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The evaluation and quantification of Southern Ocean cloud–radiation interactions simulated by climate models are essential in understanding the sources and magnitude of the radiative bias that persists in climate models for this region. To date, most evaluation methods focus on specific synoptic or cloud-type conditions that do not consider the entirety of the Southern Ocean's cloud regimes at once. Furthermore, it is difficult to directly quantify the complex and non-linear role that different cloud properties have on modulating cloud radiative effect. In this study, we present a new method of model evaluation, using machine learning that can at once identify complexities within a system and individual contributions. To do this, we use an XGBoost (eXtreme Gradient Boosting) model to predict the radiative bias within a nudged version of the Australian Community Climate and Earth System Simulator – Atmosphere-only model, using cloud property biases as predictive features. We find that the XGBoost model can explain up to 55 % of the radiative bias from these cloud properties alone. We then apply SHAP (SHapley Additive exPlanations) feature importance analysis to quantify the role each cloud property bias plays in predicting the radiative bias. We find that biases in the liquid water path are the largest contributor to the cloud radiative bias over the Southern Ocean, though important regional and cloud-type dependencies exist. We then test the usefulness of this method in evaluating model perturbations and find that it can clearly identify complex responses, including cloud property and cloud-type compensating errors.

The Southern Ocean radiative bias continues to impact climate and weather models, including the Australian Community Climate and Earth System Simulator (ACCESS). The radiative bias, characterised by too much shortwave radiation reaching the surface, is attributed to the incorrect simulation of cloud properties, including frequency and phase. To identify cloud regimes important to the Southern Ocean, we use k-means cloud histogram clustering, applied to a satellite product and then fitted to nudged simulations of the latest-generation ACCESS atmosphere model. We identify instances when the model correctly or incorrectly simulates the same cloud type as the satellite product for any point in time or space. We then evaluate the cloud and radiation biases in these instances. We find that when the ACCESS model correctly simulates the cloud type, cloud property and radiation biases of equivalent, or in some cases greater, magnitude remain compared to when cloud types are incorrectly simulated. Furthermore, we find that even when radiative biases appear small on average, cloud property biases, such as liquid or ice water paths or cloud fractions, remain large. Our results suggest that simply getting the right cloud type (or the cloud macrophysics) is not enough to reduce the Southern Ocean radiative bias. Furthermore, in instances where the radiative bias is small, it may be so for the wrong reasons. Considerable effort is still required to improve cloud microphysics, with a particular focus on cloud phase.

We investigated the radiative impact of recent process-based improvements to oceanic ozone (O3) dry deposition parameterisation and empirical improvements to lightning-generated oxides of nitrogen (LNOx) parameterisation by conducting a 5-year simulation of the Australian Community Climate and Earth System Simulator – United Kingdom Chemistry and Aerosol (ACCESS-UKCA) global chemistry–climate model, with radiative effects of O3, methane (CH4) and aerosol included. Compared to the base parameterisations, the global consequences of the two improved parameterisations on atmospheric composition are dominated by the LNOx change (which increases the LNOx production from 4.8 to 6.9 Tg N yr−1) and include (a) an increase in the O3 column of 3.75 DU, and this O3 change is centred on the tropical upper troposphere where O3 is most effective as a radiative forcer; (b) a decrease of 0.64 years in the atmospheric lifetime of CH4 due to an increase in hydroxyl radical, which corresponds to a decrease of 0.31 years in the CH4 lifetime per Tg N yr−1 change in LNOx; (c) an increase of 6.7 % in the column integrated condensation nuclei concentration; and (d) a slight increase in high-level cloud cover. The two combined parameterisation changes cause an increase of 86.3 mW m−2 in the globally-averaged all-sky net downward top-of-atmosphere (TOA) radiative flux (which is akin to instantaneous radiative forcing), and only 5 % of which is due to the dry deposition parameterisation change. Other global radiative changes from the use of the two parameterisations together include an increase in the downward longwave radiation and a decrease in the downward shortwave radiation at the earth's surface. The indirect effect of LNOx on aerosol and cloud cover can at least partly explain the differences in the downward shortwave flux at the surface. It is demonstrated that although the total global LNOx production may be the same, how LNOx is distributed spatially makes a difference to radiative transfer. We estimate that for a reported uncertainty range of 5±3 Tg N yr−1 in global estimates of LNOx, the uncertainty in the net downward TOA radiation is ±119 mW m−2. The corresponding uncertainly in the atmospheric methane lifetime is ±0.92 years. Thus, the value of LNOx used within a model will influence the effective radiative forcing (ERF) and global warming potential (GWP) of anthropogenic CH4, and influence the results of climate scenario modelling.

Coral reefs have been found to produce the sulfur compound dimethyl sulfide (DMS), a climatically relevant aerosol precursor predominantly associated with phytoplankton. Until recently, the role of coral-reef-derived DMS within the climate system had not been quantified. A study preceding the present work found that DMS produced by corals had negligible long-term climatic forcing at the global–regional scale. However, at sub-daily timescales more typically associated with aerosol and cloud formation, the influence of coral-reef-derived DMS on local aerosol radiative effects remains unquantified. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) has been used in this work to study the role of coral-reef-derived DMS at sub-daily timescales for the first time. WRF-Chem was run to coincide with an October 2016 field campaign over the Great Barrier Reef, Queensland, Australia, against which the model was evaluated. After updating and scaling the DMS surface water climatology, the model reproduced DMS and sulfur concentrations well. The inclusion of coral-reef-derived DMS resulted in no significant change in sulfate aerosol mass or total aerosol number. Subsequently, no direct or indirect aerosol effects were detected. The results suggest that the co-location of the Great Barrier Reef with significant anthropogenic aerosol sources along the Queensland coast prevents coral-reef-derived aerosol from having a modulating influence on local aerosol burdens in the current climate.

The Australian Community Climate and Earth System Simulator (ACCESS) has contributed to the World Climate Research Programme’s Coupled Model Intercomparison Project Phase 6 (CMIP6) using two fully coupled model versions (ACCESS-CM2 and ACCESS-ESM1.5) and two ocean–sea-ice model versions (1° and 0.25° resolution versions of ACCESS-OM2). The fully coupled models differ primarily in the configuration and version of their atmosphere components (including the aerosol scheme), with smaller differences in their sea-ice and land model versions. Additionally, ACCESS-ESM1.5 includes biogeochemistry in the land and ocean components and can be run with an interactive carbon cycle. CMIP6 comprises core experiments and associated thematic Model Intercomparison Projects (MIPs). This paper provides an overview of the CMIP6 submission, including the methods used for the preparation of input forcing datasets and the post-processing of model output, along with a comprehensive list of experiments performed, detailing their initialisation, duration, ensemble number and computational cost. A small selection of model output is presented, focusing on idealised experiments and their variants at global scale. Differences in the climate simulation of the two coupled models are highlighted. ACCESS-CM2 produces a larger equilibrium climate sensitivity (4.7°C) than ACCESS-ESM1.5 (3.9°C), likely a result of updated atmospheric parameterisation in recent versions of the atmospheric component of ACCESS-CM2. The idealised experiments run with ACCESS-ESM1.5 show that land and ocean carbon fluxes respond to both changing atmospheric CO2 and to changing temperature. ACCESS data submitted to CMIP6 are available from the Earth System Grid Federation (https://doi.org/10.22033/ESGF/CMIP6.2281 and https://doi.org/10.22033/ESGF/CMIP6.2288). The information provided in this paper should facilitate easier use of these significant datasets by the broader climate community.

Although lightning-generated oxides of nitrogen (LNOx) account for only approximately 10 % of the global NOx source, they have a disproportionately large impact on tropospheric photochemistry due to the conducive conditions in the tropical upper troposphere where lightning is mostly discharged. In most global composition models, lightning flash rates used to calculate LNOx are expressed in terms of convective cloud-top height via the Price and Rind (1992) (PR92) parameterisations for land and ocean, where the oceanic parameterisation is known to greatly underestimate flash rates. We conduct a critical assessment of flash-rate parameterisations that are based on cloud-top height and validate them within the Australian Community Climate and Earth System Simulator – United Kingdom Chemistry and Aerosol (ACCESS-UKCA) global chemistry–climate model using the Lightning Imaging Sensor and Optical Transient Detector (LIS/OTD) satellite data. While the PR92 parameterisation for land yields satisfactory predictions, the oceanic parameterisation, as expected, underestimates the observed flash-rate density severely, yielding a global average over the ocean of 0.33 flashes s−1 compared to the observed 9.16 flashes s−1 and leading to LNOx being underestimated proportionally. We formulate new flash-rate parameterisations following Boccippio's (2002) scaling relationships between thunderstorm electrical generator power and storm geometry coupled with available data. The new parameterisation for land performs very similarly to the corresponding PR92 one, as would be expected, whereas the new oceanic parameterisation simulates the flash-rate observations much more accurately, giving a global average over the ocean of 8.84 flashes s−1. The use of the improved flash-rate parameterisations in ACCESS-UKCA changes the modelled tropospheric composition – global LNOx increases from 4.8 to 6.6 Tg N yr−1; the ozone (O3) burden increases by 8.5 %; there is an increase in the mid- to upper-tropospheric NOx by as much as 40 pptv, a 13 % increase in the global hydroxyl radical (OH), a decrease in the methane lifetime by 6.7 %, and a decrease in the lower-tropospheric carbon monoxide (CO) by 3 %–7 %. Compared to observations, the modelled tropospheric NOx and ozone in the Southern Hemisphere and over the ocean are improved by this new flash-rate parameterisation.

Dimethyl sulfide (DMS) is a naturally occurring aerosol precursor gas which plays an important role in the global sulfur budget, aerosol formation and climate. While DMS is produced predominantly by phytoplankton, recent observational literature has suggested that corals and their symbionts produce a comparable amount of DMS, which is unaccounted for in models. It has further been hypothesised that the coral reef source of DMS may modulate regional climate. This hypothesis presents a particular concern given the current threat to coral reefs under anthropogenic climate change. In this paper, a global climate model with online chemistry and aerosol is used to explore the influence of coral-reef-derived DMS on atmospheric composition and climate. A simple representation of coral-reef-derived DMS is developed and added to a common DMS surface water climatology, resulting in an additional flux of 0.3 Tg yr−1 S, or 1.7 % of the global sulfur flux from DMS. By comparing the differences between both nudged and free-running ensemble simulations with and without coral-reef-derived DMS, the influence of coral-reef-derived DMS on regional climate is quantified. In the Maritime Continent–Australian region, where the highest density of coral reefs exists, a small decrease in nucleation- and Aitken-mode aerosol number concentration and mass is found when coral reef DMS emissions are removed from the system. However, these small responses are found to have no robust effect on regional climate via direct and indirect aerosol effects. This work emphasises the complexities of the aerosol–climate system, and the limitations of current modelling capabilities are highlighted, in particular surrounding convective responses to changes in aerosol. In conclusion, we find no robust evidence that coral-reef-derived DMS influences global and regional climate.

We document and evaluate the aerosol schemes as implemented in the physical and Earth system models, the Global Coupled 3.1 configuration of the Hadley Centre Global Environment Model version 3 (HadGEM3-GC3.1) and the United Kingdom Earth System Model (UKESM1), which are contributing to the sixth Coupled Model Intercomparison Project (CMIP6). The simulation of aerosols in the present-day period of the historical ensemble of these models is evaluated against a range of observations. Updates to the aerosol microphysics scheme are documented as well as differences in the aerosol representation between the physical and Earth system configurations. The additional Earth system interactions included in UKESM1 lead to differences in the emissions of natural aerosol sources such as dimethyl sulfide, mineral dust and organic aerosol and subsequent evolution of these species in the model. UKESM1 also includes a stratospheric–tropospheric chemistry scheme which is fully coupled to the aerosol scheme, while GC3.1 employs a simplified aerosol chemistry mechanism driven by prescribed monthly climatologies of the relevant oxidants. Overall, the simulated speciated aerosol mass concentrations compare reasonably well with observations. Both models capture the negative trend in sulfate aerosol concentrations over Europe and the eastern United States of America (US) although the models tend to underestimate sulfate concentrations in both regions. Interactive emissions of biogenic volatile organic compounds in UKESM1 lead to an improved agreement of organic aerosol over the US. Simulated dust burdens are similar in both models despite a 2-fold difference in dust emissions. Aerosol optical depth is biased low in dust source and outflow regions but performs well in other regions compared to a number of satellite and ground-based retrievals of aerosol optical depth. Simulated aerosol number concentrations are generally within a factor of 2 of the observations, with both models tending to overestimate number concentrations over remote ocean regions, apart from at high latitudes, and underestimate over Northern Hemisphere continents. Finally, a new primary marine organic aerosol source is implemented in UKESM1 for the first time. The impact of this new aerosol source is evaluated. Over the pristine Southern Ocean, it is found to improve the seasonal cycle of organic aerosol mass and cloud droplet number concentrations relative to GC3.1 although underestimations in cloud droplet number concentrations remain. This paper provides a useful characterisation of the aerosol climatology in both models and will facilitate understanding in the numerous aerosol–climate interaction studies that will be conducted as part of CMIP6 and beyond.

Global climate change and the impacts of ocean warming, ocean acidification and declining water quality are adversely affecting coral-reef ecosystems. This is of great concern, as coral reefs provide numerous ecosystem, economic and social services. Corals are also recognised as being amongst the strongest individual sources of natural atmospheric sulfur, through stress-induced emissions of dimethylsulfide (DMS). In the clean marine boundary layer, biogenic sulfates contribute to new aerosol formation and the growth of existing particles, with important implications for the radiative balance over the ocean. Evidence suggests that DMS is not only directly involved in the coral stress response, alleviating oxidative stress, but also may create an “ocean thermostat” which suppresses sea surface temperature through changes to aerosol and cloud properties. This review provides a summary of the current major threats facing coral reefs and describes the role of dimethylated sulfur compounds in coral ecophysiology and the potential influence on climate. The role of coral reefs as a source of climatically important compounds is an emerging topic of research; however the window of opportunity to understand the complex biogeophysical processes involved is closing with ongoing degradation of the world's coral reefs. The greatest uncertainty in our estimates of radiative forcing and climate change is derived from natural aerosol sources, such as marine DMS, which constitute the largest flux of oceanic reduced sulfur to the atmosphere. Given the increasing frequency of coral bleaching events, it is crucial that we gain a better understanding of the role of DMS in local climate of coral reefs.

Natural aerosol emission represents one of the largest uncertainties in our understanding of the radiation budget. Sulfur emitted by marine organisms, as dimethyl sulfide (DMS), constitutes one-fifth of the global sulfur budget and yet the distribution, fluxes and fate of DMS remain poorly constrained. This study evaluates the Australian Community Climate and Earth System Simulator (ACCESS) United Kingdom Chemistry and Aerosol (UKCA) model in terms of cloud fraction, radiation and precipitation, and then quantifies the role of DMS in the chemistry–climate system. We find that ACCESS-UKCA has similar cloud and radiation biases to other global climate models. By removing all DMS, or alternatively significantly enhancing marine DMS, we find a top of the atmosphere radiative effect of 1.7 and −1.4 W m−2 respectively. The largest responses to these DMS perturbations (removal/enhancement) are in stratiform cloud decks in the Southern Hemisphere's eastern ocean basins. These regions show significant differences in low cloud (−9∕ + 6 %), surface incoming shortwave radiation (+7∕ − 5 W m−2) and large-scale rainfall (+15∕ − 10 %). We demonstrate a precipitation suppression effect of DMS-derived aerosol in stratiform cloud deck regions due to DMS, coupled with an increase in low cloud fraction. The difference in low cloud fraction is an example of the aerosol lifetime effect. Globally, we find a sensitivity of temperature to annual DMS flux of 0.027 and 0.019 K per Tg yr−1 of sulfur, respectively. Other areas of low cloud formation, such as the Southern Ocean and stratiform cloud decks in the Northern Hemisphere, have a relatively weak response to DMS perturbations. We highlight the need for greater understanding of the DMS–climate cycle within the context of uncertainties and biases of climate models as well as those of DMS–climate observations.

Dry deposition at the Earth's surface is an important sink of atmospheric ozone. Currently, dry deposition of ozone to the ocean surface in atmospheric chemistry models has the largest uncertainty compared to deposition to other surface types, with implications for global tropospheric ozone budget and associated radiative forcing. Most global models assume that the dominant term of surface resistance in the parameterisation of ozone dry deposition velocity at the oceanic surface is constant. There have been recent mechanistic parameterisations for air–sea exchange that account for the simultaneous waterside processes of ozone solubility, molecular diffusion, turbulent transfer, and first-order chemical reaction of ozone with dissolved iodide and other compounds, but there are questions about their performance and consistency. We present a new two-layer parameterisation scheme for the oceanic surface resistance by making the following realistic assumptions: (a) the thickness of the top water layer is of the order of a reaction–diffusion length scale (a few micrometres) within which ozone loss is dominated by chemical reaction and the influence of waterside turbulent transfer is negligible; (b) in the water layer below, both chemical reaction and waterside turbulent transfer act together and are accounted for; and (c) chemical reactivity is present through the depth of the oceanic mixing layer. The new parameterisation has been evaluated against dry deposition velocities from recent open-ocean measurements. It is found that the inclusion of only the aqueous iodide–ozone reaction satisfactorily describes the measurements. In order to better quantify the global dry deposition loss and its interannual variability, modelled 3-hourly ozone deposition velocities are combined with the 3-hourly MACC (Monitoring Atmospheric Composition and Climate) reanalysis ozone for the years 2003–2012. The resulting ozone dry deposition is found to be 98.4 ± 30.0 Tg O3 yr−1 for the ocean and 722.8 ± 87.3 Tg O3 yr−1 globally. The new estimate of the ocean component is approximately a third of the current model estimates. This reduction corresponds to an approximately 20 % decrease in the total global ozone dry deposition, which (with all other components being unchanged) is equivalent to an increase of approximately 5 % in the modelled tropospheric ozone burden and a similar increase in tropospheric ozone lifetime.

Schemes used to parameterise ozone dry deposition velocity at the oceanic surface mainly differ in terms of how the dominant term of surface resistance is parameterised. We examine three such schemes and test them in a global climate–chemistry model that incorporates meteorological nudging and monthly-varying reactive-gas emissions. The default scheme invokes the commonly used assumption that the water surface resistance is constant. The other two schemes, named the one-layer and two-layer reactivity schemes, include the simultaneous influence on the water surface resistance of ozone solubility in water, waterside molecular diffusion and turbulent transfer, and a first-order chemical reaction of ozone with dissolved iodide. Unlike the one-layer scheme, the two-layer scheme can indirectly control the degree of interaction between chemical reaction and turbulent transfer through the specification of a surface reactive layer thickness. A comparison is made of the modelled deposition velocity dependencies on sea surface temperature (SST) and wind speed with recently reported cruise-based observations. The default scheme overestimates the observed deposition velocities by a factor of 2–4 when the chemical reaction is slow (e.g. under colder SSTs in the Southern Ocean). The default scheme has almost no temperature, wind speed, or latitudinal variations in contrast with the observations. The one-layer scheme provides noticeably better variations, but it overestimates deposition velocity by a factor of 2–3 due to an enhancement of the interaction between chemical reaction and turbulent transfer. The two-layer scheme with a surface reactive layer thickness specification of 2.5 µm, which is approximately equal to the reaction-diffusive length scale of the ozone–iodide reaction, is able to simulate the field measurements most closely with respect to absolute values as well as SST and wind-speed dependence. The annual global oceanic deposition of ozone determined using this scheme is approximately half of the original oceanic deposition obtained using the default scheme, and it corresponds to a 10 % decrease in the original estimate of the total global ozone deposition. The previously reported modelled estimate of oceanic deposition is roughly one-third of total deposition and with this new parameterisation it is reduced to 12 % of the modelled total global ozone deposition. Deposition parameterisation influences the predicted atmospheric ozone mixing ratios, especially in the Southern Hemisphere. For the latitudes 45–70° S, the two-layer scheme improves the prediction of ozone observed at an altitude of 1 km by 7 % and that within the altitude range 1–6 km by 5 % compared to the default scheme.

Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.

Substantial changes in anthropogenic aerosols and precursor gas emissions have occurred over recent decades due to the implementation of air pollution control legislation and economic growth. The response of atmospheric aerosols to these changes and the impact on climate are poorly constrained, particularly in studies using detailed aerosol chemistry–climate models. Here we compare the HadGEM3-UKCA (Hadley Centre Global Environment Model-United Kingdom Chemistry and Aerosols) coupled chemistry–climate model for the period 1960–2009 against extensive ground-based observations of sulfate aerosol mass (1978–2009), total suspended particle matter (SPM, 1978–1998), PM10 (1997–2009), aerosol optical depth (AOD, 2000–2009), aerosol size distributions (2008–2009) and surface solar radiation (SSR, 1960–2009) over Europe. The model underestimates observed sulfate aerosol mass (normalised mean bias factor (NMBF) = −0.4), SPM (NMBF = −0.9), PM10 (NMBF = −0.2), aerosol number concentrations (N30 NMBF = −0.85; N50 NMBF = −0.65; and N100 NMBF = −0.96) and AOD (NMBF = −0.01) but slightly overpredicts SSR (NMBF = 0.02). Trends in aerosol over the observational period are well simulated by the model, with observed (simulated) changes in sulfate of −68 % (−78 %), SPM of −42 % (−20 %), PM10 of −9 % (−8 %) and AOD of −11 % (−14 %). Discrepancies in the magnitude of simulated aerosol mass do not affect the ability of the model to reproduce the observed SSR trends. The positive change in observed European SSR (5 %) during 1990–2009 ("brightening") is better reproduced by the model when aerosol radiative effects (ARE) are included (3 %), compared to simulations where ARE are excluded (0.2 %). The simulated top-of-the-atmosphere aerosol radiative forcing over Europe under all-sky conditions increased by > 3.0 W m−2 during the period 1970–2009 in response to changes in anthropogenic emissions and aerosol concentrations.

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

The Hadley Centre Global Environmental Model (HadGEM) includes two aerosol schemes: the Coupled Large-scale Aerosol Simulator for Studies in Climate (CLASSIC), and the new Global Model of Aerosol Processes (GLOMAP-mode). GLOMAP-mode is a modal aerosol microphysics scheme that simulates not only aerosol mass but also aerosol number, represents internally-mixed particles, and includes aerosol microphysical processes such as nucleation. In this study, both schemes provide hindcast simulations of natural and anthropogenic aerosol species for the period 2000–2006. HadGEM simulations of the aerosol optical depth using GLOMAP-mode compare better than CLASSIC against a data-assimilated aerosol re-analysis and aerosol ground-based observations. Because of differences in wet deposition rates, GLOMAP-mode sulphate aerosol residence time is two days longer than CLASSIC sulphate aerosols, whereas black carbon residence time is much shorter. As a result, CLASSIC underestimates aerosol optical depths in continental regions of the Northern Hemisphere and likely overestimates absorption in remote regions. Aerosol direct and first indirect radiative forcings are computed from simulations of aerosols with emissions for the year 1850 and 2000. In 1850, GLOMAP-mode predicts lower aerosol optical depths and higher cloud droplet number concentrations than CLASSIC. Consequently, simulated clouds are much less susceptible to natural and anthropogenic aerosol changes when the microphysical scheme is used. In particular, the response of cloud condensation nuclei to an increase in dimethyl sulphide emissions becomes a factor of four smaller. The combined effect of different 1850 baselines, residence times, and abilities to affect cloud droplet number, leads to substantial differences in the aerosol forcings simulated by the two schemes. GLOMAP-mode finds a present-day direct aerosol forcing of −0.49 W m−2 on a global average, 72% stronger than the corresponding forcing from CLASSIC. This difference is compensated by changes in first indirect aerosol forcing: the forcing of −1.17 W m−2 obtained with GLOMAP-mode is 20% weaker than with CLASSIC. Results suggest that mass-based schemes such as CLASSIC lack the necessary sophistication to provide realistic input to aerosol-cloud interaction schemes. Furthermore, the importance of the 1850 baseline highlights how model skill in predicting present-day aerosol does not guarantee reliable forcing estimates. Those findings suggest that the more complex representation of aerosol processes in microphysical schemes improves the fidelity of simulated aerosol forcings.

The atmospheric oxidation of dimethyl-sulphide (DMS) derived from marine phytoplankton is a significant source of marine sulphate aerosol. DMS has been proposed to regulate climate via changes in cloud properties, though recent studies have shown that present-day global cloud condensation nuclei (CCN) concentrations have only a weak dependence on the total emission flux of DMS. Here, we use a global aerosol microphysics model to examine how efficiently CCN are produced when DMS emissions are changed in different marine regions. We find that global CCN production per unit mass of sulphur emitted varies by more than a factor of 20 depending on where the change in oceanic DMS emission flux is applied. The variation in CCN production efficiency depends upon where CCN production processes (DMS oxidation, SO2 oxidation, nucleation and growth) are most efficient and removal processes (deposition) least efficient. The analysis shows that the production of aerosol sulphate through aqueous-phase oxidation of SO2 limits the amount of H2SO4 available for nucleation and condensational growth and therefore suppresses CCN formation, leading to the weak response of CCN to changes in DMS emission. Our results show that past and future changes in the spatial distribution of DMS emissions (through changes in the phytoplankton population or wind speed patterns) could exert a stronger control on climate than net increases in biological productivity.

In the most advanced aerosol-climate models it is common to represent the aerosol particle size distribution in terms of several log-normal modes. This approach, motivated by computational efficiency, makes assumptions about the shape of the particle distribution that may not always capture the properties of global aerosol. Here, a global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that the current values for two size distribution parameter settings in the modal scheme (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Annual mean surface-level mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are within 25% in the two schemes in nearly all regions. Surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25% in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically 25–60% higher in the modal model, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g., boundary layer nucleation and ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.

Observations show that the fractional solubility of Fe (FS-Fe, percentage of dissolved to total Fe) in dust aerosol increases considerably from 0.1 % in regions of high dust mass concentration to 80 % in remote regions where concentrations are low. Here, we combined laboratory geochemical measurements with global aerosol model simulations to test the hypothesis that the increase in FS-Fe is due to physical size sorting during transport. We determined the FS-Fe and fractional solubility of Al (FS-Al) in size-fractionated dust generated from two representative soil samples collected from known Saharan dust source regions using a customized dust re-suspension and collection system. The results show that the FS-Fe is size-dependent and ranges from 0.1–0.3 % in the coarse size fractions (>1 μm) to ~0.2–0.8 % in the fine size fractions (100 μg m−3) to ~0.2 % at low concentrations (–3) due to physical size sorting (i.e., particle gravitational settling). These values are one to two orders of magnitude smaller than those observed on cruises across the tropical and sub-tropical North Atlantic Ocean under an important pathway of Saharan dust plumes for similar dust mass concentrations. Even when the FS-Fe of sub-micrometer size fractions (0.18–0.32 μm, 0.32–0.56 μm, and 0.56–1.0 μm) in the model is increased by a factor of 10 over the measured values, the calculated FS-Fe of the dust is still more than an order of magnitude lower than that measured in the field. Therefore, the physical sorting of dust particles alone is unlikely to be an important factor in the observed inverse relationship between the FS-Fe and FS-Al and the atmospheric mineral dust mass concentrations. The results suggest that processes such as chemical reactions and/or mixing with combustion particles are the main mechanisms to cause the increased FS-Fe in long-range transported dust aerosols.

The emission of dimethyl-sulphide (DMS) gas by phytoplankton and the subsequent formation of aerosol has long been suggested as an important climate regulation mechanism. The key aerosol quantity is the number concentration of cloud condensation nuclei (CCN), but until recently global models did not include the necessary aerosol physics to quantify CCN. Here we use a global aerosol microphysics model to calculate the sensitivity of CCN to changes in DMS emission using multiple present-day and future sea-surface DMS climatologies. Calculated annual fluxes of DMS to the atmosphere for the five model-derived and one observations based present day climatologies are in the range 15.1 to 32.3 Tg a−1 sulphur. The impact of DMS climatology on surface level CCN concentrations was calculated in terms of summer and winter hemispheric mean values of ΔCCN/ΔFluxDMS, which varied between −43 and +166 cm−3/(mg m−2 day−1 sulphur), with a mean of 63 cm−3/(mg m−2 day−1 sulphur). The range is due to CCN production in the atmosphere being strongly dependent on the spatial distribution of the emitted DMS. The relative sensitivity of CCN to DMS (i.e. fractional change in CCN divided by fractional change in DMS flux) depends on the abundance of non-DMS derived aerosol in each hemisphere. The relative sensitivity averaged over the five present day DMS climatologies is estimated to be 0.02 in the northern hemisphere (i.e. a 0.02% change in CCN for a 1% change in DMS) and 0.07 in the southern hemisphere where aerosol abundance is lower. In a globally warmed scenario in which the DMS flux increases by ~1% relative to present day we estimate a ~0.1% increase in global mean CCN at the surface. The largest CCN response occurs in the Southern Ocean, contributing to a Southern Hemisphere mean annual increase of less than 0.2%. We show that the changes in DMS flux and CCN concentration between the present day and global warming scenario are similar to interannual differences due to variability in windspeed. In summary, although DMS makes a significant contribution to global marine CCN concentrations, the sensitivity of CCN to potential future changes in DMS flux is very low. This finding, together with the predicted small changes in future seawater DMS concentrations, suggests that the role of DMS in climate regulation is very weak.