Aerosols affect Earth's climate both directly and indirectly, which is the largest uncertainty in the assessment of radiative forcings affecting anthropogenic climate change. The standard Aerosol Robotic Network (AERONET) aerosol products have been widely used for more than 30 years. Currently, there is strong community interest in the possibility of determining aerosol composition directly from remote sensing observations. This work presents the results of applying such a recently developed approach by Li et al. to extended datasets of the directional sky radiances and spectral aerosol optical depth (AOD) measured by AERONET for the retrievals of aerosol components. First, the validation of aerosol optical properties retrieved by this component approach with AERONET standard products shows good agreement. Then, spatiotemporal variations of the obtained aerosol component concentration are characterized globally, especially the absorbing aerosol species (black carbon, brown carbon, and iron oxides) and scattering aerosol species (organic carbon, quartz, and inorganic salts). Finally, we compared the black carbon (BC) and dust column concentration retrievals to the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), products in several regions of interest (Amazon zone, Desert, and Taklamakan Desert) for new insights on the quantitative assessment of MERRA-2 aerosol composition products (R = 0.60-0.85 for BC; R = 0.75-0.90 for dust). The new value-added and long-term aerosol composition product globally is available online (https://doi.org/10.6084/ m9.figshare.25415239.v1), which provides important measurements for the improvement and optimization of aerosol modeling to enhance estimation of the aerosol radiative forcing. SIGNIFICANCE STATEMENT: In the assessment of climate change, the uncertainty associated with aerosol radiative forcing is the largest one. The purpose of this study is to provide a new value-added and long-term aerosol composition (including absorbing and scattering aerosol species) inversion dataset derived from Aerosol Robotic Network (AERONET) measurements for characterizing their spatiotemporal variations at global scale. We find some new insights on the quantitative assessment of black carbon and dust column concentration products in the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2). Our results and aerosol composition inversion dataset will provide robust support for the overall improvement and optimization of aerosol modeling to better understand the aerosol radiative forcing.

Atmospheric observations of sources and sinks of carbon dioxide (CO2) and methane (CH4) in the pan-Arctic domain are highly sporadic, limiting our understanding of carbon turnover in this climatically sensitive environment and the fate of enormous carbon reservoirs buried in permafrost. Particular gaps apply to the Arctic latitudes of Siberia, covered by the vast tundra ecosystems underlain by permafrost, where only few atmospheric sites are available. The paper presents the first results of continuous observations of atmospheric CO2 and CH4 dry mole fractions at a newly operated station DIAMIS (73.506828 degrees N, 80.519869 degrees E) deployed on the edge of the Dikson settlement on the western coast of the Taimyr Peninsula. Atmospheric mole fractions of CO2, CH4, and H2O are measured by a CRDS analyzer Picarro G2301-f, which is regularly calibrated against WMO-traceable gases. Meteorological records permit screening of trace gas series. Here, we give the scientific rationale of the site, describe the instrumental setup, analyze the local environments, examine the seasonal footprint, and show CO2 and CH4 fluctuations for the daytime mixed atmospheric layer that is representative over a vast Arctic domain (-500-1000 km), capturing both terrestrial and oceanic signals.

We present an assessment of the impacts on atmospheric composition and radiative forcing of short-lived pollutants following a worldwide decrease in anthropogenic activity and emissions comparable to what has occurred in response to the COVID-19 pandemic, using the global composition-climate model United Kingdom Chemistry and Aerosols Model (UKCA). Emission changes reduce tropospheric hydroxyl radical and ozone burdens, increasing methane lifetime. Reduced SO2 emissions and oxidizing capacity lead to a decrease in sulfate aerosol and increase in aerosol size, with accompanying reductions to cloud droplet concentration. However, large reductions in black carbon emissions increase aerosol albedo. Overall, the changes in ozone and aerosol direct effects (neglecting aerosol-cloud interactions which were statistically insignificant but whose response warrants future investigation) yield a radiative forcing of -33 to -78 mWm(-2). Upon cessation of emission reductions, the short-lived climate forcers rapidly return to pre-COVID levels; meaning, these changes are unlikely to have lasting impacts on climate assuming emissions return to pre-intervention levels.

We describe and evaluate atmospheric chemistry in the newly developed Geophysical Fluid Dynamics Laboratory chemistry-climate model (GFDL AM3) and apply it to investigate the net impact of preindustrial (PI) to present (PD) changes in short-lived pollutant emissions (ozone precursors, sulfur dioxide, and carbonaceous aerosols) and methane concentration on atmospheric composition and climate forcing. The inclusion of online troposphere-stratosphere interactions, gas-aerosol chemistry, and aerosol-cloud interactions (including direct and indirect aerosol radiative effects) in AM3 enables a more complete representation of interactions among short-lived species, and thus their net climate impact, than was considered in previous climate assessments. The base AM3 simulation, driven with observed sea surface temperature (SST) and sea ice cover (SIC) over the period 1981-2007, generally reproduces the observed mean magnitude, spatial distribution, and seasonal cycle of tropospheric ozone and carbon monoxide. The global mean aerosol optical depth in our base simulation is within 5% of satellite measurements over the 1982-2006 time period. We conduct a pair of simulations in which only the short-lived pollutant emissions and methane concentrations are changed from PI (1860) to PD (2000) levels (i.e., SST, SIC, greenhouse gases, and ozone-depleting substances are held at PD levels). From the PI to PD, we find that changes in short-lived pollutant emissions and methane have caused the tropospheric ozone burden to increase by 39% and the global burdens of sulfate, black carbon, and organic carbon to increase by factors of 3, 2.4, and 1.4, respectively. Tropospheric hydroxyl concentration decreases by 7%, showing that increases in OH sinks (methane, carbon monoxide, nonmethane volatile organic compounds, and sulfur dioxide) dominate over sources (ozone and nitrogen oxides) in the model. Combined changes in tropospheric ozone and aerosols cause a net negative top-of-the-atmosphere radiative forcing perturbation (-1.05Wm(-2)) indicating that the negative forcing (direct plus indirect) from aerosol changes dominates over the positive forcing due to ozone increases, thus masking nearly half of the PI to PD positive forcing from long-lived greenhouse gases globally, consistent with other current generation chemistry-climate models.

Absorbing aerosols supplements the global warming caused by greenhouse gases. However, unlike greenhouse gases, the effect of absorbing aerosol on climate is not known with certainty owing to paucity of data. Also, uncertainty exists in quantifying the contributing factors whether it is biomass or fossil fuel burning. Based on the observations of absorption coefficient at seven wavelengths and aerosol optical depth (AOD) at five wavelengths carried out at Gadanki (13.5 degrees N, 79.2 degrees E), a remote village in peninsular India, from April to November 2008, as part of the Study of Atmospheric Forcing and Responses (SAFAR) pilot campaign we discuss seasonal variation of black carbon ( BC) concentration and aerosol optical depth. Also, using spectral information we estimate the fraction of fossil-fuel and non-fossil fuel contributions to absorption coefficient and contributions of soot ( Black Carbon), non-soot fine mode aerosols and coarse mode aerosols to AOD. BC concentration is found to be around 1000 ng/m(3) during monsoon months (JJAS) and around 4000 ng/m(3) during pre and post monsoon months. Non-fossil fuel sources contribute nearly 20% to absorption coefficient at 880 nm, which increases to 40% during morning and evening hours. Average AOD is found to be 0.38 +/- 0.15, with high values in May and low in September. Soot contributes nearly 10% to the AOD. This information is further used to estimate the clear sky aerosol direct radiative forcing. Top of the atmosphere aerosol radiative forcing varies between -4 to 0 W m(-2), except for April when the forcing is positive. Surface level radiative forcing is between -10 to -20 W m(-2). The net radiation absorbed within the atmosphere is in the range of 9 to 25 W m(-2), of which soot contributes about 80 to 90%.

The direct aerosol radiative forcing (DARF) has been estimated for the clear-sky conditions over Delhi from January 2006 to January 2007 using Santa Barbara DISORT Atmospheric Radiative Transfer model (SBDART) in the wavelength range 300-3000 nanometer. The single scattering albedo (SSA) and the asymmetry parameter used in this model were estimated using the Optical Properties of Aerosol and Cloud (OPAC) model. The annual average AOD observed at 500 nm was similar to 0.86 +/- 0.42 with an average Angstrom exponent similar to 0.68 +/- 0.35. The average monthly AOD throughout the year over Delhi was found to be in the range 0.56 to 1.22 with the Angstrom exponent in the range 0.38 to 0.96. A high monthly average BC concentration in the range 4-15 mu g m(-3) led to monthly average SSA in the range 0.90 +/- 0.4 to 0.74 +/- 0.3 during the year. Consequently, the monthly average clear-sky DARF at the surface was found to vary in the range -46 +/- 8 W m(-2) to -110 +/- 20 W m(-2), at TOA in the range -1.4 +/- 0.4 to 21 +/- 2 W m(-2), whereas in the atmosphere it was in the range 46 +/- 9 W m(-2) to 115 +/- 19 W m(-2) throughout the year. As the dust concentration in the atmosphere was highest (May-June) the SSA showed an increase with wavelength however when dust concentration was low the SSA decreased with the wavelength.

We have recently investigated large-scale covariability between aerosol and precipitation and other meteorological variables in the West African Monsoon (WAM) region using long term satellite observations and reanalysis data. In this study we compared the observational results to a global model simulation including only direct radiative forcing of black carbon (BC). From both observations and model simulations we found that in boreal cold seasons anomalously high African aerosols are associated with significant reductions in cloud amount, cloud top height, and surface precipitation. These results suggest that the observed precipitation reduction in the WAM region is caused by radiative effect of BC. The result also suggests that the BC effect on precipitation is nonlinear.

In the present work it is investigated the direct shortwave effect of anthropogenic aerosols on the near surface temperature over Southeastern Europe and the atmospheric circulation during summer 2000. In summer 2000, a severe heat-wave and droughts affected many countries in the Balkans. The study is based on two yearly simulations with and without the aerosol feedback of the regional climate model RegCM3 coupled with a simplified aerosol model. The surface radiative forcing associated with the anthropogenic aerosols is negative throughout the European domain with the more negative values in Central and Central-eastern Europe. A basic pattern of the aerosol induced changes in air temperature at the lower troposphere is a decrease over Southeastern Europe and the Balkan Peninsula (up to about 1.2 degrees C) thus weakening the pattern of the climatic temperature anomalies of summer 2000. The aerosol induced changes in air temperature from the lower troposphere to upper troposphere are not correlated with the respective pattern of the surface radiative forcing implying the complexity of the mechanisms linking the aerosol radiative forcing with the induced atmospheric changes through dynamical feedbacks of aerosols on atmospheric circulation. Investigation of the aerosol induced changes in the circulation indicates a southward shift of the subtropical jet stream playing a dominant role for the decrease in near surface air temperature over Southeastern Europe and the Balkan Peninsula. The southward shift of the jet exit region over the Balkan Peninsula causes a relative increase of the upward motion at the northern flank of the jet exit region, a relative increase of clouds, less solar radiation absorbed at the surface and hence relative cooler air temperatures in the lower troposphere between 45 degrees N and 50 degrees N. The southward extension of the lower troposphere aerosol induced negative temperature changes in the latitudinal band 35 degrees N-45 degrees N over the Balkan Peninsula is justified from the prevailing northerly flow advecting the relatively cooler air from the latitudinal band 45 degrees N-50 degrees N towards the lower latitudes. The present regional climate modeling study indicates the important role of anthropogenic aerosols for the regional climate and their dynamical feedback on atmospheric circulation.

Previous works have suggested that the direct radiative forcing (DRF) of black carbon (BC) aerosols are able to force a significant change in tropical convective precipitation ranging from the Pacific and Indian Ocean to the Atlantic Ocean. In this in-depth analysis, the sensitivity of this modeled effect of BC on tropical convective precipitation to the emissions of BC from 5 major regions of the world has been examined. In a zonal mean base, the effect of BC on tropical convective precipitation is a result of a displacement of ITCZ toward the forcing (warming) hemisphere. However, a substantial difference exists in this effect associated with BC over different continents. The BC effect on convective precipitation over the tropical Pacific Ocean is found to be most sensitive to the emissions from Central and North America due to a persistent presence of BC aerosols from these two regions in the lowermost troposphere over the Eastern Pacific. The BC effect over the tropical Indian and Atlantic Ocean is most sensitive to the emissions from South as well as East Asia and Africa, respectively. Interestingly, the summation of these individual effects associated with emissions from various regions mostly exceeds their actual combined effect as shown in the model run driven by the global BC emissions, so that they must offset each other in certain locations and a nonlinearity of this type of effect is thus defined. It is known that anthropogenic aerosols contain many scattering-dominant constituents that might exert an effect opposite to that of absorbing BC. The combined aerosol forcing is thus likely differing from the BC-only one. Nevertheless, this study along with others of its kind that isolates the DRF of BC from other forcings provides an insight of the potentially important climate response to anthropogenic forcings particularly related to the unique particulate solar absorption.

Seasonal distinctiveness in the microphysical and optical properties of columnar and near-surface (in the well mixed region) aerosols, associated with changes in the prevailing synoptic conditions, were delineated based on extensive (spread over 4 years) and collocated measurements at the tropical coastal location, Trivandrum (8.55 degrees N; 76.97 degrees E, 3 m a.m.s.l.), and the results were summarized in Part 1 of this two-part paper. In Part 2, we use these properties to develop empirical seasonal aerosol models, which represent the observed features fairly accurately, separately for winter monsoon season (WMS, December through March), inter-monsoon season (IMS, April and May), summer monsoon season (SMS, June through September) and post monsoon season (PMS, October and November). The models indicate a significant transformation in the aerosol environment from an anthropogenic-dominance in WMS to a natural-dominance in SMS. The modeled aerosol properties are used for estimating the direct, short wave aerosol radiative forcing, under clear-sky conditions. Our estimates show large seasonal changes. Under clear sky conditions, the daily averaged short-wave TOA forcing changes from its highest values during WMS, to the lowest values in SMS; this seasonal change being brought-in mainly by the reduction in the abundance and the mass fraction (to the composite) of black carbon aerosols and of accumulation mode aerosols. The resulting atmospheric forcing varies from the highest, (47 to 53 W m(-2)) in WMS to the lowest (22 to 26 W m(-2)) in SMS.