that in the satellite data in most of them. In a discussion of the hypotheses proposed in the literature to explain the satellite-derived strong f cldĝ€"andtau;a relationship, our results indicate that none can be identified as a unique explanation. Relationships similar to the ones found in satellite data between andtau;a and cloud top temperature or outgoing long-wave radiation (OLR) are simulated by only a few GCMs. The GCMs that simulate a negative OLRĝ€"andtau; a relationship show a strong positive correlation between andtau;a and fcld. The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of andtau;a, and parameterisation assumptions such as a lower bound on Nd. Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of andminus;1.5andplusmn;0.5 Wmandminus;2. In an alternative approach, the radiative flux perturbation due to anthropogenic aerosols can be broken down into a component over the cloud-free portion of the globe (approximately the aerosol direct effect) and a component over the cloudy portion of the globe (approximately the aerosol indirect effect). An estimate obtained by scaling these simulated clear- and cloudy-sky forcings with estimates of anthropogenic andtau;a and satellite-retrieved Ndĝ€"andtau;a regression slopes, respectively, yields a global, annual-mean aerosol direct effect estimate of andminus;0.4andplusmn;0.2 Wmandminus;2 and a cloudy-sky (aerosol indirect effect) estimate of andminus;0.7andplusmn;0.5 Wmandminus;2, with a total estimate of andminus;1.2andplusmn;0. 4 Wmandminus;2.

The AeroCom exercise diagnoses multicomponent aerosol modules in global modeling. In an initial assessment simulated global distributions for mass and mid-visible aerosol optical thickness (aot) were compared among 20 different modules. Model diversity was also explored in the context of previous comparisons. For the component combined aot general agreement has improved for the annual global mean. At 0.11 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca. 0.135) and space (satellite composite ca. 0.15). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture remain. Of particular concern are large model diversities for contributions by dust and carbonaceous aerosol, because they lead to significant uncertainty in aerosol absorption (aab). Since aot and aab, both, influence the aerosol impact on the radiative energy-balance, the aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) or space (e.g. correlations between aerosol and clouds).

The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated inter-model diversity of the global aerosol burden, and consequently global optical properties, as the results are largely controlled by modelspecific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g., the split between deposition pathways) and to a lesser extent by the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversities for these two species were caused by a few outliers. The experiment also showed that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.

Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The differences among the results (model diversities) for sources and sinks, burdens, particle sizes, water uptakes, and spatial dispersals have been established. These diversities have large consequences for the calculated radiative forcing and the aerosol concentrations at the surface. Processes and parameters are identified which deserve further research. The AeroCom all-models-average emissions are dominated by the mass of sea salt (SS), followed by dust (DU), sulfate (SO4), particulate organic matter (POM), and finally black carbon (BC). Interactive parameterizations of the emissions and contrasting particles sizes of SS and DU lead generally to higher diversities of these species, and for total aerosol. The lower diversity of the emissions of the fine aerosols, BC, POM, and SO 4, is due to the use of similar emission inventories, and does therefore not necessarily indicate a better understanding of their sources. The diversity of S04-sources is mainly caused by the disagreement on depositional loss of precursor gases and on chemical production. The diversities of the emissions are passed on to the burdens, but the latter are also strongly affected by the model-specific treatments of transport and aerosol processes. The burdens of dry masses decrease from largest to smallest: DU, SS, SO 4, POM, and BC. The all-models-average residence time is shortest for SS with about half a day, followed by SO4 and DU with four days, and POM and BC with six and seven days, respectively. The wet deposition rate is controlled by the solubility and increases from DU, BC, POM to SO4 and SS. It is the dominant sink for SO4, BC, and POM, and contributes about one third to the total removal of SS and DU species. For SS and DU we find high diversities for the removal rate coefficients and deposition pathways. Models do neither agree on the split between wet and dry deposition, nor on that between sedimentation and other dry deposition processes. We diagnose an extremely high diversity for the uptake of ambient water vapor that influences the particle size and thus the sink rate coefficients. Furthermore, we find little agreement among the model results for the partitioning of wet removal into scavenging by convective and stratiform rain. Large differences exist for aerosol dispersal both in the vertical and in the horizontal direction. In some models, a minimum of total aerosol concentration is simulated at the surface. Aerosol dispersal is most pronounced for SO4 and BC and lowest for SS. Diversities are higher for meridional than for vertical dispersal, they are similar for the individual species and highest for SS and DU. For these two components we do not find a correlation between vertical and meridional aerosol dispersal. In addition the degree of dispersals of SS and DU is not related to their residence times. SO4, BC, and POM, however, show increased meridional dispersal in models with larger vertical dispersal, and dispersal is larger for longer simulated residence times.

European loess sequences of the Marine Isotope Stage 3 (~60���25 kyr BP) show periods of strong dust accumulation alternating with episodes of reduced sedimentation, favoring soil development. In the western part of the loess belt centered around 50�� N, these variations appear to have been related to the North Atlantic rapid climate changes: the Dansgaard���Oeschger (DO) and Heinrich (H) events. It has been recently suggested that the North Atlantic climate signal can be detected further east, in loess deposits from Stayky (50��05.65' N, 30��53.92' E), Ukraine. Here we use climate and dust emission modeling to investigate this data interpretation. We focus on the areas north and northeast of the Carpathians, where loess deposits can be found, and the corresponding main dust sources must have been located as well. The simulations were performed with the LMDZ atmospheric general circulation model and the ORCHIDEE land surface model. They represent a reference "Greenland stadial" state and two perturbations, seen as sensitivity tests with respect to changes in the North Atlantic surface conditions between 30�� and 63�� N: a "Greenland interstadial" and an "H event". The main source for the loess deposits in the studied area is identified as a dust deflation band, with two very active spots located west-northwest from our reference site. Emissions only occur between February and June. Differences from one deflation spot to another, and from one climate state to another, are explained by analyzing the relevant meteorological and surface variables. Over most of the source region, the annual emission fluxes in the "interstadial" experiment are 30 to 50% lower than the "stadial" values; they would only be about 20% lower if the inhibition of dust uplift by the vegetation were not taken into account. Assuming that lower emissions result in reduced dust deposition leads us to the conclusion that the loess���paleosol stratigraphic succession in the Stayky area reflects indeed North Atlantic millennial variations. In the main deflation areas of Western Europe, the vegetation effect alone determined most of the (~50% on average) stadial���interstadial flux differences. Even if its impact in Eastern Europe is less pronounced, this effect remains a key factor in modulating aeolian emissions at the millennial timescale. Conditions favorable to initiating particularly strong dust storms within a few hundred kilometers upwind from our reference site, simulated in the month of April of the H event experiment, support the correlation of H events with peaks in grain size index in some very detailed loess profiles, indicating increased coarse sedimentation.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of 2 relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global basis, we find that the emission flux of dust with a geometric diameter up to 20 µm (PM20) is approximately 5000 Tg yr−1, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded datasets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this dataset is more accurate than current model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system. This research has been supported by the National Science Foundation (NSF) (grant nos. 1552519 and 1856389) and the Army Research Office (cooperative agreement number W911NF-20-2-0150). This research was further supported by the University of California President's Postdoctoral Fellowship awarded to Adeyemi A. Adebiyi and the European Union's Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement no. 708119 awarded to Samuel Albani and no. 789630 awarded to Martina Klose. Ramiro Checa-Garcia received funding from the European Union Horizon 2020 research and innovation grant 641816 (CRESCENDO). Akinori Ito received support from JSPS KAKENHI grant number 20H04329 and Integrated Research Program for Advancing Climate Models (TOUGOU) grant number JPMXD0717935715 from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. Peter R. Colarco and Adriana Rocha-Lima were supported by the NASA Atmospheric Composition: Modeling and Analysis Program (Richard Eckman, program manager) and the NASA Center for Climate Simulation (NCCS) for computational resources. Yue Huang was supported by NASA grant 80NSSC19K1346 awarded under the Future Investigators in NASA Earth and Space Science and Technology (FINESST) program. Ron L. Miller and Vincenzo Obiso received support from the NASA Modeling, Analysis and Prediction Program (NNG14HH42I) along with the NASA EMIT project and the Earth Venture Instrument program with computational resources from the NASA Center for Climate Simulation (NCCS). Samuel Albani received funding from MIUR (Progetto Dipartimenti di Eccellenza 2018-2022). Carlos Pérez García-Pando received support from the European Research Council (grant no. 773051, FRAGMENT), the EU H2020 project FORCES (grant no. 821205), the AXA Research Fund, and the Spanish Ministry of Science, Innovation and Universities (RYC-2015-18690 and CGL2017-88911-R). Longlei Li received support from the NASA EMIT project and the Earth Venture – Instrument program (grant no. E678605). Yves Balkanski and Ramiro Checa-Garcia received funding from the PolEASIA ANR project under allocation ANR-15-CE04-0005. Peer Reviewed "Article signat per 20 autors/es: Jasper F. Kok, Adeyemi A. Adebiyi, Samuel Albani, Yves Balkanski, Ramiro Checa-Garcia, Mian Chin, Peter R. Colarco, Douglas S. Hamilton, Yue Huang, Akinori Ito, Martina Klose, Danny M. Leung, Longlei Li, Natalie M. Mahowald, Ron L. Miller, Vincenzo Obiso, Carlos Pérez García-Pando, Adriana Rocha-Lima, Jessica S. Wan, and Chloe A. Whicker"

International audience; Purpose of Review: Natural archives are imprinted with signs of the past variability of some aerosol species in connection to major climate changes. In certain cases, it is possible to use these paleo-observations as a quantitative tool for benchmarking climate model simulations. Where are we on the path to use observations and models in connection to define an envelope on aerosol feedback onto climate? Recent Findings: On glacial-interglacial time scales, the major advances in our understanding refer to mineral dust, in terms of quantifying its global mass budget, as well as in estimating its direct impacts on the atmospheric radiation budget and indirect impacts on the oceanic carbon cycle. Summary: Even in the case of dust, major uncertainties persist. More detailed observational studies and model intercomparison experiments such as in the Paleoclimate Modelling Intercomparison Project phase 4 will be critical in advancing the field. The inclusion of new processes such as cloud feedbacks and studies focusing on other aerosol species are also envisaged.