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Constraining dust models to understand and quantify the effect of dust upon climate and ecosystems requires comprehensive analyses of the physiochemical properties of dust-emitting sediments in arid regions. Building upon previous studies in the Moroccan Sahara and Iceland, we analyse a diverse set of crusts and aeolian ripples (n=55) from various potential dust-emitting basins within the Mojave Desert, California, USA. Our focus is on characterizing the particle size distribution (PSD), mineralogy, aggregation/cohesion state, and Fe mode of occurrence. Our results show differences in fully and minimally dispersed PSDs, with crusts exhibiting average median diameters of 92 and 37 µm, respectively, compared to aeolian ripples with 226 and 213 µm, respectively. Mineralogical analyses unveiled strong variations between crusts and ripples, with crusts being enriched in phyllosilicates (24 % vs. 7.8 %), carbonates (6.6 % vs. 1.1 %), Na salts (7.3 % vs. 1.1 %), and zeolites (1.2 % and 0.12 %) and ripples being enriched in feldspars (48 % vs. 37 %), quartz (32 % vs. 16 %), and gypsum (4.7 % vs. 3.1 %). The size fractions from crust sediments display a homogeneous mineralogy, whereas those of aeolian ripples display more heterogeneity, mostly due to different particle aggregation. Bulk Fe content analyses indicate higher concentrations in crusts (3.0 ± 1.3 wt %) compared to ripples (1.9 ± 1.1 wt %), with similar proportions in their Fe mode of occurrence: nano-sized Fe oxides and readily exchangeable Fe represent ∼1.6 %, hematite and goethite ∼15 %, magnetite/maghemite ∼2.0 %, and structural Fe in silicates ∼80 % of the total Fe. We identified segregation patterns in the PSD and mineralogy differences in Na salt content within the Mojave basins, which can be explained by sediment transportation dynamics and precipitates due to groundwater table fluctuations described in previous studies in the region. Mojave Desert crusts show similarities with previously sampled crusts in the Moroccan Sahara in terms of the PSD and readily exchangeable Fe yet exhibit substantial differences in mineralogical composition, which should significantly influence the characteristic of the emitted dust particles.

Mineralogical composition drives dust impacts on Earth's climate systems. However, most climate models still use homogeneous dust, without accounting for the temporal and spatial variation in mineralogy. To quantify the radiative impact of resolving dust mineralogy on Earth's climate, we implement and simulate the distribution of dust minerals (i.e., illite, kaolinite, smectite, hematite, calcite, feldspar, quartz, and gypsum) from Claquin et al. (1999) (C1999) and activate their interaction with radiation in the GFDL AM4.0 model. Resolving mineralogy reduces dust absorption compared to the homogeneous dust used in the standard GFDL AM4.0 model that assumes a globally uniform hematite volume content of 2.7 % (HD27). The reduction in dust absorption results in improved agreement with observation-based single-scattering albedo (SSA), radiative fluxes from CERES (the Clouds and the Earth's Radiant Energy System), and land surface temperature from the CRU (Climatic Research Unit) compared to the baseline HD27 model version. It also results in distinct radiative impacts on Earth's climate over North Africa. Over the 19-year (from 2001 to 2019) modeled period during JJA (June–July–August), the reduction in dust absorption in AM4.0 leads to a reduction of over 50 % in net downward radiation across the Sahara and approximately 20 % over the Sahel at the top of the atmosphere (TOA) compared to the baseline HD27 model version. The reduced dust absorption weakens the atmospheric warming effect of dust aerosols and leads to an alteration in land surface temperature, resulting in a decrease of 0.66 K over the Sahara and an increase of 0.7 K over the Sahel. The less warming in the atmosphere suppresses ascent and weakens the monsoon inflow from the Gulf of Guinea. This brings less moisture to the Sahel, which combined with decreased ascent induces a reduction of precipitation. To isolate the effect of reduced absorption compared to resolving spatial and temporal mineralogy, we carry out a simulation where the hematite volume content of homogeneous dust is reduced from 2.7 % to 0.9 % (HD09). The dust absorption (e.g., single-scattering albedo) of HD09 is comparable to that of the mineralogically speciated model on a global mean scale, albeit with a lower spatial variation that arises solely from particle size. Comparison of the two models indicates that the spatial inhomogeneity in dust absorption resulting from resolving mineralogy does not have significant impacts on Earth's radiation and climate, provided there is a similar level of dust absorption on a global mean scale before and after resolving dust mineralogy. However, uncertainties related to emission and distribution of minerals may blur the advantages of resolving minerals to study their impact on radiation, cloud properties, ocean biogeochemistry, air quality, and photochemistry. On the other hand, lumping together clay minerals (i.e., illite, kaolinite, and smectite), but excluding externally mixed hematite and gypsum, appears to provide both computational efficiency and relative accuracy. Nevertheless, for specific research, it may be necessary to fully resolve mineralogy to achieve accuracy.

Volatile organic compounds (VOCs) significantly impact air quality and atmospheric chemistry, influencing ozone formation and secondary organic aerosol production. Despite their importance, the uncertainties associated with representing VOCs in atmospheric emission inventories are considerable. This work presents a spatiotemporal assessment and evaluation of benzene, toluene, and xylene (BTX) emissions and concentrations in Spain by combining bottom-up emissions, air quality modelling techniques, and ground-based observations. The emissions produced by High-Elective Resolution Modelling Emission System (HERMESv3) were used as input to the Multiscale Online Nonhydrostatic AtmospheRe CHemistry (MONARCH) chemical transport model to simulate surface concentrations across Spain. Comparing modelled and observed levels revealed uncertainty in the anthropogenic emissions, which were further explored through sensitivity tests. The largest levels of observed benzene and xylene were found in industrial sites near coke ovens, refineries, and car manufacturing facilities, where the modelling results show large underestimations. Official emissions reported for these facilities were replaced by alternative estimates, resulting in varied improvements in the model's performance across different stations. However, uncertainties associated with industrial emission processes persist, emphasising the need for further refinement. For toluene, consistent overestimations in background stations were mainly related to uncertainties in the spatial disaggregation of emissions from industrial-use solvent activities, mainly wood paint applications. Observed benzene levels in Barcelona's urban traffic areas were 5 times larger than the ones observed in Madrid. MONARCH failed to reproduce the observed gradient between the two cities due to uncertainties arising from estimating emissions from motorcycles and mopeds, as well as from different measurement methods and the model's capacity to accurately simulate meteorological conditions. Our results are constrained by the spatial and temporal coverage of available BTX observations, posing a key challenge in evaluating the spatial distribution of modelled levels and associated emissions.

Characterising the physico-chemical properties of dust-emitting sediments in arid regions is fundamental to understanding the effects of dust on climate and ecosystems. However, knowledge regarding high-latitude dust (HLD) remains limited. This study focuses on analysing the particle size distribution (PSD), mineralogy, cohesion, iron (Fe) mode of occurrence, and visible–near infrared (VNIR) reflectance spectra of dust-emitting sediments from dust hotspots in Iceland (HLD region). Extensive analysis was conducted on samples of top sediments, sediments, and aeolian ripples collected from seven dust sources, with particular emphasis on the Jökulsá basin, encompassing the desert of Dyngjunsandur. Both fully and minimally dispersed PSDs and their respective mass median particle diameters revealed remarkable similarities (56 ± 69 and 55 ± 62 µm, respectively). Mineralogical analyses indicated the prevalence of amorphous phases (68 ± 26 %), feldspars (17 ± 13 %), and pyroxenes (9.3 ± 7.2 %), consistent with thorough analyses of VNIR reflectance spectra. The Fe content reached 9.5 ± 0.40 wt %, predominantly within silicate structures (80 ± 6.3 %), complemented by magnetite (16 ± 5.5 %), hematite/goethite (4.5 ± 2.7 %), and readily exchangeable Fe ions or Fe nano-oxides (1.6 ± 0.63 %). Icelandic top sediments exhibited coarser PSDs compared to the high dust-emitting crusts from mid-latitude arid regions, distinctive mineralogy, and a 3-fold bulk Fe content, with a significant presence of magnetite. The congruence between fully and minimally dispersed PSDs underscores reduced particle aggregation and cohesion of Icelandic top sediments, suggesting that aerodynamic entrainment of dust could also play a role upon emission in this region, alongside saltation bombardment. The extensive analysis in Dyngjusandur enabled the development of a conceptual model to encapsulate Iceland's rapidly evolving high dust-emitting environments.

The composition of soil dust aerosols derives from the mineral abundances in the parent soils that vary across dust source regions. Nonetheless, Earth system models (ESMs) have traditionally represented mineral dust as a globally homogeneous species. The growing interest in modeling dust mineralogy, facilitated by the recognized sensitivity of the dust climate impacts to composition, has motivated state-of-the-art ESMs to incorporate the mineral speciation of dust along with its effect upon the dust direct radiative effect (DRE). In this work, we enable the NASA Goddard Institute for Space Studies ModelE2.1 to calculate the shortwave (SW) DRE accounting for the regionally varying soil mineralogy. Mineral–radiation interaction at solar wavelengths is calculated according to two alternative coupling schemes: (1) external mixing of three mineral components that are optically distinguished, one of which contains embedded iron oxides; (2) a single internal mixture of all dust minerals with a dynamic fraction of iron oxides that varies regionally and temporally. We link dust absorption to the fractional mass of iron oxides based on recent chamber measurements using natural dust aerosol samples. We show that coupled mineralogy overall enhances the scattering by dust, and thus the global cooling, compared to our control run with globally uniform composition. According to the external mixing scheme, the SW DRE at the top of atmosphere (TOA) changes from −0.25 to -0.30Wm-2, corresponding to a change in the net DRE, including the longwave effect, from −0.08 to -0.12Wm-2. The cooling increase is accentuated when the internal mixing scheme is configured: the SW DRE at the TOA becomes -0.34Wm-2 with a net DRE of -0.15Wm-2. The varying composition modifies the regional distribution of single scattering albedo (SSA), whose variations in specific regions can be remarkable (above 0.03) and significantly modify the regional SW DRE. Evaluation against the AErosol RObotic NETwork (AERONET) shows that explicit representation of soil mineralogy and its regional variations reduces the low bias of model dust SSA while improving the range of variability across stations and calendar months. Despite these improvements, the moderate spatiotemporal correlation with AERONET reveals remaining modeling challenges and the need for more accurate measurements of mineral fractions in soils.

Desert dust is an important atmospheric aerosol that affects the Earth's climate, biogeochemistry, and air quality. However, current Earth system models (ESMs) struggle to accurately capture the impact of dust on the Earth's climate and ecosystems, in part because these models lack several essential aeolian processes that couple dust with climate and land surface processes. In this study, we address this issue by implementing several new parameterizations of aeolian processes detailed in our companion paper in the Community Earth System Model version 2 (CESM2). These processes include (1) incorporating a simplified soil particle size representation to calculate the dust emission threshold friction velocity, (2) accounting for the drag partition effect of rocks and vegetation in reducing wind stress on erodible soils, (3) accounting for the intermittency of dust emissions due to unresolved turbulent wind fluctuations, and (4) correcting the spatial variability of simulated dust emissions from native to higher spatial resolutions on spatiotemporal dust variability. Our results show that the modified dust emission scheme significantly reduces the model bias against observations compared with the default scheme and improves the correlation against observations of multiple key dust variables such as dust aerosol optical depth (DAOD), surface particulate matter (PM) concentration, and deposition flux. Our scheme's dust also correlates strongly with various meteorological and land surface variables, implying higher sensitivity of dust to future climate change than other schemes' dust. These findings highlight the importance of including additional aeolian processes for improving the performance of ESM aerosol simulations and potentially enhancing model assessments of how dust impacts climate and ecosystem changes.

We present a high-resolution global emission catalogue of CO2 and co-emitted species (NOx, SO2, CO, CH4) from thermal power plants for the year 2018. The construction of the database follows a bottom-up approach, which combines plant-specific information with national energy consumption statistics and fuel-dependent emission factors for CO2 and emission ratios for co-emitted species (e.g. the amount of NOx emitted relative to CO2: NOx/CO2). The resulting catalogue contains annual emission information for more than 16 000 individual facilities at their exact geographical locations. Each facility is linked to a country- and fuel-dependent temporal profile (i.e. monthly, day of the week and hourly) and a plant-level vertical profile, which were derived from national electricity generation statistics and plume rise calculations that combine stack parameters with meteorological information. The combination of the aforementioned information allows us to derive high-resolution spatial and temporal emissions for modelling purposes. Estimated annual emissions were compared against independent plant- and country-level inventories, including Carbon Monitoring for Action (CARMA), the Global Infrastructure emission Database (GID) and the Emissions Database for Global Atmospheric Research (EDGAR), as well as officially reported emission data. Overall good agreement is observed between datasets when comparing the CO2 emissions. The main discrepancies are related to the non-inclusion of auto-producer or heat-only facilities in certain countries due to a lack of data. Larger inconsistencies are obtained when comparing emissions from co-emitted species due to uncertainties in the fuel-, country- and region-dependent emission ratios and gap-filling procedures. The temporal distribution of emissions obtained in this work was compared against traditional sector-dependent profiles that are widely used in modelling efforts. This highlighted important differences and the need to consider country dependencies when temporally distributing emissions. The resulting catalogue (https://doi.org/10.24380/0a9o-v7xe, Guevara et al., 2023) is developed in the framework of the Prototype System for a Copernicus CO2 service (CoCO2) European Union (EU)-funded project to support the development of the Copernicus CO2 Monitoring and Verification Support capacity (CO2MVS).

The effects of desert dust upon climate and ecosystems depend strongly on its particle size and size-resolved mineralogical composition. However, there is very limited quantitative knowledge on the particle size and composition of the parent sediments along with their variability within dust-source regions, particularly in dust emission hotspots. The lower Drâa Valley, an inland drainage basin and dust hotspot region located in the Moroccan Sahara, was chosen for a comprehensive analysis of sediment particle size and mineralogy. Different sediment type samples (n= 42) were collected, including paleo-sediments, paved surfaces, crusts, and dunes, and analysed for particle-size distribution (minimally and fully dispersed samples) and mineralogy. Furthermore, Fe sequential wet extraction was carried out to characterise the modes of occurrence of Fe, including Fe in Fe (oxyhydr)oxides, mainly from goethite and hematite, which are key to dust radiative effects; the poorly crystalline pool of Fe (readily exchangeable ionic Fe and Fe in nano-Fe oxides), relevant to dust impacts upon ocean biogeochemistry; and structural Fe. Results yield a conceptual model where both particle size and mineralogy are segregated by transport and deposition of sediments during runoff of water across the basin and by the precipitation of salts, which causes a sedimentary fractionation. The proportion of coarser particles enriched in quartz is higher in the highlands, while that of finer particles rich in clay, carbonates, and Fe oxides is higher in the lowland dust emission hotspots. There, when water ponds and evaporates, secondary carbonates and salts precipitate, and the clays are enriched in readily exchangeable ionic Fe, due to sorption of dissolved Fe by illite. The results differ from currently available mineralogical atlases and highlight the need for observationally constrained global high-resolution mineralogical data for mineral-speciated dust modelling. The dataset obtained represents an important resource for future evaluation of surface mineralogy retrievals from spaceborne spectroscopy.

Soil dust aerosols are a key component of the climate system, as they interact with short- and long-wave radiation, alter cloud formation processes, affect atmospheric chemistry and play a role in biogeochemical cycles by providing nutrient inputs such as iron and phosphorus. The influence of dust on these processes depends on its physicochemical properties, which, far from being homogeneous, are shaped by its regionally varying mineral composition. The relative amount of minerals in dust depends on the source region and shows a large geographical variability. However, many state-of-the-art Earth system models (ESMs), upon which climate analyses and projections rely, still consider dust mineralogy to be invariant. The explicit representation of minerals in ESMs is more hindered by our limited knowledge of the global soil composition along with the resulting size-resolved airborne mineralogy than by computational constraints. In this work we introduce an explicit mineralogy representation within the state-of-the-art Multiscale Online Nonhydrostatic AtmospheRe CHemistry (MONARCH) model. We review and compare two existing soil mineralogy datasets, which remain a source of uncertainty for dust mineralogy modeling and provide an evaluation of multiannual simulations against available mineralogy observations. Soil mineralogy datasets are based on measurements performed after wet sieving, which breaks the aggregates found in the parent soil. Our model predicts the emitted particle size distribution (PSD) in terms of its constituent minerals based on brittle fragmentation theory (BFT), which reconstructs the emitted mineral aggregates destroyed by wet sieving. Our simulations broadly reproduce the most abundant mineral fractions independently of the soil composition data used. Feldspars and calcite are highly sensitive to the soil mineralogy map, mainly due to the different assumptions made in each soil dataset to extrapolate a handful of soil measurements to arid and semi-arid regions worldwide. For the least abundant or more difficult-to-determine minerals, such as iron oxides, uncertainties in soil mineralogy yield differences in annual mean aerosol mass fractions of up to ∼ 100 %. Although BFT restores coarse aggregates including phyllosilicates that usually break during soil analysis, we still identify an overestimation of coarse quartz mass fractions (above 2 µm in diameter). In a dedicated experiment, we estimate the fraction of dust with undetermined composition as given by a soil map, which makes up ∼ 10 % of the emitted dust mass at the global scale and can be regionally larger. Changes in the underlying soil mineralogy impact our estimates of climate-relevant variables, particularly affecting the regional variability of the single-scattering albedo at solar wavelengths or the total iron deposited over oceans. All in all, this assessment represents a baseline for future model experiments including new mineralogical maps constrained by high-quality spaceborne hyperspectral measurements, such as those arising from the NASA Earth Surface Mineral Dust Source Investigation (EMIT) mission.

The 2020 COVID-19 crisis caused an unprecedented drop in anthropogenic emissions of air pollutants and greenhouse gases. Given that emissions estimates from official national inventories for the year 2020 were not reported until 2 years later, new and non-traditional datasets to estimate near-real-time emissions became particularly relevant and widely used in international monitoring and modelling activities during the pandemic. This study investigates the impact of the COVID-19 pandemic on 2020 European (the 27 EU member states and the UK) emissions by comparing a selection of such near-real-time emission estimates, with the official inventories that were subsequently reported in 2022 under the Convention on Long-Range Transboundary Air Pollution (CLRTAP) and the United Nations Framework Convention on Climate Change (UNFCCC). Results indicate that annual changes in total 2020 emissions reported by official and near-real-time estimates are fairly in line for most of the chemical species, with NOx and fossil fuel CO2 being reported as the ones that experienced the largest reduction in Europe in all cases. However, large discrepancies arise between the official and non-official datasets when comparing annual results at the sector and country level, indicating that caution should be exercised when estimating changes in emissions using specific near-real-time activity datasets, such as time mobility data derived from smartphones. The main examples of these differences are observed for the manufacturing industry NOx (relative changes ranging between −21.4 % and −5.4 %) and road transport CO2 (relative changes ranging between −29.3 % and −5.6 %) total European emissions. Additionally, significant discrepancies are observed between the quarterly and monthly distribution of emissions drops reported by the various near-real-time inventories, with differences of up to a factor of 1.5 for total NOx during April 2020, when restrictions were at their maximum. For residential combustion, shipping and the public energy industry, results indicate that changes in emissions that occurred between 2019 and 2020 were mainly dominated by non-COVID-19 factors, including meteorology, the implementation of the Global Sulphur Cap and the shutdown of coal-fired power plants as part of national decarbonization efforts, respectively. The potential increase in NMVOC emissions from the intensive use of personal protective equipment such as hand sanitizer gels is considered in a heterogeneous way across countries in officially reported inventories, indicating the need for some countries to base their calculations on more advanced methods. The findings of this study can be used to better understand the uncertainties in near-real-time emissions and how such emissions could be used in the future to provide timely updates to emission datasets that are critical for modelling and monitoring applications.

The particle size distribution (PSD) of mineral dust has a strong effect on the impacts of dust on climate. However, our understanding of the emitted dust PSD, including its variability and the fraction of super-coarse dust (diameter >10 µm), remains limited. Here, we provide new insights into the size-resolved dust emission process based on a field campaign performed in the Moroccan Sahara in September 2019 in the context of the FRontiers in dust minerAloGical coMposition and its Effects upoN climaTe (FRAGMENT) project. The obtained dust concentration and diffusive flux PSDs show significant dependencies upon the friction velocity (u*), wind direction and type of event (regular events versus haboob events). For instance, the number fraction of sub-micrometre particles increases with u*, along with a large decrease in the mass fraction of super-coarse dust. We identify dry deposition, which is modulated by u* and fetch length, as a potential cause for this PSD variability. Using a resistance model constrained with field observations to estimate the dry deposition flux and thereby also the emitted dust flux, we show that deposition could represent up to ∼90 % of the emission of super-coarse particles (>10 µm) and up to ∼65 % of the emission of particles as small as ∼5 µm in diameter. Importantly, removing the deposition component significantly reduces the variability with u* in the PSD of the emitted dust flux compared with the diffusive flux, particularly for super-coarse dust. The differences between regular and haboob event concentration and diffusive flux PSDs are suspected to result from a smaller and variable dust source fetch during the haboob events, and/or an increased resistance of soil aggregates to fragmentation associated with the observed increase in relative humidity along the haboob outflow. Finally, compared to the invariant emitted dust flux PSD estimated based on brittle fragmentation theory, we obtain a substantially higher proportion of super-micrometre particles in the dust flux. Overall, our results suggest that dry deposition needs to be adequately considered to estimate the emitted PSD, even in studies limited to the fine and coarse size ranges ( µm).

Desert dust accounts for most of the atmosphere's aerosol burden by mass and produces numerous important impacts on the Earth system. However, current global climate models (GCMs) and land-surface models (LSMs) struggle to accurately represent key dust emission processes, in part because of inadequate representations of soil particle sizes that affect the dust emission threshold, surface roughness elements that absorb wind momentum, and boundary-layer characteristics that control wind fluctuations. Furthermore, because dust emission is driven by small-scale (∼ 1 km or smaller) processes, simulating the global cycle of desert dust in GCMs with coarse horizontal resolutions (∼ 100 km) presents a fundamental challenge. This representation problem is exacerbated by dust emission fluxes scaling nonlinearly with wind speed above a threshold wind speed that is sensitive to land-surface characteristics. Here, we address these fundamental problems underlying the simulation of dust emissions in GCMs and LSMs by developing improved descriptions of (1) the effect of soil texture on the dust emission threshold, (2) the effects of nonerodible roughness elements (both rocks and green vegetation) on the surface wind stress, and (3) the effects of boundary-layer turbulence on driving intermittent dust emissions. We then use the resulting revised dust emission parameterization to simulate global dust emissions in a standalone model forced by reanalysis meteorology and land-surface fields. We further propose (4) a simple methodology to rescale lower-resolution dust emission simulations to match the spatial variability of higher-resolution emission simulations in GCMs. The resulting dust emission simulation shows substantially improved agreement against regional dust emissions observationally constrained by inverse modeling. We thus find that our revised dust emission parameterization can substantially improve dust emission simulations in GCMs and LSMs.

Aerosol reanalysis datasets are model-based, observationally constrained, continuous 3D aerosol fields with a relatively high temporal frequency that can be used to assess aerosol variations and trends, climate effects, and impacts on socioeconomic sectors, such as health. Here we compare and assess the recently published MONARCH (Multiscale Online Non-hydrostatic AtmospheRe CHemistry) high-resolution regional desert dust reanalysis over northern Africa, the Middle East, and Europe (NAMEE) with a combination of ground-based observations and space-based dust retrievals and products. In particular, we compare the total and coarse dust optical depth (DOD) from the new reanalysis with DOD products derived from MODIS (MODerate resolution Imaging Spectroradiometer), MISR (Multi-angle Imaging SpectroRadiometer), and IASI (Infrared Atmospheric Sounding Interferometer) spaceborne instruments. Despite the larger uncertainties, satellite-based datasets provide a better geographical coverage than ground-based observations, and the use of different retrievals and products allows at least partially overcoming some single-product weaknesses in the comparison. Nevertheless, limitations and uncertainties due to the type of sensor, its operating principle, its sensitivity, its temporal and spatial resolution, and the methodology for retrieving or further deriving dust products are factors that bias the reanalysis assessment. We, therefore, also use ground-based DOD observations provided by 238 stations of the AERONET (AErosol RObotic NETwork) located within the NAMEE region as a reference evaluation dataset. In particular, prior to the reanalysis assessment, the satellite datasets were evaluated against AERONET, showing moderate underestimations in the vicinities of dust sources and downwind regions, whereas small or significant overestimations, depending on the dataset, can be found in the remote regions. Taking these results into consideration, the MONARCH reanalysis assessment shows that total and coarse-DOD simulations are consistent with satellite- and ground-based data, qualitatively capturing the major dust sources in the area in addition to the dust transport patterns. Moreover, the MONARCH reanalysis reproduces the seasonal dust cycle, identifying the increased dust activity that occurred in the NAMEE region during spring and summer. The quantitative comparison between the MONARCH reanalysis DOD and satellite multi-sensor products shows that the reanalysis tends to slightly overestimate the desert dust that is emitted from the source regions and underestimate the transported dust over the outflow regions, implying that the model's removal of dust particles from the atmosphere, through deposition processes, is too effective. More specifically, small positive biases are found over the Sahara desert (0.04) and negative biases over the Atlantic Ocean and the Arabian Sea (−0.04), which constitute the main pathways of the long-range dust transport. Considering the DOD values recorded on average there, such discrepancies can be considered low, as the low relative bias in the Sahara desert (< 50 %) and over the adjacent maritime regions (< 100 %) certifies. Similarly, over areas with intense dust activity, the linear correlation coefficient between the MONARCH reanalysis simulations and the ensemble of the satellite products is significantly high for both total and coarse DOD, reaching 0.8 over the Middle East, the Atlantic Ocean, and the Arabian Sea and exceeding it over the African continent. Moreover, the low relative biases and high correlations are associated with regions for which large numbers of observations are available, thus allowing for robust reanalysis assessment.

Over the last century, our societies have experienced a sharp increase in urban population and fossil-fuelled transportation, turning air pollution into a critical issue. It is therefore key to accurately characterize the spatiotemporal variability of surface air pollution in order to understand its effects upon the environment, knowledge that can then be used to design effective pollution reduction policies. Global atmospheric composition reanalyses offer great capabilities towards this characterization through assimilation of satellite measurements. However, they generally do not integrate surface measurements and thus remain affected by significant biases at ground level. In this study, we thoroughly evaluate two global atmospheric composition reanalyses, the Copernicus Atmosphere Monitoring Service (CAMSRA) and the Modern-Era Retrospective Analysis for Research and Applications v2 (MERRA-2), between 2003 and 2020, against independent surface measurements of O3, NO2, CO, SO2 and particulate matter (PM; both PM10 and PM2.5) over the European continent. Overall, both reanalyses present significant and persistent biases for almost all examined pollutants. CAMSRA clearly outperforms MERRA-2 in capturing the spatiotemporal variability of most pollutants, as shown by generally lower biases (all pollutants except for PM2.5), lower errors (all pollutants) and higher correlations (all pollutants except SO2). CAMSRA also outperforms MERRA-2 in capturing the annual trends found in all pollutants (except for SO2). Overall, CAMSRA tends to perform best for O3 and CO, followed by NO2 and PM10, while poorer results are typically found for SO2 and PM2.5. Higher correlations are generally found in autumn and/or winter for reactive gases. Compared to MERRA-2, CAMSRA assimilates a wider range of satellite products which, while enhancing the performance of the reanalysis in the troposphere (as shown by other studies), has a limited impact on the surface. The biases found in both reanalyses are likely explained by a combination of factors, including errors in emission inventories and/or sinks, a lack of surface data assimilation, and their relatively coarse resolution. Our results highlight the current limitations of reanalyses to represent surface pollution, which limits their applicability for health and environmental impact studies. When applied to reanalysis data, bias-correction methodologies based on surface observations should help to constrain the spatiotemporal variability of surface pollution and its associated impacts.

Comprehensive monitoring of NO2 exceedances is imperative for protecting human health, especially in urban areas with traffic. However, an accurate spatial characterization of the exceedances is challenging due to the typically low density of air quality monitoring stations and the inherent uncertainties in urban air quality models. We study how observational data from different sources and timescales can be combined with a dispersion air quality model to obtain bias-corrected NO2 hourly maps at the street scale. We present a kriging-based data fusion workflow that merges dispersion model output with continuous hourly observations and uses a machine-learning-based land use regression (LUR) model constrained with past short intensive passive dosimeter campaign measurements. While the hourly observations allow the bias adjustment of the temporal variability in the dispersion model, the microscale LUR model adds information on the NO2 spatial patterns. Our method includes an uncertainty calculation based on the estimated error variance of the universal kriging technique, which is subsequently used to produce urban maps of probability of exceeding the 200 µg m−3 hourly and the 40 µg m−3 annual NO2 average limits. We assess the statistical performance of this approach in the city of Barcelona for the year 2019. Our results show that simply merging the monitoring stations with the model output already significantly increases the correlation coefficient (r) by +29 % and decreases the root mean square error (RMSE) by −32 %. When adding the time-invariant microscale LUR model in the data fusion workflow, the improvement is even more remarkable, with +46 % and −48 % for the r and RMSE, respectively. Our work highlights the usefulness of high-resolution spatial information in data fusion methods to better estimate exceedances at the street scale.

In orbit since late 2017, the Tropospheric Monitoring Instrument (TROPOMI) is offering new outstanding opportunities for better understanding the emission and fate of nitrogen dioxide (NO2) pollution in the troposphere. In this study, we provide a comprehensive analysis of the spatio-temporal variability of TROPOMI NO2 tropospheric columns (TrC-NO2) over the Iberian Peninsula during 2018–2021, considering the recently developed Product Algorithm Laboratory (PAL) product. We complement our analysis with estimates of NOx anthropogenic and natural soil emissions. Closely related to cloud cover, the data availability of TROPOMI observations ranges from 30 %–45 % during April and November to 70 %–80 % during summertime, with strong variations between northern and southern Spain. Strongest TrC-NO2 hotspots are located over Madrid and Barcelona, while TrC-NO2 enhancements are also observed along international maritime routes close the strait of Gibraltar, and to a lesser extent along specific major highways. TROPOMI TrC-NO2 appear reasonably well correlated with collocated surface NO2 mixing ratios, with correlations around 0.7–0.8 depending on the averaging time. We investigate the changes of weekly and monthly variability of TROPOMI TrC-NO2 depending on the urban cover fraction. Weekly profiles show a reduction of TrC-NO2 during the weekend ranging from −10 % to −40 % from least to most urbanized areas, in reasonable agreement with surface NO2. In the largest agglomerations like Madrid or Barcelona, this weekend effect peaks not in the city center but in specific suburban areas/cities, suggesting a larger relative contribution of commuting to total NOx anthropogenic emissions. The TROPOMI TrC-NO2 monthly variability also strongly varies with the level of urbanization, with monthly differences relative to annual mean ranging from −40 % in summer to +60 % in winter in the most urbanized areas, and from −10 % to +20 % in the least urbanized areas. When focusing on agricultural areas, TROPOMI observations depict an enhancement in June–July that could come from natural soil NO emissions. Some specific analysis of surface NO2 observations in Madrid show that the relatively sharp NO2 minimum used to occur in August (drop of road transport during holidays) has now evolved into a much broader minimum partly de-coupled from the observed local road traffic counting; this change started in 2018, thus before the COVID-19 outbreak. Over 2019–2021, a reasonable consistency of the inter-annual variability of NO2 is also found between both datasets. Our study illustrates the strong potential of TROPOMI TrC-NO2 observations for complementing the existing surface NO2 monitoring stations, especially in the poorly covered rural and maritime areas where NOx can play a key role, notably for the production of tropospheric O3.

The chemical and morphological properties of mineral dust aerosols emitted by wind erosion from arid and semi-arid regions influence climate, ocean, and land ecosystems; air quality; and multiple socio-economic sectors. However, there is an incomplete understanding of the emitted dust particle size distribution (PSD) in terms of its constituent minerals that typically result from the fragmentation of soil aggregates during wind erosion. The emitted dust PSD affects the duration of particle transport and thus each mineral's global distribution, along with its specific effect upon climate. This lack of understanding is largely due to the scarcity of relevant in situ measurements in dust sources. To advance our understanding of the physicochemical properties of the emitted dust PSD, we present insights into the elemental composition and morphology of individual dust particles collected during the FRontiers in dust minerAloGical coMposition and its Effects upoN climaTe (FRAGMENT) field campaign in the Moroccan Sahara in September 2019. We analyzed more than 300 000 freshly emitted individual particles by performing offline analysis in the laboratory using scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectrometry (EDX). Eight major particle-type classes were identified with clay minerals making up the majority of the analyzed particles both by number and mass, followed by quartz, whereas carbonates and feldspar contributed to a lesser extent. We provide an exhaustive analysis of the PSD and potential mixing state of different particle types, focusing largely on iron-rich (Fe oxide-hydroxides) and feldspar particles, which are key to the effects of dust upon radiation and clouds, respectively. Nearly pure or externally mixed Fe oxide-hydroxides are present mostly in diameters smaller than 2 µm, with the highest fraction below 1 µm at about 3.75 % abundance by mass. Fe oxide-hydroxides tend to be increasingly internally mixed with other minerals, especially clays, as particle size increases; i.e., the volume fraction of Fe oxide-hydroxides in aggregates decreases with particle size. Pure (externally mixed) feldspar represented 3.2 % of all the particles by mass, of which we estimated about a 10th to be K-feldspar. The externally mixed total feldspar and K-feldspar abundances are relatively invariant with particle size, in contrast to the increasing abundance of feldspar-like (internally mixed) aggregates with particle size with mass fractions ranging from 5 % to 18 %. We also found that overall the median aspect ratio is rather constant across particle size and mineral groups, although we obtain slightly higher aspect ratios for internally mixed particles. The detailed information on the composition of freshly emitted individual dust particles and quantitative analysis of their mixing state presented here can be used to constrain climate models including mineral species in their representation of the dust cycle.

Ice-nucleating particles (INPs) enable ice formation, profoundly affecting the microphysical and radiative properties, lifetimes, and precipitation rates of clouds. Mineral dust emitted from arid regions, particularly potassium-containing feldspar (K-feldspar), has been shown to be a very effective INP through immersion freezing in mixed-phase clouds. However, despite the fact that quartz has a significantly lower ice nucleation activity, it is more abundant than K-feldspar in atmospheric desert dust and therefore may be a significant source of INPs. In this contribution, we test this hypothesis by investigating the global and regional importance of quartz as a contributor to INPs in the atmosphere relative to K-feldspar. We have extended a global 3-D chemistry transport model (TM4-ECPL) to predict INP concentrations from both K-feldspar and quartz mineral dust particles with state-of-the-art parameterizations using the ice-active surface-site approach for immersion freezing. Our results show that, although K-feldspar remains the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds, the contribution of quartz can also be significant. Quartz dominates the lowest and the highest altitudes of dust-derived INPs, affecting mainly low-level and high-level mixed-phase clouds. The consideration of quartz INPs also improves the comparison between simulations and observations at low temperatures. Our simulated INP concentrations predict ∼ 51 % of the observations gathered from different campaigns within 1 order of magnitude and ∼ 69 % within 1.5 orders of magnitude, despite the omission of other potentially important INP aerosol precursors like marine bioaerosols. Our findings support the inclusion of quartz in addition to K-feldspar as an INP in climate models and highlight the need for further constraining their abundance in arid soil surfaces along with their abundance, size distribution, and mixing state in the emitted dust atmospheric particles.

We present a European dataset of daily sector-, pollutant- and country-dependent emission adjustment factors associated with the COVID-19 mobility restrictions for the year 2020. We considered metrics traditionally used to estimate emissions, such as energy statistics or traffic counts, as well as information derived from new mobility indicators and machine learning techniques. The resulting dataset covers a total of nine emission sectors, including road transport, the energy industry, the manufacturing industry, residential and commercial combustion, aviation, shipping, off-road transport, use of solvents, and fugitive emissions from transportation and distribution of fossil fuels. The dataset was produced to be combined with the Copernicus CAMS-REG_v5.1 2020 business-as-usual (BAU) inventory, which provides high-resolution (0.1∘×0.05∘) emission estimates for 2020 omitting the impact of the COVID-19 restrictions. The combination of both datasets allows quantifying spatially and temporally resolved reductions in primary emissions from both criteria pollutants (NOx, SO2, non-methane volatile organic compounds – NMVOCs, NH3, CO, PM10 and PM2.5) and greenhouse gases (CO2 fossil fuel, CO2 biofuel and CH4), as well as assessing the contribution of each emission sector and European country to the overall emission changes. Estimated overall emission changes in 2020 relative to BAU emissions were as follows: −10.5 % for NOx (−602 kt), −7.8 % (−260.2 Mt) for CO2 from fossil fuels, −4.7 % (−808.5 kt) for CO, −4.6 % (−80 kt) for SO2, −3.3 % (−19.1 Mt) for CO2 from biofuels, −3.0 % (−56.3 kt) for PM10, −2.5 % (−173.3 kt) for NMVOCs, −2.1 % (−24.3 kt) for PM2.5, −0.9 % (−156.1 kt) for CH4 and −0.2 % (−8.6 kt) for NH3. The most pronounced drop in emissions occurred in April (up to −32.8 % on average for NOx) when mobility restrictions were at their maxima. The emission reductions during the second epidemic wave between October and December were 3 to 4 times lower than those occurred during the spring lockdown, as mobility restrictions were generally softer (e.g. curfews, limited social gatherings). Italy, France, Spain, the United Kingdom and Germany were, together, the largest contributors to the total EU27 + UK (27 member states of the European Union and the UK) absolute emission decreases. At the sectoral level, the largest emission declines were found for aviation (−51 % to −56 %), followed by road transport (−15.5 % to −18.8 %), the latter being the main driver of the estimated reductions for the majority of pollutants. The collection of COVID-19 emission adjustment factors (https://doi.org/10.24380/k966-3957, Guevara et al., 2022) and the CAMS-REG_v5.1 2020 BAU gridded inventory (https://doi.org/10.24380/eptm-kn40, Kuenen et al., 2022b) have been produced in support of air quality modelling studies.

One of the challenges in studying desert dust aerosol along with its numerous interactions and impacts is the paucity of direct in situ measurements, particularly in the areas most affected by dust storms. Satellites typically provide column-integrated aerosol measurements, but observationally constrained continuous 3D dust fields are needed to assess dust variability, climate effects and impacts upon a variety of socio-economic sectors. Here, we present a high-resolution regional reanalysis data set of desert dust aerosols that covers Northern Africa, the Middle East and Europe along with the Mediterranean Sea and parts of central Asia and the Atlantic and Indian oceans between 2007 and 2016. The horizontal resolution is 0.1∘ latitude × 0.1∘ longitude in a rotated grid, and the temporal resolution is 3 h. The reanalysis was produced using local ensemble transform Kalman filter (LETKF) data assimilation in the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (MONARCH) developed at the Barcelona Supercomputing Center (BSC). The assimilated data are coarse-mode dust optical depth retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue Level 2 products. The reanalysis data set consists of upper-air variables (dust mass concentrations and the extinction coefficient), surface variables (dust deposition and solar irradiance fields among them) and total column variables (e.g. dust optical depth and load). Some dust variables, such as concentrations and wet and dry deposition, are expressed for a binned size distribution that ranges from 0.2 to 20 µm in particle diameter. Both analysis and first-guess (analysis-initialized simulation) fields are available for the variables that are diagnosed from the state vector. A set of ensemble statistics is archived for each output variable, namely the ensemble mean, standard deviation, maximum and median. The spatial and temporal distribution of the dust fields follows well-known dust cycle features controlled by seasonal changes in meteorology and vegetation cover. The analysis is statistically closer to the assimilated retrievals than the first guess, which proves the consistency of the data assimilation method. Independent evaluation using Aerosol Robotic Network (AERONET) dust-filtered optical depth retrievals indicates that the reanalysis data set is highly accurate (mean bias = −0.05, RMSE = 0.12 and r = 0.81 when compared to retrievals from the spectral de-convolution algorithm on a 3-hourly basis). Verification statistics are broadly homogeneous in space and time with regional differences that can be partly attributed to model limitations (e.g. poor representation of small-scale emission processes), the presence of aerosols other than dust in the observations used in the evaluation and differences in the number of observations among seasons. Such a reliable high-resolution historical record of atmospheric desert dust will allow a better quantification of dust impacts upon key sectors of society and economy, including health, solar energy production and transportation. The reanalysis data set (Di Tomaso et al., 2021) is distributed via Thematic Real-time Environmental Distributed Data Services (THREDDS) at BSC and is freely available at http://hdl.handle.net/21.12146/c6d4a608-5de3-47f6-a004-67cb1d498d98 (last access: 10 June 2022).

Understanding how multiphase processes affect the iron-containing aerosol cycle is key to predicting ocean biogeochemistry changes and hence the feedback effects on climate. For this work, the EC-Earth Earth system model in its climate–chemistry configuration is used to simulate the global atmospheric oxalate (OXL), sulfate (SO42-), and iron (Fe) cycles after incorporating a comprehensive representation of the multiphase chemistry in cloud droplets and aerosol water. The model considers a detailed gas-phase chemistry scheme, all major aerosol components, and the partitioning of gases in aerosol and atmospheric water phases. The dissolution of Fe-containing aerosols accounts kinetically for the solution's acidity, oxalic acid, and irradiation. Aerosol acidity is explicitly calculated in the model, both for accumulation and coarse modes, accounting for thermodynamic processes involving inorganic and crustal species from sea salt and dust. Simulations for present-day conditions (2000–2014) have been carried out with both EC-Earth and the atmospheric composition component of the model in standalone mode driven by meteorological fields from ECMWF's ERA-Interim reanalysis. The calculated global budgets are presented and the links between the (1) aqueous-phase processes, (2) aerosol dissolution, and (3) atmospheric composition are demonstrated and quantified. The model results are supported by comparison to available observations. We obtain an average global OXL net chemical production of 12.615 ± 0.064 Tg yr−1 in EC-Earth, with glyoxal being by far the most important precursor of oxalic acid. In comparison to the ERA-Interim simulation, differences in atmospheric dynamics and the simulated weaker oxidizing capacity in EC-Earth overall result in a ∼ 30 % lower OXL source. On the other hand, the more explicit representation of the aqueous-phase chemistry in EC-Earth compared to the previous versions of the model leads to an overall ∼ 20 % higher sulfate production, but this is still well correlated with atmospheric observations. The total Fe dissolution rate in EC-Earth is calculated at 0.806 ± 0.014 Tg yr−1 and is added to the primary dissolved Fe (DFe) sources from dust and combustion aerosols in the model (0.072 ± 0.001 Tg yr−1). The simulated DFe concentrations show a satisfactory comparison with available observations, indicating an atmospheric burden of ∼0.007 Tg, resulting in an overall atmospheric deposition flux into the global ocean of 0.376 ± 0.005 Tg yr−1, which is well within the range reported in the literature. All in all, this work is a first step towards the development of EC-Earth into an Earth system model with fully interactive bioavailable atmospheric Fe inputs to the marine biogeochemistry component of the model.

Atmospheric mineral dust has a rich tri-dimensional spatial and temporal structure that is poorly constrained in forecasts and analyses when only column-integrated aerosol optical depth (AOD) is assimilated. At present, this is the case of most operational global aerosol assimilation products. Aerosol vertical distributions obtained from spaceborne lidars can be assimilated in aerosol models, but questions about the extent of their benefit upon analyses and forecasts along with their consistency with AOD assimilation remain unresolved. Our study thoroughly explores the added value of assimilating spaceborne vertical dust profiles, with and without the joint assimilation of dust optical depth (DOD). We also discuss the consistency in the assimilation of both sources of information and analyse the role of the smaller footprint of the spaceborne lidar profiles in the results. To that end, we have performed data assimilation experiments using dedicated dust observations for a period of 2 months over northern Africa, the Middle East, and Europe. We assimilate DOD derived from the Visible Infrared Imaging Radiometer Suite (VIIRS) on board Suomi National Polar-Orbiting Partnership (SUOMI-NPP) Deep Blue and for the first time Cloud-Aerosol Lidar with Orthogonal Polarisation (CALIOP)-based LIdar climatology of Vertical Aerosol Structure for space-based lidar simulation studies (LIVAS) pure-dust extinction coefficient profiles on an aerosol model. The evaluation is performed against independent ground-based DOD derived from AErosol RObotic NETwork (AERONET) Sun photometers and ground-based lidar dust extinction profiles from the Cyprus Clouds Aerosol and Rain Experiment (CyCARE) and PREparatory: does dust TriboElectrification affect our ClimaTe (Pre-TECT) field campaigns. Jointly assimilating LIVAS and Deep Blue data reduces the root mean square error (RMSE) in the DOD by 39 % and in the dust extinction coefficient by 65 % compared to a control simulation that excludes assimilation. We show that the assimilation of dust extinction coefficient profiles provides a strong added value to the analyses and forecasts. When only Deep Blue data are assimilated, the RMSE in the DOD is reduced further, by 42 %. However, when only LIVAS data are assimilated, the RMSE in the dust extinction coefficient decreases by 72 %, the largest improvement across experiments. We also show that the assimilation of dust extinction profiles yields better skill scores than the assimilation of DOD under an equivalent sensor footprint. Our results demonstrate the strong potential of future lidar space missions to improve desert dust forecasts, particularly if they foresee a depolarization lidar channel to allow discrimination of desert dust from other aerosol types.

We present the dust module in the Multiscale Online Non-hydrostatic AtmospheRe CHemistry model (MONARCH) version 2.0, a chemical weather prediction system that can be used for regional and global modeling at a range of resolutions. The representations of dust processes in MONARCH were upgraded with a focus on dust emission (emission parameterizations, entrainment thresholds, considerations of soil moisture and surface cover), lower boundary conditions (roughness, potential dust sources), and dust–radiation interactions. MONARCH now allows modeling of global and regional mineral dust cycles using fundamentally different paradigms, ranging from strongly simplified to physics-based parameterizations. We present a detailed description of these updates along with four global benchmark simulations, which use conceptually different dust emission parameterizations, and we evaluate the simulations against observations of dust optical depth. We determine key dust parameters, such as global annual emission/deposition flux, dust loading, dust optical depth, mass-extinction efficiency, single-scattering albedo, and direct radiative effects. For dust-particle diameters up to 20 µm, the total annual dust emission and deposition fluxes obtained with our four experiments range between about 3500 and 6000 Tg, which largely depend upon differences in the emitted size distribution. Considering ellipsoidal particle shapes and dust refractive indices that account for size-resolved mineralogy, we estimate the global total (longwave and shortwave) dust direct radiative effect (DRE) at the surface to range between about −0.90 and −0.63 W m−2 and at the top of the atmosphere between −0.20 and −0.28 W m−2. Our evaluation demonstrates that MONARCH is able to reproduce key features of the spatiotemporal variability of the global dust cycle with important and insightful differences between the different configurations.

This paper documents the global climate model EC-Earth3-AerChem, one of the members of the EC-Earth3 family of models participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). EC-Earth3-AerChem has interactive aerosols and atmospheric chemistry and contributes to the Aerosols and Chemistry Model Intercomparison Project (AerChemMIP). In this paper, we give an overview of the model, describe in detail how it differs from the other EC-Earth3 configurations, and outline the new features compared with the previously documented version of the model (EC-Earth 2.4). We explain how the model was tuned and spun up under preindustrial conditions and characterize the model's general performance on the basis of a selection of coupled simulations conducted for CMIP6. The net energy imbalance at the top of the atmosphere in the preindustrial control simulation is on average −0.09 W m−2 with a standard deviation due to interannual variability of 0.25 W m−2, showing no significant drift. The global surface air temperature in the simulation is on average 14.08 ∘C with an interannual standard deviation of 0.17 ∘C, exhibiting a small drift of 0.015 ± 0.005 ∘C per century. The model's effective equilibrium climate sensitivity is estimated at 3.9 ∘C, and its transient climate response is estimated at 2.1 ∘C. The CMIP6 historical simulation displays spurious interdecadal variability in Northern Hemisphere temperatures, resulting in a large spread across ensemble members and a tendency to underestimate observed annual surface temperature anomalies from the early 20th century onwards. The observed warming of the Southern Hemisphere is well reproduced by the model. Compared with the ECMWF (European Centre for Medium-Range Weather Forecasts) Reanalysis version 5 (ERA5), the surface air temperature climatology for 1995–2014 has an average bias of −0.86 ± 0.05 ∘C with a standard deviation across ensemble members of 0.35 ∘C in the Northern Hemisphere and 1.29 ± 0.02 ∘C with a corresponding standard deviation of 0.05 ∘C in the Southern Hemisphere. The Southern Hemisphere warm bias is largely caused by errors in shortwave cloud radiative effects over the Southern Ocean, a deficiency of many climate models. Changes in the emissions of near-term climate forcers (NTCFs) have significant effects on the global climate from the second half of the 20th century onwards. For the SSP3-7.0 Shared Socioeconomic Pathway, the model gives a global warming at the end of the 21st century (2091–2100) of 4.9 ∘C above the preindustrial mean. A 0.5 ∘C stronger warming is obtained for the AerChemMIP scenario with reduced emissions of NTCFs. With concurrent reductions of future methane concentrations, the warming is projected to be reduced by 0.5 ∘C.

This study provides a comprehensive assessment of NO2 changes across the main European urban areas induced by COVID-19 lockdowns using satellite retrievals from the Tropospheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5p satellite, surface site measurements, and simulations from the Copernicus Atmosphere Monitoring Service (CAMS) regional ensemble of air quality models. Some recent TROPOMI-based estimates of changes in atmospheric NO2 concentrations have neglected the influence of weather variability between the reference and lockdown periods. Here we provide weather-normalized estimates based on a machine learning method (gradient boosting) along with an assessment of the biases that can be expected from methods that omit the influence of weather. We also compare the weather-normalized satellite-estimated NO2 column changes with weather-normalized surface NO2 concentration changes and the CAMS regional ensemble, composed of 11 models, using recently published estimates of emission reductions induced by the lockdown. All estimates show similar NO2 reductions. Locations where the lockdown measures were stricter show stronger reductions, and, conversely, locations where softer measures were implemented show milder reductions in NO2 pollution levels. Average reduction estimates based on either satellite observations (−23 %), surface stations (−43 %), or models (−32 %) are presented, showing the importance of vertical sampling but also the horizontal representativeness. Surface station estimates are significantly changed when sampled to the TROPOMI overpasses (−37 %), pointing out the importance of the variability in time of such estimates. Observation-based machine learning estimates show a stronger temporal variability than model-based estimates.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, atmospheric models struggle to accurately represent its spatial and temporal distribution. These model errors are partially caused by fundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of 2 relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global basis, we find that the emission flux of dust with a geometric diameter up to 20 µm (PM20) is approximately 5000 Tg yr−1, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded datasets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this dataset is more accurate than current model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world's major source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world's main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global aerosol model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth (DAOD). We obtain a dataset that constrains the relative contribution of nine major source regions to size-resolved dust emission, atmospheric loading, DAOD, concentration, and deposition flux. We find that the 22–29 Tg (1 standard error range) global loading of dust with a geometric diameter up to 20 µm is partitioned as follows: North African source regions contribute ∼ 50 % (11–15 Tg), Asian source regions contribute ∼ 40 % (8–13 Tg), and North American and Southern Hemisphere regions contribute ∼ 10 % (1.8–3.2 Tg). These results suggest that current models on average overestimate the contribution of North African sources to atmospheric dust loading at ∼ 65 %, while underestimating the contribution of Asian dust at ∼ 30 %. Our results further show that each source region's dust loading peaks in local spring and summer, which is partially driven by increased dust lifetime in those seasons. We also quantify the dust deposition flux to the Amazon rainforest to be ∼ 10 Tg yr−1, which is a factor of 2–3 less than inferred from satellite data by previous work that likely overestimated dust deposition by underestimating the dust mass extinction efficiency. The data obtained in this paper can be used to obtain improved constraints on dust impacts on clouds, climate, biogeochemical cycles, and other parts of the Earth system.

The large uncertainty in the mineral dust direct radiative effect (DRE) hinders projections of future climate change due to anthropogenic activity. Resolving modeled dust mineral speciation allows for spatially and temporally varying refractive indices consistent with dust aerosol composition. Here, for the first time, we quantify the range in dust DRE at the top of the atmosphere (TOA) due to current uncertainties in the surface soil mineralogical content using a dust mineral-resolving climate model. We propagate observed uncertainties in soil mineral abundances from two soil mineralogy atlases along with the optical properties of each mineral into the DRE and compare the resultant range with other sources of uncertainty across six climate models. The shortwave DRE responds region-specifically to the dust burden depending on the mineral speciation and underlying shortwave surface albedo: positively when the regionally averaged annual surface albedo is larger than 0.28 and negatively otherwise. Among all minerals examined, the shortwave TOA DRE and single scattering albedo at the 0.44–0.63 µm band are most sensitive to the fractional contribution of iron oxides to the total dust composition. The global net (shortwave plus longwave) TOA DRE is estimated to be within −0.23 to +0.35 W m−2. Approximately 97 % of this range relates to uncertainty in the soil abundance of iron oxides. Representing iron oxide with solely hematite optical properties leads to an overestimation of shortwave DRE by +0.10 W m−2 at the TOA, as goethite is not as absorbing as hematite in the shortwave spectrum range. Our study highlights the importance of iron oxides to the shortwave DRE: they have a disproportionally large impact on climate considering their small atmospheric mineral mass fractional burden (∼2 %). An improved description of iron oxides, such as those planned in the Earth Surface Mineral Dust Source Investigation (EMIT), is thus essential for more accurate estimates of the dust DRE.

We present the Copernicus Atmosphere Monitoring Service TEMPOral profiles (CAMS-TEMPO), a dataset of global and European emission temporal profiles that provides gridded monthly, daily, weekly and hourly weight factors for atmospheric chemistry modelling. CAMS-TEMPO includes temporal profiles for the priority air pollutants (NOx; SOx; NMVOC, non-methane volatile organic compound; NH3; CO; PM10; and PM2.5) and the greenhouse gases (CO2 and CH4) for each of the following anthropogenic source categories: energy industry (power plants), residential combustion, manufacturing industry, transport (road traffic and air traffic in airports) and agricultural activities (fertilizer use and livestock). The profiles are computed on a global 0.1 × 0.1∘ and regional European 0.1 × 0.05∘ grid following the domain and sector classification descriptions of the global and regional emission inventories developed under the CAMS programme. The profiles account for the variability of the main emission drivers of each sector. Statistical information linked to emission variability (e.g. electricity production and traffic counts) at national and local levels were collected and combined with existing meteorology-dependent parametrizations to account for the influences of sociodemographic factors and climatological conditions. Depending on the sector and the temporal resolution (i.e. monthly, weekly, daily and hourly) the resulting profiles are pollutant-dependent, year-dependent (i.e. time series from 2010 to 2017) and/or spatially dependent (i.e. the temporal weights vary per country or region). We provide a complete description of the data and methods used to build the CAMS-TEMPO profiles, and whenever possible, we evaluate the representativeness of the proxies used to compute the temporal weights against existing observational data. We find important discrepancies when comparing the obtained temporal weights with other currently used datasets. The CAMS-TEMPO data product including the global (CAMS-GLOB-TEMPOv2.1, https://doi.org/10.24380/ks45-9147, Guevara et al., 2020a) and regional European (CAMS-REG-TEMPOv2.1, https://doi.org/10.24380/1cx4-zy68, Guevara et al., 2020b) temporal profiles are distributed from the Emissions of atmospheric Compounds and Compilation of Ancillary Data (ECCAD) system (https://eccad.aeris-data.fr/, last access: February 2021).

Monitoring and describing the spatiotemporal variability in dust aerosols is crucial for understanding their multiple effects, related feedbacks, and impacts within the Earth system. This study describes the development of the ModIs Dust AeroSol (MIDAS) data set. MIDAS provides columnar daily dust optical depth (DOD) at 550 nm at a global scale and fine spatial resolution (0.1∘ × 0.1∘) over a 15-year period (2003–2017). This new data set combines quality filtered satellite aerosol optical depth (AOD) retrievals from MODIS-Aqua at swath level (Collection 6.1; Level 2), along with DOD-to-AOD ratios provided by the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) reanalysis to derive DOD on the MODIS native grid. The uncertainties of the MODIS AOD and MERRA-2 dust fraction, with respect to the AEronet RObotic NETwork (AERONET) and LIdar climatology of vertical Aerosol Structure for space-based lidar simulation (LIVAS), respectively, are taken into account for the estimation of the total DOD uncertainty. MERRA-2 dust fractions are in very good agreement with those of LIVAS across the dust belt in the tropical Atlantic Ocean and the Arabian Sea; the agreement degrades in North America and the Southern Hemisphere, where dust sources are smaller. MIDAS, MERRA-2, and LIVAS DODs strongly agree when it comes to annual and seasonal spatial patterns, with colocated global DOD averages of 0.033, 0.031, and 0.029, respectively; however, deviations in dust loading are evident and regionally dependent. Overall, MIDAS is well correlated with AERONET-derived DODs (R=0.89) and only shows a small positive bias (0.004 or 2.7 %). Among the major dust areas of the planet, the highest R values (>0.9) are found at sites of North Africa, the Middle East, and Asia. MIDAS expands, complements, and upgrades the existing observational capabilities of dust aerosols, and it is suitable for dust climatological studies, model evaluation, and data assimilation.

We quantify the reductions in primary emissions due to the COVID-19 lockdowns in Europe. Our estimates are provided in the form of a dataset of reduction factors varying per country and day that will allow the modelling and identification of the associated impacts upon air quality. The country- and daily-resolved reduction factors are provided for each of the following source categories: energy industry (power plants), manufacturing industry, road traffic and aviation (landing and take-off cycle). We computed the reduction factors based on open-access and near-real-time measured activity data from a wide range of information sources. We also trained a machine learning model with meteorological data to derive weather-normalized electricity consumption reductions. The time period covered is from 21 February, when the first European localized lockdown was implemented in the region of Lombardy (Italy), until 26 April 2020. This period includes 5 weeks (23 March until 26 April) with the most severe and relatively unchanged restrictions upon mobility and socio-economic activities across Europe. The computed reduction factors were combined with the Copernicus Atmosphere Monitoring Service's European emission inventory using adjusted temporal emission profiles in order to derive time-resolved emission reductions per country and pollutant sector. During the most severe lockdown period, we estimate the average emission reductions to be −33 % for NOx, −8 % for non-methane volatile organic compounds (NMVOCs), −7 % for SOx and −7 % for PM2.5 at the EU-30 level (EU-28 plus Norway and Switzerland). For all pollutants more than 85 % of the total reduction is attributable to road transport, except SOx. The reductions reached −50 % (NOx), −14 % (NMVOCs), −12 % (SOx) and −15 % (PM2.5) in countries where the lockdown restrictions were more severe such as Italy, France or Spain. To show the potential for air quality modelling, we simulated and evaluated NO2 concentration decreases in rural and urban background regions across Europe (Italy, Spain, France, Germany, United-Kingdom and Sweden). We found the lockdown measures to be responsible for NO2 reductions of up to −58 % at urban background locations (Madrid, Spain) and −44 % at rural background areas (France), with an average contribution of the traffic sector to total reductions of 86 % and 93 %, respectively. A clear improvement of the modelled results was found when considering the emission reduction factors, especially in Madrid, Paris and London where the bias is reduced by more than 90 %. Future updates will include the extension of the COVID-19 lockdown period covered, the addition of other pollutant sectors potentially affected by the restrictions (commercial and residential combustion and shipping) and the evaluation of other air quality pollutants such as O3 and PM2.5. All the emission reduction factors are provided in the Supplement.

The spread of the new coronavirus SARS-CoV-2 that causes COVID-19 forced the Spanish Government to implement extensive lockdown measures to reduce the number of hospital admissions, starting on 14 March 2020. Over the following days and weeks, strong reductions in nitrogen dioxide (NO2) pollution were reported in many regions of Spain. A substantial part of these reductions was obviously due to decreased local and regional anthropogenic emissions. Yet, the confounding effect of meteorological variability hinders a reliable quantification of the lockdown's impact upon the observed pollution levels. Our study uses machine-learning (ML) models fed by meteorological data along with other time features to estimate the “business-as-usual” NO2 mixing ratios that would have been observed in the absence of the lockdown. We then quantify the so-called meteorology-normalized NO2 reductions induced by the lockdown measures by comparing the estimated business-as-usual values with the observed NO2 mixing ratios. We applied this analysis for a selection of urban background and traffic stations covering the more than 50 Spanish provinces and islands. The ML predictive models were found to perform remarkably well in most locations, with an overall bias, root mean square error and correlation of +4 %, 29 % and 0.86, respectively. During the period of study, from the enforcement of the state of alarm in Spain on 14 March to 23 April, we found the lockdown measures to be responsible for a 50 % reduction in NO2 levels on average over all provinces and islands. The lockdown in Spain has gone through several phases with different levels of severity with respect to mobility restrictions. As expected, the meteorology-normalized change in NO2 was found to be stronger during phase II (the most stringent phase) and phase III of the lockdown than during phase I. In the largest agglomerations, where both urban background and traffic stations were available, a stronger meteorology-normalized NO2 change is highlighted at traffic stations compared with urban background sites. Our results are consistent with foreseen (although still uncertain) changes in anthropogenic emissions induced by the lockdown. We also show the importance of taking the meteorological variability into account for accurately assessing the impact of the lockdown on NO2 levels, in particular at fine spatial and temporal scales. Meteorology-normalized estimates such as those presented here are crucial to reliably quantify the health implications of the lockdown due to reduced air pollution.

We describe the bottom–up module of the High-Elective Resolution Modelling Emission System version 3 (HERMESv3), a Python-based and multi-scale modelling tool intended for the processing and computation of atmospheric emissions for air quality modelling. HERMESv3 is composed of two separate modules: the global_regional module and the bottom_up module. In a companion paper (Part 1, Guevara et al., 2019a) we presented the global_regional module. The bottom_up module described in this contribution is an emission model that estimates anthropogenic emissions at high spatial- (e.g. road link level,) and temporal- (hourly) resolution using state-of-the-art calculation methods that combine local activity and emission factors along with meteorological data. The model computes bottom–up emissions from point sources, road transport, residential and commercial combustion, other mobile sources, and agricultural activities. The computed pollutants include the main criteria pollutants (i.e. NOx, CO, NMVOCs (non-methane volatile organic compounds), SOx, NH3, PM10 and PM2.5) and greenhouse gases (i.e. CO2 and CH4, only related to combustion processes). Specific emission estimation methodologies are provided for each source and are mostly based on (but not limited to) the calculation methodologies reported by the European EMEP/EEA air pollutant emission inventory guidebook. Meteorologically dependent functions are also included to take into account the dynamical component of the emission processes. The model also provides several functionalities for automatically manipulating and performing spatial operations on georeferenced objects (shapefiles and raster files). The model is designed so that it can be applicable to any European country or region where the required input data are available. As in the case of the global_regional module, emissions can be estimated on several user-defined grids, mapped to multiple chemical mechanisms and adapted to the input requirements of different atmospheric chemistry models (CMAQ, WRF-Chem and MONARCH) as well as a street-level dispersion model (R-LINE). Specific emission outputs generated by the model are presented and discussed to illustrate its capabilities.

Dust emission is initiated when surface wind velocities exceed the threshold of wind erosion. Many dust models used constant threshold values globally. Here we use satellite products to characterize the frequency of dust events and land surface properties. By matching this frequency derived from Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue aerosol products with surface winds, we are able to retrieve a climatological monthly global distribution of the wind erosion threshold (Vthreshold) over dry and sparsely vegetated surfaces. This monthly two-dimensional threshold velocity is then implemented into the Geophysical Fluid Dynamics Laboratory coupled land–atmosphere model (AM4.0/LM4.0). It is found that the climatology of dust optical depth (DOD) and total aerosol optical depth, surface PM10 dust concentrations, and the seasonal cycle of DOD are better captured over the “dust belt” (i.e., northern Africa and the Middle East) by simulations with the new wind erosion threshold than those using the default globally constant threshold. The most significant improvement is the frequency distribution of dust events, which is generally ignored in model evaluation. By using monthly rather than annual mean Vthreshold, all comparisons with observations are further improved. The monthly global threshold of wind erosion can be retrieved under different spatial resolutions to match the resolution of dust models and thus can help improve the simulations of dust climatology and seasonal cycles as well as dust forecasting.

The NO2 annual air quality limit value is systematically exceeded in many European cities. In this context, understanding human exposure, improving policy and planning, and providing forecasts requires the development of accurate air quality models at the urban (street level) scale. We describe CALIOPE-Urban, a system coupling CALIOPE – an operational mesoscale air quality forecast system based on the HERMES (emissions), WRF (meteorology) and CMAQ (chemistry) models – with the urban roadway dispersion model R-LINE. Our developments have focused on Barcelona city (Spain), but the methodology may be replicated for other cities in the future. WRF drives pollutant dispersion and CMAQ provides background concentrations to R-LINE. Key features of our system include the adaptation of R-LINE to street canyons, the use of a new methodology that considers upwind grid cells in CMAQ to avoid double counting traffic emissions, a new method to estimate local surface roughness within street canyons, and a vertical mixing parameterisation that considers urban geometry and atmospheric stability to calculate surface level background concentrations. We show that the latter is critical to correct the night-time overestimations in our system. Both CALIOPE and CALIOPE-Urban are evaluated using two sets of observations. The temporal variability is evaluated against measurements from five traffic sites and one urban background site for April–May 2013. While both systems show a fairly good agreement at the urban background site, CALIOPE-Urban shows a better agreement at traffic sites. The spatial variability is evaluated using 182 passive dosimeters that were distributed across Barcelona during 2 weeks for February–March 2017. In this case, the coupled system also shows a more realistic distribution than the mesoscale system, which systematically underpredicts NO2 close to traffic emission sources. Overall CALIOPE-Urban improves mesoscale model results, demonstrating that the combination of both scales provides a more realistic representation of NO2 spatio-temporal variability in Barcelona.

We present the High-Elective Resolution Modelling Emission System version 3 (HERMESv3), an open source, parallel and stand-alone multi-scale atmospheric emission modelling framework that computes gaseous and aerosol emissions for use in atmospheric chemistry models. HERMESv3 is coded in Python and consists of a global_regional module and a bottom_up module that can be either combined or executed separately. In this contribution (Part 1) we describe the global_regional module, a customizable emission processing system that calculates emissions from different sources, regions and pollutants on a user-specified global or regional grid. The user can flexibly define combinations of existing up-to-date global and regional emission inventories and apply country-specific scaling factors and masks. Each emission inventory is individually processed using user-defined vertical, temporal and speciation profiles that allow obtaining emission outputs compatible with multiple chemical mechanisms (e.g. Carbon-Bond 05). The selection and combination of emission inventories and databases is done through detailed configuration files providing the user with a widely applicable framework for designing, choosing and adjusting the emission modelling experiment without modifying the HERMESv3 source code. The generated emission fields have been successfully tested in different atmospheric chemistry models (i.e. CMAQ, WRF-Chem and NMMB-MONARCH) at multiple spatial and temporal resolutions. In a companion article (Part 2; Guevara et al., 2019) we describe the bottom_up module, which estimates emissions at the source level (e.g. road link) combining state-of-the-art bottom–up methods with local activity and emission factors.

It is well established that in Europe, high O3 concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to O3 formation within each country relative to the imported (regional and hemispheric) O3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the O3 target value set by the European air quality directive. O3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O3 and precursors from neighbouring regions, O3 regional and hemispheric transport and stratospheric O3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O3 events in Spain relative to the contribution of imported (regional and hemispheric) O3. We also assess the potential of our source apportionment method to improve O3 modelling. Our study applies and thoroughly evaluates a countrywide O3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4 km2) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O3 and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NOx local sources to high O3 concentrations compared with the contribution of imported O3. We show, for the first time, that imported O3 is the largest input to the ground-level O3 concentration in the IP, accounting for 46 %–68 % of the daily mean O3 concentration during exceedances of the European target value. The hourly imported O3 increases during typical northwestern advections (70 %–90 %, 60–80 µg m−3), and decreases during typical stagnant conditions (30 %–40 %, 30–60 µg m−3) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the O3 peaks in areas downwind of the main urban and industrial regions (up to 40 % in hourly peaks). We also show that ground-level O3 concentrations are strongly affected by vertical mixing of O3-rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported O3 at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high O3 concentrations for local O3 management, and show O3 source apportionment to be an essential analysis prior to the design of O3 mitigation plans in any non-attainment area. Achieving the European O3 objectives in southern Europe requires not only ad hoc local actions but also decided national and European-wide strategies.

The direct radiative effect (DRE) during 20 intense and widespread dust outbreaks, which affected the broader Mediterranean basin over the period March 2000–February 2013, has been calculated with the NMMB-MONARCH model at regional (Sahara and European continent) and short-term temporal (84 h) scales. According to model simulations, the maximum dust aerosol optical depths (AODs) range from ∼ 2.5 to ∼ 5.5 among the identified cases. At midday, dust outbreaks locally induce a NET (shortwave plus longwave) strong atmospheric warming (DREATM values up to 285 W m−2; Niger–Chad; dust AODs up to ∼ 5.5) and a strong surface cooling (DRENETSURF values down to −337 W m−2), whereas they strongly reduce the downward radiation at the ground level (DRESURF values down to −589 W m−2 over the Eastern Mediterranean, for extremely high dust AODs, 4.5–5). During night-time, reverse effects of smaller magnitude are found. At the top of the atmosphere (TOA), positive (planetary warming) DREs up to 85 W m−2 are found over highly reflective surfaces (Niger–Chad; dust AODs up to ∼ 5.5) while negative (planetary cooling) DREs down to −184 W m−2 (Eastern Mediterranean; dust AODs 4.5–5) are computed over dark surfaces at noon. Dust outbreaks significantly affect the mean regional radiation budget, with NET DREs ranging from −8.5 to 0.5 W m−2, from −31.6 to 2.1 W m−2, from −22.2 to 2.2 W m−2 and from −1.7 to 20.4 W m−2 for TOA, SURF, NETSURF and ATM, respectively. Although the shortwave DREs are larger than the longwave ones, the latter are comparable or even larger at TOA, particularly over the Sahara at midday. As a response to the strong surface day-time cooling, dust outbreaks cause a reduction in the regional sensible and latent heat fluxes by up to 45 and 4 W m−2, respectively, averaged over land areas of the simulation domain. Dust outbreaks reduce the temperature at 2 m by up to 4 K during day-time, whereas a reverse tendency of similar magnitude is found during night-time. Depending on the vertical distribution of dust loads and time, mineral particles heat (cool) the atmosphere by up to 0.9 K (0.8 K) during day-time (night-time) within atmospheric dust layers. Beneath and above the dust clouds, mineral particles cool (warm) the atmosphere by up to 1.3 K (1.2 K) at noon (night-time). On a regional mean basis, negative feedbacks on the total emitted dust (reduced by 19.5 %) and dust AOD (reduced by 6.9 %) are found when dust interacts with the radiation. Through the consideration of dust radiative effects in numerical simulations, the model positive and negative biases for the downward surface SW or LW radiation, respectively, with respect to Baseline Surface Radiation Network (BSRN) measurements, are reduced. In addition, they also reduce the model near-surface (at 2 m) nocturnal cold biases by up to 0.5 K (regional averages), as well as the model warm biases at 950 and 700 hPa, where the dust concentration is maximized, by up to 0.4 K. However, improvements are relatively small and do not happen in all episodes because other model first-order errors may dominate over the expected improvements, and the misrepresentation of the dust plumes' spatiotemporal features and optical properties may even produce a double penalty effect. The enhancement of dust forecasts via data assimilation techniques may significantly improve the results.

A data assimilation capability has been built for the NMMB-MONARCH chemical weather prediction system, with a focus on mineral dust, a prominent type of aerosol. An ensemble-based Kalman filter technique (namely the local ensemble transform Kalman filter – LETKF) has been utilized to optimally combine model background and satellite retrievals. Our implementation of the ensemble is based on known uncertainties in the physical parametrizations of the dust emission scheme. Experiments showed that MODIS AOD retrievals using the Dark Target algorithm can help NMMB-MONARCH to better characterize atmospheric dust. This is particularly true for the analysis of the dust outflow in the Sahel region and over the African Atlantic coast. The assimilation of MODIS AOD retrievals based on the Deep Blue algorithm has a further positive impact in the analysis downwind from the strongest dust sources of the Sahara and in the Arabian Peninsula. An analysis-initialized forecast performs better (lower forecast error and higher correlation with observations) than a standard forecast, with the exception of underestimating dust in the long-range Atlantic transport and degradation of the temporal evolution of dust in some regions after day 1. Particularly relevant is the improved forecast over the Sahara throughout the forecast range thanks to the assimilation of Deep Blue retrievals over areas not easily covered by other observational datasets. The present study on mineral dust is a first step towards data assimilation with a complete aerosol prediction system that includes multiple aerosol species.

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT). We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3–0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error – RMSE – below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability). The resulting ozone (O3) burden (348 Tg) lies within the range of other state-of-the-art global atmospheric chemistry models. The model generally captures the spatial and seasonal trends of background surface O3 and its vertical distribution. However, the model tends to overestimate O3 throughout the troposphere in several stations. This may be attributed to an overestimation of CO concentration over the Southern Hemisphere leading to an excessive production of O3 or to the lack of specific chemistry (e.g., halogen chemistry, aerosol chemistry). Overall, O3 correlations range between 0.6 and 0.8 for daily mean values. The overall performance of the NMMB-MONARCH is comparable to that of other state-of-the-art global chemistry models.

We review the major features of desert dust outbreaks that are relevant to the assessment of dust impacts upon human health. Our ultimate goal is to provide scientific guidance for the acquisition of relevant population exposure information for epidemiological studies tackling the short and long term health effects of desert dust. We first describe the source regions and the typical levels of dust particles in regions close and far away from the source areas, along with their size, composition, and bio-aerosol load. We then describe the processes by which dust may become mixed with anthropogenic particulate matter (PM) and/or alter its load in receptor areas. Short term health effects are found during desert dust episodes in different regions of the world, but in a number of cases the results differ when it comes to associate the effects to the bulk PM, the desert dust-PM, or non-desert dust-PM. These differences are likely due to the different monitoring strategies applied in the epidemiological studies, and to the differences on atmospheric and emission (natural and anthropogenic) patterns of desert dust around the world. We finally propose methods to allow the discrimination of health effects by PM fraction during dust outbreaks, and a strategy to implement desert dust alert and monitoring systems for health studies and air quality management. Keywords: Mineral dust, Atmospheric particulate matter, Aerosols, Epidemiology, Natural and anthropogenic contributions

In the framework of the World Meteorological Organisation's Sand and Dust Storm Warning Advisory and Assessment System, we evaluated the predictions of five state-of-the-art dust forecast models during an intense Saharan dust outbreak affecting western and northern Europe in April 2011. We assessed the capacity of the models to predict the evolution of the dust cloud with lead times of up to 72 h using observations of aerosol optical depth (AOD) from the AErosol RObotic NETwork (AERONET) and the Moderate Resolution Imaging Spectroradiometer (MODIS) and dust surface concentrations from a ground-based measurement network. In addition, the predicted vertical dust distribution was evaluated with vertical extinction profiles from the Cloud and Aerosol Lidar with Orthogonal Polarization (CALIOP). To assess the diversity in forecast capability among the models, the analysis was extended to wind field (both surface and profile), synoptic conditions, emissions and deposition fluxes. Models predict the onset and evolution of the AOD for all analysed lead times. On average, differences among the models are larger than differences among lead times for each individual model. In spite of large differences in emission and deposition, the models present comparable skill for AOD. In general, models are better in predicting AOD than near-surface dust concentration over the Iberian Peninsula. Models tend to underestimate the long-range transport towards northern Europe. Our analysis suggests that this is partly due to difficulties in simulating the vertical distribution dust and horizontal wind. Differences in the size distribution and wet scavenging efficiency may also account for model diversity in long-range transport.

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the model extensions result in better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

One of the major sources of uncertainty in model estimates of the global sea-salt aerosol distribution is the emission parameterization. We evaluate a new sea-salt aerosol life cycle module coupled to the online multiscale chemical transport model NMMB/BSC-CTM. We compare 5 yr global simulations using five state-of-the-art sea-salt open-ocean emission schemes with monthly averaged coarse aerosol optical depth (AOD) from selected AERONET sun photometers, surface concentration measurements from the University of Miami's Ocean Aerosol Network, and measurements from two NOAA/PMEL cruises (AEROINDOEX and ACE1). Model results are highly sensitive to the introduction of sea-surface-temperature (SST)-dependent emissions and to the accounting of spume particles production. Emission ranges from 3888 Tg yr−1 to 8114 Tg yr−1, lifetime varies between 7.3 h and 11.3 h, and the average column mass load is between 5.0 Tg and 7.2 Tg. Coarse AOD is reproduced with an overall correlation of around 0.5 and with normalized biases ranging from +8.8% to +38.8%. Surface concentration is simulated with normalized biases ranging from −9.5% to +28% and the overall correlation is around 0.5. Our results indicate that SST-dependent emission schemes improve the overall model performance in reproducing surface concentrations. On the other hand, they lead to an overestimation of the coarse AOD at tropical latitudes, although it may be affected by uncertainties in the comparison due to the use of all-sky model AOD, the treatment of water uptake, deposition and optical properties in the model and/or an inaccurate size distribution at emission.

No abstract available.