Global source attribution of sulfate concentration and direct and indirect radiative forcing

The global source–receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is −0.42 W m−2, with −0.31 W m−2 contributed by anthropogenic sulfate and −0.11 W m−2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of −0.44 W m−2. DMS has the largest contribution, explaining −0.23 W m−2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.

Global source attribution of sulfate concentration, direct and indirect radiative forcing

The global source-receptor relationships of sulfate concentration, direct and indirect radiative forcing (DRF and IRF) from sixteen regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. The export of SO2 and sulfate from Europe contributes 16–20 % of near-surface sulfate concentrations over North Africa, Russia/Belarus/Ukraine (RBU) region and Central Asia. Sources from the Middle East account for 15–24 % of sulfate over North Africa, Southern Africa and Central Asia in winter and autumn, and 19 % over South Asia in spring. Sources in RBU account for 21–42 % of sulfate concentrations over Central Asia. East Asia accounts for about 50 % of sulfate over Southeast Asia in winter and autumn, 15 % over RBU in summer, and 11 % over North America in spring. South Asia contributes to 11–24 % of sulfate over Southeast Asia in winter and spring. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is −0.42 W m−2, with 0.31 W m−2 contributed by anthropogenic sulfate and −0.11 W m−2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high-latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of −0.44 W m−2. DMS has the largest contribution, explaining −0.23 W m−2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than those over the polluted Northern Hemisphere.

Systematic satellite observations of the impact of aerosols from passive volcanic degassing on local cloud properties

The impact of volcanic emissions is a significant source of uncertainty in estimations of aerosol indirect radiative forcing, especially with respect to emissions from passive degassing and minor explosions. Understanding the impact of volcanic emissions on indirect radiative forcing is important for assessing present day atmospheric properties and also to define the pre-industrial baseline to assess anthropogenic perturbations. We present observations of the time-averaged indirect aerosol effect within 200 km downwind of isolated island volcanoes in regions of low present-day aerosol burden using MODIS and AATSR data. Retrievals of aerosol and cloud properties at Kīlauea (Hawai'i), Yasur (Vanuatu) and Piton de la Fournaise (Réunion) are rotated about the volcanic vent according to wind direction, so that retrievals downwind of the volcano can be averaged to improve signal to noise ratio. The emissions from all three volcanoes, including those from passive degassing, strombolian activity and minor explosions lead to measurably increased aerosol optical depth downwind of the active vent. Average cloud droplet effective radius is lower downwind of the volcano in all cases, with the peak difference in effective radius of 4–8 μm at the different volcanoes. A comparison of these observations with cloud properties at isolated islands with no significant source of aerosol suggests that these patterns are not purely orographic in origin. This approach sets out a first step for the systematic measurement of the effects of present day low altitude volcanic emissions on cloud properties. Our observations of unpolluted, isolated marine settings may also capture processes similar to those in the pre-industrial marine atmosphere.

Estimates of aerosol radiative forcing from the MACC re-analysis

The European Centre for Medium-range Weather Forecast (ECMWF) provides an aerosol re-analysis starting from year 2003 for the Monitoring Atmospheric Composition and Climate (MACC) project. The re-analysis assimilates total aerosol optical depth retrieved by the Moderate Resolution Imaging Spectroradiometer (MODIS) to correct for model departures from observed aerosols. The re-analysis therefore combines satellite retrievals with the full spatial coverage of a numerical model. Re-analysed products are used here to estimate the shortwave direct and first indirect radiative forcing of anthropogenic aerosols over the period 2003–2010, using methods previously applied to satellite retrievals of aerosols and clouds. The best estimate of globally-averaged, all-sky direct radiative forcing is −0.7 ± 0.3 Wm−2. The standard deviation is obtained by a Monte-Carlo analysis of uncertainties, which accounts for uncertainties in the aerosol anthropogenic fraction, aerosol absorption, and cloudy-sky effects. Further accounting for differences between the present-day natural and pre-industrial aerosols provides a direct radiative forcing estimate of −0.4 ± 0.3 Wm−2. The best estimate of globally-averaged, all-sky first indirect radiative forcing is −0.6 ± 0.4 Wm−2. Its standard deviation accounts for uncertainties in the aerosol anthropogenic fraction, and in cloud albedo and cloud droplet number concentration susceptibilities to aerosol changes. The distribution of first indirect radiative forcing is asymmetric and is bounded by −0.1 and −2.0 Wm−2. In order to decrease uncertainty ranges, better observational constraints on aerosol absorption and sensitivity of cloud droplet number concentrations to aerosol changes are required.

Aerosol–climate interactions in the Norwegian Earth System Model – NorESM1-M

The objective of this study is to document and evaluate recent changes and updates to the module for aerosols and aerosol–cloud–radiation interactions in the atmospheric module CAM4-Oslo of the core version of the Norwegian Earth System Model (NorESM), NorESM1-M. Particular attention is paid to the role of natural organics, sea salt, and mineral dust in determining the gross aerosol properties as well as the anthropogenic contribution to these properties and the associated direct and indirect radiative forcing. The aerosol module is extended from earlier versions that have been published, and includes life-cycling of sea salt, mineral dust, particulate sulphate, black carbon, and primary and secondary organics. The impacts of most of the numerous changes since previous versions are thoroughly explored by sensitivity experiments. The most important changes are: modified prognostic sea salt emissions; updated treatment of precipitation scavenging and gravitational settling; inclusion of biogenic primary organics and methane sulphonic acid (MSA) from oceans; almost doubled production of land-based biogenic secondary organic aerosols (SOA); and increased ratio of organic matter to organic carbon (OM/OC) for biomass burning aerosols from 1.4 to 2.6. Compared with in situ measurements and remotely sensed data, the new treatments of sea salt and dust aerosols give smaller biases in near-surface mass concentrations and aerosol optical depth than in the earlier model version. The model biases for mass concentrations are approximately unchanged for sulphate and BC. The enhanced levels of modeled OM yield improved overall statistics, even though OM is still underestimated in Europe and overestimated in North America. The global anthropogenic aerosol direct radiative forcing (DRF) at the top of the atmosphere has changed from a small positive value to −0.08 W m−2 in CAM4-Oslo. The sensitivity tests suggest that this change can be attributed to the new treatment of biomass burning aerosols and gravitational settling. Although it has not been a goal in this study, the new DRF estimate is closer both to the median model estimate from the AeroCom intercomparison and the best estimate in IPCC AR4. Estimated DRF at the ground surface has increased by ca. 60%, to −1.89 W m−2. We show that this can be explained by new emission data and omitted mixing of constituents between updrafts and downdrafts in convective clouds. The increased abundance of natural OM and the introduction of a cloud droplet spectral dispersion formulation are the most important contributions to a considerably decreased estimate of the indirect radiative forcing (IndRF). The IndRF is also found to be sensitive to assumptions about the coating of insoluble aerosols by sulphate and OM. The IndRF of −1.2 W m−2, which is closer to the IPCC AR4 estimates than the previous estimate of −1.9 W m−2, has thus been obtained without imposing unrealistic artificial lower bounds on cloud droplet number concentrations.