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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.

This study investigates the hydrometeor development and response to cloud droplet number concentration (CDNC) perturbations in convection-permitting model configurations. We present results from a real-data simulation of deep convection in the Congo basin, an idealised supercell case, and a warm-rain large-eddy simulation (LES). In each case we compare two frequently used double-moment bulk microphysics schemes and investigate the response to CDNC perturbations. We find that the variability among the two schemes, including the response to aerosol, differs widely between these cases. In all cases, differences in the simulated cloud morphology and precipitation are found to be significantly greater between the microphysics schemes than due to CDNC perturbations within each scheme. Further, we show that the response of the hydrometeors to CDNC perturbations differs strongly not only between microphysics schemes, but the inter-scheme variability also differs between cases of convection. Sensitivity tests show that the representation of autoconversion is the dominant factor that drives differences in rain production between the microphysics schemes in the idealised precipitating shallow cumulus case and in a subregion of the Congo basin simulations dominated by liquid-phase processes. In this region, rain mass is also shown to be relatively insensitive to the radiative effects of an overlying layer of ice-phase cloud. The conversion of cloud ice to snow is the process responsible for differences in cold cloud bias between the schemes in the Congo. In the idealised supercell case, thermodynamic impacts on the storm system using different microphysics parameterisations can equal those due to aerosol effects. These results highlight the large uncertainty in cloud and precipitation responses to aerosol in convection-permitting simulations and have important implications not only for process studies of aerosol–convection interaction, but also for global modelling studies of aerosol indirect effects. These results indicate the continuing need for tighter observational constraints of cloud processes and response to aerosol in a range of meteorological regimes.

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 ...

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.

The interactions between aerosols and convective clouds represent some of the greatest uncertainties in the climate impact of aerosols in the atmosphere. A wide variety of mechanisms have been proposed by which aerosols may invigorate, suppress or change the properties of individual convective clouds, some of which can be reproduced in high-resolution limited-area models. However, there may also be mesoscale, regional or global adjustments which modulate or dampen such impacts which cannot be captured in the limited domain of such models. The Convective Cloud Field Model (CCFM) provides a mechanism to simulate a population of convective clouds, complete with microphysics and interactions between clouds, within each grid column at resolutions used for global climate modelling, so that a representation of the microphysical aerosol response within each parameterised cloud type is possible. Using CCFM within the global aerosol–climate model ECHAM–HAM, we demonstrate how the parameterised cloud field responds to the present-day anthropogenic aerosol perturbation in different regions. In particular, we show that in regions with strongly forced deep convection and/or significant aerosol effects via large-scale processes, the changes in the convective cloud field due to microphysical effects are rather small; however in a more weakly forced regime such as the Caribbean, where large-scale aerosol effects are small, a signature of convective invigoration does become apparent.

This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

We investigate the dust forecasts from two operational global atmospheric models in comparison with in situ and remote sensing measurements obtained during the AERosol properties – Dust (AER-D) field campaign. Airborne elastic backscatter lidar measurements were performed on board the Facility for Airborne Atmospheric Measurements during August 2015 over the eastern Atlantic, and they permitted us to characterise the dust vertical distribution in detail, offering insights on transport from the Sahara. They were complemented with airborne in situ measurements of dust size distribution and optical properties, as well as datasets from the Cloud–Aerosol Transport System (CATS) spaceborne lidar and the Moderate Resolution Imaging Spectroradiometer (MODIS). We compare the airborne and spaceborne datasets to operational predictions obtained from the Met Office Unified Model (MetUM) and the Copernicus Atmosphere Monitoring Service (CAMS). The dust aerosol optical depth predictions from the models are generally in agreement with the observations but display a low bias. However, the predicted vertical distribution places the dust lower in the atmosphere than highlighted in our observations. This is particularly noticeable for the MetUM, which does not transport coarse dust high enough in the atmosphere or far enough away from the source.We also found that both model forecasts underpredict coarse-mode dust and at times overpredict fine-mode dust, but as they are fine-tuned to represent the observed optical depth, the fine mode is set to compensate for the underestimation of the coarse mode. As aerosol–cloud interactions are dependent on particle numbers rather than on the optical properties, this behaviour is likely to affect their correct representation. This leads us to propose an augmentation of the set of aerosol observations available on a global scale for constraining models, with a better focus on the vertical distribution and on the particle size distribution. Mineral dust is a major component of the climate system; therefore, it is important to work towards improving how models reproduce its properties and transport mechanisms.

We present an Arctic aerosol optical depth (AOD) climatology and trend analysis for 2003–2019 spring and summertime periods derived from a combination of multi-agency aerosol reanalyses, remote-sensing retrievals, and ground observations. This includes the U.S. Navy Aerosol Analysis and Prediction System ReAnalysis version 1 (NAAPS-RA v1), the NASA Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), and the Copernicus Atmosphere Monitoring Service ReAnalysis (CAMSRA). Spaceborne remote-sensing retrievals of AOD are considered from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Multi-angle Imaging SpectroRadiometer (MISR), and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Ground-based data include sun photometer data from AErosol RObotic NETwork (AERONET) sites and oceanic Maritime Aerosol Network (MAN) measurements. Aerosol reanalysis AODs and spaceborne retrievals show consistent climatological spatial patterns and trends for both spring and summer seasons over the lower Arctic (60–70∘ N). Consistent AOD trends are also found for the high Arctic (north of 70∘ N) from reanalyses. The aerosol reanalyses yield more consistent AOD results than climate models, can be verified well with AERONET, and corroborate complementary climatological and trend analysis. Speciated AODs are more variable than total AOD among the three reanalyses and a little more so for March–May (MAM) than for June–August (JJA). Black carbon (BC) AOD in the Arctic comes predominantly from biomass burning (BB) sources in both MAM and JJA, and BB overwhelms anthropogenic sources in JJA for the study period. AOD exhibits a multi-year negative MAM trend and a positive JJA trend in the Arctic during 2003–2019, due to an overall decrease in sulfate/anthropogenic pollution and a significant JJA increase in BB smoke. Interannual Arctic AOD variability is significantly large, driven by fine-mode and, specifically, BB smoke, with both smoke contribution and interannual variation larger in JJA than in MAM. It is recommended that climate models should account for BB emissions and BB interannual variabilities and trends in Arctic climate change studies.

Atmospheric aerosol particle concentrations are strongly affected by various wet processes, including below and in-cloud wet scavenging and in-cloud aqueous-phase oxidation. We studied how wet scavenging and cloud processes affect particle concentrations and composition during transport to a rural boreal forest site in northern Europe. For this investigation, we employed air mass history analysis and observational data. Long-term particle number size distribution (∼15 years) and composition measurements (∼8 years) were combined with air mass trajectories with relevant variables from reanalysis data. Some such variables were rainfall rate, relative humidity, and mixing layer height. Additional observational datasets, such as temperature and trace gases, helped further evaluate wet processes along trajectories with mixed effects models. All chemical species investigated (sulfate, black carbon, and organics) exponentially decreased in particle mass concentration as a function of accumulated precipitation along the air mass route. In sulfate (SO4) aerosols, clear seasonal differences in wet removal emerged, whereas organics (Org) and equivalent black carbon (eBC) exhibited only minor differences. The removal efficiency varied slightly among the different reanalysis datasets (ERA-Interim and Global Data Assimilation System; GDAS) used for the trajectory calculations due to the difference in the average occurrence of precipitation events along the air mass trajectories between the reanalysis datasets. Aqueous-phase processes were investigated by using a proxy for air masses travelling inside clouds. We compared air masses with no experience of approximated in-cloud conditions or precipitation during the past 24 h to air masses recently inside non-precipitating clouds before they entered SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). Significant increases in SO4 mass concentration were observed for the latter air masses (recently experienced non-precipitating clouds). Our mixed effects model considered other contributing factors affecting particle mass concentrations in SMEAR II: examples were trace gases, local meteorology, and diurnal variation. This model also indicated in-cloud SO4 production. Despite the reanalysis dataset used in the trajectory calculations, aqueous-phase SO4 formation was observed. Particle number size distribution measurements revealed that most of the in-cloud SO4 formed can be attributed to particle sizes larger than 200 nm (electrical mobility diameter). Aqueous-phase secondary organic aerosol (aqSOA) formation was non-significant.

The Copernicus Atmosphere Monitoring Service (CAMS) provides near-real-time forecast and reanalysis of aerosols using the ECMWF Integrated Forecasting System with atmospheric composition extension, constrained by the assimilation of MODIS and the Polar Multi-Sensor Aerosol Optical Properties (PMAp) aerosol optical depth (AOD). The objective of this work is to evaluate two new near-real-time AOD products to prepare for their assimilation into CAMS, namely the Copernicus AOD (collection 1) from the Sea and Land Surface Temperature Radiometer (SLSTR) on board Sentinel 3-A/B over ocean and the NOAA EPS AOD (v2.r1) from VIIRS on board S-NPP and NOAA20 over both land and ocean. The differences between MODIS (C6.1), PMAp (v2.1), VIIRS (v2.r1), and SLSTR (C1) AOD as well as their departure from the modeled AOD were assessed at the model grid resolution (i.e., level-3) using the 3-month AOD average (December 2019–February 2020 and March–May 2020). VIIRS and MODIS show the best consistency across the products, which is explained by instrument and retrieval algorithm similarities. VIIRS AOD is frequently lower over the ocean background and higher over biomass burning and dust source land regions compared to MODIS. VIIRS shows larger spatial coverage over land and resolves finer spatial structures such as the transport of Australian biomass burning smoke over the Pacific, which can be explained by the use of a heavy aerosol detection test in the retrieval algorithm. Our results confirm the positive offset over ocean (i) between Terra/MODIS and Aqua/MODIS due to the non-corrected radiometric calibration degradation of Terra/MODIS in the Dark Target algorithm and (ii) between SNPP/VIIRS and NOAA20/VIIRS due to the positive bias in the solar reflective bands of SNPP/VIIRS. SLSTR AOD shows much smaller level-3 values than the rest of the products, which is mainly related to differences in spatial representativity at the IFS grid spatial resolution due to the stringent cloud filtering applied to the SLSTR radiances. Finally, the geometry characteristics of the instrument, which drive the range of scattering angles sampled by the instrument, can explain a large part of the differences between retrievals such as the positive offset between PMAp datasets from MetOp-B and MetOp-A.