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Global atmospheric dust is simulated using the Dust Entrainment and Deposition (DEAD) model in combination with the global-scale Oslo chemical transport model CTM2 using meteorological data for 1996. Dust sources are calculated using both mean wind speeds with model resolution T63 and subgrid wind speeds. Different data sets are used to describe soil erodibility. We explain how the different assumptions about dust production affect atmospheric dust burden and deposition. Some aspects of the annual dust cycle, such as the east Asian dust emissions, are largely dependent on the data used to determine soil erodibility. Other aspects, such as the timing of the maximum in the African plume at Northern Hemisphere summer, are well modeled with all data sets applied here. We show that the daily variation in optical depth at Cape Verde on the west coast of Africa is well simulated when we assume that erodibility is correlated with surface reflectivity from Moderate-Resolution Imaging Spetroradiometer (MODIS) satellite data. Using a subgrid probability density function of wind speed to drive the dust sources facilitates dust emissions in areas with low wind speeds. Dust concentrations in remote areas are sensitive to the parameterization of wet deposition. Our results point out the need for a detailed soil erodibility data set for global dust modeling, and they suggest that surface reflectivity is potentially valuable for producing or evaluating such data sets.

An observationally constrained time series of historical aerosol effective radiative forcing (ERF) from 1750 to 2019 is developed in this study. We find that the time history of aerosol ERFs diagnosed in CMIP6 models exhibits considerable variation and explore how the time history of aerosol forcing influences the probability distributions of present‐day aerosol forcing and emergent metrics such as climate sensitivity. Using a simple energy balance model, trained on CMIP6 climate models and constrained by observed near‐surface warming and ocean heat uptake, we derive estimates for the historical aerosol forcing. We find 2005–2014 mean aerosol ERF to be −1.1 (−1.8 to −0.5) W m−2 relative to 1750. Assuming recently published historical emissions from fossil fuel and industrial sectors and biomass burning emissions from SSP2‐4.5, aerosol ERF in 2019 is −0.9 (−1.5 to −0.4) W m−2. There is a modest recovery in aerosol forcing (+0.025 W m−2 decade−1) between 1980 and 2014. This analysis also gives a 5%–95% range of equilibrium climate sensitivity of 1.8°C –5.1°C (best estimate 3.1°C) with a transient climate response of 1.2°C –2.6°C (best estimate 1.8°C). Plain Language Summary: There are two main human drivers of climate change: (a) Greenhouse gas emissions, which warm the planet; and (b) air pollution (aerosols) that offset some of this warming. Unfortunately, disentangling the effects of historical aerosol cooling is difficult based on the available observations. Therefore, we often use climate models to estimate how much aerosols have cooled the Earth since the start of the Industrial Revolution. Over the mid‐to‐late 20th Century, some climate models simulate less warming compared to 1850 than has been observed. This may be because aerosol cooling in some climate models is too strong. Our approach combines the relationships between aerosol emissions and their cooling effects on temperature from 11 climate models with simpler representations of the underlying physics. This simpler mathematical framework allows us to more fully account for uncertainty in both aerosol cooling and its effects on surface temperature and ocean heat uptake by running a much larger set of simulations. Our results suggest that the effect of aerosol cooling has only unwound slowly since 1980, and that it is difficult to determine how sensitive the climate is from this method. Key Points: We determine the most plausible time history of aerosol forcing that matches surface temperature and Earth energy uptake constraintsConstrained aerosol forcing shows a modest recovery between 1980 and 2014, slower than the rate simulated by many CMIP6 modelsThe best estimate aerosol forcing using this method is −1.10 W m−2 for 2005–2014 relative to 1750 [ABSTRACT FROM AUTHOR]

The response of the hydrological cycle to climate forcings can be understood within the atmospheric energy budget framework. In this study precipitation and energy budget responses to five forcing agents are analyzed using 10 climate models from the Precipitation Driver Response Model Intercomparison Project (PDRMIP). Precipitation changes are split into a forcing-dependent fast response and a temperature-driven hydrological sensitivity. Globally, when normalized by top-of-atmosphere (TOA) forcing, fast precipitation changes are most sensitive to strongly absorbing drivers (CO2, black carbon). However, over land fast precipitation changes are most sensitive to weakly absorbing drivers (sulfate, solar) and are linked to rapid circulation changes. Despite this, land-mean fast responses to CO2 and black carbon exhibit more intermodel spread. Globally, the hydrological sensitivity is consistent across forcings, mainly associated with increased longwave cooling, which is highly correlated with intermodel spread. The land-mean hydrological sensitivity is weaker, consistent with limited moisture availability. The PDRMIP results are used to construct a simple model for land-mean and sea-mean precipitation change based on sea surface temperature change and TOA forcing. The model matches well with CMIP5 ensemble mean historical and future projections, and is used to understand the contributions of different drivers. During the twentieth century, temperature-driven intensification of land-mean precipitation has been masked by fast precipitation responses to anthropogenic sulfate and volcanic forcing, consistent with the small observed trend. However, as projected sulfate forcing decreases, and warming continues, land-mean precipitation is expected to increase more rapidly, and may become clearly observable by the mid-twenty-first century. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols such as sulfate and black carbon (BC) generate inhomogeneous radiative forcing and can affect precipitation in distinct ways compared to greenhouse gases (GHGs). Their regional effects on the atmospheric energy budget and circulation can be important for understanding and predicting global and regional precipitation changes, which act on top of the background GHG-induced hydrological changes. Under the framework of the Precipitation Driver Response Model Intercomparison Project (PDRMIP), multiple models were used for the first time to simulate the influence of regional (Asian and European) sulfate and BC forcing on global and regional precipitation. The results show that, as in the case of global aerosol forcing, the global fast precipitation response to regional aerosol forcing scales with global atmospheric absorption, and the slow precipitation response scales with global surface temperature response. Asian sulfate aerosols appear to be a stronger driver of global temperature and precipitation change compared to European aerosols, but when the responses are normalized by unit radiative forcing or by aerosol burden change, the picture reverses, with European aerosols being more efficient in driving global change. The global apparent hydrological sensitivities of these regional forcing experiments are again consistent with those for corresponding global aerosol forcings found in the literature. However, the regional responses and regional apparent hydrological sensitivities do not align with the corresponding global values. Through a holistic approach involving analysis of the energy budget combined with exploring changes in atmospheric dynamics, we provide a framework for explaining the global and regional precipitation responses to regional aerosol forcing. [ABSTRACT FROM AUTHOR]

Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO2, NO2, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. This reduction in UV-E over the industrial period is particularly large in highly populated regions. [ABSTRACT FROM AUTHOR]

The effect of anthropogenic emissions from China on global burdens of ozone, sulphate, organic carbon (OC) and black carbon (BC) aerosols is examined, using the three-dimensional chemistry transport model Oslo CTM2. Two model simulations were performed, the first with global present-day emissions and the second with the anthropogenic emissions from China set to their pre-industrial levels. The global radiative forcing for these species is then calculated. Industrial emissions from China are found to account for a 4–5% increase in the global burden of OC aerosol, the change in secondary organic aerosol being slightly less than that of primary organic aerosol. A 10% increase in the global sulphate aerosol burden is calculated, and the increase in BC is 23%. The global radiative forcing of aerosols from China was calculated to be −62, −3.7, −13 and 89 mW m−2, for sulphate, secondary organic, primary organic and BC aerosols, respectively. The increase in ozone causes a forcing of 77 mW m−2. [ABSTRACT FROM AUTHOR]

The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA). Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics). A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr-1 by allowing semivolatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA) values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA) is the dominant OA component) than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%-60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes. Reducing the yield for β-pinene and limonene oxidation in line with recent measurements reduces the global fraction of SOA formed from NO3 oxidation products from 27% to about 21%. This study underscores the need for SOA to be represented in a more realistic way in global aerosol models in order to better reproduce observations of organic aerosol burdens in industrialised and biomass burning regions. [ABSTRACT FROM AUTHOR]

We have used the MODIS satellite data and two global aerosol models to investigate the relationships between aerosol optical depth (AOD) and cloud parameters that may be affected by the aerosol concentration. The relationships that are studied are mainly between AOD, on the one hand, and cloud cover, cloud liquid water path, and water vapour, on the other. Additionally, cloud droplet effective radius, cloud optical depth, cloud top pressure and aerosol Ångström exponent, have been analysed in a few cases. In the MODIS data we found, as in earlier studies, an enhancement in the cloud cover with increasing AOD. We find it likely that most of the strong increase in cloud cover with AOD, at least for AOD<0.2, is a result of aerosol-cloud interactions and a prolonged cloud lifetime. Large and mesoscale weather systems seem not to be a cause for the increase in cloud cover with AOD in this range. Sensitivity simulations show that when water uptake of the aerosols is not taken into account in the models the modelled cloud cover mostly decreases with AOD. Part of the relationship found in the MODIS data for AOD>0.2 can be explained by larger water uptake close to the clouds since relative humidity is higher in regions with higher cloud cover. The efficiency of the hygroscopic growth depends on aerosol type, the hygroscopic nature of the aerosol, the relative humidity, and to some extent the cloud screening. By analysing the Ångström exponent we find that the hygroscopic growth of the aerosol is not likely to be a main contributor to the cloud cover increase with AOD. Since the largest increase in cloud cover with AOD is for low AOD (~0.2) and thus also for low cloud cover, we argue that cloud contamination is not likely to play a large role. However, interpretation of the complex relationships between AOD and cloud parameters should be made with great care and further work is clearly needed. [ABSTRACT FROM AUTHOR]

Nine different global models with detailed aerosol modules have independently produced instantaneous direct radiative forcing due to anthropogenic aerosols. The anthropogenic impact is derived from the difference of two model simulations with prescribed aerosol emissions, one for present-day and one for pre-industrial conditions. The difference in the solar energy budget at the top of the atmosphere (ToA) yields a new harmonized estimate for the aerosol direct radiative forcing (RF) under all-sky conditions. On a global annual basis RF is -0.22Wm-2, ranging from +0.04 to -0.41Wm-2, with a standard deviation of ±0.16Wm-2. Anthropogenic nitrate and dust are not included in this estimate. No model shows a significant positive all-sky RF. The corresponding clear-sky RF is -0.68Wm-2. The cloud-sky RF was derived based on all-sky and clear-sky RF and modelled cloud cover. It was significantly different from zero and ranged between -0.16 and +0.34Wm-2. A sensitivity analysis shows that the total aerosol RF is influenced by considerable diversity in simulated residence times, mass extinction coefficients and most importantly forcing efficiencies (forcing per unit optical depth). The clear-sky forcing efficiency (forcing per unit optical depth) has diversity comparable to that for the all-sky/ clear-sky forcing ratio. While the diversity in clear-sky forcing efficiency is impacted by factors such as aerosol absorption, size, and surface albedo, we can show that the all-sky/clear-sky forcing ratio is important because all-sky forcing estimates require proper representation of cloud fields and the correct relative altitude placement between absorbing aerosol and clouds. The analysis of the sulphate RF shows that long sulphate residence times are compensated by low mass extinction coefficients and vice versa. This is explained by more sulphate particle humidity growth and thus higher extinction in those models where short-lived sulphate is present at lower altitude and vice versa. Solar atmospheric forcing within the atmospheric column is estimated at +0.82±0.17Wm-2. The local annual average maxima of atmospheric forcing exceed +5Wm-2 confirming the regional character of aerosol impacts on climate. The annual average surface forcing is -1.02±0.23Wm-2. With the current uncertainties in the modelling of the radiative forcing due to the direct aerosol effect we show here that an estimate from one model is not sufficient but a combination of several model estimates is necessary to provide a mean and to explore the uncertainty. [ABSTRACT FROM AUTHOR]

A thermodynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on nitrate partitioning to the aerosol phase and if particulate nitrate is expected to form in fine or coarse mode aerosols. Modelling of the formation of fine mode nitrate particles is complicated since it depends on other aerosol components and aerosol precursors as well as meteorological condition. The surface concentrations from the model are compared to observed surface concentrations at around 20 sites around Europe for nitrate and ammonium. The agreement for nitrate is good but the modelled values are somewhat underestimated compared to observations at high concentrations, whereas for ammonium the agreement is very good. However, we underscore that such a comparison is not of large importance for the aerosol optical depth of particulate nitrate since the vertical profile of aerosol components and their precursors are so important. Fine mode nitrate formation depends on vertical profiles of both ammonia/ammonium and sulphate. The model results show that fine mode particulate nitrate play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of fine mode nitrate is relatively small due to limited availability of ammonia and loss to larger sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of fine mode nitrate by 25% on a global scale but with large regional variations. [ABSTRACT FROM AUTHOR]

The indirect effect of aerosols via liquid clouds is investigated by comparing aerosol and cloud characteristics from the Global Climate Model CAM-Oslo to those observed by the MODIS instrument onboard the TERRA and AQUA satellites (http://modis.gsfc.nasa.gov). The comparison is carried out for 15 selected regions ranging from remote and clean to densely populated and polluted. For each region, the regression coefficient and correlation coefficient for the following parameters are calculated: Aerosol Optical Depth vs. Liquid Cloud Optical Thickness, Aerosol Optical Depth vs. Liquid Cloud Droplet Effective Radius and Aerosol Optical Depth vs. Cloud Liquid Water Path. Modeled and observed correlation coefficients and regression coefficients are then compared for a 3-year period starting in January 2001. Additionally, global maps for a number of aerosol and cloud parameters crucial for the understanding of the aerosol indirect effect are compared for the same period of time. Significant differences are found between MODIS and CAM-Oslo both in the regional and global comparison. However, both the model and the observations show a positive correlation between Aerosol Optical Depth and Cloud Optical Depth in practically all regions and for all seasons, in agreement with the current understanding of aerosol-cloud interactions. The correlation between Aerosol Optical Depth and Liquid Cloud Droplet Effective Radius is variable both in the model and the observations. However, the model reports the expected negative correlation more often than the MODIS data. Aerosol Optical Depth is overall positively correlated to Cloud Liquid Water Path both in the model and the observations, with a few regional exceptions. [ABSTRACT FROM AUTHOR]

Monthly mean aerosol optical depth (AOD) over ocean is compared from a total of 9 aerosol retrievals during a 40 months period. Comparisons of AOD have been made both for the entire period and sub periods. We identify regions where there is large disagreement and good agreement between the aerosol satellite retrievals. Significant differences in AOD have been identified in most of the oceanic regions. Several analyses are performed including spatial correlation between the retrievals as well as comparison with AERONET data. During the 40 months period studied there have been several major aerosol field campaigns as well as events of high aerosol content. It is studied how the aerosol retrievals compare during such circumstances. The differences found in this study are larger than found in a previous study where 5 aerosol retrievals over an 8 months period were compared. Part of the differences can be explained by limitations and deficiencies in some of the aerosol retrievals. In particular, results in coastal regions are promising especially for aerosol retrievals from satellite instruments particularly suited for aerosol research. In depth analyses explaining the differences between AOD obtained in different retrievals are clearly needed. We limit this study to identifying differences and similarities and indicating possible sources that affect the quality of the retrievals. This is a necessary first step towards understanding the differences and improving the retrievals. [ABSTRACT FROM AUTHOR]

Abstract: Chemically active climate compounds are either primary compounds like methane (CH4), removed by oxidation in the atmosphere, or secondary compounds like ozone (O3), sulfate and organic aerosols, both formed and removed in the atmosphere. Man-induced climate–chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate–chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds like O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds like O3, and of particles inducing both direct and indirect effects. Through EU projects like ACCENT, QUANTIFY, and the AeroCom project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric–tropospheric exchange of ozone, more frequent periods with stable conditions favoring pollution build up over industrial areas, enhanced temperature induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 5–10 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modeling of composition changes, access to new observational data has improved modeling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact. [Copyright &y& Elsevier]