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The Copernicus Atmosphere Monitoring Service (CAMS) provides daily analyses and forecasts of the composition of the atmosphere, including the reactive gases such as O3, CO, NO2, HCHO and SO2; aerosol species; and greenhouse gases. The global CAMS analysis system (IFS-COMPO) is based on the ECMWF Integrated Forecasting System (IFS) for numerical weather prediction (NWP) and assimilates a large number of composition satellite products on top of the meteorological observations ingested in IFS. The CAMS system receives regular upgrades, following the upgrades of IFS. The last upgrade, Cy48R1, operational since 27 June 2023, was major with a large number of code changes, both for IFS-COMPO and for NWP. The main IFS-COMPO innovations include the introduction of full stratospheric chemistry; a major update of the emissions; a major update of the aerosol model, including the representation of secondary organic aerosol; several updates of the dust life cycle and optics; updates to the inorganic chemistry in the troposphere; and the assimilation of Visible Infrared Imaging Radiometer Suite (VIIRS) aerosol optical depth (AOD) and TROPOspheric Monitoring Instrument (TROPOMI) CO. The CAMS Cy48R1 upgrade was validated using a large number of independent measurement datasets, including surface in situ, surface remote sensing, routine aircraft, and balloon and satellite observations. In this paper we present the validation results for Cy48R1 by comparing them with the skill of the previous operational system (Cy47R3), with the independent observations as reference, for the period October 2022 to June 2023, during which daily forecasts from both cycles are available. Major improvements in skill are found for the ozone profile in the lower–middle stratosphere and for stratospheric NO2 due to the inclusion of full stratospheric chemistry. Stratospheric trace gases compare well with the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) observations between 10 and 200 hPa, with larger deviations between 1 and 10 hPa. The impact of the updated emissions is especially visible over East Asia and is beneficial for the trace gases O3, NO2 and SO2. The CO column assimilation is now anchored by the Infrared Atmospheric Sounding Interferometer (IASI) instead of the Measurements Of Pollution in The Troposphere (MOPITT) instrument, which is beneficial for most of the CO comparisons, and the assimilation of TROPOMI CO data improves the model CO field in the troposphere. In general the aerosol optical depth has improved globally, but the dust evaluation shows more mixed results. The results of the 47 comparisons are summarised in a scorecard, which shows that 83 % of the evaluation datasets show a neutral or improved performance of Cy48R1 compared to the previous operational CAMS system, while 17 % indicate a (slight) degradation. This demonstrates the overall success of this upgrade.

Atmospheric mineral dust aerosol constitutes a threat to aircraft engines from deterioration of internal components. Here we fulfil an overdue need to quantify engine dust ingestion at airports worldwide. The vertical distribution of dust is of key importance since ascent/descent rates and engine power both vary with altitude and affect dust ingestion. We use representative jet engine power profile information combined with vertically and seasonally varying dust concentrations to calculate the “dust dose” ingested by an engine over a single ascent or descent. Using the Copernicus Atmosphere Monitoring Service (CAMS) model reanalysis, we calculate climatological and seasonal dust dose at 10 airports for 2003–2019. Dust doses are mostly largest in Northern Hemisphere summer for descent, with the largest at Delhi in June–August (JJA; 6.6 g) followed by Niamey in March–May (MAM; 4.7 g) and Dubai in JJA (4.3 g). Holding patterns at altitudes coincident with peak dust concentrations can lead to substantial quantities of dust ingestion, resulting in a larger dose than the take-off, climb, and taxi phases. We compare dust dose calculated from CAMS to spaceborne lidar observations from two dust datasets derived from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP). In general, seasonal and spatial patterns are similar between CAMS and CALIOP, though large variations in dose magnitude are found, with CAMS producing lower doses by a factor of 1.9 to 2.8, particularly when peak dust concentration is very close to the surface. We show that mitigating action to reduce engine dust damage could be achieved, firstly by moving arrivals and departures to after sunset and secondly by altering the altitude of the holding pattern away from that of the local dust peak altitude, reducing dust dose by up to 44 % and 41 % respectively. We suggest that a likely low bias of dust concentration in the CAMS reanalysis should be considered by aviation stakeholders when estimating dust-induced engine wear.

The emergence of aerosol reanalyses in recent years has facilitated a comprehensive and systematic evaluation of aerosol optical depth (AOD) trends and attribution over multi-decadal timescales. Notable multi-year aerosol reanalyses currently available include NAAPS-RA from the US Naval Research Laboratory, the NASA MERRA-2, JRAero from the Japan Meteorological Agency (JMA), and CAMSRA from Copernicus/ECMWF. These aerosol reanalyses are based on differing underlying meteorology models, representations of aerosol processes, as well as data assimilation methods and treatment of AOD observations. This study presents the basic verification characteristics of these four reanalyses versus both AERONET and MODIS retrievals in monthly AOD properties and identifies the strength of each reanalysis and the regions where divergence and challenges are prominent. Regions with high pollution and often mixed fine-mode and coarse-mode aerosol environments, such as South Asia, East Asia, Southeast Asia, and the Maritime Continent, pose significant challenges, as indicated by higher monthly AOD root mean square error. Moreover, regions that are distant from major aerosol source areas, including the polar regions and remote oceans, exhibit large relative differences in speciated AODs and fine-mode versus coarse-mode AODs among the four reanalyses. To ensure consistency across the globe, a multi-reanalysis consensus (MRC, i.e., ensemble mean) approach was developed similarly to the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME). Like the ICAP-MME, while the MRC does not consistently rank first among the reanalyses for individual regions, it performs well by ranking first or second globally in AOD correlation and RMSE, making it a suitable candidate for climate studies that require robust and consistent assessments.

Global monitoring of aerosols is required to analyse the impacts of aerosols on air quality and to understand their role in modulating the climate variability. The Copernicus Atmosphere Monitoring Service (CAMS) provides near-real-time forecasts and reanalyses of aerosols using the ECMWF Integrated Forecasting System (IFS), constrained by the assimilation of MODIS and Polar Multi-Sensor Aerosol Optical Properties (PMAp) aerosol optical depth (AOD). Given the potential end of lifetime of MODIS AOD, implementing new AOD observations in the CAMS operational suite is a priority to ensure the continuity of the CAMS forecast performances. The objective of this work is to test the assimilation of the NOAA VIIRS AOD product from S-NPP and NOAA20 satellites in the IFS model. Simulation experiments assimilating VIIRS on top or in place of MODIS were carried out from June 2021 to November 2021 to evaluate the impacts on the AOD analysis. For maritime aerosol background, the assimilation of VIIRS and the use of VIIRS from NOAA20 as an anchor reduce the analysis AOD values compared to MODIS-based experiments, in which the analysis values were too high due to the positive bias of MODIS/Terra over ocean. Over land, the assimilation of VIIRS induces a large increase in the analysis over biomass burning regions where VIIRS shows larger AOD than MODIS due to differences in the aerosol models and cloud filtering between MODIS and VIIRS retrieval algorithms. For dust source regions, the analysis is reduced when VIIRS is assimilated on top of or in place of MODIS, particularly over the Sahara, the Arabian Peninsula and a few places in Asia in the July–August period. The assimilation of VIIRS leads to an overall reduction of the bias in AOD analysis evaluated against AERONET measurements, with the largest bias reduction over Europe and desert and maritime sites.

The Copernicus Atmosphere Monitoring Service (CAMS) has recently produced a greenhouse gas reanalysis (version egg4) that covers almost 2 decades from 2003 to 2020 and which will be extended in the future. This reanalysis dataset includes carbon dioxide (CO2) and methane (CH4). The reanalysis procedure combines model data with satellite data into a globally complete and consistent dataset using the European Centre for Medium-Range Weather Forecasts' Integrated Forecasting System (IFS). This dataset has been carefully evaluated against independent observations to ensure validity and to point out deficiencies to the user. The greenhouse gas reanalysis can be used to examine the impact of atmospheric greenhouse gas concentrations on climate change (such as global and regional climate radiative forcing), assess intercontinental transport, and serve as boundary conditions for regional simulations, among other applications and scientific uses. The caveats associated with changes in assimilated observations and fixed underlying emissions are highlighted, as is their impact on the estimation of trends and annual growth rates of these long-lived greenhouse gases.

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.

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.

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.

Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

This article describes the Integrated Forecasting System aerosol scheme (IFS-AER) used operationally in the IFS cycle 47R1, which was operated by the European Centre for Medium Range Weather Forecasts (ECMWF) in the framework of the Copernicus Atmospheric Monitoring Services (CAMS). It represents an update of the Rémy et al. (2019) article, which described cycle 45R1 of IFS-AER in detail. Here, we detail only the parameterisations of sources and sinks that have been updated since cycle 45R1, as well as recent changes in the configuration used operationally within CAMS. Compared to cycle 45R1, a greater integration of aerosol and chemistry has been achieved. Primary aerosol sources have been updated, with the implementation of new dust and sea salt aerosol emission schemes. New dry and wet deposition parameterisations have also been implemented. Sulfate production rates are now provided by the global chemistry component of IFS. This paper aims to describe most of the updates that have been implemented since cycle 45R1, not just the ones that are used operationally in cycle 47R1; components that are not used operationally will be clearly flagged. Cycle 47R1 of IFS-AER has been evaluated against a wide range of surface and total column observations. The final simulated products, such as particulate matter (PM) and aerosol optical depth (AOD), generally show a significant improvement in skill scores compared to results obtained with cycle 45R1. Similarly, the simulated surface concentration of sulfate, organic matter and sea salt aerosol are improved by cycle 47R1 compared to cycle 45R1. Some biases persist, such as the surface concentrations of nitrate and organic matter being simulated too high. The new wet and dry deposition schemes that have been implemented into cycle 47R1 have a mostly positive impact on simulated AOD, PM and speciated aerosol surface concentration.

Concentrations of atmospheric methane (CH4), the second most important greenhouse gas, continue to grow. In recent years this growth rate has increased further (2020: +15.6 ppb), the cause of which remains largely unknown. Here, we demonstrate a high-resolution (∼80 km), short-window (24 h) 4D-Var global inversion system based on the ECMWF Integrated Forecasting System (IFS) and newly available satellite observations. The largest national disagreement found between prior (5.3 Tg per month) and posterior (5.0 Tg per month) CH4 emissions is from China, mainly attributed to the energy sector. Emissions estimated from our global system are in good agreement with those of previous regional studies and point source-specific studies. Emission events (leaks or blowouts) > 10 t CH4 h−1 were detected, but without appropriate prior uncertainty information, were not well quantified. Our results suggest that global anthropogenic CH4 emissions for the first 6 months of 2020 were, on average, 470 Gg per month (+1.6 %) higher than for 2019, mainly attributed to the energy and agricultural sectors. Regionally, the largest increases were seen from China (+220 Gg per month, 4.3 %), with smaller increases from India (+50 Gg per month, 1.5 %) and the USA (+40 Gg per month, 2.2 %). When assuming a consistent year-on-year positive trend in emissions, results show that during the onset of the global slowdown (March–April 2020) energy sector CH4 emissions from China increased above expected levels; however, during later months (May–June 2020) emissions decreased below expected levels. Results for the first 6 months of 2019/20 suggest that the accumulated impact of the COVID-19 slowdown on CH4 emissions from March–June 2020 might be small relative to the long-term positive trend in emissions. Changes in OH concentration, not investigated here, may have contributed to the observed growth in 2020.

Aerosol-induced absorption of shortwave radiation can modify the climate through local atmospheric heating, which affects lapse rates, precipitation, and cloud formation. Presently, the total amount of aerosol absorption is poorly constrained, and the main absorbing aerosol species (black carbon (BC), organic aerosols (OA), and mineral dust) are diversely quantified in global climate models. As part of the third phase of the Aerosol Comparisons between Observations and Models (AeroCom) intercomparison initiative (AeroCom phase III), we here document the distribution and magnitude of aerosol absorption in current global aerosol models and quantify the sources of intermodel spread, highlighting the difficulties of attributing absorption to different species. In total, 15 models have provided total present-day absorption at 550 nm (using year 2010 emissions), 11 of which have provided absorption per absorbing species. The multi-model global annual mean total absorption aerosol optical depth (AAOD) is 0.0054 (0.0020 to 0.0098; 550 nm), with the range given as the minimum and maximum model values. This is 28 % higher compared to the 0.0042 (0.0021 to 0.0076) multi-model mean in AeroCom phase II (using year 2000 emissions), but the difference is within 1 standard deviation, which, in this study, is 0.0023 (0.0019 in Phase II). Of the summed component AAOD, 60 % (range 36 %–84 %) is estimated to be due to BC, 31 % (12 %–49 %) is due to dust, and 11 % (0 %–24 %) is due to OA; however, the components are not independent in terms of their absorbing efficiency. In models with internal mixtures of absorbing aerosols, a major challenge is the lack of a common and simple method to attribute absorption to the different absorbing species. Therefore, when possible, the models with internally mixed aerosols in the present study have performed simulations using the same method for estimating absorption due to BC, OA, and dust, namely by removing it and comparing runs with and without the absorbing species. We discuss the challenges of attributing absorption to different species; we compare burden, refractive indices, and density; and we contrast models with internal mixing to models with external mixing. The model mean BC mass absorption coefficient (MAC) value is 10.1 (3.1 to 17.7) m2 g−1 (550 nm), and the model mean BC AAOD is 0.0030 (0.0007 to 0.0077). The difference in lifetime (and burden) in the models explains as much of the BC AAOD spread as the difference in BC MAC values. The difference in the spectral dependency between the models is striking. Several models have an absorption Ångstrøm exponent (AAE) close to 1, which likely is too low given current knowledge of spectral aerosol optical properties. Most models do not account for brown carbon and underestimate the spectral dependency for OA.

Aerosol forecasts by the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System aerosol module (IFS-AER) for the years 2016–2019 (cycles 41r1–46r1) are compared to vertical profiles of particle backscatter from the Deutscher Wetterdienst (DWD) ceilometer network. The system has been developed in the Copernicus Atmosphere Monitoring Service (CAMS) and its precursors. The focus of this article is to evaluate the realism of the vertical aerosol distribution from 0.4 to 8 km above ground, coded in the shape, bias and temporal variation of the profiles. The common physical quantity, the attenuated backscatter β∗(z), is directly measured and calculated from the model mass mixing ratios of the different particle types using the model's inherent aerosol microphysical properties. Pearson correlation coefficients of daily average simulated and observed vertical profiles between r=0.6–0.8 in summer and 0.7–0.95 in winter indicate that most of the vertical structure is captured. It is governed by larger β∗(z) in the mixing layer and comparably well captured with the successive model versions. The aerosol load tends to be biased high near the surface, underestimated in the mixing layer and realistic at small background values in the undisturbed free troposphere. A seasonal cycle of the bias below 1 km height indicates that aerosol sources and/or lifetimes are overestimated in summer and pollution episodes are not fully resolved in winter. Long-range transport of Saharan dust or fire smoke is captured and timely, only the dispersion to smaller scales is not resolved in detail. Over Germany, β∗(z) values from Saharan dust and sea salt are considerably overestimated. Differences between model and ceilometer profiles are investigated using observed in situ mass concentrations of organic matter (OM), black carbon, SO4, NO3, NH4 and proxies for mineral dust and sea salt near the surface. Accordingly, SO4 and OM sources as well as gas-to-particle partitioning of the NO3–NH4 system are too strong. The top of the mixing layer on average appears too smooth and several hundred meters too low in the model. Finally, a discussion is included of the considerable uncertainties in the observations as well as the conversion from modeled to observed physical quantities and from necessary adaptions of varying resolutions and definitions.

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 %.

Previous studies have noted a relationship between African dust and Atlantic tropical cyclone (TC) activity. However, due to the limitations of past dust analyses, the strength of this relationship remains uncertain. The emergence of aerosol reanalyses, including the Navy Aerosol Analysis and Prediction System (NAAPS) aerosol optical depth (AOD) reanalysis, NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and ECMWF Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA), enables an investigation of the relationship between African dust and TC activity over the tropical Atlantic and Caribbean in a consistent temporal and spatial manner for 2003–2018. Although June–July–August (JJA) 550 nm dust AOD (DAOD) from all three reanalysis products correlates significantly over the tropical Atlantic and Caribbean, the difference in DAOD magnitude between products can be as large as 60 % over the Caribbean and 20 % over the tropical North Atlantic. Based on the three individual reanalyses, we have created an aerosol multi-reanalysis consensus (MRC). The MRC presents overall better root mean square error over the tropical Atlantic and Caribbean compared to individual reanalyses when verified with ground-based AErosol RObotic NETwork (AERONET) AOD measurements. Each of the three individual reanalyses and the MRC have significant negative correlations between JJA Caribbean DAOD and seasonal Atlantic accumulated cyclone energy (ACE), while the correlation between JJA tropical North Atlantic DAOD and seasonal ACE is weaker. Possible reasons for this regional difference are provided. A composite analysis of 3 high-JJA-Caribbean-DAOD years versus 3 low-JJA-Caribbean-DAOD years reveals large differences in overall Atlantic TC activity. We also show that JJA Caribbean DAOD is significantly correlated with large-scale fields associated with variability in interannual Atlantic TC activity including zonal wind shear, mid-level moisture, and sea surface temperature (SST), as well as the El Niño–Southern Oscillation (ENSO) and the Atlantic Meridional Mode (AMM), implying confounding effects of these factors on the dust–TC relationship. We find that seasonal Atlantic DAOD and the AMM, the leading mode of coupled Atlantic variability, are inversely related and intertwined in the dust–TC relationship. Overall, DAOD in both the tropical Atlantic and Caribbean is negatively correlated with Atlantic hurricane frequency and intensity, with stronger correlations in the Caribbean than farther east in the tropical North Atlantic.

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.

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.

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f(RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f(RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f(RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f(RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided.

Atmospheric flux inversions use observations of atmospheric CO2 to provide anthropogenic and biogenic CO2 flux estimates at a range of spatio-temporal scales. Inversions require prior flux, a forward model and observation errors to estimate posterior fluxes and uncertainties. Here, we investigate the forward transport error and the associated biogenic feedback in an Earth system model (ESM) context. These errors can occur from uncertainty in the initial meteorology, the analysis fields used, or the advection schemes and physical parameterisation of the model. We also explore the spatio-temporal variability and flow-dependent error covariances. We then compare the error with the atmospheric response to uncertainty in the prior anthropogenic emissions. Although transport errors are variable, average total-column CO2 (XCO2) transport errors over anthropogenic emission hotspots (0.1–0.8 ppm) are comparable to, and often exceed, prior monthly anthropogenic flux uncertainties projected onto the same space (0.1–1.4 ppm). Average near-surface transport errors at three sites (Paris, Caltech and Tsukuba) range from 1.7 to 7.2 ppm. The global average XCO2 transport error standard deviation plateaus at ∼0.1 ppm after 2–3 d, after which atmospheric mixing significantly dampens the concentration gradients. Error correlations are found to be highly flow dependent, with XCO2 spatio-temporal correlation length scales ranging from 0 to 700 km and 0 to 260 min. Globally, the average model error caused by the biogenic response to atmospheric meteorological uncertainties is small ( ppm); however, this increases over high flux regions and is seasonally dependent (e.g. the Amazon; January and July: 0.24±0.18 ppm and 0.13±0.07 ppm). In general, flux hotspots are well-correlated with model transport errors. Our model error estimates, combined with the atmospheric response to anthropogenic flux uncertainty, are validated against three Total Carbon Observing Network (TCCON) XCO2 sites. Results indicate that our model and flux uncertainty account for 21 %–65 % of the total uncertainty. The remaining uncertainty originates from additional sources, such as observation, numerical and representation errors, as well as structural errors in the biogenic model. An underrepresentation of transport and flux uncertainties could also contribute to the remaining uncertainty. Our quantification of CO2 transport error can be used to help derive accurate posterior fluxes and error reductions in future inversion systems. The model uncertainty diagnosed here can be used with varying degrees of complexity and with different modelling techniques by the inversion community.

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.

An aerosol climatology to represent aerosols in the radiation schemes of global atmospheric models was recently developed. We derived the climatology from a reanalysis of atmospheric composition produced by the Copernicus Atmosphere Monitoring Service (CAMS). As an example of an application in a global atmospheric model, we discuss the technical aspects of the implementation in the European Centre for Medium Range Weather Forecasts Integrated Forecasting System (ECMWF-IFS) and the impact of the new climatology on the medium-range weather forecasts and 1-year simulations. The new aerosol climatology was derived by combining a set of model simulations with constrained meteorological conditions and an atmospheric composition reanalysis for the period 2003–2013 produced by the IFS. The aerosol fields of the reanalysis are constrained by assimilating the aerosol optical thickness (AOT) retrievals product by the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. In a further step, we used modelled aerosol fields to correct the aerosol speciation and the vertical profiles of the aerosol reanalysis fields. The new climatology provides the monthly-mean mass mixing ratio of five aerosol species constrained by assimilated MODIS AOT. Using the new climatology in the ECMWF-IFS leads to changes in the direct aerosol radiative effect compared to the climatology previously implemented, which have a small but non-impact on the forecast skill of large-scale weather patterns in the medium-range. However, details of the regional distribution of aerosol radiative forcing can have a large local impact. This is the case for the area of the Arabian Peninsula and the northern Indian Ocean. Here changes in the radiative forcing of the mineral dust significantly improve the summer monsoon circulation.

Abstract 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.

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.

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.

The Convective Cloud Field Model (CCFM) attempts to address some of the shortcomings of both the commonly used bulk mass-flux parameterisations and those using a prescribed spectrum of clouds. By considering the cloud spectrum as a competitive system in which cloud types interact through their environment in competition for convective available potential energy (CAPE), the spectrum is able to respond dynamically to changes in the environment. An explicit Lagrangian entraining plume model for each cloud type allows for the representation of convective-cloud microphysics, paving the way for the study of aerosol–convection interactions at the global scale where their impact remains highly uncertain. In this paper, we introduce a new treatment of convective triggering, extending the entraining plume model below cloud base to explicitly represent the unsaturated thermals which initiate convection. This allows for a realistic vertical velocity to develop at cloud base, so that the cloud microphysics can begin with physically based activation of cloud condensation nuclei (CCN). We evaluate this new version of CCFM in the context of the global model ECHAM6–HAM, comparing its performance to the standard Tiedtke–Nordeng parameterisation used in that model. We find that the spatio-temporal distribution of precipitation is improved, both against a climatology from the Global Precipitation Climatology Project (GPCP) and also against diurnal cycles from the Tropical Rainfall Measurement Mission (TRMM) with a reduced tendency for precipitation to peak too early in the afternoon. Cloud cover is quite sensitive to the vertical level from which the dry convection is initiated, but when this is chosen appropriately the cloud cover compares well with that from Tiedtke–Nordeng. CCFM can thus perform as well as, or better than, the standard scheme while providing additional capabilities to represent convective-cloud microphysics and dynamic cloud morphology at the global scale.

The Community Intercomparison Suite (CIS) is an easy-to-use command-line tool which has been developed to allow the straightforward intercomparison of remote sensing, in situ and model data. While there are a number of tools available for working with climate model data, the large diversity of sources (and formats) of remote sensing and in situ measurements necessitated a novel software solution. Developed by a professional software company, CIS supports a large number of gridded and ungridded data sources "out-of-the-box", including climate model output in NetCDF or the UK Met Office pp file format, CloudSat, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization), MODIS (MODerate resolution Imaging Spectroradiometer), Cloud and Aerosol CCI (Climate Change Initiative) level 2 satellite data and a number of in situ aircraft and ground station data sets. The open-source architecture also supports user-defined plugins to allow many other sources to be easily added. Many of the key operations required when comparing heterogenous data sets are provided by CIS, including subsetting, aggregating, collocating and plotting the data. Output data are written to CF-compliant NetCDF files to ensure interoperability with other tools and systems. The latest documentation, including a user manual and installation instructions, can be found on our website (http://cistools.net). Here, we describe the need which this tool fulfils, followed by descriptions of its main functionality (as at version 1.4.0) and plugin architecture which make it unique in the field.

Aerosol–cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (ω500 −1) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is close to that in subsidence regimes, which indicates that regimes with strong large-scale ascent are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm day−1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.

The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3–UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3–UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN > 3 nm), while the profiles of larger particles (e.g. CN > 100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. We also show that the processes that affect the AOD-normalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions.

Satellite studies of aerosol–cloud interactions usually make use of retrievals of both aerosol and cloud properties, but these retrievals are rarely spatially co-located. While it is possible to retrieve aerosol properties above clouds under certain circumstances, aerosol properties are usually only retrieved in cloud-free scenes. Generally, the smaller spatial variability of aerosols compared to clouds reduces the importance of this sampling difference. However, as precipitation generates an increase in spatial variability of aerosols, the imperfect co-location of aerosol and cloud property retrievals may lead to changes in observed aerosol–cloud–precipitation relationships in precipitating environments. In this work, we use a regional-scale model, satellite observations and reanalysis data to investigate how the non-coincidence of aerosol, cloud and precipitation retrievals affects correlations between them. We show that the difference in the aerosol optical depth (AOD)–precipitation relationship between general circulation models (GCMs) and satellite observations can be explained by the wet scavenging of aerosol. Using observations of the development of precipitation from cloud regimes, we show how the influence of wet scavenging can obscure possible aerosol influences on precipitation from convective clouds. This obscuring of aerosol–cloud–precipitation interactions by wet scavenging suggests that even if GCMs contained a perfect representation of aerosol influences on convective clouds, the difficulty of separating the "clear-sky" aerosol from the "all-sky" aerosol in GCMs may prevent them from reproducing the correlations seen in satellite data.

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.

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.

Absorbing aerosols emitted from biomass burning (BB) greatly affect the radiation balance, cloudiness, and circulation over tropical regions. Assessments of these impacts rely heavily on the modeled aerosol absorption from poorly constrained global models and thus exhibit large uncertainties. By combining the AeroCom model ensemble with satellite and in situ observations, we provide constraints on the aerosol absorption optical depth (AAOD) over the Amazon and Africa. Our approach enables identification of error contributions from emission, lifetime, and MAC (mass absorption coefficient) per model, with MAC and emission dominating the AAOD errors over Amazon and Africa, respectively. In addition to primary emissions, our analysis suggests substantial formation of secondary organic aerosols over the Amazon but not over Africa. Furthermore, we find that differences in direct aerosol radiative effects between models decrease by threefold over the BB source and outflow regions after correcting the identified errors. This highlights the potential to greatly reduce the uncertainty in the most uncertain radiative forcing agent.

Biomass burning (BB) is a major source of aerosols that remain the most uncertain components of the global radiative forcing. Current global models have great difficulty matching observed aerosol optical depth (AOD) over BB regions. A common solution to address modelled AOD biases is scaling BB emissions. Using the relationship from an ensemble of aerosol models and satellite observations, we show that the bias in aerosol modelling results primarily from incorrect lifetimes and underestimated mass extinction coefficients. In turn, these biases seem to be related to incorrect precipitation and underestimated particle sizes. We further show that boosting BB emissions to correct AOD biases over the source region causes an overestimation of AOD in the outflow from Africa by 48%, leading to a double warming effect compared with when biases are simultaneously addressed for both aforementioned factors. Such deviations are particularly concerning in a warming future with increasing emissions from fires., (© 2022. The Author(s).)

Since the first International Cooperative for Aerosol Prediction (ICAP) multi-model ensemble (MME) study, the number of ICAP global operational aerosol models has increased from five to nine. An update of the current ICAP status is provided, along with an evaluation of the performance of ICAP-MME over 2012-2017, with a focus on June 2016-May 2017. Evaluated with ground-based Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) and data assimilation quality MODerate-resolution Imaging Spectroradiometer (MODIS) retrieval products, the ICAP-MME AOD consensus remains the overall top-scoring and most consistent performer among all models in terms of root-mean-square error (RMSE), bias and correlation for total, fine- and coarse-mode AODs as well as dust AOD; this is similar to the first ICAP-MME study. Further, over the years, the performance of ICAP-MME is relatively stable and reliable compared to more variability in the individual models. The extent to which the AOD forecast error of ICAP-MME can be predicted is also examined. Leading predictors are found to be the consensus mean and spread. Regression models of absolute forecast errors were built for AOD forecasts of different lengths for potential applications. ICAP-MME performance in terms of modal AOD RMSEs of the 21 regionally representative sites over 2012-2017 suggests a general tendency for model improvements in fine-mode AOD, especially over Asia. No significant improvement in coarse-mode AOD is found overall for this time period., (© 2019 The Authors. Quarterly Journal of the Royal Meteorological Society published by John Wiley & Sons Ltd on behalf of the Royal Meteorological Society.)

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.