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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 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.

The Lagrangian particle dispersion model FLEXPART was originally designed for calculating long-range and mesoscale dispersion of air pollutants from point sources, such that occurring after an accident in a nuclear power plant. In the meantime, FLEXPART has evolved into a comprehensive tool for atmospheric transport modeling and analysis at different scales. A need for further multiscale modeling and analysis has encouraged new developments in FLEXPART. In this paper, we present a FLEXPART version that works with the Weather Research and Forecasting (WRF) mesoscale meteorological model. We explain how to run this new model and present special options and features that differ from those of the preceding versions. For instance, a novel turbulence scheme for the convective boundary layer has been included that considers both the skewness of turbulence in the vertical velocity as well as the vertical gradient in the air density. To our knowledge, FLEXPART is the first model for which such a scheme has been developed. On a more technical level, FLEXPART-WRF now offers effective parallelization, and details on computational performance are presented here. FLEXPART-WRF output can either be in binary or Network Common Data Form (NetCDF) format, both of which have efficient data compression. In addition, test case data and the source code are provided to the reader as a Supplement. This material and future developments will be accessible at http://www.flexpart.eu.

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.

Black carbon (BC) particles over the Himalayas and Tibetan Plateau (HTP), both airborne and those deposited on snow, have been shown to affect snowmelt and glacier retreat. Since BC over the HTP may originate from a variety of geographical regions and emission sectors, it is essential to quantify the source–receptor relationships of BC in order to understand the contributions of natural and anthropogenic emissions and provide guidance for potential mitigation actions. In this study, we use the Community Atmosphere Model version 5 (CAM5) with a newly developed source-tagging technique, nudged towards the MERRA meteorological reanalysis, to characterize the fate of BC particles emitted from various geographical regions and sectors. Evaluated against observations over the HTP and surrounding regions, the model simulation shows a good agreement in the seasonal variation in the near-surface airborne BC concentrations, providing confidence to use this modeling framework for characterizing BC source–receptor relationships. Our analysis shows that the relative contributions from different geographical regions and source sectors depend on season and location in the HTP. The largest contribution to annual mean BC burden and surface deposition in the entire HTP region is from biofuel and biomass (BB) emissions in South Asia, followed by fossil fuel (FF) emissions from South Asia, then FF from East Asia. The same roles hold for all the seasonal means except for the summer, when East Asia FF becomes more important. For finer receptor regions of interest, South Asia BB and FF have the largest impact on BC in the Himalayas and central Tibetan Plateau, while East Asia FF and BB contribute the most to the northeast plateau in all seasons and southeast plateau in the summer. Central Asia and Middle East FF emissions have relatively more important contributions to BC reaching the northwest plateau, especially in the summer. Although local emissions only contribute about 10% of BC in the HTP, this contribution is extremely sensitive to local emission changes. Lastly, we show that the annual mean radiative forcing (0.42 W m−2) due to BC in snow outweighs the BC dimming effect (−0.3 W m−2) at the surface over the HTP. We also find strong seasonal and spatial variation with a peak value of 5 W m−2 in the spring over the northwest plateau. Such a large forcing of BC in snow is sufficient to cause earlier snow melting and potentially contribute to the acceleration of glacier retreat.

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.

This paper describes and evaluates a new framework for modeling kinetic gas-particle partitioning of secondary organic aerosol (SOA) that takes into account diffusion and chemical reaction within the particle phase. The framework uses a combination of (a) an analytical quasi-steady-state treatment for the diffusion–reaction process within the particle phase for fast-reacting organic solutes, and (b) a two-film theory approach for slow- and nonreacting solutes. The framework is amenable for use in regional and global atmospheric models, although it currently awaits specification of the various gas- and particle-phase chemistries and the related physicochemical properties that are important for SOA formation. Here, the new framework is implemented in the computationally efficient Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) to investigate the competitive growth dynamics of the Aitken and accumulation mode particles. Results show that the timescale of SOA partitioning and the associated size distribution dynamics depend on the complex interplay between organic solute volatility, particle-phase bulk diffusivity, and particle-phase reactivity (as exemplified by a pseudo-first-order reaction rate constant), each of which can vary over several orders of magnitude. In general, the timescale of SOA partitioning increases with increase in volatility and decrease in bulk diffusivity and rate constant. At the same time, the shape of the aerosol size distribution displays appreciable narrowing with decrease in volatility and bulk diffusivity and increase in rate constant. A proper representation of these physicochemical processes and parameters is needed in the next generation models to reliably predict not only the total SOA mass, but also its composition- and number-diameter distributions, all of which together determine the overall optical and cloud-nucleating properties.

The Energy Exascale Earth System Model Atmosphere Model version 1, the atmospheric component of the Department of Energy's Energy Exascale Earth System Model is described. The model began as a fork of the well‐known Community Atmosphere Model, but it has evolved in new ways, and coding, performance, resolution, physical processes (primarily cloud and aerosols formulations), testing and development procedures now differ significantly. Vertical resolution was increased (from 30 to 72 layers), and the model top extended to 60 km (~0.1 hPa). A simple ozone photochemistry predicts stratospheric ozone, and the model now supports increased and more realistic variability in the upper troposphere and stratosphere. An optional improved treatment of light‐absorbing particle deposition to snowpack and ice is available, and stronger connections with Earth system biogeochemistry can be used for some science problems. Satellite and ground‐based cloud and aerosol simulators were implemented to facilitate evaluation of clouds, aerosols, and aerosol‐cloud interactions. Higher horizontal and vertical resolution, increased complexity, and more predicted and transported variables have increased the model computational cost and changed the simulations considerably. These changes required development of alternate strategies for tuning and evaluation as it was not feasible to “brute force” tune the high‐resolution configurations, so short‐term hindcasts, perturbed parameter ensemble simulations, and regionally refined simulations provided guidance on tuning and parameterization sensitivity to higher resolution. A brief overview of the model and model climate is provided. Model fidelity has generally improved compared to its predecessors and the CMIP5 generation of climate models. Plain Language Summary This study provides an overview of a new computer model of the Earth's atmosphere that is used as one component of the Department of Energy's latest Earth system model. The model can be used to help understand past, present, and future changes in Earth's behavior as the system responds to changes in atmospheric composition (like pollution and greenhouse gases), land, and water use and to explore how the atmosphere interacts with other components of the Earth system (ocean, land, biology, etc.). Physical, chemical, and biogeochemical processes treated within the atmospheric model are described, and pointers to previous and recent work are listed to provide additional information. The model is compared to present‐day observations and evaluated for some important tests that provide information about what could happen to clouds and the environment as changes occur. Strengths and weaknesses of the model are listed, as well as opportunities for future work. Key Points A brief description and evaluation is provided for the atmospheric component of the Department of Energy's Energy Exascale Earth System Model Model fidelity has generally improved compared to predecessors and models participating in past international model evaluations Strengths and weaknesses of the model, as well as opportunities for future work, are described

The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity, and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle‐resolved model PartMC‐MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach tracks the evolution of the mixing state of particles due to emission, dilution, condensation, and coagulation. To make this direct stochastic particle‐based method practical, we implemented a new multiscale stochastic coagulation method. With this method we achieved high computational efficiency for situations when the coagulation kernel is highly nonuniform, as is the case for many realistic applications. PartMC‐MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the evolution of carbonaceous aerosols of different types due to coagulation and condensation. For this urban plume scenario we quantified the individual processes that contributed to the aging of the aerosol distribution, illustrating the capabilities of our modeling approach. The results showed for the first time the multidimensional structure of particle composition, which is usually lost in sectional or modal aerosol models.

A fully coupled meteorology-chemistry-aerosol model (WRF-Chem) is applied to simulate mineral dust and its shortwave (SW) radiative forcing over North Africa. Two dust emission schemes (GOCART and DUSTRAN) and two aerosol models (MADE/SORGAM and MOSAIC) are adopted in simulations to investigate the modeling sensitivities to dust emissions and aerosol size treatments. The modeled size distribution and spatial variability of mineral dust and its radiative properties are evaluated using measurements (ground-based, aircraft, and satellites) during the AMMA SOP0 campaign from 6 January to 3 February of 2006 (the SOP0 period) over North Africa. Two dust emission schemes generally simulate similar spatial distributions and temporal evolutions of dust emissions. Simulations using the GOCART scheme with different initial (emitted) dust size distributions require ~40% difference in total emitted dust mass to produce similar SW radiative forcing of dust over the Sahel region. The modal approach of MADE/SORGAM retains 25% more fine dust particles (radius<1.25 μm) but 8% less coarse dust particles (radius>1.25 μm) than the sectional approach of MOSAIC in simulations using the same size-resolved dust emissions. Consequently, MADE/SORGAM simulates 11% higher AOD, up to 13% lower SW dust heating rate, and 15% larger (more negative) SW dust radiative forcing at the surface than MOSAIC over the Sahel region. In the daytime of the SOP0 period, the model simulations show that the mineral dust heats the lower atmosphere with an average rate of 0.8 ± 0.5 K day−1 over the Niamey vicinity and 0.5 ± 0.2 K day−1 over North Africa and reduces the downwelling SW radiation at the surface by up to 58 W m−2 with an average of 22 W m−2 over North Africa. This highlights the importance of including dust radiative impact in understanding the regional climate of North Africa. When compared to the available measurements, the WRF-Chem simulations can generally capture the measured features of mineral dust and its radiative properties over North Africa, suggesting that the model is suitable for more extensive simulations of dust impact on regional climate over North Africa.