Abstract. The Copernicus Atmosphere Monitoring Service (CAMS) reanalysis is the latest global reanalysis dataset of atmospheric composition produced by the European Centre for Medium-Range Weather Forecasts (ECMWF), consisting of three-dimensional time-consistent atmospheric composition fields, including aerosols and chemical species. The dataset currently covers the period 2003–2016 and will be extended in the future by adding 1 year each year. A reanalysis for greenhouse gases is being produced separately. The CAMS reanalysis builds on the experience gained during the production of the earlier Monitoring Atmospheric Composition and Climate (MACC) reanalysis and CAMS interim reanalysis. Satellite retrievals of total column CO; tropospheric column NO2; aerosol optical depth (AOD); and total column, partial column and profile ozone retrievals were assimilated for the CAMS reanalysis with ECMWF's Integrated Forecasting System. The new reanalysis has an increased horizontal resolution of about 80 km and provides more chemical species at a better temporal resolution (3-hourly analysis fields, 3-hourly forecast fields and hourly surface forecast fields) than the previously produced CAMS interim reanalysis. The CAMS reanalysis has smaller biases compared with most of the independent ozone, carbon monoxide, nitrogen dioxide and aerosol optical depth observations used for validation in this paper than the previous two reanalyses and is much improved and more consistent in time, especially compared to the MACC reanalysis. The CAMS reanalysis is a dataset that can be used to compute climatologies, study trends, evaluate models, benchmark other reanalyses or serve as boundary conditions for regional models for past periods.

A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.

Abstract. Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

Abstract. This article describes the IFS-AER aerosol module used operationally in the Integrated Forecasting System (IFS) cycle 45R1, operated by the European Centre for Medium-Range Weather Forecasts (ECMWF) in the framework of the Copernicus Atmospheric Monitoring Services (CAMS). We describe the different parameterizations for aerosol sources, sinks, and its chemical production in IFS-AER, as well as how the aerosols are integrated in the larger atmospheric composition forecasting system. The focus is on the entire 45R1 code base, including some components that are not used operationally, in which case this will be clearly specified. This paper is an update to the Morcrette et al. (2009) article that described aerosol forecasts at the ECMWF using cycle 32R2 of the IFS. Between cycles 32R2 and 45R1, a number of source and sink processes have been reviewed and/or added, notably increasing the complexity of IFS-AER. A greater integration with the tropospheric chemistry scheme of the IFS has been achieved for the sulfur cycle and for nitrate production. Two new species, nitrate and ammonium, have also been included in the forecasting system. Global budgets and aerosol optical depth (AOD) fields are shown, as is an evaluation of the simulated particulate matter (PM) and AOD against observations, showing an increase in skill from cycle 40R2, used in the CAMS interim ReAnalysis (CAMSiRA), to cycle 45R1.

Abstract. 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 (σ 2 w ) of a Gaussian pdf (probability density function) of vertical velocity. Fixed values of σ w (spanning the range measured in situ by nine flight campaigns found in the literature) and a configuration in which σ w depends on turbulent kinetic energy are tested. Results from the mid-range fixed σ w 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 σ w = 0.1 m s −1 , −2.1 W m −2 with σ w derived from TKE, −2.25 W m −2 with σ w = 0.4 m s −1 , and −2.3 W m −2 with σ w = 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 σ w 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.