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The Geoengineering Model Intercomparison Project (GeoMIP) has proposed multiple model experiments during phases 5 and 6 of the Climate Model Intercomparison Project (CMIP), with the latest set of model experiments proposed in 2015. With phase 7 of CMIP in preparation and with multiple efforts ongoing to better explore the potential space of outcomes for different solar radiation modifications (SRMs) both in terms of deployment strategies and scenarios and in terms of potential impacts, the GeoMIP community has identified the need to propose and conduct a new experiment that could serve as a bridge between past iterations and future CMIP7 experiments. Here we report the details of such a proposed experiment, named G6-1.5K-SAI, to be conducted with the current generation of scenarios and models from CMIP6 and clarify the reasoning behind many of the new choices introduced. Namely, compared to the CMIP6 GeoMIP scenario G6sulfur, we decided on (1) an intermediate emission scenario as a baseline (the Shared Socioeconomic Pathway 2-4.5), (2) a start date set in the future that includes both considerations for the likelihood of exceeding 1.5 °C above preindustrial levels and some considerations for a likely start date for an SRM implementation, and (3) a deployment strategy for stratospheric aerosol injection that does not inject in the tropical pipe in order to obtain a more latitudinally uniform aerosol distribution. We also offer more details regarding the preferred experiment length and number of ensemble members and include potential options for second-tier experiments that some modeling groups might want to run. The specifics of the proposed experiment will further allow for a more direct comparison between results obtained from CMIP6 models and those obtained from future scenarios for CMIP7.

The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

Ship tracks in subtropical marine low clouds are simulated and investigated using large-eddy simulations. Five variants of a shallow subtropical stratocumulus-topped marine boundary layer (MBL) are chosen to span a range of background aerosol concentrations and variations in free-tropospheric moisture. Idealized time-invariant meteorological forcings and approximately steady-state aerosol concentrations constitute the background conditions. We investigate processes controlling cloud microphysical, macrophysical, and radiative responses to aerosol injections. For the analysis, we use novel methods to decompose the liquid water path (LWP) adjustment into changes in cloud and boundary-layer properties and to decompose the cloud radiative effect (CRE) into contributions from cloud macro- and microphysics. The key results are that (a) the cloud-top entrainment rate increases in all cases, with stronger increases for thicker than thinner clouds; (b) the drying and warming induced by increased entrainment is offset to differing degrees by corresponding responses in surface fluxes, precipitation, and radiation; (c) MBL turbulence responds to changes caused by the aerosol perturbation, and this significantly affects cloud macrophysics; (d) across 2 d of simulation, clouds were brightened in all cases. In a pristine MBL, significant drizzle suppression by aerosol injections results not only in greater water retention but also in turbulence intensification, leading to a significant increase in cloud amount. In this case, Twomey brightening is strongly augmented by an increase in cloud thickness and cover. In addition, a reduction in the loss of aerosol through coalescence scavenging more than offsets the entrainment dilution. This interplay precludes estimation of the lifetime of the aerosol perturbation. The combined responses of cloud macro- and microphysics lead to 10–100 times more effective cloud brightening in these cases relative to those in the non-precipitating MBL cases. In moderate and polluted MBLs, entrainment enhancement makes the boundary layer drier, warmer, and more stratified, leading to a decrease in cloud thickness. This LWP response offsets the greatest fraction of the Twomey brightening in a moderately moist free troposphere. This finding differs from previous studies that found larger offsets in a drier free troposphere, and it results from a greater entrainment enhancement of initially thicker clouds, so the offsetting effects are weaker. The injected aerosol lifetime in cases with polluted MBLs is estimated to be 2–3 d, which is much longer than estimates of typical ship track lifetimes from satellite images.

Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (∼1–2 K) and greatly enhanced moisture (>2 g kg−1) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ∼350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ∼100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2∘ grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16∘ S, 6∘ E, and 10∘ S, 0∘ E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

The Community Atmosphere Model (CAM5), equipped with a technique to tag black carbon (BC) emissions by source regions and types, has been employed to establish source–receptor relationships for atmospheric BC and its deposition to snow over western North America. The CAM5 simulation was conducted with meteorological fields constrained by reanalysis for year 2013 when measurements of BC in both near-surface air and snow are available for model evaluation. We find that CAM5 has a significant low bias in predicted mixing ratios of BC in snow but only a small low bias in predicted atmospheric concentrations over northwestern USA and western Canada. Even with a strong low bias in snow mixing ratios, radiative transfer calculations show that the BC-in-snow darkening effect is substantially larger than the BC dimming effect at the surface by atmospheric BC. Local sources contribute more to near-surface atmospheric BC and to deposition than distant sources, while the latter are more important in the middle and upper troposphere where wet removal is relatively weak. Fossil fuel (FF) is the dominant source type for total column BC burden over the two regions. FF is also the dominant local source type for BC column burden, deposition, and near-surface BC, while for all distant source regions combined the contribution of biomass/biofuel (BB) is larger than FF. An observationally based positive matrix factorization (PMF) analysis of the snow-impurity chemistry is conducted to quantitatively evaluate the CAM5 BC source-type attribution. While CAM5 is qualitatively consistent with the PMF analysis with respect to partitioning of BC originating from BB and FF emissions, it significantly underestimates the relative contribution of BB. In addition to a possible low bias in BB emissions used in the simulation, the model is likely missing a significant source of snow darkening from local soil found in the observations.

Black carbon (BC) in snow lowers its albedo, increasing the absorption of sunlight, leading to positive radiative forcing, climate warming and earlier snowmelt. A series of recent studies have used prescribed-aerosol deposition flux fields in climate model runs to assess the forcing by black carbon in snow. In these studies, the prescribed mass deposition flux of BC to surface snow is decoupled from the mass deposition flux of snow water to the surface. Here we compare prognostic- and prescribed-aerosol runs and use a series of offline calculations to show that the prescribed-aerosol approach results, on average, in a factor of about 1.5–2.5 high bias in annual-mean surface snow BC mixing ratios in three key regions for snow albedo forcing by BC: Greenland, Eurasia and North America. These biases will propagate directly to positive biases in snow and surface albedo reduction by BC. The bias is shown be due to coupling snowfall that varies on meteorological timescales (daily or shorter) with prescribed BC mass deposition fluxes that are more temporally and spatially smooth. The result is physically non-realistic mixing ratios of BC in surface snow. We suggest that an alternative approach would be to prescribe BC mass mixing ratios in snowfall, rather than BC mass fluxes, and we show that this produces more physically realistic BC mixing ratios in snowfall and in the surface snow layer.

We examine the impacts of atmospheric aerosols on Arctic and global climate using a series of 20th century transient simulations from Community Climate System Model version 4 (CCSM4). We focus on the response of surface air temperature to the direct radiative forcing driven by changes in sulfate and black carbon (BC) concentrations from 1975 to 2005 and we also examine the response to changes in sulfate, BC, and organic carbon (OC) aerosols collectively. The direct forcing from sulfate dominates the aerosol climate effect. Globally averaged, simultaneous changes in all three aerosols produce a cooling trend of 0.015 K decade−1 during the period 1975–2005. In the Arctic, surface air temperature has large spatial variations in response to changes in aerosol concentrations. Over the European Arctic, aerosols induce about 0.6 K decade−1 warming, which is about 1.8 K warming over the 30-year period. This warming is triggered mainly by the reduction in sulfate and BC emissions over Europe since the 1970s and is reinforced by sea ice loss and a strengthening in atmospheric northward heat transport. Changes in sulfate concentrations account for about two thirds of the warming and BC for the remaining one third. Over the Siberian and North American Arctic, surface air temperature is likely influenced by changes in aerosol concentrations over Asia. An increase in sulfate optical depth over Asia induces a large cooling while an increase in BC over Asia causes a significant warming.

We use observations of the absorption properties of black carbon and non-black carbon impurities in near-surface snow collected near the research stations at South Pole and Dome C, Antarctica, and Summit, Greenland, combined with a snowpack actinic flux parameterization to estimate the vertical profile and e-folding depth of ultraviolet/near-visible (UV/near-vis) actinic flux in the snowpack at each location. We have developed a simple and broadly applicable parameterization to calculate depth and wavelength dependent snowpack actinic flux that can be easily integrated into large-scale (e.g., 3-D) models of the atmosphere. The calculated e-folding depths of actinic flux at 305 nm, the peak wavelength of nitrate photolysis in the snowpack, are 8–12 cm near the stations and 15–31 cm away (>11 km) from the stations. We find that the e-folding depth is strongly dependent on impurity content and wavelength in the UV/near-vis region, which explains the relatively shallow e-folding depths near stations where local activities lead to higher snow impurity levels. We calculate the lifetime of NOx in the snowpack interstitial air produced by photolysis of snowpack nitrate against wind pumping (τwind pumping) from the snowpack, and compare this to the calculated lifetime of NOx against chemical conversion to HNO3 (τchemical) to determine whether the NOx produced at a given depth can escape from the snowpack to the overlying atmosphere. Comparison of τwind pumping and τchemical suggests efficient escape of photoproduced NOx in the snowpack to the overlying atmosphere throughout most of the photochemically active zone. Calculated vertical actinic flux profiles and observed snowpack nitrate concentrations are used to estimate the potential flux of NOx from the snowpack. Calculated NOx fluxes of 4.4 × 108–3.8 × 109 molecules cm−2 s−1 in remote polar locations and 3.2–8.2 × 108 molecules cm−2 s−1 near polar stations for January at Dome C and South Pole and June at Summit suggest that NOx flux measurements near stations may be underestimating the amount of NOx emitted from the clean polar snowpack.

We evaluate the performance of the Single Particle Soot Photometer (SP2) and the Integrating Sphere/Integrating Sandwich Spectrophotometer (ISSW) in quantifying the concentration of refractory black carbon (BC) in snow samples. We find that the SP2 can be used to measure BC mass concentration in snow with substantially larger uncertainty (60%) than for atmospheric sampling (

The presence of light-absorbing aerosol particles deposited on arctic snow and sea ice influences the surface albedo, causing greater shortwave absorption, warming, and loss of snow and sea ice, lowering the albedo further. The Community Earth System Model version 1 (CESM1) now includes the radiative effects of light-absorbing particles in snow on land and sea ice and in sea ice itself. We investigate the model response to the deposition of black carbon and dust to both snow and sea ice. For these purposes we employ a slab ocean version of CESM1, using the Community Atmosphere Model version 4 (CAM4), run to equilibrium for year 2000 levels of CO2 and fixed aerosol deposition. We construct experiments with and without aerosol deposition, with dust or black carbon deposition alone, and with varying quantities of black carbon and dust to approximate year 1850 and 2000 deposition fluxes. The year 2000 deposition fluxes of both dust and black carbon cause 1–2 °C of surface warming over large areas of the Arctic Ocean and sub-Arctic seas in autumn and winter and in patches of Northern land in every season. Atmospheric circulation changes are a key component of the surface-warming pattern. Arctic sea ice thins by on average about 30 cm. Simulations with year 1850 aerosol deposition are not substantially different from those with year 2000 deposition, given constant levels of CO2. The climatic impact of particulate impurities deposited over land exceeds that of particles deposited over sea ice. Even the surface warming over the sea ice and sea ice thinning depends more upon light-absorbing particles deposited over land. For CO2 doubled relative to year 2000 levels, the climate impact of particulate impurities in snow and sea ice is substantially lower than for the year 2000 equilibrium simulation.

We use a global chemical transport model (GEOS-Chem CTM) to interpret observations of black carbon (BC) and organic aerosol (OA) from the NASA ARCTAS aircraft campaign over the North American Arctic in April 2008, as well as longer-term records in surface air and in snow (2007–2009). BC emission inventories for North America, Europe, and Asia in the model are tested by comparison with surface air observations over these source regions. Russian open fires were the dominant source of OA in the Arctic troposphere during ARCTAS but we find that BC was of prevailingly anthropogenic (fossil fuel and biofuel) origin, particularly in surface air. This source attribution is confirmed by correlation of BC and OA with acetonitrile and sulfate in the model and in the observations. Asian emissions are the main anthropogenic source of BC in the free troposphere but European, Russian and North American sources are also important in surface air. Russian anthropogenic emissions appear to dominate the source of BC in Arctic surface air in winter. Model simulations for 2007–2009 (to account for interannual variability of fires) show much higher BC snow content in the Eurasian than the North American Arctic, consistent with the limited observations. We find that anthropogenic sources contribute 90% of BC deposited to Arctic snow in January-March and 60% in April–May 2007–2009. The mean decrease in Arctic snow albedo from BC deposition is estimated to be 0.6% in spring, resulting in a regional surface radiative forcing consistent with previous estimates.

Absorption of radiation by ice is extremely weak at visible and near-ultraviolet wavelengths, so small amounts of light-absorbing impurities in snow can dominate the absorption of solar radiation at these wavelengths, reducing the albedo relative to that of pure snow, contributing to the surface energy budget and leading to earlier snowmelt. In this study Arctic snow is surveyed for its content of light-absorbing impurities, expanding and updating the 1983–1984 survey of Clarke and Noone. Samples were collected in Alaska, Canada, Greenland, Svalbard, Norway, Russia, and the Arctic Ocean during 1998 and 2005–2009, on tundra, glaciers, ice caps, sea ice, frozen lakes, and in boreal forests. Snow was collected mostly in spring, when the entire winter snowpack is accessible for sampling. Sampling was carried out in summer on the Greenland Ice Sheet and on the Arctic Ocean, of melting glacier snow and sea ice as well as cold snow. About 1200 snow samples have been analyzed for this study. The snow is melted and filtered; the filters are analyzed in a specially designed spectrophotometer system to infer the concentration of black carbon (BC), the fraction of absorption due to non-BC light-absorbing constituents and the absorption Ångstrom exponent of all particles. This is done using BC calibration standards having a mass absorption efficiency of 6.0 m2 g−1 at 550 nm and by making an assumption that the absorption Angstrom exponent for BC is 1.0 and for non-BC light-absorbing aerosol is 5.0. The reduction of snow albedo is primarily due to BC, but other impurities, principally brown (organic) carbon, are typically responsible for ~40% of the visible and ultraviolet absorption. The meltwater from selected snow samples was saved for chemical analysis to identify sources of the impurities. Median BC amounts in surface snow are as follows (nanograms of carbon per gram of snow): Greenland 3, Arctic Ocean snow 7, melting sea ice 8, Arctic Canada 8, subarctic Canada 14, Svalbard 13, Northern Norway 21, western Arctic Russia 27, northeastern Siberia 34. Concentrations are more variable in the European Arctic than in Arctic Canada or the Arctic Ocean, probably because of the proximity to BC sources. Individual samples of falling snow were collected on Svalbard, documenting the springtime decline of BC from March through May. Absorption Ångstrom exponents are 1.5–1.7 in Norway, Svalbard, and western Russia, 2.1–2.3 elsewhere in the Arctic, and 2.5 in Greenland. Correspondingly, the estimated contribution to absorption by non-BC constituents in these regions is ~25%, 40%, and 50% respectively. It has been hypothesized that when the snow surface layer melts some of the BC is left at the top of the snowpack rather than being carried away in meltwater. This process was observed in a few locations and would cause a positive feedback on snowmelt. The BC content of the Arctic atmosphere has declined markedly since 1989, according to the continuous measurements of near-surface air at Alert (Canada), Barrow (Alaska), and Ny-Ålesund (Svalbard). Correspondingly, the new BC concentrations for Arctic snow are somewhat lower than those reported by Clarke and Noone for 1983–1984, but because of methodological differences it is not clear that the differences are significant. Nevertheless, the BC content of Arctic snow appears to be no higher now than in 1984, so it is doubtful that BC in Arctic snow has contributed to the rapid decline of Arctic sea ice in recent years.

In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines.