Modal Aerosol Module Research Articles

Enhanced Aging of Black Carbon under Recent Clean Air Actions and Future Carbon Neutrality Scenario in China.

China has implemented strict emission control measures, but it is unclear how they affect black carbon (BC) aging and light absorption. Here, we use the Community Atmosphere Model version 6 (CAM6) with the four-mode version of the Modal Aerosol Module coupled with machine learning (MAM4-ML) to simulate BC aging during 2011-2018 and 2050/2100 following a carbon neutrality scenario (SSP1-2.6), respectively. During 2011-2018, the mass ratio of coatings to BC (RBC) widely increased (5.4% yr-1) over the east of China. The increased secondary organic aerosol (SOA) coatings dominate (88%) the increased RBC, while the sulfate coatings decrease. The drivers of BC coating changes come from the different magnitudes of emission reductions in secondary aerosol precursors (i.e., volatile organic compounds (VOCs) and SO2) and BC. During 2011-2018, the increased RBC enhances the BC mass absorption cross section (MAC, 0.7% yr-1). In 2050/2100 for SSP1-2.6, emission control leads to further increased RBC (95/145%) and BC MAC (12/17%). For both 2011-2018 and 2050/2100, the enhanced BC MAC partly offsets the declining direct radiative effect (DRE) of BC due to direct emission reduction. As a result, the full impact of direct emission reductions of BC on BC DRE is only 75% for 2011-2018 and 90/94% for 2050/2100.

Validating a microphysical prognostic stratospheric aerosol implementation in E3SMv2 using observations after the Mount Pinatubo eruption

Abstract. This paper describes the addition of a stratospheric prognostic aerosol (SPA) capability – developed with the goal of accurately simulating sulfate aerosol formation and evolution in the stratosphere – in the Department of Energy (DOE) Energy Exascale Earth System Model, version 2 (E3SMv2). The implementation includes changes to the four-mode Modal Aerosol Module microphysics in the stratosphere to allow for larger particle growth and more accurate stratospheric aerosol lifetime following the Pinatubo eruption. E3SMv2-SPA reasonably reproduces stratospheric aerosol lifetime, burden, aerosol optical depth, and top-of-atmosphere flux when compared to remote sensing observations. E3SMv2-SPA also has close agreement with the interactive chemistry–climate model CESM2-WACCM (Community Earth System Model version 2–Whole Atmosphere Community Climate Model) – which has a more complete chemical treatment – and the observationally constrained, prescribed volcanic aerosol treatment in E3SMv2. Global stratospheric aerosol size distributions identify the nucleation and growth of sulfate aerosol from volcanically injected SO2 from both major and minor volcanic eruptions from 1991 to 1993. The modeled aerosol effective radius is consistently lower than satellite and in situ measurements (max differences of ∼ 30 %). Comparisons with in situ size distribution samples indicate that this simulated underestimation in both E3SMv2-SPA and CESM2-WACCM is due to overly small accumulation and coarse-mode aerosols 6–18 months post-eruption, with E3SMv2-SPA simulating ∼ 50 % of the coarse-mode geometric mean diameters of observations 11 months post-eruption. Effective radii from the models and observations are used to calculate offline scattering and absorption efficiencies to explore the implications of smaller simulated aerosol size for the Pinatubo climate impacts. Scattering efficiencies at wavelengths of peak solar irradiance (∼ 0.5 µm) are 10 %–80 % higher for daily samples in models relative to observations through 1993, suggesting higher diffuse radiation at the surface and a larger cooling effect in the models due to the smaller simulated aerosol; absorption efficiencies at the peak wavelengths of outgoing terrestrial radiation (∼ 10 µm) are 15 %–40 % lower for daily samples in models relative to observations, suggesting an underestimation in stratospheric heating in the models due to the smaller simulated aerosol. These potential biases are based on aerosol size alone and do not take into account differences in the aerosol number. The overall agreement of E3SMv2-SPA with observations and its similar performance to the well-validated CESM2-WACCM makes E3SMv2-SPA a viable alternative to simulating climate impacts from stratospheric sulfate aerosols.

Quantifying structural errors in cloud condensation nuclei activity from reduced representation of aerosol size distributions

Aerosol effects on clouds and radiation are a large source of uncertainty in our understanding of human impacts on the climate system. Uncertainty in aerosol effects results from uncertainty in parameter values, known as parametric uncertainty, and from uncertainty from the model’s structure, known as structural uncertainty. While previous studies have assessed the impact of parametric uncertainty on modeled forcing, structural errors from the numerical representation of particle distributions and their dynamics have not been well quantified. Here we present a framework for quantifying error in aerosol size distributions and cloud condensation nuclei activity, which we apply to the widely used 4-mode version of the Modal Aerosol Module (MAM4). Box model predictions from the MAM4 are evaluated against the Particle Monte Carlo Model for Simulating Aerosol Interactions and Chemistry (PartMC-MOSAIC), a benchmark model that tracks the evolution of individual particles. We show that size distributions simulated by MAM4 diverge from those simulated by PartMC-MOSAIC after only a few hours of aging by condensation and coagulation in polluted conditions, which leads to large errors in modeled cloud condensation nuclei concentrations. We find that differences between MAM4 and PartMC-MOSAIC are largest under polluted conditions, where the size distribution evolves rapidly though aging. These findings indicate that structural error in modeled aerosol properties is a key factor contributing to uncertainty in aerosol forcing.

Improving BC Mixing State and CCN Activity Representation With Machine Learning in the Community Atmosphere Model Version 6 (CAM6)

AbstractRepresenting mixing state of black carbon (BC) is challenging for global climate models (GCMs). The Community Atmosphere Model version 6 (CAM6) with the four‐mode version of the Modal Aerosol Module (MAM4) represents aerosols as fully internal mixtures with uniform composition within each aerosol mode, resulting in high degree of internal mixing of BC with non‐BC species and large mass ratio of coating to BC (RBC, the mass ratio of non‐BC species to BC in BC‐containing particles). To improve BC mixing state representation, we coupled a machine learning (ML) model of BC mixing state index trained on particle‐resolved simulations to the CAM6 with MAM4 (MAM4‐ML). In MAM4‐ML, we use RBC to partition accumulation mode particles into two new modes, BC‐free particles and BC‐containing particles. We adjust RBC to make the modeled BC mixing state index (χmode) match the one predicted by the ML model (χML). On a global average, the mass fraction of BC‐containing particles in accumulation mode decreases from 100% (MAM4‐default) to 48% (MAM4‐ML). The globally averaged χmode decreases from 78% (MAM4‐default) to 63% (MAM4‐ML, 19% reduction) and agrees well with χML (66%). The RBC decreases by 52% for accumulation mode and better agrees with observations. The hygroscopicity drops by 9% for BC‐containing particles in accumulation mode, leading to a 20% reduction in the BC activation fraction. The surface BC concentration increases most (6.9%) in the Arctic, and the BC burden increases by 4%, globally. Our study highlights the application of the ML model for improving key aerosol processes in GCMs.

Evaluating BC Aging Processes in the Community Atmosphere Model Version 6 (CAM6)

AbstractThe uncertainty of the climatic effect of Black carbon (BC) remains large. One critical uncertainty source that needs to be captured is BC aging. Here we use the Community Atmosphere Model version 6 (CAM6) configured with the four‐mode version of the Modal Aerosol Module (MAM4) to evaluate the modeled BC aging process with recent laboratory and in‐situ measurements over China. As revealed by the comparison of BC aging timescale and number fraction of aged BC against recent measurements, the modeled condensation aging timescale is estimated to be about 0.8 hr (17%) faster than the chamber measurement, and the diurnal variations of modeled BC aging degree are typically higher than observations mainly due to the fast increase in modeled BC aging degree during daytime. Further analysis shows that the condensation aging dominates (>70%) BC aging across China. More specifically, the condensation of secondary organic aerosol (SOA) vapor contributes most to BC aging over China. Slowing down BC aging increases the modeled surface BC concentration over remote Western China and BC burden, but hardly changes surface BC concentration over Eastern China. Our results suggest that BC aging representation in the MAM4 needs to be further improved toward slowing down the BC aging rate, especially the condensation aging by SOA, to improve the BC simulation over remote areas and its impact on BC transport in MAM4.

Development and Evaluation of E3SM‐MOSAIC: Spatial Distributions and Radiative Effects of Nitrate Aerosol

AbstractNitrate aerosol plays an important role in affecting regional air quality as well as Earth's climate. However, it is not well represented or even neglected in many global climate models. In this study, we couple the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module with the four‐mode version of the Modal Aerosol Module (MAM4) in DOE's Energy Exascale Earth System Model version 2 (E3SMv2) to simulate nitrate aerosol and its radiative effects. We find that nitrate aerosol simulated by E3SMv2‐MAM4‐MOSAIC is sensitive to the treatment of gaseous HNO3 transfer to/from interstitial particles related to accommodation coefficients of HNO3 () on dust and non‐dust particles. We compare three different treatments of HNO3 transfer: (a) a treatment (MTC_SLOW) that uses a low in the mass transfer coefficient (MTC) calculation; (b) a dust‐weighted MTC treatment (MTC_WGT) that uses a high on non‐dust particles; and (c) a dust‐weighted MTC treatment that also splits coarse mode aerosols into the coarse dust and sea salt sub‐modes in MOSAIC (MTC_SPLC). MTC_WGT and MTC_SPLC increase the global annual mean (2005–2014) nitrate burden from 0.096 (MTC_SLOW) to 0.237 and 0.185 Tg N, respectively, mostly in the coarse mode. MTC_WGT and MTC_SPLC also produce stronger nitrate direct radiative forcing (−0.048 and −0.051 W m−2, respectively) and indirect forcing (−0.33 and −0.35 W m−2, respectively) than MTC_SLOW (−0.021 and −0.24 W m−2). MTC_WGT and MTC_SPLC improve nitrate surface concentrations over remote oceans based on limited observations and vertical profiles of nitrate concentrations against aircraft measurements below 400 hPa.

Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model

Abstract. Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. This study aims to verify the global distribution of aerosol mixing state represented by modal models. To quantify the aerosol mixing state, we used the aerosol mixing state indices for submicron aerosol based on the mixing of optically absorbing and non-absorbing species (χo), the mixing of primary carbonaceous and non-primary carbonaceous species (χc), and the mixing of hygroscopic and non-hygroscopic species (χh). To achieve a spatiotemporal comparison, we calculated the mixing state indices using output from the Community Earth System Model with the four-mode version of the Modal Aerosol Module (MAM4) and compared the results with the mixing state indices from a benchmark machine-learned model trained on high-detail particle-resolved simulations from the particle-resolved stochastic aerosol model PartMC-MOSAIC. The two methods yielded very different spatial patterns of the mixing state indices. In some regions, the yearly averaged χ value computed by the MAM4 model differed by up to 70 percentage points from the benchmark values. These errors tended to be zonally structured, with the MAM4 model predicting a more internally mixed aerosol at low latitudes and a more externally mixed aerosol at high latitudes compared to the benchmark. Our study quantifies potential model bias in simulating mixing state in different regions and provides insights into potential improvements to model process representation for a more realistic simulation of aerosols towards better quantification of radiative forcing and aerosol–cloud interactions.

Radiative Forcing of Nitrate Aerosols From 1975 to 2010 as Simulated by MOSAIC Module in CESM2‐MAM4

AbstractWe incorporate the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model Version 6 with interactive chemistry (CAM6‐chem), and couple it with the four mode version of the Modal Aerosol Module (MAM4). The MOSAIC module is used to simulate the thermodynamics of the gas‐aerosol mass exchange, with a special focus on simulating nitrate aerosol. By comparing against ground and satellite observations, we found that the MOSAIC/MAM4 scheme performs reasonably well in simulating spatiotemporal distributions of aerosols, including nitrate aerosol. We conducted a series of model experiments with and without nitrate aerosols, and examined the radiative effect (RE) associated with nitrate aerosols in 1975, 2000, and 2010, and accessed the radiative forcing (RF) of nitrate aerosols between the present day and pre‐industrial periods. Comparing with the nitrate aerosol RE, we predicted relatively small RF of anthropogenic nitrate aerosol from aerosol‐radiation interactions (RFari: −0.014 W m−2) and large RF from aerosol‐cloud interactions (RFaci: −0.219 W m−2). Regional signatures of nitrate RE/RF are noticeable and important: for instance, very small changes in REari in Europe and USA, but 2.8–3 times increases in REari in India and China from 1975 to 2010, while REaci/RFaci in China is a warming effect due to the competing effect between sulfate and nitrate aerosols as cloud condensation nuclei.

Development and Evaluation of Chemistry-Aerosol-Climate Model CAM5-Chem-MAM7-MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol.

An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m−2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m−2. Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m−2. Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m−2.

Effective radiative forcing in the aerosol–climate model CAM5.3-MARC-ARG

Abstract. We quantify the effective radiative forcing (ERF) of anthropogenic aerosols modelled by the aerosol–climate model CAM5.3-MARC-ARG. CAM5.3-MARC-ARG is a new configuration of the Community Atmosphere Model version 5.3 (CAM5.3) in which the default aerosol module has been replaced by the two-Moment, Multi-Modal, Mixing-state-resolving Aerosol model for Research of Climate (MARC). CAM5.3-MARC-ARG uses the ARG aerosol-activation scheme, consistent with the default configuration of CAM5.3. We compute differences between simulations using year-1850 aerosol emissions and simulations using year-2000 aerosol emissions in order to assess the radiative effects of anthropogenic aerosols. We compare the aerosol lifetimes, aerosol column burdens, cloud properties, and radiative effects produced by CAM5.3-MARC-ARG with those produced by the default configuration of CAM5.3, which uses the modal aerosol module with three log-normal modes (MAM3), and a configuration using the modal aerosol module with seven log-normal modes (MAM7). Compared with MAM3 and MAM7, we find that MARC produces stronger cooling via the direct radiative effect, the shortwave cloud radiative effect, and the surface albedo radiative effect; similarly, MARC produces stronger warming via the longwave cloud radiative effect. Overall, MARC produces a global mean net ERF of -1.79±0.03 W m−2, which is stronger than the global mean net ERF of -1.57±0.04 W m−2 produced by MAM3 and -1.53±0.04 W m−2 produced by MAM7. The regional distribution of ERF also differs between MARC and MAM3, largely due to differences in the regional distribution of the shortwave cloud radiative effect. We conclude that the specific representation of aerosols in global climate models, including aerosol mixing state, has important implications for climate modelling.

Aviation impact on air quality present day and mid-century simulated in the Community Atmosphere Model (CAM)

The projected increase in global air traffic raises concerns about the potential impact aviation emissions have on climate and air quality. Previous studies have shown that aircraft non-landing and take-off (non-LTO) emissions (emitted above 1 km) can affect surface air quality by increasing concentrations of ozone (O3) and fine particles (PM2.5). Here, we examine the global impacts of aviation non-LTO emissions on surface air quality for present day and mid-century (2050) using the Community Atmosphere Model with Chemistry, version 5 (CAM5). An important update in CAM5 over previous versions is the modal aerosol module (MAM), which provides a more accurate aerosol representation. Additionally we evaluate of the aviation impact at mid-century with two fuel scenarios, a fossil fuel (SC1) and a biofuel (Alt). Monthly-mean results from the present day simulations show a northern hemisphere (NH) mean surface O3 increase of 1.3 ppb (2.7% of the background) and a NH maximum surface PM2.5 increase of 1.4 μg/m3 in January. Mid-century simulations show slightly greater surface O3 increases (mean of 1.9 ppb (4.2%) for both scenarios) and greater PM2.5 increases (maximum of 3.5 μg/m3 for SC1 and 2.2 μg/m3 for Alt). While these perturbations do not significantly increase the frequency of extreme air quality events (increase is less than 1.5%), they do contribute to the background concentrations of O3 and PM2.5, making it easier for urban areas to surpass these standards.

Constraining Aging Processes of Black Carbon in the Community Atmosphere Model Using Environmental Chamber Measurements.

The direct radiative forcing of black carbon aerosol (BC) on the Earth system remains unsettled, largely due to the uncertainty with physical properties of BC throughout their lifecycle. Here we show that ambient chamber measurements of BC properties provide a novel constraint on the crude BC aging representation in climate models. Observational evidence for significant absorption enhancement of BC can be reproduced when the aging processes in the four‐mode version of the Modal Aerosol Module (MAM4) aerosol scheme in the Community Atmosphere Model version 5 are calibrated by the recent in situ chamber measurements. An observation‐based scaling method is developed in the aging timescale calculation to alleviate the influence of biases in the simulated model chemical composition. Model sensitivity simulations suggest that the different monolayer settings in the BC aging parameterization of MAM4 can cause as large as 26% and 24% differences in BC burden and radiative forcing, respectively. We also find that an increase in coating materials (e.g., sulfate and secondary organic aerosols) reduces BC lifetime by increasing the hygroscopicity of the mixture but enhances its absorption, resulting in a net increase in BC direct radiative forcing. Our results suggest that accurate simulations of BC aging processes as well as other aerosol species are equally important in reducing the uncertainty of BC forcing estimation.

Description and evaluation of a new four-mode version of the Modal Aerosol Module (MAM4) within version 5.3 of the Community Atmosphere Model

Abstract. 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.

A new chemistry option in WRF-Chem v. 3.4 for the simulation of direct and indirect aerosol effects using VBS: evaluation against IMPACT-EUCAARI data

Abstract. A parameterization for secondary organic aerosol (SOA) production based on the volatility basis set (VBS) approach has been coupled with microphysics and radiative schemes in the Weather Research and Forecasting model with Chemistry (WRF-Chem) model. The new chemistry option called "RACM-MADE-VBS-AQCHEM" was evaluated on a cloud resolving scale against ground-based and aircraft measurements collected during the IMPACT-EUCAARI (Intensive Cloud Aerosol Measurement Campaign – European Integrated project on Aerosol Cloud Climate and Air quality interaction) campaign, and complemented with satellite data from MODIS. The day-to-day variability and the diurnal cycle of ozone (O3) and nitrogen oxides (NOx) at the surface are captured by the model. Surface aerosol mass concentrations of sulfate (SO4), nitrate (NO3), ammonium (NH4), and organic matter (OM) are simulated with correlations larger than 0.55. WRF-Chem captures the vertical profile of the aerosol mass concentration in both the planetary boundary layer (PBL) and free troposphere (FT) as a function of the synoptic condition, but the model does not capture the full range of the measured concentrations. Predicted OM concentration is at the lower end of the observed mass concentrations. The bias may be attributable to the missing aqueous chemistry processes of organic compounds and to uncertainties in meteorological fields. A key role could be played by assumptions on the VBS approach such as the SOA formation pathways, oxidation rate, and dry deposition velocity of organic condensable vapours. Another source of error in simulating SOA is the uncertainties in the anthropogenic emissions of primary organic carbon. Aerosol particle number concentration (condensation nuclei, CN) is overestimated by a factor of 1.4 and 1.7 within the PBL and FT, respectively. Model bias is most likely attributable to the uncertainties of primary particle emissions (mostly in the PBL) and to the nucleation rate. Simulated cloud condensation nuclei (CCN) are also overestimated, but the bias is more contained with respect to that of CN. The CCN efficiency, which is a characterization of the ability of aerosol particles to nucleate cloud droplets, is underestimated by a factor of 1.5 and 3.8 in the PBL and FT, respectively. The comparison with MODIS data shows that the model overestimates the aerosol optical thickness (AOT). The domain averages (for 1 day) are 0.38 ± 0.12 and 0.42 ± 0.10 for MODIS and WRF-Chem data, respectively. The droplet effective radius (Re) in liquid-phase clouds is underestimated by a factor of 1.5; the cloud liquid water path (LWP) is overestimated by a factor of 1.1–1.6. The consequence is the overestimation of average liquid cloud optical thickness (COT) from a few percent up to 42 %. The predicted cloud water path (CWP) in all phases displays a bias in the range +41–80 %, whereas the bias of COT is about 15 %. In sensitivity tests where we excluded SOA, the skills of the model in reproducing the observed patterns and average values of the microphysical and optical properties of liquid and all phase clouds decreases. Moreover, the run without SOA (NOSOA) shows convective clouds with an enhanced content of liquid and frozen hydrometers, and stronger updrafts and downdrafts. Considering that the previous version of WRF-Chem coupled with a modal aerosol module predicted very low SOA content (secondary organic aerosol model (SORGAM) mechanism) the new proposed option may lead to a better characterization of aerosol–cloud feedbacks.

Stratospheric sulfur and its implications for radiative forcing simulated by the chemistry climate model EMAC.

Multiyear simulations with the atmospheric chemistry general circulation model EMAC with a microphysical modal aerosol module at high vertical resolution demonstrate that the sulfur gases COS and SO2, the latter from low-latitude and midlatitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. Marine dimethyl sulfide (DMS) and other SO2 sources, including strong anthropogenic emissions in China, are found to play a minor role except in the lowermost stratosphere. Estimates of volcanic SO2 emissions are based on satellite observations using Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument for total injected mass and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat or Stratospheric Aerosol and Gases Experiment for the spatial distribution. The 10 year SO2 and COS data set of MIPAS is also used for model evaluation. The calculated radiative forcing of stratospheric background aerosol including sulfate from COS and small contributions by DMS oxidation, and organic aerosol from biomass burning, is about 0.07W/m2. For stratospheric sulfate aerosol from medium and small volcanic eruptions between 2005 and 2011 a global radiative forcing up to 0.2W/m2 is calculated, moderating climate warming, while for the major Pinatubo eruption the simulated forcing reaches 5W/m2, leading to temporary climate cooling. The Pinatubo simulation demonstrates the importance of radiative feedback on dynamics, e.g., enhanced tropical upwelling, for large volcanic eruptions.

Modeling dust as component minerals in the Community Atmosphere Model: development of framework and impact on radiative forcing

Abstract. The mineralogy of desert dust is important due to its effect on radiation, clouds and biogeochemical cycling of trace nutrients. This study presents the simulation of dust radiative forcing as a function of both mineral composition and size at the global scale, using mineral soil maps for estimating emissions. Externally mixed mineral aerosols in the bulk aerosol module in the Community Atmosphere Model version 4 (CAM4) and internally mixed mineral aerosols in the modal aerosol module in the Community Atmosphere Model version 5.1 (CAM5) embedded in the Community Earth System Model version 1.0.5 (CESM) are speciated into common mineral components in place of total dust. The simulations with mineralogy are compared to available observations of mineral atmospheric distribution and deposition along with observations of clear-sky radiative forcing efficiency. Based on these simulations, we estimate the all-sky direct radiative forcing at the top of the atmosphere as + 0.05 Wm−2 for both CAM4 and CAM5 simulations with mineralogy. We compare this to the radiative forcing from simulations of dust in release versions of CAM4 and CAM5 (+0.08 and +0.17 Wm−2) and of dust with optimized optical properties, wet scavenging and particle size distribution in CAM4 and CAM5, −0.05 and −0.17 Wm−2, respectively. The ability to correctly include the mineralogy of dust in climate models is hindered by its spatial and temporal variability as well as insufficient global in situ observations, incomplete and uncertain source mineralogies and the uncertainties associated with data retrieved from remote sensing methods.

Aviation 2006 NO<sub>x</sub>-induced effects on atmospheric ozone and HO<sub>x</sub> in Community Earth System Model (CESM)

Abstract. The interaction between atmospheric chemistry and ozone (O3) in the upper troposphere–lower stratosphere (UTLS) presents a major uncertainty in understanding the effects of aviation on climate. In this study, two configurations of the atmospheric model from the Community Earth System Model (CESM), Community Atmosphere Model with Chemistry, Version 4 (CAM4) and Version 5 (CAM5), are used to evaluate the effects of aircraft nitrogen oxide (NOx = NO + NO2) emissions on ozone and the background chemistry in the UTLS. CAM4 and CAM5 simulations were both performed with extensive tropospheric and stratospheric chemistry including 133 species and 330 photochemical reactions. CAM5 includes direct and indirect aerosol effects on clouds using a modal aerosol module (MAM), whereby CAM4 uses a bulk aerosol module, which can only simulate the direct effect. To examine the accuracy of the aviation NOx-induced ozone distribution in the two models, results from the CAM5 and CAM4 simulations are compared to ozonesonde data. Aviation NOx emissions for 2006 were obtained from the AEDT (Aviation Environmental Design Tool) global commercial aircraft emissions inventory. Differences between simulated O3 concentrations and ozonesonde measurements averaged at representative levels in the troposphere and different regions are 13% in CAM5 and 18% in CAM4. Results show a localized increase in aviation-induced O3 concentrations at aviation cruise altitudes that stretches from 40° N to the North Pole. The results indicate a greater and more disperse production of aviation NOx-induced ozone in CAM5, with the annual tropospheric mean O3 perturbation of 1.2 ppb (2.4%) for CAM5 and 1.0 ppb (1.9%) for CAM4. The annual mean O3 perturbation peaks at about 8.2 ppb (6.4%) and 8.8 ppb (5.2%) in CAM5 and CAM4, respectively. Aviation emissions also result in increased hydroxyl radical (OH) concentrations and methane (CH4) loss rates, reducing the tropospheric methane lifetime in CAM5 and CAM4 by 1.69 and 1.40%, respectively. Aviation NOx emissions are associated with an instantaneous change in global mean short-term O3 radiative forcing (RF) of 40.3 and 36.5 mWm−2 in CAM5 and CAM4, respectively.

Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

Abstract. We present the implementation and evaluation of a sectional aerosol microphysics module SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by minimising the number of variables needed to describe the size and composition distribution. The aerosol size distribution is described using 10 size classes with parallel sections which can have different chemical compositions. Thus in total, the module tracks 20 size sections which cover diameters ranging from 3 nm to 10 μm and are divided into three subranges, each with an optimised selection of processes and compounds. The implementation of SALSA into ECHAM5-HAM includes the main aerosol processes in the atmosphere: emissions, removal, radiative effects, liquid and gas phase sulphate chemistry, and the aerosol microphysics. The aerosol compounds treated in the module are sulphate, organic carbon, sea salt, black carbon, and mineral dust. In its default configuration, ECHAM5-HAM treats aerosol size distribution using the modal method. In this implementation, the aerosol processes were converted to be used in a sectional model framework. The ability of the module to describe the global aerosol properties was evaluated by comparing against (1) measured continental and marine size distributions, (2) observed variability of continental number concentrations, (3) measured sulphate, organic carbon, black carbon and sea-salt mass concentrations, (4) observations of aerosol optical depth (AOD) and other aerosol optical properties from satellites and AERONET network, (5) global aerosol budgets and concentrations from previous model studies, and (6) model results using M7, which is the default aerosol microphysics module in ECHAM5-HAM. The evaluation shows that the global aerosol properties can be reproduced reasonably well using a coarse resolution of 10 sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sulphate and carbonaceous species have an annual mean within a factor of two of the observations. The simulated sea-salt concentrations reproduce the observations within a factor of two, apart from the Southern Ocean over which the concentrations are within a factor of five. Regionally, AOD is in a relatively good agreement with the observations (within a factor of two). At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and dust regions the modelled AOD is significantly lower than observed. Regarding most of the investigated aerosol properties, the SALSA and the modal aerosol module M7 perform comparably well against observations. However, SALSA reproduces the observed number concentrations and the size distribution of CCN sized particles much more accurately than M7, and is therefore a good choice for aerosol-cloud interaction studies in global models. Our study also shows that when activation type nucleation in the boundary layer is included, the observed concentration of particles under 50 nm in diameter are reproduced much better compared to when only binary nucleation in the free troposphere is assumed.

Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5

Abstract. A modal aerosol module (MAM) has been developed for the Community Atmosphere Model version 5 (CAM5), the atmospheric component of the Community Earth System Model version 1 (CESM1). MAM is capable of simulating the aerosol size distribution and both internal and external mixing between aerosol components, treating numerous complicated aerosol processes and aerosol physical, chemical and optical properties in a physically-based manner. Two MAM versions were developed: a more complete version with seven lognormal modes (MAM7), and a version with three lognormal modes (MAM3) for the purpose of long-term (decades to centuries) simulations. In this paper a description and evaluation of the aerosol module and its two representations are provided. Sensitivity of the aerosol lifecycle to simplifications in the representation of aerosol is discussed. Simulated sulfate and secondary organic aerosol (SOA) mass concentrations are remarkably similar between MAM3 and MAM7. Differences in primary organic matter (POM) and black carbon (BC) concentrations between MAM3 and MAM7 are also small (mostly within 10%). The mineral dust global burden differs by 10% and sea salt burden by 30–40% between MAM3 and MAM7, mainly due to the different size ranges for dust and sea salt modes and different standard deviations of the log-normal size distribution for sea salt modes between MAM3 and MAM7. The model is able to qualitatively capture the observed geographical and temporal variations of aerosol mass and number concentrations, size distributions, and aerosol optical properties. However, there are noticeable biases; e.g., simulated BC concentrations are significantly lower than measurements in the Arctic. There is a low bias in modeled aerosol optical depth on the global scale, especially in the developing countries. These biases in aerosol simulations clearly indicate the need for improvements of aerosol processes (e.g., emission fluxes of anthropogenic aerosols and precursor gases in developing countries, boundary layer nucleation) and properties (e.g., primary aerosol emission size, POM hygroscopicity). In addition, the critical role of cloud properties (e.g., liquid water content, cloud fraction) responsible for the wet scavenging of aerosol is highlighted.

Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

Abstract. Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS−) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr−1, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA and particulate MS− (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr−1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m−3, with values up to 400 ng m−3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2), both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20%) in CCN (at a supersaturation (S) of 0.2%) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea-salt provides diverse results with increases and decreases in the concentration of CCN over different parts of the ocean. The sign of the CCN change due to the addition of marine organics to sea-salt aerosol is determined by the relative significance of the increase in mean modal diameter due to addition of mass, and the decrease in particle hygroscopicity due to compositional changes in marine aerosol. Based on emerging evidence for increased CCN concentration over biologically active surface ocean areas/periods, our study suggests that treatment of sea spray in global climate models (GCMs) as an internal mixture of marine organic aerosols and sea-salt will likely lead to an underestimation in CCN number concentration.