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Anthropogenic aerosols exert a cooling influence that offsets part of the greenhouse gas warming. Due to their short tropospheric lifetime of only several days, the aerosol forcing responds quickly to emissions. Here, we present and discuss the evolution of the aerosol forcing since 2000. There are multiple lines of evidence that allow us to robustly conclude that the anthropogenic aerosol effective radiative forcing (ERF) - both aerosol- radiation interactions (ERFari) and aerosol-cloud interactions (ERFaci) - has become less negative globally, i.e. the trend in aerosol effective radiative forcing changed sign from negative to positive. Bottom-up inventories show that anthropogenic primary aerosol and aerosol precursor emissions declined in most regions of the world; observations related to aerosol burden show declining trends, in particular of the fine-mode particles that make up most of the anthropogenic aerosols; satellite retrievals of cloud droplet numbers show trends in regions with aerosol declines that are consistent with these in sign, as do observations of top-of-atmosphere radiation. Climate model results, including a revised set that is constrained by observations of the ocean heat content evolution show a consistent sign and magnitude for a positive forcing relative to the year 2000 due to reduced aerosol effects. This reduction leads to an acceleration of the forcing of climate change, i.e. an increase in forcing by 0.1 to 0.3 W m(-2), up to 12 % of the total climate forcing in 2019 compared to 1750 according to the Intergovernmental Panel on Climate Change (IPCC)., Atmospheric Chemistry and Physics, 22 (18), ISSN:1680-7375, ISSN:1680-7367

This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550 nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550 nm), with the range given as the minimum and maximum model values. This is 28 % higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60 % (range 36 %–84 %) is estimated to be due to BC, 31 % (12 %–49 %) is due to dust, and 11 % (0 %–24 %) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7) m2 g−1 (550 nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

The effective radiative forcing, which includes the instantaneous forcing plus adjustments from the atmosphere and surface, has emerged as the key metric of evaluating human and natural influence on the climate. We evaluate effective radiative forcing and adjustments in 13 contemporary climate models that are participating in CMIP6 and have contributed to the Radiative Forcing Model Intercomparison Project (RFMIP). Present-day (2014) global mean anthropogenic forcing relative to pre-industrial (1850) from climate models stands at 1.97 (± 0.26) W m−2, comprised of 1.80 (± 0.11) W m−2 from CO2, 1.07 (± 0.21) W m−2 from other well-mixed greenhouse gases, −1.04 (± 0.23) W m−2 from aerosols and −0.08 (± 0.14) W m−2 from land use change. Quoted uncertainties are one standard deviation across model best estimates, and 90 % confidence in the reported forcings, due to internal variability, is typically within 0.1 W m−2. The majority of the remaining 0.17 W m−2 is likely to be from ozone. As determined in previous studies, cancellation of tropospheric and surface adjustments means that the traditional stratospherically adjusted radiative forcing is approximately equal to ERF for greenhouse gas forcing, but not for aerosols, and consequentially, not for the anthropogenic total. The spread of aerosol forcing ranges from −0.63 to −1.37 W m−2, exhibiting a less negative mean and narrower range compared to 10 CMIP5 models. The spread in 4 × CO2 forcing has also narrowed in CMIP6 compared to 13 CMIP5 models. Aerosol forcing is uncorrelated with equilibrium climate sensitivity. Therefore, there is no evidence to suggest that the increasing spread in climate sensitivity in CMIP6 models, particularly related to high-sensitivity models, is a consequence of a stronger negative present-day aerosol forcing.

Shortwave cloud radiative effects (SWCREs), defined as the difference of the shortwave radiative flux between all-sky and clear-sky conditions at the surface, have been reported to play an important role in influencing the Earth's energy budget and temperature extremes. In this study, we employed a set of global climate models to examine the SWCRE responses to CO2, black carbon (BC) aerosols, and sulfate aerosols in boreal summer over the Northern Hemisphere. We found that CO2 causes positive SWCRE changes over most of the NH, and BC causes similar positive responses over North America, Europe, and eastern China but negative SWCRE over India and tropical Africa. When normalized by effective radiative forcing, the SWCRE from BC is roughly 3–5 times larger than that from CO2. SWCRE change is mainly due to cloud cover changes resulting from changes in relative humidity (RH) and, to a lesser extent, changes in cloud liquid water, circulation, dynamics, and stability. The SWCRE response to sulfate aerosols, however, is negligible compared to that for CO2 and BC because part of the radiation scattered by clouds under all-sky conditions will also be scattered by aerosols under clear-sky conditions. Using a multilinear regression model, it is found that mean daily maximum temperature (Tmax) increases by 0.15 and 0.13 K per watt per square meter (W m−2) increase in local SWCRE under the CO2 and BC experiment, respectively. When domain-averaged, the contribution of SWCRE change to summer mean Tmax changes was 10 %–30 % under CO2 forcing and 30 %–50 % under BC forcing, varying by region, which can have important implications for extreme climatic events and socioeconomic activities.

The diurnal temperature range (DTR) (or difference between the maximum and minimum temperature within a day) is one of many climate parameters that affects health, agriculture and society. Understanding how DTR evolves under global warming is therefore crucial. Physically different drivers of climate change, such as greenhouse gases and aerosols, have distinct influences on global and regional climate. Therefore, predicting the future evolution of DTR requires knowledge of the effects of individual climate forcers, as well as of the future emissions mix, in particular in high-emission regions. Using global climate model simulations from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP), we investigate how idealized changes in the atmospheric levels of a greenhouse gas (CO2) and aerosols (black carbon and sulfate) influence DTR (globally and in selected regions). We find broad geographical patterns of annual mean change that are similar between climate drivers, pointing to a generalized response to global warming which is not defined by the individual forcing agents. Seasonal and regional differences, however, are substantial, which highlights the potential importance of local background conditions and feedbacks. While differences in DTR responses among drivers are minor in Europe and North America, there are distinctly different DTR responses to aerosols and greenhouse gas perturbations over India and China, where present aerosol emissions are particularly high. BC induces substantial reductions in DTR, which we attribute to strong modeled BC-induced cloud responses in these regions.

A primary goal of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) was to characterize the short-lived drivers of preindustrial to 2100 climate change in the current generation of climate models. Here we evaluate historical and future radiative forcing in the 10 ACCMIP models that included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5). The models generally reproduce present-day climatological total aerosol optical depth (AOD) relatively well. They have quite different contributions from various aerosol components to this total, however, and most appear to underestimate AOD over East Asia. The models generally capture 1980–2000 AOD trends fairly well, though they underpredict AOD increases over the Yellow/Eastern Sea. They appear to strongly underestimate absorbing AOD, especially in East Asia, South and Southeast Asia, South America and Southern Hemisphere Africa. We examined both the conventional direct radiative forcing at the tropopause (RF) and the forcing including rapid adjustments (adjusted forcing; AF, including direct and indirect effects). The models' calculated all aerosol all-sky 1850 to 2000 global mean annual average RF ranges from −0.06 to −0.49 W m−2, with a mean of −0.26 W m−2 and a median of −0.27 W m−2. Adjusting for missing aerosol components in some models brings the range to −0.12 to −0.62 W m−2, with a mean of −0.39 W m−2. Screening the models based on their ability to capture spatial patterns and magnitudes of AOD and AOD trends yields a quality-controlled mean of −0.42 W m−2 and range of −0.33 to −0.50 W m−2 (accounting for missing components). The CMIP5 subset of ACCMIP models spans −0.06 to −0.49 W m−2, suggesting some CMIP5 simulations likely have too little aerosol RF. A substantial, but not well quantified, contribution to historical aerosol RF may come from climate feedbacks (35 to −58 %). The mean aerosol AF during this period is −1.12 W m−2 (median value −1.16 W m−2, range −0.72 to −1.44 W m−2), indicating that adjustments to aerosols, which include cloud, water vapor and temperature, lead to stronger forcing than the aerosol direct RF. Both negative aerosol RF and AF are greatest over and near Europe, South and East Asia and North America during 1850 to 2000. AF, however, is positive over both polar regions, the Sahara, and the Karakoram. Annual average AF is stronger than 0.5 W m−2 over parts of the Arctic and more than 1.5 W m−2 during boreal summer. Examination of the regional pattern of RF and AF shows that the multi-model spread relative to the mean of AF is typically the same or smaller than that for RF over areas with substantial forcing. Historical aerosol RF peaks in nearly all models around 1980, declining thereafter. Aerosol RF declines greatly in most models over the 21st century and is only weakly sensitive to the particular Representative Concentration Pathway (RCP). One model, however, shows approximate stabilization at current RF levels under RCP 8.5, while two others show increasingly negative RF due to the influence of nitrate aerosols (which are not included in most models). Aerosol AF, in contrast, continues to become more negative during 1980 to 2000 despite the turnaround in RF. Total anthropogenic composition forcing (RF due to well-mixed greenhouse gases (WMGHGs) and ozone plus aerosol AF) shows substantial masking of greenhouse forcing by aerosols towards the end of the 20{th} century and in the early 21st century at the global scale. Regionally, net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over East and Southeast Asia by 2000 and only over a very small part of Southeast Asia by 2030 (under RCP8.5). Net forcing is strongly positive by 1980 over the Sahara, Arabian peninsula, the Arctic, Southern Hemisphere South America, Australia and most of the oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter. There is no clear relationship between aerosol AF and climate sensitivity in the CMIP5 subset of ACCMIP models. There is a clear link between the strength of aerosol+ozone forcing and the global mean historical climate response to anthropogenic non-WMGHG forcing (ANWF). The models show ~20–35% greater climate sensitivity to ANWF than to WMGHG forcing, at least in part due to geographic differences in climate sensitivity. These lead to ~50% more warming in the Northern Hemisphere in response to increasing WMGHGs. This interhemispheric asymmetry is enhanced for ANWF by an additional 10–30%. At smaller spatial scales, response to ANWF and WMGHGs show distinct differences.

The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of −0.44 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 9.3 (B1) or −32 ± 18 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −19 ± 5.3 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 9 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m−2 in 2000 to a slightly negative net RF of −3.1 ± 2.2 (B1) or −3.1 ± 3.4 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.6 ± 2.2 mW m−2 in 2000.

The distribution of black carbon (BC) in the atmosphere and the deposition of BC on snow surfaces since pre-industrial time until present are modelled with the Oslo CTM2 model. The model results are compared with observations including recent measurements of BC in snow in the Arctic. The global mean burden of BC from fossil fuel and biofuel sources increased during two periods. The first period, until 1920, is related to increases in emissions in North America and Europe, and the last period after 1970 are related mainly to increasing emissions in East Asia. Although the global burden of BC from fossil fuel and biofuel increases, in the Arctic the maximum atmospheric BC burden as well as in the snow was reached in 1960s, with a slight reduction thereafter. The global mean burden of BC from open biomass burning sources has not changed significantly since 1900. With current inventories of emissions from open biomass sources, the modelled burden of BC in snow and in the atmosphere north of 65° N is small compared to the BC burden of fossil fuel and biofuel origin. From the concentration changes radiative forcing time series due to the direct aerosol effect as well as the snow-albedo effect is calculated for BC from fossil fuel and biofuel. The calculated radiative forcing in 2000 for the direct aerosol effect is 0.35 W m−2 and for the snow-albedo effect 0.016 W m−2 in this study. Due to a southward shift in the emissions there is an increase in the lifetime of BC as well as an increase in normalized radiative forcing, giving a change in forcing per unit of emissions of 26 % since 1950.