Tropospheric aerosol radiative forcing has persisted for many years as one of the major causes of uncertainty in global climate model simulations. To sample the range of plausible aerosol and atmospheric states and perform robust statistical analyses of the radiative forcing, it is important to account for the combined effects of many sources of model uncertainty, which is rarely done due to the high computational cost. This paper describes the designs of two ensembles of the Met Office Hadley Centre Global Environment Model‐U.K. Chemistry and Aerosol global climate model and provides the first analyses of the uncertainties in aerosol radiative forcing and their causes. The first ensemble was designed to comprehensively sample uncertainty in the aerosol state, while the other samples additional uncertainties in the physical model related to clouds, humidity, and radiation, thereby allowing an analysis of uncertainty in the aerosol effective radiative forcing. Each ensemble consists of around 200 simulations of the preindustrial and present‐day atmospheres. The uncertainty in aerosol radiative forcing in our ensembles is comparable to the range of estimates from multimodel intercomparison projects. The mean aerosol effective radiative forcing is −1.45 W/m2 (credible interval of −2.07 to −0.81 W/m2), which encompasses but is more negative than the −1.17 W/m2 in the 2013 Atmospheric Chemistry and Climate Model Intercomparison Project and −0.90 W/m2 in the Intergovernmental Panel on Climate Change Fifth Assessment Report. The ensembles can be used to reduce aerosol radiative forcing uncertainty by challenging them with multiple measurements as well as to isolate potential causes of multimodel differences.

Aerosol processes and, in particular, aerosol-cloud interactions cut across the traditional physical-Earth system boundary of coupled Earth system models and remain one of the key uncertainties in estimating anthropogenic radiative forcing of climate. Here we calculate the historical aerosol effective radiative forcing (ERF) in the HadGEM3-GA7 climate model in order to assess the suitability of this model for inclusion in the UK Earth system model, UKESM1. The aerosol ERF, calculated for the year 2000 relative to 1850, is large and negative in the standard GA7 model leading to an unrealistic negative total anthropogenic forcing over the twentieth century. We show how underlying assumptions and missing processes in both the physical model and aerosol parameterizations lead to this large aerosol ERF. A number of model improvements are investigated to assess their impact on the aerosol ERF. These include an improved representation of cloud droplet spectral dispersion, updates to the aerosol activation scheme, and black carbon optical properties. One of the largest contributors to the aerosol forcing uncertainty is insufficient knowledge of the preindustrial aerosol climate. We evaluate the contribution of uncertainties in the natural marine emissions of dimethyl sulfide and organic aerosol to the ERF. The combination of model improvements derived from these studies weakens the aerosol ERF by up to 50% of the original value and leads to a total anthropogenic historical forcing more in line with assessed values.

European air quality legislation has reduced emissions of air pollutants across Europe since the 1970s, affecting air quality, human health and regional climate. We used a coupled composition-climate model to simulate the impacts of European air quality legislation and technology measures implemented between 1970 and 2010. We contrast simulations using two emission scenarios; one with actual emissions in 2010 and the other with emissions that would have occurred in 2010 in the absence of technological improvements and end-of-pipe treatment measures in the energy, industrial and road transport sectors. European emissions of sulphur dioxide, black carbon (BC) and organic carbon in 2010 are 53%, 59% and 32% lower respectively compared to emissions that would have occurred in 2010 in the absence of legislative and technology measures. These emission reductions decreased simulated European annual mean concentrations of fine particulate matter (PM2.5) by 35%, sulphate by 44%, BC by 56% and particulate organic matter by 23%. The reduction in PM2.5 concentrations is calculated to have prevented 80 000 (37 000–116 000, at 95% confidence intervals) premature deaths annually across the European Union, resulting in a perceived financial benefit to society of US$232 billion annually (1.4% of 2010 EU GDP). The reduction in aerosol concentrations due to legislative and technology measures caused a positive change in the aerosol radiative effect at the top of atmosphere, reduced atmospheric absorption and also increased the amount of solar radiation incident at the surface over Europe. We used an energy budget approximation to estimate that these changes in the radiative balance have increased European annual mean surface temperatures and precipitation by 0.45 ± 0.11 °C and by 13 ± 0.8 mm yr−1 respectively. Our results show that the implementation of European legislation and technological improvements to reduce the emission of air pollutants has improved air quality and human health over Europe, as well as having an unintended impact on the regional radiative balance and climate.

Introduction Conclusions References Tables Figures

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.

In this paper, we present a description of the tropospheric chemistry component of the UK Chemistry and Aerosols (UKCA) model which has been coupled to the Met Office Hadley Centre's HadGEM family of climate models. We assess the model's transport and scavenging processes, in particular focussing on convective transport, boundary layer mixing, wet scavenging and inter-hemispheric exchange. Simulations with UKCA of the short-lived radon tracer suggest that modelled distributions are comparable to those of other models and the comparison with observations indicate that apart from a few locations, boundary layer mixing and convective transport are effective in the model as a means of vertically redistributing surface emissions of radon. Comparisons of modelled lead tracer concentrations with observations suggest that UKCA captures surface concentrations in both hemispheres very well, although there is a tendency to underestimate the observed geographical and interannual variability in the Northern Hemisphere. In particular, UKCA replicates the shape and absolute concentrations of observed lead profiles, a key test in the evaluation of a model's wet scavenging scheme. The timescale for inter-hemispheric transport, calculated in the model using a simple krypton tracer experiment, does appear to be long relative to other models and could indicate deficiencies in tropical deep convection and/or insufficient boundary layer mixing. We also describe the main components of the tropospheric chemistry and evaluate it against observations and other tropospheric chemistry models. In particular, from a climate forcing perspective, present-day observed surface methane concentrations and tropospheric ozone concentrations are reproduced very well by the model, thereby making it suitable for long centennial integrations as well as studies of biogeochemical feedbacks. Results from both historical and future simulations with UKCA tropospheric chemistry are presented. Future projections of tropospheric ozone vary with the Representative Concentration Pathway (RCP). In RCP2.6, for example, tropospheric ozone increases up to 2010 and then declines by 13% of its year-2000 global mean by the end of the century. In RCP8.5, tropospheric ozone continues to rise steadily throughout the 21st century, with methane being the main driving factor. Finally, we highlight aspects of the UKCA model which are undergoing and/or have undergone recent developments and are suitable for inclusion in a next-generation Earth System Model.

The activation of aerosols to form cloud droplets is dependent upon vertical velocities whose local variability is not typically resolved at the GCM grid scale. Consequently, it is necessary to represent the subgrid-scale variability of vertical velocity in the calculation of cloud droplet number concentration. This study uses the UK Chemistry and Aerosols community model (UKCA) within the Hadley Centre Global Environmental Model (HadGEM3), coupled for the first time to an explicit aerosol activation parameterisation, and hence known as UKCA-Activate. We explore the range of uncertainty in estimates of the indirect aerosol effects attributable to the choice of parameterisation of the subgrid-scale variability of vertical velocity in HadGEM-UKCA. Results of simulations demonstrate that the use of a characteristic vertical velocity cannot replicate results derived with a distribution of vertical velocities, and is to be discouraged in GCMs. This study focuses on the effect of the variance (σw2) of a Gaussian pdf (probability density function) of vertical velocity. Fixed values of σw (spanning the range measured in situ by nine flight campaigns found in the literature) and a configuration in which σw depends on turbulent kinetic energy are tested. Results from the mid-range fixed σw and TKE-based configurations both compare well with observed vertical velocity distributions and cloud droplet number concentrations. The radiative flux perturbation due to the total effects of anthropogenic aerosol is estimated at −1.9 W m−2 with σw = 0.1 m s−1, −2.1 W m−2 with σw derived from TKE, −2.25 W m−2 with σw = 0.4 m s−1, and −2.3 W m−2 with σw = 0.7 m s−1. The breadth of this range is 0.4 W m−2, which is comparable to a substantial fraction of the total diversity of current aerosol forcing estimates. Reducing the uncertainty in the parameterisation of σw would therefore be an important step towards reducing the uncertainty in estimates of the indirect aerosol effects. Detailed examination of regional radiative flux perturbations reveals that aerosol microphysics can be responsible for some climate-relevant radiative effects, highlighting the importance of including microphysical aerosol processes in GCMs.

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 multimodel-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.

Abstract. We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

We use a stratosphere–troposphere composition– climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO 2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H 2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO 2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO 2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloonborne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41 ◦ N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, Published by Copernicus Publications on behalf of the European Geosciences Union. 11222 S. S. Dhomse et al.: Simulation of Pinatubo aerosol in a CCM whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

The on-line air quality model AQUM (Air Quality in the Unified Model) is a limited-area forecast configuration of the Met Office Unified Model which uses the UKCA (UK Chemistry and Aerosols) sub-model. AQUM has been developed with two aims: as an operational system to deliver regional air quality forecasts and as a modelling system to conduct air quality studies to inform policy decisions on emissions controls. This paper presents a description of the model and the methods used to evaluate the performance of the forecast system against the automated UK surface network of air quality monitors. Results are presented of evaluation studies conducted for a year-long period of operational forecast trials and several past cases of poor air quality episodes. The results demonstrate that AQUM tends to over-predict ozone (~8 μg m−3 mean bias for the year-long forecast), but has a good level of responsiveness to elevated ozone episode conditions – a characteristic which is essential for forecasting poor air quality episodes. AQUM is shown to have a negative bias for PM10, while for PM2.5 the negative bias is much smaller in magnitude. An analysis of speciated PM2.5 data during an episode of elevated particulate matter (PM) suggests that the PM bias occurs mainly in the coarse component. The sensitivity of model predictions to lateral boundary conditions (LBCs) has been assessed by using LBCs from two different global reanalyses and by comparing the standard, single-nested configuration with a configuration having an intermediate European nest. We conclude that, even with a much larger regional domain, the LBCs remain an important source of model error for relatively long-lived pollutants such as ozone. To place the model performance in context we compare AQUM ozone forecasts with those of another forecasting system, the MACC (Monitoring Atmospheric Composition and Climate) ensemble, for a 5-month period. An analysis of the variation of model skill with forecast lead time is presented and the insights this provides to the relative sources of error in air quality modelling are discussed.

Abstract. Evaluation of the aerosol schemes in current climate models is dependent upon the available observational data. In-situ observations from flight campaigns can provide valuable data about the vertical distribution of aerosol that is difficult to obtain from satellite or ground-based platforms, although they are localised in space and time. Using single-particle soot-photometer (SP2) measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign, which consists of many vertical profiles over a large region of the Pacific, we evaluate the meridional and vertical distribution of black carbon (BC) aerosol simulated by the HadGEM3–UKCA and ECHAM5–HAM2 models. Both models show a similar pattern of overestimating the BC column burden compared to that derived from the observations, in many areas by an order of magnitude. However, by sampling the simulated BC mass mixing ratio along the flight track and comparing to the observations, we show that this discrepancy has a rather different vertical structure in the two models: in HadGEM3–UKCA the discrepancy is dominated by excess aerosol in the tropical upper troposphere, while in ECHAM5–HAM2 areas of discrepancy are spread across many different latitudes and altitudes. Using this methodology, we conduct sensitivity tests on two specific elements of the models: biomass-burning emissions and scavenging by convective precipitation. We show that, by coupling the convective scavenging more tightly with convective transport, both the column burden and vertical distribution of BC in HadGEM3–UKCA are much improved with respect to the observations, with a substantial and statistically significant increase in correlation – this demonstrates the importance of a realistic representation of this process. In contrast, updating from GFED2 to GFED3.1 biomass-burning emissions makes a more modest improvement in both models, which is not statistically significant. By comparing our results with a more traditional approach using regional- and monthly-mean vertical profile curves, we show that the point-by-point analysis allows the model improvements to be demonstrated more clearly. We also demonstrate the important role that nudged simulations (where the large-scale model dynamics are continuously relaxed towards a reanalysis) can play in this type of evaluation, allowing statistically significant differences between configurations of the aerosol scheme to be seen where the differences between the corresponding free-running simulations would not be significant.

We describe the HadGEM2 family of climate configurations of the Met Office Unified Model, MetUM. The concept of a model "family" comprises a range of specific model configurations incorporating different levels of complexity but with a common physical framework. The HadGEM2 family of configurations includes atmosphere and ocean components, with and without a vertical extension to include a well-resolved stratosphere, and an Earth-System (ES) component which includes dynamic vegetation, ocean biology and atmospheric chemistry. The HadGEM2 physical model includes improvements designed to address specific systematic errors encountered in the previous climate configuration, HadGEM1, namely Northern Hemisphere continental temperature biases and tropical sea surface temperature biases and poor variability. Targeting these biases was crucial in order that the ES configuration could represent important biogeochemical climate feedbacks. Detailed descriptions and evaluations of particular HadGEM2 family members are included in a number of other publications, and the discussion here is limited to a summary of the overall performance using a set of model metrics which compare the way in which the various configurations simulate present-day climate and its variability.

The eruption of Mt. Pinatubo in June 1991 was the largest in the twentieth century. One of its effects was to produce cooler and drier conditions in the years following the eruption. We present the results of an integrated model study of the effect of these climatic changes on the emissions of isoprene from the biosphere. Our emissions model simulations showed that global isoprene emissions were reduced by 9% from 1990 to 1992. When incorporated into our model of global atmospheric chemistry this reduction of isoprene emissions led to an increase in the tropospheric OH burden of 2%. This caused an increase in the removal of methane via oxidation by OH of up to 5 Tg per year. This could have contributed to the observed changes in methane growth rate at this time.

We describe the HadGEM2 family of climate configurations of the Met Office Unified Model, MetUM. The concept of a model “family” comprises a range of specific model configurations incorporating different levels of complexity but with a common physical framework. The HadGEM2 family of configurations includes atmosphere and ocean components, with and without a vertical extension to include a well-resolved stratosphere, and an Earth-System (ES) component which includes dynamic vegetation, ocean biology and atmospheric chemistry. The HadGEM2 physical model includes improvements designed to address specific systematic errors encountered in the previous climate configuration, HadGEM1, namely Northern Hemisphere continental temperature biases and tropical sea surface temperature biases and poor variability. Targeting these biases was crucial in order that the ES configuration could represent important biogeochemical climate feedbacks. Detailed descriptions and evaluations of particular HadGEM2 family memCorrespondence to: G. M. Martin (gill.martin@metoffice.gov.uk) bers are included in a number of other publications, and the discussion here is limited to a summary of the overall performance using a set of model metrics which compare the way in which the various configurations simulate present-day climate and its variability.

The HadGEM2 Development Team: G. M. Martin, N. Bellouin, W. J. Collins, I. D. Culverwell, P. R. Halloran, S. C. Hardiman, T. J. Hinton, C. D. Jones, R. E. McDonald, A. J. McLaren, F. M. O’Connor, M. J. Roberts, J. M. Rodriguez, S. Woodward, M. J. Best, M. E. Brooks, A. R. Brown, N. Butchart, C. Dearden, S. H. Derbyshire, I. Dharssi, M. Doutriaux-Boucher, J. M. Edwards, P. D. Falloon, N. Gedney, L. J. Gray, H. T. Hewitt, M. Hobson, M. R. Huddleston, J. Hughes, S. Ineson, W. J. Ingram, P. M. James, T. C. Johns, C. E. Johnson, A. Jones, C. P. Jones, M. M. Joshi, A. B. Keen, S. Liddicoat, A. P. Lock, A. V. Maidens, J. C. Manners, S. F. Milton, J. G. L. Rae, J. K. Ridley, A. Sellar, C. A. Senior, I. J. Totterdell, A. Verhoef, P. L. Vidale, and A. Wiltshire Met Office, FitzRoy Road, Exeter, UK School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK Centre for Australian Weather and Climate, Bureau of Meteorology, Melbourne, Australia

A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.