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Estimating anthropogenic aerosol effects on the planetary energy balance through the aerosol influence on clouds using the difference in cloud radiative forcing from simulations with and without anthropogenic emissions produces estimates that are positively biased. A more representative method is suggested using the difference in cloud radiative forcing calculated as a diagnostic with aerosol scattering and absorption neglected. The method also yields an aerosol radiative forcing decomposition that includes a term quantifying the impact of changes in surface albedo. The method requires only two additional diagnostic calculations: the whole-sky and clear-sky top-of-atmosphere radiative flux with aerosol scattering and absorption neglected.

Atmospheric carbonaceous aerosols play an important role in the climate system by influencing the Earth's radiation budgets and modifying the cloud properties. Despite the importance, their representations in large-scale atmospheric models are still crude, which can influence model simulated burden, lifetime, physical, chemical and optical properties, and the climate forcing of carbonaceous aerosols. In this study, we improve the current three-mode version of the Modal Aerosol Module (MAM3) in the Community Atmosphere Model version 5 (CAM5) by introducing an additional primary carbon mode to explicitly account for the microphysical ageing of primary carbonaceous aerosols in the atmosphere. Compared to MAM3, the four-mode version of MAM (MAM4) significantly increases the column burdens of primary particulate organic matter (POM) and black carbon (BC) by up to 40 % in many remote regions, where in-cloud scavenging plays an important role in determining the aerosol concentrations. Differences in the column burdens for other types of aerosol (e.g., sulfate, secondary organic aerosols, mineral dust, sea salt) are less than 1 %. Evaluating the MAM4 simulation against in situ surface and aircraft observations, we find that MAM4 significantly improves the simulation of seasonal variation of near-surface BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons. However, it exacerbates the overestimation of modeled BC concentrations in the upper troposphere in the Pacific regions. The comparisons suggest that, to address the remaining model POM and BC biases, future improvements are required related to (1) in-cloud scavenging and vertical transport in convective clouds and (2) emissions of anthropogenic and biomass burning aerosols.

The authors have decomposed the anthropogenic aerosol radiative forcing into direct contributions from each aerosol species to the planetary energy balance through absorption and scattering of solar radiation, indirect effects of anthropogenic aerosol on solar and infrared radiation through droplet and crystal nucleation on aerosol, and semidirect effects through the influence of solar absorption on the distribution of clouds. A three-mode representation of the aerosol in version 5.1 of the Community Atmosphere Model (CAM5.1) yields global annual mean radiative forcing estimates for each of these forcing mechanisms that are within 0.1 W m−2of estimates using a more complex seven-mode representation that distinguishes between fresh and aged black carbon and primary organic matter. Simulating fresh black carbon particles separately from internally mixed accumulation mode particles is found to be important only near fossil fuel sources. In addition to the usual large indirect effect on solar radiation, this study finds an unexpectedly large positive longwave indirect effect (because of enhanced cirrus produced by homogenous nucleation of ice crystals on anthropogenic sulfate), small shortwave and longwave semidirect effects, and a small direct effect (because of cancelation and interactions of direct effects of black carbon and sulfate). Differences between the three-mode and seven-mode versions are significantly larger (up to 0.2 W m−2) when the hygroscopicity of primary organic matter is decreased from 0.1 to 0 and transfer of the primary carbonaceous aerosol to the accumulation mode in the seven-mode version requires more hygroscopic material coating the primary particles. Radiative forcing by cloudborne anthropogenic black carbon is only −0.07 W m−2.

We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present day (year 2000 ACCMIP time slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of approximately 50 Tg(N) yr-1 from nitrogen oxide emissions, 60 Tg(N) yr-1 from ammonia emissions, and 83 Tg(S) yr-1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards a potential misrepresentation of 1980 NH3 emissions over North America. Based on ice core records, the 1850 deposition fluxes agree well with Greenland ice cores, but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways (RCPs) to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double their 2000 counterpart in some scenarios and reaching > 1300 mg(N) m-2 yr-1 averaged over regional to continental-scale regions in RCP 2.6 and 8.5, ~ 30-50% larger than the values in any region currently (circa 2000). However, sulfur deposition rates in 2100 are in all regions lower than in 2000 in all the RCPs. The new ACCMIP multi-model deposition dataset provides state-of-the-science, consistent and evaluated time slice (spanning 1850-2100) global gridded deposition fields for use in a wide range of climate and ecological studies.

A process‐based treatment of ice supersaturation and ice nucleation is implemented in the National Center for Atmospheric Research Community Atmosphere Model (CAM). The new scheme is designed to allow (1) supersaturation with respect to ice, (2) ice nucleation by aerosol particles, and (3) ice cloud cover consistent with ice microphysics. The scheme is implemented with a two‐moment microphysics code and is used to evaluate ice cloud nucleation mechanisms and supersaturation in CAM. The new model is able to reproduce field observations of ice mass and mixed phase cloud occurrence better than previous versions. The model is able to reproduce observed patterns and frequency of ice supersaturation. Simulations indicate homogeneous freezing of sulfate and heterogeneous freezing on dust are both important ice nucleation mechanisms, in different regions. Simulated cloud forcing and climate is sensitive to different formulations of the ice microphysics. Arctic surface radiative fluxes are sensitive to the parameterization of ice clouds. These results indicate that ice clouds are potentially an important part of understanding cloud forcing and potential cloud feedbacks, particularly in the Arctic.

The global performance of a new two-moment cloud microphysics scheme for a general circulation model (GCM) is presented and evaluated relative to observations. The scheme produces reasonable representations of cloud particle size and number concentration when compared to observations, and it represents expected and observed spatial variations in cloud microphysical quantities. The scheme has smaller particles and higher number concentrations over land than the standard bulk microphysics in the GCM and is able to balance the top-of-atmosphere radiation budget with 60% the liquid water of the standard scheme, in better agreement with retrieved values. The new scheme diagnostically treats both the mixing ratio and number concentration of rain and snow, and it is therefore able to differentiate the two key regimes, consisting of drizzle in shallow, warm clouds and larger rain drops in deeper cloud systems. The modeled rain and snow size distributions are consistent with observations.

Nudging as an assimilation technique has seen increased use in recent years in the development and evaluation of climate models. Constraining the simulated wind and temperature fields using global weather reanalysis facilitates more straightforward comparison between simulation and observation, and reduces uncertainties associated with natural variabilities of the large-scale circulation. On the other hand, the forcing introduced by nudging can be strong enough to change the basic characteristics of the model climate. In the paper we show that for the Community Atmosphere Model version 5 (CAM5), due to the systematic temperature bias in the standard model and the sensitivity of simulated ice formation to anthropogenic aerosol concentration, nudging towards reanalysis results in substantial reductions in the ice cloud amount and the impact of anthropogenic aerosols on long-wave cloud forcing. In order to reduce discrepancies between the nudged and unconstrained simulations, and meanwhile take the advantages of nudging, two alternative experimentation methods are evaluated. The first one constrains only the horizontal winds. The second method nudges both winds and temperature, but replaces the long-term climatology of the reanalysis by that of the model. Results show that both methods lead to substantially improved agreement with the free-running model in terms of the top-of-atmosphere radiation budget and cloud ice amount. The wind-only nudging is more convenient to apply, and provides higher correlations of the wind fields, geopotential height and specific humidity between simulation and reanalysis. Results from both CAM5 and a second aerosol–climate model ECHAM6-HAM2 also indicate that compared to the wind-and-temperature nudging, constraining only winds leads to better agreement with the free-running model in terms of the estimated shortwave cloud forcing and the simulated convective activities. This suggests nudging the horizontal winds but not temperature is a good strategy for the investigation of aerosol indirect effects since it provides well-constrained meteorology without strongly perturbing the model's mean climate.

The impact of black carbon (BC) aerosols on the global radiation balance is not well constrained. Here twelve global aerosol models are used to show that at least 20% of the present uncertainty in modeled BC direct radiative forcing (RF) is due to diversity in the simulated vertical profile of BC mass. Results are from phases 1 and 2 of the global aerosol model intercomparison project (AeroCom). Additionally, a significant fraction of the variability is shown to come from high altitudes, as, globally, more than 40% of the total BC RF is exerted above 5 km. BC emission regions and areas with transported BC are found to have differing characteristics. These insights into the importance of the vertical profile of BC lead us to suggest that observational studies are needed to better characterize the global distribution of BC, including in the upper troposphere.

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02 Wm−2, with a mean of −0.27 Wm−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35 Wm−2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.

Atmospheric black carbon (BC) absorbs solar radiation, and exacerbates global warming through exerting positive radiative forcing (RF). However, the contribution of BC to ongoing changes in global climate is under debate. Anthropogenic BC emissions, and the resulting distribution of BC concentration, are highly uncertain. In particular, long-range transport and processes affecting BC atmospheric lifetime are poorly understood. Here we discuss whether recent assessments may have overestimated present-day BC radiative forcing in remote regions. We compare vertical profiles of BC concentration from four recent aircraft measurement campaigns to simulations by 13 aerosol models participating in the AeroCom Phase II intercomparison. An atmospheric lifetime of BC of less than 5 days is shown to be essential for reproducing observations in remote ocean regions, in line with other recent studies. Adjusting model results to measurements in remote regions, and at high altitudes, leads to a 25% reduction in AeroCom Phase II median direct BC forcing, from fossil fuel and biofuel burning, over the industrial era. The sensitivity of modelled forcing to BC vertical profile and lifetime highlights an urgent need for further flight campaigns, close to sources and in remote regions, to provide improved quantification of BC effects for use in climate policy.