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Mineral dust interacts with incoming/outgoing electromagnetic radiation in the atmosphere. This interaction depends on the microphysical properties of the dust particles, including size, mineral composition, external morphology, and internal structure. Ideally all these properties should be accounted for in dust remote sensing, the modeling of single-scattering properties, and radiative effect assessment. There have been many reports on the microphysical characterizations of mineral dust, but no investigations of the internal structures or mineral composition of individual dust particles. We explored the interiors of Asian dust particles using the combined application of focused ion beam thin-slice preparation and high-resolution transmission electron microscopy. The results showed that individual dust particles consisted of numerous mineral grains, which were organized into several types of internal structure: single and polycrystalline cores of quartz, feldspars, calcite, and amphibole often with oriented clay coatings; individual clay agglomerates of nano-thin clay platelets showing preferred to random orientations commonly with coarser mineral inclusions; and platy coarse phyllosilicates (muscovite, biotite, and chlorite). Micron to submicron pores were scattered throughout the interior of particles. Clays in the coatings and agglomerates were dominated by nano-thin platelets of the clay minerals of illite-smectite series including illite, smectite, and their mixed layers with subordinate kaolinite and clay-size chlorite. Submicron iron oxide grains, dominantly goethite, were distributed throughout the clay agglomerates and coatings. Unlike the common assumptions and simplifications, we found that the analyzed dust particles were irregularly shaped with birefringent, polycrystalline, and polymineralic heterogeneous compositions. Accounting for this structural and mineralogical makeup may improve the remote sensing retrieval of dust and the evaluation of radiation effects, but will also require sophisticated single-scattering modeling. In particular, the observed internal structures of dust particles such as clay coatings, preferred orientation, embedded grains in clays, and pores, likely have a great impact on the light scattering of dust particles. The distribution and size of structural components with contrasting dielectric properties, such as iron oxides, should also be explicitly accounted for. [ABSTRACT FROM AUTHOR]

The occurrence of African dust outbreaks over the western Mediterranean basin were identified on an 11 year period (2001-2011). PM10 daily data from nine regional background air quality monitoring sites across the study area were compiled and the net dust load transported during each event was estimated. Then, the main atmospheric circulation patterns causing the transport of African air masses, were characterized by mean of an objective classification methodology of atmospheric variables fields. Next, the potential source areas of mineral dust, associated to each circulation pattern were identified by trajectory statistical methods. Finally, an impact index was calculated to 10 estimate the incidence of the African dust outbreaks produced during each circulation pattern, on the levels of dust load in PM10 concentrations recorded in the different regions. Our results indicate that the values of the impact index and the areas affected by African dust, strongly depended on the atmospheric circulation pattern. Four circulation types were obtained by the classification procedure. Two of them (CT-1 and CT-4) occurred predominantly during the warm season, bringing dust from areas of Algeria, Tunisia, Western Sahara, western Libya and Mauritania. African dust outbreaks produced during the CT-4 were the most frequent across the period of study, generating the highest impact index over southern, central and eastern regions of the Iberian Peninsula as well as over the Balearic Islands. Conversely, the events caused by the CT-1 encompassed the highest impact index over the western areas of the Iberian Peninsula. The two remaining circulation types (CT-2 and CT-3) were more frequently observed during the spring season. The prevailing flows generated by these two atmospheric circulation patterns, carried mineral dust from areas of Algeria, Tunisia and Western Sahara, giving rise to higher values of the impact index from eastern to western areas of the western Mediterranean basin. [ABSTRACT FROM AUTHOR]

The predictions of two road dust suspension emission models were compared with the on-site mobile measurements of suspension emission factors. Such a quantitative comparison has not previously been reported in the reviewed literature. The models used were the Nordic collaboration model NORTRIP (NOn-exhaust Road TRaffic Induced Particle emissions) and the Swedish-Finnish FORE model (Forecasting Of Road dust Emissions). These models describe particulate matter generated by the wear of road surface due to traction control methods and processes that control the suspension of road dust particles into the air. An experimental measurement campaign was conducted using a mobile laboratory called SNIFFER, along two selected road segments in central Helsinki in 2007 and 2008. The suspended PM10 concentration was measured behind the left rear tyre and the street background PM10 concentration in front of the van. Both models reproduced the measured seasonal variation of suspension emission factors fairly well during both years at both measurement sites. However, both models substantially under-predicted the measured emission values. The results indicate that road dust emission models can be directly compared with mobile measurements; however, more extensive and versatile measurement campaigns will be needed in the future. [ABSTRACT FROM AUTHOR]

Long-term (1984-2012) surface observations from 70 stations in the Sahara and Sahel are used to explore the diurnal, seasonal and geographical variations in dust emission events and thresholds. The frequency of dust emission (FDE) is calculated using the present weather codes of SYNOP reports. Thresholds are estimated as the wind speed for which there is a 50% probability of dust emission and are then used to calculate strong wind frequency (SWF) and dust uplift potential (DUP), where the latter is an estimate of the dust-generating power of winds. Stations are grouped into six coherent geographical areas for more in-depth analysis. FDE is highest at stations in Sudan and overall peaks in spring north of 23° N. South of this, where stations are directly influenced by the summer monsoon, the annual cycle in FDE is more variable. Thresholds are highest in northern Algeria, lowest in the latitude band 16-21° N and have greatest seasonal variations in the Sahel. Spatial variability in thresholds partly explain spatial variability in frequency of dust emission events on an annual basis. However, seasonal variations in thresholds for the six grouped areas are not the main control on seasonal variations in FDE. This is demonstrated by highly correlated seasonal cycles of FDE and SWF which are not significantly changed by using a fixed, or seasonally varying, threshold. The likely meteorological mechanisms generating these patterns such as low-level jets and haboobs are discussed. [ABSTRACT FROM AUTHOR]

Simulations of the global dust cycle and its interactions with a changing Earth system are hindered by the empirical nature of dust emission parameterizations in climate models. Here we take a step towards improving global dust cycle simulations by presenting a physically-based dust emission model. The resulting dust flux parameterization depends only on the wind friction speed and the soil's threshold friction speed, and can therefore be readily implemented into climate models. We show that our parameterization's functional form is supported by a compilation of quality-controlled vertical dust flux measurements, and that it better reproduces these measurements than existing parameterizations. Both our theory and measurements indicate that many climate models underestimate the dust flux's sensitivity to soil erodibility. This finding can explain why dust cycle simulations in many models are improved by using an empirical preferential sources function that shifts dust emissions towards the most erodible regions. In fact, implementing our parameterization in a climate model produces even better agreement against aerosol optical depth measurements than simulations that use such a source function. These results indicate that the need to use a source function is at least partially eliminated by the additional physics accounted for by our parameterization. Since soil erodibility is affected by climate changes, our results further suggest that many models have underestimated the climate sensitivity of the global dust cycle. [ABSTRACT FROM AUTHOR]

Uptake coefficients for HO2 radicals onto Arizona Test Dust (ATD) aerosols were measured at room temperature and atmospheric pressure using an aerosol flow tube and the sensitive Fluorescence Assay by Gas Expansion (FAGE) technique, enabling HO2 concentrations in the range 3-10 × 108 molecule cm-3 to be investigated. The uptake coefficients were measured as 0.031 ± 0.008 and 0.018 ± 0.006 for the lower and higher HO2 concentrations, respectively, over a range of relative humidities (5-76%). A time dependence for the HO2 uptake onto the ATD aerosols was observed, with larger uptake coefficients observed at shorter reaction times. The combination of time and HO2 concentration dependencies suggest either the partial saturation of the dust surface or that a chemical component of the dust is partially consumed whilst the aerosols are exposed to HO2. A constrained box model is used to show that HO2 uptake to dust surfaces may be an important loss pathway of HO2 in the atmosphere. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

In order to investigate the impact of different treatments for the contact angle (α) in heterogeneous ice nucleating properties of natural dust and black carbon (BC) particles, we implement the classical-nucleation-theory-based parameterization of hetero- geneous ice nucleation (Hoose et al., 2010) in the Community Atmospheric Model version 5 (CAM5), and then improve it by replacing the original single contact angle model with the probability density function of α (α-PDF) model to better represent the ice nucleation behavior of natural dust found in observations. We re-fit the classical nucleation theory (CNT) to constrain the uncertain parameters (i.e., onset α and activation energy in the single α model; mean contact angle and standard deviation in the α-PDF model) using recent observation datasets for Saharan natural dust and BC (soot). We investigate the impact of time-dependence of droplet freezing on mixedphase clouds and climate in CAM5, and the roles of natural dust and soot by different nucleation mechanisms. Our results show that when comparing with observations, the potential ice nuclei (IN) calculated by the α-PDF model has a better agreement than that calculated by the single-α model at warm temperatures (T > -20°C). Ice crystals can form at lower altitudes (with warmer temperatures) simulated by the α-PDF model compared with the single-α model in CAM5. All of these can be attributed to different ice nucleation efficiencies among aerosol particles with some particles having smaller contact angles (higher efficiencies) in the α-PDF model. In the sensitivity tests with the α-PDF model, we find that the change of mean contact angle has larger impact on the active fraction than that of standard deviation, even though the change of standard deviation can lead to the transition of freezing behavior. Both the single α and the α-PDF model indicates that the immersion freezing of natural dust plays a more important role in the heterogeneous nucleation than that of soot in mixed-phase clouds. [ABSTRACT FROM AUTHOR]

HONO is a major precursor for OH radicals in early mornings. Its formation has been mainly attributed to the heterogeneous hydrolysis of NO2 on surfaces such as soot, glass, mineral oxides and aerosol surfaces. In particular, dust events which are loaded with mineral oxide aerosols have been associated with higher HONO concentrations in the gas phase. In order to understand the mechanism of reactions related to this process, samples during dusty and non-dusty days were collected between October 2009 and April 2011. Based on HYSPLIT backward trajectories, data were divided between wind trajectories originating from Arabian or African deserts. In this study an increase of HONO levels was observed during dusty days. The increase in the acidic gas concentrations was accompanied by an increase in the PM nitrate and sulfate ion concentrations. During high relative humidity (African dusty days), it is proposed that the mechanism of NO2 hydrolysis predominates whereas during Arabian dusty days, where the air is relatively dry, a synergistic mechanism of adsorption and reaction between NO2 and SO2 on dust particles to produce HONO and sulfate in the particle phase is suggested. This study implies that the NOx reactivity on mineral oxide surfaces leads to a higher mixing level of OH. An increase in the sulfate forming capacity could account for the underestimation of sulfates in aerosols when the reactive uptake of SO2 alone is considered. [ABSTRACT FROM AUTHOR]

The direct radiative forcing efficiency of dust aerosol (DRFE dust) is an important indicator to measure the climate effect of dust. The DRFE dust is determined by the microphysical properties of dust, which vary with dust source regions. However, there are only sparse in situ measurements of them, such as the distribution of the dust aerosol particle size and the complex refractive index in the main dust source regions. Furthermore, recent studies have shown that the non-spherical effect of the dust particle is not negligible. The DRFE dust is often evaluated by estimating given microphysical properties of the dust aerosols in the radiative transfer model (RTM). However, considerable uncertainties exist due to the complex and variable dust properties, including the complex refractive index and the shape of the dust. The DRFE dust over the Taklimakan Desert and Sahara is derived from the satellite observations in this paper. The advantage of the proposed satellite-based method is that there is no need to consider the microphysical properties of the dust aerosols in estimating the DRFE dust. For comparison, the observed DRFE dust is compared with that simulated by the RTM. The differences in the dust microphysical properties in these two regions and their impacts on DRFE dust are analyzed. The DRFE dust derived from the satellite observation is -39.6±10.0 W m -2τ-1 in March 2019 over Tamanrasset in the Sahara and -48.6±13.7 W m -2τ-1 in April 2019 over Kashi in the Taklimakan Desert. According to the analyses of their microphysical properties and optical properties, the dust aerosols from the Taklimakan Desert (Kashi) scatter strongly. The RTM-simulated results (-41.5 to -47.4 W m -2τ-1 over Kashi and - 32.2 to - 44.3 W m -2τ-1 over Tamanrasset) are in good agreement with the results estimated by satellite observations. According to previous studies, the results in this paper are proven to be reasonable and reliable. The results also show that the microphysical properties of the dust can significantly influence the DRFE dust. The satellite-derived results can represent the influence of the dust microphysical properties on the DRFE dust , which can also validate the direct radiative effect of the dust aerosol and the DRFE dust derived from the numerical model more directly. [ABSTRACT FROM AUTHOR]

This paper is the companion paper of Córdoba-Jabonero et al. (2021). It deals with the estimation of the long-wave (LW) and net dust direct radiative effect (DRE) during the dust episode that occurred between 23 and 30 June 2019 and was paired with a mega-heatwave. The analysis is performed at two European sites where polarized micro-pulse lidars ran continuously to retrieve the vertical distribution of the dust optical properties: Barcelona, Spain, 23–30 June, and Leipzig, Germany, 29–30 June. The radiative effect is computed with the GAME (global atmospheric model) radiative transfer model separately for the fine- and coarse-mode dust. The instantaneous and daily radiative effect and radiative efficiency (DREff) are provided for the fine-mode, coarse-mode and total dust at the surface, top of the atmosphere (TOA) and in the atmosphere. The fine-mode daily LW DRE is low (< 6 % of the short-wave (SW) component), which makes the coarse-mode LW DRE the main modulator of the total net dust DRE. The coarse-mode LW DRE starts exceeding (in absolute values) the SW component in the middle of the episode, which produces positive coarse-mode net DRE at both the surface and TOA. Such an unusual tendency is attributed to increasing coarse-mode size and surface temperature throughout the episode. This has the effect of reducing the SW cooling in Barcelona up to the point of reaching total net positive dust DRE (+ 0.9 W m -2) on one occasion at the surface and quasi-neutral (- 0.6 W m -2) at TOA. When adding the LW component, the total dust SW radiative efficiency is reduced by a factor of 1.6 at both surface (on average over the episode the total dust net DREff is - 54.1 W m -2 τ-1) and TOA (- 37.3 W m -2 τ-1). A sensitivity study performed on the surface temperature and the air temperature in the dust layer, both linked to the heatwave and upon which the LW DRE strongly depends, shows that the heatwave contributed to reducing the dust net cooling effect at the surface and that it had nearly no effect at TOA. Its subsequent effect was thus to reduce the heating of the atmosphere produced by the dust particles. [ABSTRACT FROM AUTHOR]

Particle size distribution of dust at emission (dust PSD) is an essential quantity to estimate in dust studies. It has been recognized in earlier research that dust PSD is dependent on soil properties (e.g. whether soil is sand or clay) and friction velocity, u∗ , which is a surrogate for surface shear stress and a descriptor for saltation-bombardment intensity. This recognition has been challenged in some recent papers, causing a debate on whether dust PSD is "invariant" and the search for its justification. In this paper, we analyse the dust PSD measured in the Japan Australian Dust Experiment and show that dust PSD is dependent on u∗ and on atmospheric boundary-layer (ABL) stability. By simple theoretical and numerical analysis, we explain the two reasons for the latter dependency, which are both related to enhanced saltation bombardment in convective turbulent flows. First, u∗ is stochastic and its probability distribution profoundly influences the magnitude of the mean saltation flux due to the non-linear relationship between saltation flux and u∗. Second, in unstable conditions, turbulence is usually stronger, which leads to higher saltation-bombardment intensity. This study confirms that dust PSD depends on u∗ and, more precisely, on the probability distribution of u∗ , which in turn is dependent on ABL stability; consequently, dust PSD is also dependent on ABL. We also show that the dependency of dust PSD on u∗ and ABL stability is made complicated by soil surface conditions. In general, our analysis reinforces the basic conceptual understanding that dust PSD depends on saltation bombardment and inter-particle cohesion. [ABSTRACT FROM AUTHOR]

In this paper we show that the origin of the ice phase in tropical cumulus clouds over the sea may occur by primary ice nucleation of small crystals at temperatures just between 0 and -5 ∘ C. This was made possible through use of a holographic instrument able to image cloud particles at very high resolution and small size (6 µ m). The environment in which the observations were conducted was notable for the presence of desert dust advected over the ocean from the Sahara. However, there is no laboratory evidence to suggest that these dust particles can act as ice nuclei at temperatures warmer than about -10 ∘ C, the zone in which the first ice was observed in these clouds. The small ice particles were observed to grow rapidly by vapour diffusion, riming, and possibly through collisions with supercooled raindrops, causing these to freeze and potentially shatter. This in turn leads to the further production of secondary ice in these clouds. Hence, although the numbers of primary ice particles are small, they are very effective in initiating the rapid glaciation of the cloud, altering the dynamics and precipitation production processes. [ABSTRACT FROM AUTHOR]

In this paper, a long-term large-scale Saharan dust transport event which occurred between 14 and 27 June 2020 is tracked with the spaceborne lidars ALADIN (Atmospheric Laser Doppler Instrument) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) together with ECMWF (European Centre for Medium-Range Forecasts) and HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory model) analysis. We evaluate the performance of ALADIN and CALIOP on the observations of dust optical properties and wind fields and explore the possibility of tracking the dust events and calculating the dust mass advection with the combination of satellite and model data. The dust plumes are identified with the AIRS/Aqua Dust Score Index and with the vertical feature mask product from CALIOP. The emission, dispersion, transport and deposition of the dust event are monitored using the data from AIRS/Aqua, CALIOP and HYSPLIT. With the quasi-synchronized observations by ALADIN and CALIOP, combined with the wind field and relative humidity, the dust advection values are calculated. From this study, it is found that the dust event generated on 14 and 15 June 2020 from the Sahara in North Africa dispersed and moved westward over the Atlantic Ocean, finally being deposited in the western Atlantic Ocean, the Americas and the Caribbean Sea. During the transport and deposition processes, the dust plumes are trapped in the northeasterly trade-wind zone between latitudes of 5∘ and 30∘ N and altitudes of 0 and 6 km. Aeolus provided the observations of the dynamics of this dust transport event in the Saharan Air Layer (SAL). From the measurement results on 19 June 2020, the dust plumes are captured quasi-simultaneously over the emission region (Western Sahara), the transport region (middle Atlantic) and the deposition region (western Atlantic) individually, which indicates that the dust plume area over the Atlantic on the morning of this day is quite enormous and that this dust transport event is massive and extensive. The quasi-synchronization observation results of 15, 16, 19, 24 and 27 June by ALADIN and CALIOP during the entire transport process show good agreement with the Dust Score Index data and the HYSPLIT trajectories, which indicates that the transport process of the same dust event is tracked by ALADIN and CALIOP, verifies that the dust transport spent around 2 weeks from the emission to the deposition and achieved the respective observations of this dust event's emission phase, development phase, transport phase, descent phase and deposition phase. Finally, the advection values for different dust parts and heights on 19 June and on the entire transport routine during transportation are computed. On 19 June, the mean dust advection values are about 1.91±1.21 mg m -2 s -1 over the emission region, 1.38±1.28 mg m -2 s -1 over the transport region and 0.75±0.68mgm-2s-1 over the deposition region. In the whole lifetime of the dust event, the mean dust advection values were about 1.51±1.03mgm-2s-1 on 15 June 2020, 2.19±1.72mgm-2s-1 on 16 June 2020, 1.38±1.28mgm-2s-1 on 19 June 2020, 1.60±1.08mgm-2s-1 on 24 June 2020 and 1.03±0.60mgm-2s-1 on 27 June 2020. During the dust development stage, the mean advection values gradually increased and reached their maximum on 16 June with the enhancement of the dust event. Then, the mean advection values decreased during the transport and the deposition of the dust over the Atlantic Ocean, the Americas and the Caribbean Sea. [ABSTRACT FROM AUTHOR]

This paper concerns an in-depth analysis of an exceptional incursion of mineral dust over southern Europe in late March 2020 (27–30 March 2020). This event was associated with an anomalous circulation pattern leading to several days of PM 10 (particulate matter with an aerodynamic diameter less than 10 µ m) exceedances in connection with a dust source located in central Asia; this is a rare source of dust for Europe, which is more frequently affected by dust outbreaks from the Sahara Desert. The synoptic meteorological configuration was analyzed in detail, and the aerosol evolution during the transit of the dust plume over northern Italy was assessed at high time resolution by means of optical particle counting at three stations, namely Bologna, Trieste, and Mt. Cimone, allowing for the revelation of the transport timing among the three locations. Back-trajectory analyses supported by Copernicus Atmosphere Monitoring Service (CAMS) maps allowed for the location of the mineral dust source area in the Aralkum region. Therefore, the event was analyzed by observing the particle number size distribution with the support of chemical composition analysis. It is shown that the PM 10 exceedance recorded is associated with a large fraction of coarse particles, which is in agreement with mineral dust properties. Both the in situ number size distribution and the vertical distribution of the dust plume were cross-checked using lidar ceilometer and aerosol optical depth (AOD) data from two nearby stations and showed that the dust plume (in contrast to those originating from the Sahara Desert) traveled close to the ground (up to a height of about 2 km). The limited mixing layer height caused by high concentrations of absorbing and scattering aerosols caused the mixing of mineral dust with other locally produced ambient aerosols, thereby potentially increasing its morbidity effects. [ABSTRACT FROM AUTHOR]

This paper examines the mechanisms responsible for the production of ice in convective clouds influenced by mineral dust. Observations were made in the Ice in Clouds Experiment – Dust (ICE-D) field campaign which took place in the vicinity of Cape Verde during August 2015. Measurements made with instruments on the Facility for Airborne Atmospheric Measurements (FAAM) aircraft through the clouds on 21 August showed that ice particles were observed in high concentrations at temperatures greater than about -8 ∘ C. Sensitivity studies were performed using existing parameterization schemes in a cloud model to explore the impact of the freezing onset temperature, the efficiency of freezing, mineral dust as efficient ice nuclei, and multi-thermals on secondary ice production by the rime-splintering process. The simulation with the default Morrison microphysics scheme that involved a single thermal produced a concentration of secondary ice that was much lower than the observed value of total ice number concentration. Relaxing the onset temperature to a higher value, enhancing the freezing efficiency, or combinations of these increased the secondary ice particle concentration but not by a sufficient amount. Simulations that involved only dust particles as ice-nucleating particles produced a lower concentration of secondary ice particles, since the freezing onset temperature is low. The simulations implicate that a higher concentration of ice-nucleating particles with a higher freezing onset temperature may explain some of the observed high concentrations of secondary ice. However, a simulation with two thermals that used the original Morrison scheme without enhancement of the freezing efficiency or relaxation of the onset temperature produced the greatest concentration of secondary ice particles. It did so because of the increased time that graupel particles were exposed to significant cloud liquid water in the Hallett–Mossop temperature zone. The forward-facing camera and measurements of the vertical wind in repeated passes of the same cloud suggested that these tropical clouds contained multiple thermals. It is possible of course that several mechanisms, some of them only recently discovered, may be responsible for producing the ice particles in clouds. This study highlights the fact that the dynamics of the clouds likely play an important role in producing high concentrations of secondary ice particles in clouds. [ABSTRACT FROM AUTHOR]

An increase in the sulfate aerosols observed in the period 1–6 April 2014 over Austria is analyzed using in situ measurements at an Austrian air quality background station, lidar measurements at the closest EARLINET stations around Austria, CAMS near-real-time data, and particle dispersion modeling using FLEXPART, a Lagrangian transport model. In situ measurements of SO2 , PM 2.5 , PM 10 , and O3 were performed at the air quality background station Pillersdorf, Austria (EMEP station AT30, 48 ∘ 43 ′ N, 15 ∘ 55 ′ E). A CAMS aerosol mixing ratio analysis for Pillersdorf and the lidar stations Leipzig, Munich, Garmisch, and Bucharest indicates the presence of an event of aerosol transport, with sulfate and dust as principal components. For the sulfate layers identified at Pillersdorf from the CAMS analysis, backward- and forward-trajectory analyses were performed, associating lidar stations with the trajectories. The lidar measurements for the period corresponding to trajectory overpass of associated stations were analyzed, obtaining the aerosol layers, the optical properties, and the aerosol types. The potential sources of transported aerosols were determined for Pillersdorf and the lidar stations using the source–receptor sensitivity computed with FLEXPART, combined with the MACCity source inventory. A comparative analysis for Pillersdorf and the trajectory-associated lidar stations showed consistent aerosol layers, optical properties and types, and potential sources. A complex pattern of contributions to sulfate over Austria was found in this paper. For the lower layers (below 2000 m) of sulfate, it was found that central Europe was the main source of sulfate. Medium to smaller contributions come from sources in eastern Europe, northwest Africa, and the eastern US. For the middle-altitude layers (between 2000 and 5000 m), sources from central Europe (northern Italy, Serbia, Hungary) contribute with similar emissions. Northwest Africa and the eastern US also have important contributions. For the high-altitude layers (above 5000 m), the main contributions come from northwest Africa, but sources from the southern and eastern US also contribute significantly. No contributions from Europe are seen for these layers. The methodology used in this paper can be used as a general tool to correlate measurements at in situ stations and EARLINET lidar stations around these in situ stations. [ABSTRACT FROM AUTHOR]

This paper presents an analysis of the mineral dust aerosol modelled by five Earth system models (ESMs) within the project entitled Coordinated Research in Earth Systems and Climate: Experiments, kNowledge, Dissemination and Outreach (CRESCENDO). We quantify the global dust cycle described by each model in terms of global emissions, together with dry and wet deposition, reporting large differences in the ratio of dry over wet deposition across the models not directly correlated with the range of particle sizes emitted. The multi-model mean dust emissions with five ESMs is 2836 Tgyr-1 but with a large uncertainty due mainly to the difference in the maximum dust particle size emitted. The multi-model mean of the subset of four ESMs without particle diameters larger than 10 µm is 1664 (σ=651) Tgyr-1. Total dust emissions in the simulations with identical nudged winds from reanalysis give us better consistency between models; i.e. the multi-model mean global emissions with three ESMs are 1613 (σ=278) Tgyr-1 , but 1834 (σ=666) Tgyr-1 without nudged winds and the same models. Significant discrepancies in the globally averaged dust mass extinction efficiency explain why even models with relatively similar global dust load budgets can display strong differences in dust optical depth. The comparison against observations has been done in terms of dust optical depths based on MODIS (Moderate Resolution Imaging Spectroradiometer) satellite products, showing global consistency in terms of preferential dust sources and transport across the Atlantic. The global localisation of source regions is consistent with MODIS, but we found regional and seasonal differences between models and observations when we quantified the cross-correlation of time series over dust-emitting regions. To faithfully compare local emissions between models we introduce a re-gridded normalisation method that can also be compared with satellite products derived from dust event frequencies. Dust total deposition is compared with an instrumental network to assess global and regional differences. We find that models agree with observations within a factor of 10 for data stations distant from dust sources, but the approximations of dust particle size distribution at emission contributed to a misrepresentation of the actual range of deposition values when instruments are close to dust-emitting regions. The observed dust surface concentrations also are reproduced to within a factor of 10. The comparison of total aerosol optical depth with AERONET (AErosol RObotic NETwork) stations where dust is dominant shows large differences between models, although with an increase in the inter-model consistency when the simulations are conducted with nudged winds. The increase in the model ensemble consistency also means better agreement with observations, which we have ascertained for dust total deposition, surface concentrations and optical depths (against both AERONET and MODIS retrievals). We introduce a method to ascertain the contributions per mode consistent with the multi-modal direct radiative effects, which we apply to study the direct radiative effects of a multi-modal representation of the dust particle size distribution that includes the largest particles. [ABSTRACT FROM AUTHOR]

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 µ m 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. [ABSTRACT FROM AUTHOR]

This paper presents measurements of mineral dust concentration in the diameter range from 0.4 to 14.0 µ m with a novel balloon-borne optical particle counter, the Universal Cloud and Aerosol Sounding System (UCASS). The balloon launches were coordinated with ground-based active and passive remote-sensing observations and airborne in situ measurements with a research aircraft during a Saharan dust outbreak over Cyprus from 20 to 23 April 2017. The aerosol optical depth at 500 nm reached values up to 0.5 during that event over Cyprus, and particle number concentrations were as high as 50 cm -3 for the diameter range between 0.8 and 13.9 µ m. Comparisons of the total particle number concentration and the particle size distribution from two cases of balloon-borne measurements with aircraft observations show reasonable agreement in magnitude and shape despite slight mismatches in time and space. While column-integrated size distributions from balloon-borne measurements and ground-based remote sensing show similar coarse-mode peak concentrations and diameters, they illustrate the ambiguity related to the missing vertical information in passive sun photometer observations. Extinction coefficient inferred from the balloon-borne measurements agrees with those derived from coinciding Raman lidar observations at height levels with particle number concentrations smaller than 10 cm -3 for the diameter range from 0.8 to 13.9 µ m. An overestimation of the UCASS-derived extinction coefficient of a factor of 2 compared to the lidar measurement was found for layers with particle number concentrations that exceed 25 cm -3 , i.e. in the centre of the dust plume where particle concentrations were highest. This is likely the result of a variation in the refractive index and the shape and size dependency of the extinction efficiency of dust particles along the UCASS measurements. In the future, profile measurements of the particle number concentration and particle size distribution with the UCASS could provide a valuable addition to the measurement capabilities generally used in field experiments that are focussed on the observation of coarse aerosols and clouds. [ABSTRACT FROM AUTHOR]

The short-wave (SW) direct radiative effect (DRE) during the summer 2019 heatwave produced partly by a moderate, long-lasting Saharan dust outbreak over Europe is analysed in this study. Two European sites (periods) are considered: Barcelona, Spain (23–30 June), and Leipzig, Germany (29 and 30 June), 1350 km apart from each other. Major data are obtained from AERONET and polarised Micro-Pulse Lidar (P-MPL) observations. Modelling is used to describe the different dust pathways, as observed at both sites. The coarse dust (Dc) and fine dust (Df) components (with total dust, DD = Dc + Df) are identified in the profiles of the total particle backscatter coefficient using the POLIPHON (POlarisation LIdar PHOtometer Networking) method in synergy with P-MPL measurements. This information is used to calculate the relative mass loading and the centre-of-mass height, as well as the contribution of each dust mode to the total dust DRE. Several aspects of the ageing of dust are put forward. The mean dust optical depth and its Df/DD ratios are, respectively, 0.153 and 24 % in Barcelona and 0.039 and 38 % in Leipzig; this Df increase in Leipzig is attributed to a longer dust transport path in comparison to Barcelona. The dust produced a cooling effect on the surface with a mean daily DRE of - 9.1 and - 2.5 Wm-2 , respectively, in Barcelona and Leipzig, but the Df/DD DRE ratio is larger for Leipzig (52 %) than for Barcelona (37 %). Cooling is also observed at the top of the atmosphere (TOA), although less intense than on the surface. However, the Df/DD DRE ratio at the TOA is even higher (45 % and 60 %, respectively, in Barcelona and Leipzig) than on the surface. Despite the predominance of Dc particles under dusty conditions, the SW radiative impact of Df particles can be comparable to, even higher than, that induced by the Dc ones. In particular, the Df/DD DRE ratio in Barcelona increases by + 2.4 %d-1 (surface) and + 2.9 %d-1 (TOA) during the dusty period. This study is completed by a second paper about the long-wave and net radiative effects. These results are especially relevant for the next ESA EarthCARE mission (planned in 2022) as it is devoted to aerosol–cloud–radiation interaction research. [ABSTRACT FROM AUTHOR]

Feedbacks play a fundamental role in determining the magnitude of the response of the climate system to external forcing, such as from anthropogenic emissions. The latest generation of Earth system models includes aerosol and chemistry components that interact with each other and with the biosphere. These interactions introduce a complex web of feedbacks that is important to understand and quantify. This paper addresses multiple pathways for aerosol and chemical feedbacks in Earth system models. These focus on changes in natural emissions (dust, sea salt, dimethyl sulfide, biogenic volatile organic compounds (BVOCs) and lightning) and changes in reaction rates for methane and ozone chemistry. The feedback terms are then given by the sensitivity of a pathway to climate change multiplied by the radiative effect of the change. We find that the overall climate feedback through chemistry and aerosols is negative in the sixth Coupled Model Intercomparison Project (CMIP6) Earth system models due to increased negative forcing from aerosols in a climate with warmer surface temperatures following a quadrupling of CO2 concentrations. This is principally due to increased emissions of sea salt and BVOCs which are sensitive to climate change and cause strong negative radiative forcings. Increased chemical loss of ozone and methane also contributes to a negative feedback. However, overall methane lifetime is expected to increase in a warmer climate due to increased BVOCs. Increased emissions of methane from wetlands would also offset some of the negative feedbacks. The CMIP6 experimental design did not allow the methane lifetime or methane emission changes to affect climate, so we found a robust negative contribution from interactive aerosols and chemistry to climate sensitivity in CMIP6 Earth system models. [ABSTRACT FROM AUTHOR]

The optical properties of airborne mineral dust depend on its mineralogy, size distribution, and shape, and they might vary between different source regions. To date, large differences in refractive index values found in the literature have not been fully explained. In this paper we present a new dataset of complex refractive indices (m=n-ik) and single-scattering albedos (SSAs) for 19 mineral dust aerosols over the 370–950 nm range in dry conditions. Dust aerosols were generated from natural parent soils from eight source regions (northern Africa, Sahel, Middle East, eastern Asia, North and South America, southern Africa, and Australia). They were selected to represent the global-scale variability of the dust mineralogy. Dust was resuspended into a 4.2 m 3 smog chamber where its spectral shortwave scattering (βsca) and absorption (βabs) coefficients, number size distribution, and bulk composition were measured. The complex refractive index was estimated by Mie calculations combining optical and size data, while the spectral SSA was directly retrieved from βsca and βabs measurements. Dust is assumed to be spherical in the whole data treatment, which introduces a potential source of uncertainty. Our results show that the imaginary part of the refractive index (k) and the SSA vary widely from sample to sample, with values for k in the range 0.0011 to 0.0088 at 370 nm, 0.0006 to 0.0048 at 520 nm, and 0.0003 to 0.0021 at 950 nm, as well as values for SSA in the range 0.70 to 0.96 at 370 nm, 0.85 to 0.98 at 520 nm, and 0.95 to 0.99 at 950 nm. In contrast, the real part of the refractive index (n) is mostly source (and wavelength) independent, with an average value between 1.48 and 1.55. The sample-to-sample variability in our dataset of k and SSA is mostly related to differences in the dust iron content. In particular, a wavelength-dependent linear relationship is found between the magnitude of k and SSA and the mass concentrations of both iron oxide and total elemental iron, with iron oxide better correlated than total elemental iron with both k and SSA. The value of k was found to be independent of size. When the iron oxide content exceeds 3 %, the SSA linearly decreases with an increasing fraction of coarse particles at short wavelengths (< 600 nm). Compared to the literature, our values for the real part of the refractive index and SSA are in line with past results, while we found lower values of k compared to most of the literature values currently used in climate models. We recommend that source-dependent values of the SW spectral refractive index and SSA be used in models and remote sensing retrievals instead of generic values. In particular, the close relationships found between k or SSA and the iron content in dust enable the establishment of predictive rules for spectrally resolved SW absorption based on particle composition. [ABSTRACT FROM AUTHOR]

Aerosol–cloud interactions in mixed-phase clouds (MPCs) are one of the most uncertain drivers of the hydrological cycle and climate change. A synergy of in situ, remote-sensing and modelling experiments were used to determine the source of ice-nucleating particles (INPs) for MPCs at Mount Helmos in the eastern Mediterranean. The influences of boundary layer turbulence, vertical aerosol distributions and meteorological conditions were also examined. When the observation site is in the free troposphere (FT), approximately 1 in ×106 aerosol particles serve as INPs around -25 °C. The INP abundance spans 3 orders of magnitude and increases in the following order: marine aerosols; continental aerosols; and, finally, dust plumes. Biological particles are important INPs observed in continental and marine aerosols, whereas they play a secondary, although important, role during Saharan dust events. Air masses in the planetary boundary layer (PBL) show both enriched INP concentrations and a higher proportion of INPs to total aerosol particles, compared with cases in the FT. The presence of precipitation/clouds enriches INPs in the FT but decreases INPs in the PBL. Additionally, new INP parameterizations are developed that incorporate the ratio of fluorescent-to-nonfluorescent or coarse-to-fine particles and predict >90 % of the observed INPs within an uncertainty range of a factor of 10; these new parameterizations exhibit better performance than current widely used parameterizations and allow ice formation in models to respond to variations in dust and biological particles. The improved parameterizations can help MPC formation simulations in regions with various INP sources or different regions with prevailing INP sources. [ABSTRACT FROM AUTHOR]

Remote marine regions comprise a high fraction of Earth's surface, but in situ vertically resolved measurements over these locations remain scarce. Here we use airborne data during 15 vertical spiral soundings (0.15–8.5 km) over Bermuda during the NASA Aerosol Cloud meTeorology Interactions over the western ATlantic Experiment (ACTIVATE) to investigate the impact of different source regions on the vertical structure of trace gases, aerosol particles, and meteorological variables over 1000 km offshore of the US East Coast. Results reveal significant differences in vertical profiles of variables between three different air mass source categories (North America, Ocean, Caribbean/North Africa) identified using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model: (i) the strongest pollution signature is from air masses from the North America category, while the weakest one is from the Ocean category; (ii) North America air has the highest levels of CO, CH 4 , submicron particle number concentration, aerosol mass spectrometer (AMS) mass, and organic mass fraction along with smoke layers in the free troposphere (FT); (iii) Ocean air has the highest relative amount of nitrate, non-sea-salt sulfate, and oxalate, which are key acidic species participating in chloride depletion; (iv) air masses from the Caribbean/North Africa showed a pronounced coarse aerosol signature in the FT and reduced aerosol hygroscopicity, which is associated with dust transport; and (v) there is considerable vertical heterogeneity for almost all variables examined, including higher O 3 and submicron particle concentrations with altitude, suggesting that the FT is a potential contributor of both constituents in the marine boundary layer. This study highlights the importance of considering air mass source origin and vertical resolution to capture aerosol and trace gas properties over remote marine areas. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Infrared "Desert Dust" composite imagery taken by the Spinning Enhanced Visible and InfraRed Imager (SEVIRI), onboard the Meteosat Second Generation (MSG) series of satellites above the equatorial East Atlantic, has been widely used for more than a decade to identify and track the presence of dust storms from and over the Sahara Desert, the Middle East, and southern Africa. Dust is characterised by distinctive pink colours in the Desert Dust false-colour imagery; however, the precise colour is influenced by numerous environmental properties, such as the surface thermal emissivity and skin temperature, the atmospheric water vapour content, the quantity and height of dust in the atmosphere, and the infrared optical properties of the dust itself. For this paper, simulations of SEVIRI infrared measurements and imagery have been performed using a modelling system, which combines dust concentrations simulated by the aerosol transport model COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdelling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model) with radiative transfer simulations from the RTTOV (Radiative Transfer for TOVS) model. Investigating the sensitivity of the synthetic infrared imagery to the environmental properties over a 6-month summertime period from 2011 to 2013, it is confirmed that water vapour is a major control on the apparent colour of dust, obscuring its presence when the moisture content is high. Of the three SEVIRI channels used in the imagery (8.7, 10.8, and 12.0 µm), the channel at 10.8 µm has the highest atmospheric transmittance and is therefore the most sensitive to the surface skin temperature. A direct consequence of this sensitivity is that the background desert surface exhibits a strong diurnal cycle in colour, with light blue colours possible during the day and purple hues prevalent at night. In dusty scenes, the clearest pink colours arise from high-altitude dust in dry atmospheres. Elevated dust influences the dust colour primarily by reducing the contrast in atmospheric transmittance above the dust layer between the SEVIRI channels at 10.8 and 12.0 µm , thereby boosting red and pink colours in the imagery. Hence, the higher the dust altitude, the higher the threshold column moisture needed for dust to be obscured in the imagery: for a sample of dust simulated to have an aerosol optical depth (AOD) at 550 nm of 2–3 at an altitude of 3–4 km, the characteristic colour of the dust may only be impaired when the total column water vapour is particularly moist (⪆39 mm). Meanwhile, dust close to the surface (altitude <1 km) is only likely to be apparent when the atmosphere is particularly dry and when the surface is particularly hot, requiring column moisture ⪅13 mm and skin temperatures ⪆314 K, and is highly unlikely to be apparent when the skin temperature is ⪅300 K. Such low-altitude dust will regularly be almost invisible within the imagery, since it will usually be beneath much of the atmospheric water vapour column. It is clear that the interpretation of satellite-derived dust imagery is greatly aided by knowledge of the background environment. [ABSTRACT FROM AUTHOR]

The Saharan Air Layer (SAL) in the summertime eastern Atlantic is typically well mixed and 3–4 km deep, overlying the marine boundary layer (MBL). In this paper, we show experimental evidence that at times a very different structure can be observed. During the AERosol properties – Dust (AER-D) airborne campaign in August 2015, the typical structure described above was observed most of the time, and was associated with a moderate dust content yielding an aerosol optical depth (AOD) of 0.3–0.4 at 355 nm. In an intense event, however, an unprecedented vertical structure was observed close to the eastern boundary of the basin, displaying an uneven vertical distribution and a very large AOD (1.5–2), with most of the dust in a much lower level than usual (0.3–2 km). Estimated dust concentrations and column loadings for all flights during the campaign spanned 300–5500 and 0.8–7.5 g m -2 , respectively. The shortwave direct radiative impact of the intense dust event has been evaluated to be as large as -260±30 and -120±15 W m -2 at the surface and top of atmosphere (TOA), respectively. We also report the correlation of this event with anomalous lightning activity in the Canary Islands. In all cases, our measurements detected a broad distribution of aerosol sizes, ranging from ∼0.1 to ∼80 µ m (diameter), thus highlighting the presence of giant particles. Giant dust particles were also found in the MBL. We note that most aerosol models may miss the giant particles due to the fact that they use size bins up to 10–25 µ m. The unusual vertical structure and the giant particles may have implications for dust transport over the Atlantic during intense events and may affect the estimate of dust deposited to the ocean. We believe that future campaigns could focus more on events with high aerosol load and that instrumentation capable of detecting giant particles will be key to dust observations in this part of the world. [ABSTRACT FROM AUTHOR]

The complex nature of mineral dust aerosol emission makes it a difficult process to represent accurately in weather and climate models. Indeed, results in the companion paper indicate that many large-scale models underestimate the dust flux's sensitivity to the soil's threshold friction velocity for erosion. We hypothesize that this finding explains why many dust cycle simulations are improved by using an empirical dust source function that shifts emissions towards the world's most erodible regions. Here, we both test this hypothesis and evaluate the performance of the new dust emission parameterization presented in the companion paper. We do so by implementing the new emission scheme into the Community Earth System Model (CESM) and comparing the resulting dust cycle simulations against an array of measurements. We find that the new scheme shifts emissions towards the world's most erodible regions in a manner that is strikingly similar to the effect of implementing a widely used source function based on satellite observations of dust source regions. Furthermore, model comparisons against aerosol optical depth measurements show that the new physically based scheme produces a statistically significant improvement in CESM's representation of dust emission, which exceeds the improvement produced by implementing a source function. These results indicate that the need to use an empirical source function is eliminated, at least in CESM, by the additional physics in the new scheme, and in particular by its increased sensitivity to the soil's threshold friction velocity. Since the threshold friction velocity is affected by climate changes, our results further suggest that many large-scale models underestimate the global dust cycle's climate sensitivity. [ABSTRACT FROM AUTHOR]

Understanding the role atmospheric aerosols play in the Earth-atmosphere system is limited by uncertainties in the knowledge of their distribution, composition and sources. In this paper, we use the GEOS-Chem based inverse modelling framework for retrieving desert dust (DD), black carbon (BC) and organic carbon (OC) aerosol emissions simultaneously. Aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) retrieved from the multi-angular and polarimetric POLDER/PARASOL measurements generated by the GRASP algorithm (hereafter PARASOL/GRASP) have been assimilated. First, the inversion framework is validated in a series of numerical tests conducted with synthetic PARASOL-like data. These tests show that the framework allows for retrieval of the distribution and strength of aerosol emissions. The uncertainty of retrieved daily emissions in error free conditions is below 25.8% for DD, 5.9% for BC and 26.9% for OC. In addition, the BC emission retrieval is sensitive to BC refractive index, which could produce an additional factor of 1.8 differences for total BC emissions. The approach is then applied to 1 year (December 2007 to November 2008) of data over the African and Arabian Peninsula region using PARASOL/GRASP spectral AOD and AAOD at six wavelengths (443, 490, 565, 670, 865 and 1020 nm). Analysis of the resulting retrieved emissions indicates 1.8 times overestimation of the prior DD online mobilization and entrainment model. For total BC and OC, the retrieved emissions show a significant increase of 209.9%-271.8% in comparison to the prior carbonaceous aerosol emissions. The model posterior simulation with retrieved emissions shows good agreement with both the AOD and AAOD PARASOL/GRASP products used in the inversion. The fidelity of the results is evaluated by comparison of posterior simulations with measurements from AERONET that are completely independent measurements and more temporally frequent than PARASOL observations. To further test the robustness of our posterior emissions constrained using PARASOL/GRASP, the posterior emissions are implemented in the GEOS-5/GOCART model and the consistency of simulated AOD and AAOD with other independent measurements (MODIS and OMI) demonstrates promise in applying this database for modelling studies. [ABSTRACT FROM AUTHOR]

The climatic and health effects of aerosols are strongly dependent on the intra-annual variations in their loading and properties. While the seasonal variations of regional aerosol optical depth (AOD) have been extensively studied, understanding the temporal variations in aerosol vertical distribution and particle types is also important for an accurate estimate of aerosol climatic effects. In this paper, we combine the observations from four satellite-borne sensors and several ground-based networks to investigate the seasonal variations of aerosol column loading, vertical distribution, and particle types over three populous regions: the Eastern United States (EUS), Western Europe (WEU), and Eastern and Central China (ECC). In all three regions, column AOD, as well as AOD at heights above 800 m, peaks in summer/spring, probably due to accelerated formation of secondary aerosols and hygroscopic growth. In contrast, AOD below 800m peaks in winter over WEU and ECC regions because more aerosols are confined to lower heights due to the weaker vertical mixing. In the EUS region, AOD below 800m shows two maximums, one in summer and the other in winter. The temporal trends in low-level AOD are consistent with those in surface fine particle (PM2:5) concentrations. AOD due to fine particles (< 0:7 µm diameter) is much larger in spring/summer than in winter over all three regions. However, the coarse mode AOD (> 1:4 µm diameter), generally shows small variability, except that a peak occurs in spring in the ECC region due to the prevalence of airborne dust during this season. When aerosols are classified according to sources, the dominant type is associated with anthropogenic air pollution, which has a similar seasonal pattern as total AOD. Dust and sea-spray aerosols in the WEU region peak in summer and winter, respectively, but do not show an obvious seasonal pattern in the EUS region. Smoke aerosols, as well as absorbing aerosols, present an obvious unimodal distribution with a maximum occurring in summer over the EUS and WEU regions, whereas they follow a bimodal distribution with peaks in August and March (due to crop residue burning) over the ECC region. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 µ m, 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. [ABSTRACT FROM AUTHOR]

Heterogeneous uptake of SO2 on mineral dust is a predominant formation pathway of sulfates, whereas the contribution of photo-induced SO2 oxidation to sulfates on the dust interfaces still remains unclear. Here, we investigated heterogeneous photochemical reactions of SO2 on five mineral oxides (SiO2 , kaolinite, Al2O3 , MgO , and CaO) without photocatalytic activity. Light enhanced the uptake of SO2 , and its enhancement effects negatively depended on the basicity of mineral oxides. The initial uptake coefficient (γ0,BET) and the steady-state uptake coefficient (γs,BET) of SO2 positively relied on light intensity, relative humidity (RH), and O2 content, while they exhibited a negative relationship with the initial SO2 concentration. Rapid sulfate formation during photo-induced heterogeneous reactions of SO2 with all mineral oxides was confirmed to be ubiquitous, and H2O and O2 played key roles in the conversion of SO2 to sulfates. In particular, triplet states of SO2 (3SO2) were suggested to be the trigger for photochemical sulfate formation. Atmospheric implications supported a potential contribution of interfacial SO2 photochemistry on non-photoactive mineral dust to atmospheric sulfate sources. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The Taklamakan Desert (TD) is a major source of mineral dust emissions into the atmosphere. These dust particles have the ability to darken the surface of snow on the surrounding high mountains after deposition, significantly impacting the regional radiation balance. However, previous field measurements have been unable to capture the effects of severe dust storms accurately, and their representation on regional scales has been inadequate. In this study, we propose a modified remote-sensing approach that combines data from the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite and simulations from the Snow, Ice, and Aerosol Radiative (SNICAR) model. This approach allows us to detect and analyze the substantial snow darkening resulting from dust storm deposition. We focus on three typical dust events originating from the Taklamakan Desert and observe significant snow darkening over an area of ∼ 2160, ∼ 610, and ∼ 640 km 2 in the Tien Shan, Kunlun, and Qilian mountains, respectively. Our findings reveal that the impact of dust storms extends beyond the local high mountains, reaching mountains located approximately 1000 km away from the source. Furthermore, we observe that dust storms not only darken the snowpack during the spring but also in the summer and autumn seasons, leading to increased absorption of solar radiation. Specifically, the snow albedo reduction (radiative forcing) triggered by severe dust deposition is up to 0.028–0.079 (11–31.5 W m -2), 0.088–0.136 (31–49 W m -2), and 0.092–0.153 (22–38 W m -2) across the Tien Shan, Kunlun, and Qilian mountains, respectively. This further contributes to the aging of the snow, as evidenced by the growth of snow grain size. Comparatively, the impact of persistent but relatively slow dust deposition over several months during non-event periods is significantly lower than that of individual dust events. This highlights the necessity of giving more attention to the influence of extreme events on the regional radiation balance. This study provides a deeper understanding of how a single dust event can affect the extensive snowpack and demonstrates the potential of employing satellite remote sensing to monitor large-scale snow darkening. [ABSTRACT FROM AUTHOR]

During transport by advection, atmospheric nonspherical particles, such as volcanic ash, desert dust or seasalt particles experience several chemical and physical processes, leading to a complex vertical atmospheric layering at remote sites where intrusion episodes occur. In this paper, a new methodology is proposed to analyse this complex vertical layering in the case of a two/three-component particle external mixtures. This methodology relies on an analysis of the spectral and polarization properties of the light backscattered by atmospheric particles. It is based on combining a sensitive and accurate UV-VIS polarization lidar experiment with T-matrix numerical simulations and air mass back trajectories. The Lyon UV-VIS polarization lidar is used to efficiently partition the particle mixture into its nonspherical components, while the T-matrix method is used for simulating the backscattering and depolarization properties of nonspherical volcanic ash, desert dust and sea-salt particles. It is shown that the particle mixtures' depolarization ratio δp differs from the nonspherical particles' depolarization ratio δns due to the presence of spherical particles in the mixture. Hence, after identifying a tracer for nonspherical particles, particle backscattering coefficients specific to each nonspherical component can be retrieved in a two-component external mixture. For three-component mixtures, the spectral properties of light must in addition be exploited by using a dualwavelength polarization lidar. Hence, for the first time, in a three-component external mixture, the nonsphericity of each particle is taken into account in a so-called 2β + 2β formalism. Applications of this new methodology are then demonstrated in two case studies carried out in Lyon, France, related to the mixing of Eyjafjallajökull volcanic ash with sulfate particles (case of a two-component mixture) and to the mixing of dust with sea-salt and water-soluble particles (case of a three-component mixture). This new methodology, which is able to provide separate vertical profiles of backscattering coefficient for mixed atmospheric dust, sea-salt and watersoluble particles, may be useful for accurate radiative forcing assessments. [ABSTRACT FROM AUTHOR]

In our previous works, it was demonstrated that the combined use of quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), which is also known as low-Z particle EPMA, and attenuated total reflectance Fourier transform infrared spectroscopy (ATRFTIR) imaging has great potential for a detailed characterization of individual aerosol particles. In this study, extensively chemically modified (aged) individual Asian dust particles collected during an Asian dust storm event on 11 November 2002 in Korea were characterized by the combined use of low-Z particle EPMA and ATR-FTIR imaging. Overall, 109 individual particles were classified into four particle types based on their morphology, elemental concentrations, and molecular species and/or functional groups of individual particles available from the two analytical techniques: Ca-containing (38 %), NaNO3-containing (30 %), silicate (22%), and miscellaneous particles (10 %). Among the 41 Ca-containing particles, 10, 8, and 14 particles contained nitrate, sulfate, and both, respectively, whereas only two particles contained unreacted CaCO3. Airborne amorphous calcium carbonate (ACC) particles were observed in this Asian dust sample for the first time, where their IR peaks for the insufficient symmetric environment of CO32- ions of ACC were clearly differentiated from those of crystalline CaCO3. This paper also reports the first inland field observation of CaCl2 particles probably converted from CaCO3 through the reaction with HCl(g). HCl(g) was likely released from the reaction of sea salt with NOx/HNO3, as all 33 particles of marine origin contained NaNO3 (no genuine sea salt particle was encountered). Some silicate particles with minor amounts of calcium were observed to be mixed with nitrate, sulfate, and water. Among 24 silicate particles, 10 particles are mixed with water, the presence of which could facilitate atmospheric heterogeneous reactions of silicate particles including swelling minerals, such as montmorillonite and vermiculite, and nonswelling ones, such as feldspar and quartz. This paper provides detailed information on the physicochemical characteristics of these aged individual Asia dust particles through the combined use of the two single-particle analytical techniques, and using this analytical methodology it is clearly shown that internal mixing states of the aged particles are highly complicated. [ABSTRACT FROM AUTHOR]

The new NMMB/BSC-Dust model is intended to provide short to medium-range weather and dust forecasts from regional to global scales. It is an online model in which the dust aerosol dynamics and physics are solved at each model time step. The companion paper (Pérez et al., 2011) develops the dust model parameterizations and provides daily to annual evaluations of the model for its global and regional configurations. Modeled aerosol optical depth (AOD) was evaluated against AERONET Sun photometers over Northern Africa, Middle East and Europe with correlations around 0.6-0.7 on average without dust data assimilation. In this paper we analyze in detail the behavior of the model using data from the Saharan Mineral dUst experiment (SAMUM-1) in 2006 and the Bodélé Dust Experiment (BoDEx) in 2005. AOD from satellites and Sun photometers, vertically resolved extinction coefficients from lidars and particle size distributions at the ground and in the troposphere are used, complemented by wind profile data and surface meteorological measurements. All simulations were performed at the regional scale for the Northern African domain at the expected operational horizontal resolution of 25 km. Model results for SAMUM-1 generally show good agreement with satellite data over the most active Saharan dust sources. The model reproduces the AOD from Sun photometers close to sources and after long-range transport, and the dust size spectra at different height levels. At this resolution, the model is not able to reproduce a large haboob that occurred during the campaign. Some deficiencies are found concerning the vertical dust distribution related to the representation of the mixing height in the atmospheric part of the model. For the BoDEx episode, we found the diurnal temperature cycle to be strongly dependant on the soil moisture, which is underestimated in the NCEP analysis used for model initialization. The low level jet (LLJ) and the dust AOD over the Bodélé are well reproduced. The remaining negative AOD bias (due to underestimated surface wind speeds) can be substantially reduced by decreasing the threshold friction velocity in the model. [ABSTRACT FROM AUTHOR]

We describe and evaluate the NMMB/BSC-Dust, a new dust aerosol cycle model embedded online within the NCEP Non-hydrostatic Multiscale Model (NMMB). NMMB is a further evolution of the operational Nonhydrostatic Mesoscale Model (WRF-NMM), which together with other upgrades has been extended from meso to global scales. Its unified non-hydrostatic dynamical core is prepared for regional and global simulation domains. The new NMMB/BSC-Dust is intended to provide short to medium-range weather and dust forecasts from regional to global scales and represents a first step towards the development of a unified chemical-weather model. This paper describes the parameterizations used in the model to simulate the dust cycle including sources, transport, deposition and interaction with radiation. We evaluate monthly and annual means of the global configuration of the model against the AEROCOM dust benchmark dataset for year 2000 including surface concentration, deposition and aerosol optical depth (AOD), and we evaluate the daily AOD variability in a regional domain at high resolution covering Northern Africa, Middle East and Europe against AERONET AOD for year 2006. The NMMB/BSC-Dust provides a good description of the horizontal distribution and temporal variability of the dust. Daily AOD correlations at the regional scale are around 0.6-0.7 on average without dust data assimilation. At the global scale the model lies within the top range of AEROCOM dust models in terms of performance statistics for surface concentration, deposition and AOD. This paper discusses the current strengths and limitations of the modeling system and points towards future improvements. [ABSTRACT FROM AUTHOR]

Massive amounts of Saharan dust are blown from the coast of northern Africa across the Atlantic Ocean towards the Americas each year. This dust has, depending on its chemistry, direct and indirect effects on global climate which include reflection and absorption of solar radiation as well as transport and deposition of nutrients and metals fertilizing both ocean and land. To determine the temporal and spatial variability of Saharan dust transport and deposition and their marine environmental effects across the equatorial North Atlantic Ocean, we have set up a monitoring experiment using deep-ocean sediment traps as well as land-based dust collectors. The sediment traps were deployed at five ocean sites along a transatlantic transect between north-west Africa and the Caribbean along 12° N, in a downwind extension of the land-based dust collectors placed at 19° N on the Mauritanian coast in Iouîk. In this paper, we lay out the setup of the monitoring experiment and present the particle fluxes from sediment trap sampling over 24 continuous and synchronized intervals from October 2012 through to November 2013. We establish the temporal distribution of the particle fluxes deposited in the Atlantic and compare chemical compositions with the land-based dust collectors propagating to the downwind sediment trap sites, and with satellite observations of Saharan dust outbreaks. First-year results show that the total mass fluxes in the ocean are highest at the sampling sites in the east and west, closest to the African continent and the Caribbean, respectively. Element ratios reveal that the lithogenic particles deposited nearest to Africa are most similar in composition to the Saharan dust collected in Iouîk. Downwind increasing Al, Fe and K contents suggest a downwind change in the mineralogical composition of Saharan dust and indicate an increasing contribution of clay minerals towards the west. In the westernmost Atlantic Ocean, admixture of re-suspended clay-sized sediments advected towards the deep sediment trap cannot be excluded. Seasonality is most prominent near both continents but generally weak, with mass fluxes dominated by calcium carbonate and clear seasonal maxima of biogenic silica towards the west. The monitoring experiment is now extended, with autonomous dust sampling buoys for better quantification of Saharan dust transport and deposition from source to sink and their impact on fertilization and carbon export to the deep ocean. [ABSTRACT FROM AUTHOR]

Most of the dust models underestimate the load of the large dust particles, consider spherical shapes instead of irregular ones, and have to deal with a wide range of the dust refractive index (RI) to be used. This leads to an incomplete assessment of the dust radiative effects and dust-related impacts on climate and weather. The current work aims to provide an assessment, through a sensitivity study, of the limitations of models to calculate the dust direct radiative effect (DRE) due to the underrepresentation of its size, RI, and shape. We show that the main limitations stem from the size and RI, while using a more realistic shape plays only a minor role, with our results agreeing with recent findings in the literature. At the top of the atmosphere (TOA) close to dust sources, the underestimation of size issues an underestimation of the direct warming effect of dust of ∼ 18–25 W m -2 , for DOD = 1 (dust optical depth) at 0.5 µ m, depending on the solar zenith angle (SZA) and RI. The underestimation of the dust size in models is less above the ocean than above dust sources, resulting in an underestimation of the direct cooling effect of dust above the ocean by up to 3 W m -2 , for aerosol optical depth (AOD) of 1 at 0.5 µ m. We also show that the RI of dust may change its DRE by 80 W m -2 above the dust sources and by 50 W m -2 at downwind oceanic areas for DOD = 1 at 0.5 µ m at TOA. These results indicate the necessity of including more realistic sizes and RIs for dust particles in dust models, in order to derive better estimations of the dust DRE, especially near the dust sources and mostly for studies dealing with local radiation effects of dust aerosols. [ABSTRACT FROM AUTHOR]

The radiative effects of biomass burning aerosols (BBAs) on low-level atmospheric circulation over southern Africa are investigated on 5 September 2017 during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign. This is conducted using a variety of in situ and remote sensing observations, as well as two 5 d ensemble simulations made with the Meso-NH mesoscale model, one including the direct and semi-direct radiative effects of aerosols and one in which these effects are not included. We show that the radiative impact of BBA building up over a period of 5 d in the Meso-NH simulations can lead to significantly different circulations at low and middle levels, thereby affecting dust emissions over southern Namibia and northwestern South Africa as well as the transport of BBA in a so-called "river of smoke". While most of the regional-scale dynamics, thermodynamics and composition features are convincingly represented in the simulation with BBA radiative effects, neglecting the radiative impact of BBA leads to unrealistic representations of (i) the low-level jet (LLJ) over the plateau, which is the main low-level dynamic feature fostering dust emission, and (ii) the mid-level dynamics pertaining to the transport of BBA from the fire-prone regions in the tropics to the mid-latitudes. For instance, when the BBA radiative impacts are not included, the LLJ is too weak and not well established over night, and the developing convective planetary boundary layer (PBL) is too deep compared to observations. The deeper convective PBL over Etosha and surrounding areas is related to the enhanced anomalous upward motion caused by the eastern displacement of the river of smoke. This eastern displacement is, in turn, related to the weaker southerly African easterly jet. Both ensemble simulations provide clear evidence that the enhanced near-surface extinction coefficient values detected from observations over Etosha are related to the downward mixing of BBA in the developing convective boundary layer rather than dust being emitted as a result of the LLJ breakdown after sunrise. This study suggests that the radiative effect of BBAs needs to be taken into account to properly forecast dust emissions in Namibia. [ABSTRACT FROM AUTHOR]

During the months of February–March (FM) of the 2020–2022 period, several intense dust intrusions from northern Africa affected Europe. The frequency of dust events was exceptional, considering that wintertime is the season with minimum dust activity in the Mediterranean, and some episodes displayed a duration and/or intensity never recorded before, affecting large areas of the western Euro-Mediterranean (WEM) region. The main objective of this work is to construct a catalogue of FM dust events over the WEM for the 2003–2022 period based on satellite aerosol retrievals and to analyse their atmospheric drivers at the synoptic and large scales, paying special attention to the recent 2020–2022 period of high dust activity. Overall, our results indicate large intraseasonal and interannual variability in the occurrence of wintertime dust events over the WEM. Dust events of FM 2020–2022 were characterized by enhanced dust concentration and high maximum altitudes in comparison with those of previous years (2003–2019). WEM dust events are associated with enhanced activity of high-pressure systems over the Euro-Atlantic sector, which favour the obstruction of the westerlies and the occurrence of cut-off lows at subtropical latitudes. However, these high-pressure systems can exhibit a large variety of configurations, including meridional dipole blocking patterns with poleward shifted jets or Mediterranean subtropical ridges with an intensified mid-latitude jet. The former is the dominant favourable pattern for WEM dust occurrence, but the latter was relatively common during the 2020–2022 period. [ABSTRACT FROM AUTHOR]

Spatial and temporal variations in the level of dust activity can provide valuable information for policymaking and climate research. Recently, Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol products have been successfully used for retrieving dust aerosol optical depth (DAOD), especially over bright dust source areas, and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) aerosol reanalysis provides DAOD and additionally other dust-aerosol-related parameters. In this study, spatial and temporal variations in dust activity in Australia were analyzed using MODIS and MERRA-2 combined (M&M) DAOD and MERRA-2 near-surface dust concentrations and estimated PM 10 for the period 1980–2020. Validation results show that M&M DAOD has an expected error of ±(0.016+0.15τ) compared to the ground observations at the AErosol RObotic NETwork (AERONET) dust storms on populated areas sites. MERRA-2 near-surface dust concentrations show a power-law relationship with visibility data collected at meteorological stations with an r2 value from 0.18 to 0.44, and the estimated MERRA-2 PM 10 shows similar temporal variations and correlates with ground-based PM 10 data with an r2 value from 0.14 to 0.44 at six selected stations in Australia. Moreover, MERRA-2 horizontal dust flux shows the same major dust pathways as those in previous studies and similar dust emissions and deposition areas identified using ground-based observations. Dust events based on DAOD over eastern Australia are concentrated in the north in December, are concentrated in the south in February, and can occur anywhere in January. Near-surface dust concentration was found to be the highest (over 200 µ g m -3) over the center of Lake Eyre basin in central Australia and radially decreased toward the coast to below 20 µ g m -3 via the two main pathways in the southwest and northeast. The ratio of near-surface dust concentration to PM 10 shows a similar spatial pattern. Total dust emission was estimated to be 40 Mt (megatonnes) per year over the period 1980–2020, of which nearly 50 % was deposited on land and the rest exported away from the Australian continent. [ABSTRACT FROM AUTHOR]

Chloride (Cl -) displacement from sea salt particles is an extensively studied phenomenon with implications for human health, visibility, and the global radiation budget. Past works have investigated Cl - depletion over the northwest Atlantic (NWA); however, an updated, multi-seasonal, and geographically expanded account of sea salt reactivity over the region is needed. This study uses chemically resolved mass concentrations and meteorological data from the airborne Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) to quantify seasonal, spatial, and meteorological trends in Cl - depletion and to explore the importance of quantifying (1) non-sea salt sources of Na + and (2) mass concentrations of lost Cl - (instead of relative amounts displaced). Lost Cl - mass concentrations are lowest in December–February and March, moderate around Bermuda in June, and highest in May (median losses of 0.04, 0.04, 0.66, and 1.76 µ g m -3 , respectively), with losses in May that are high enough to potentially accelerate tropospheric oxidation rates. Inorganic acidic species can account for all Cl - depletion in December–February, March, and June near Bermuda but none of the lost Cl - in May, suggesting that organic acids may be of importance for Cl - displacement in certain months. Contributions of dust to Na + are not important seasonally but may cause relevant overestimates of lost Cl - in smoke and dust plumes. Higher percentages of Cl - depletion often do not correspond to larger mass concentrations of lost Cl - , so it is highly recommended to quantify the latter to place depletion reactions in context with their role in atmospheric oxidation and radiative forcing. [ABSTRACT FROM AUTHOR]

Satellite observations and ground-based measurements have indicated a high variability in the aerosol optical depth (AOD) in the Middle East region in recent decades. In the period that extends from 2003 to 2012, observations show a positive AOD trend of 0.01–0.04 per year or a total increase of 0.1–0.4 per decade. This study aimed to investigate if the observed trend was also captured by the NASA Goddard Earth Observing System (GEOS) model. To this end, we examined changes in the simulated dust emissions and dust AOD during this period. To understand the factors driving the increase in AOD in this region we also examined meteorological and surface parameters important for dust emissions, such as wind fields and soil moisture. Two GEOS model simulations were used in this study: the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) reanalysis (with meteorological and aerosol AOD data assimilated) and MERRA-2 Global Modeling Initiative (GMI) Replay (with meteorology constrained by the MERRA-2 reanalysis but without aerosol assimilation). We did not find notable changes in the modeled 10 m wind speed and soil moisture. However, analysis of Moderate Resolution Imaging Spectroradiometer (MODIS) normalized difference vegetation index (NDVI) data did show an average decrease of 8 % per year in the region encompassing Syria and Iraq, which prompted us to quantify the effects of vegetation on dust emissions and AOD in the Middle East region. This was done by performing a sensitivity experiment in which we enhanced dust emissions in grid cells where the NDVI decreased. The simulation results supported our hypothesis that the loss of vegetation cover and the associated increase in dust emissions over Syria and Iraq can partially explain the increase in AOD downwind. The model simulations indicated dust emissions need to be 10-fold larger in those grid cells in order to reproduce the observed AOD and trend in the model. [ABSTRACT FROM AUTHOR]

The spring 2020 COVID-19 lockdowns led to a rapid reduction in aerosol and aerosol precursor emissions. These emission reductions provide a unique opportunity for model evaluation and to assess the potential efficacy of future emission control measures. We investigate changes in observed regional aerosol optical depth (AOD) during the COVID-19 lockdowns and use these observed anomalies to evaluate Earth system model simulations forced with COVID-19-like reductions in aerosols and greenhouse gases. Most anthropogenic source regions do not exhibit statistically significant changes in satellite retrievals of total or dust-subtracted AOD, despite the dramatic economic and lifestyle changes associated with the pandemic. Of the regions considered, only India exhibits an AOD anomaly that exceeds internal variability. Earth system models reproduce the observed responses reasonably well over India but initially appear to overestimate the magnitude of response in East China and when averaging over the Northern Hemisphere (0–70 ∘ N) as a whole. We conduct a series of sensitivity tests to systematically assess the contributions of internal variability, model input uncertainty, and observational sampling to the aerosol signal, and we demonstrate that the discrepancies between observed and simulated AOD can be partially resolved through the use of an updated emission inventory. The discrepancies can also be explained in part by characteristics of the observational datasets. Overall our results suggest that current Earth system models have potential to accurately capture the effects of future emission reductions. [ABSTRACT FROM AUTHOR]

A huge amount of dust is transported every year from north Africa into the Caribbean region. This paper presents an investigation of this long-range transport process based on airborne Doppler wind lidar (DWL) measurements conducted during the SALTRACE campaign (June- July 2013), as well as an evaluation of the ability of the MACC (Monitoring Atmospheric Composition and Climate) global aerosol model to reproduce it and its associated features. Although both the modeled winds from MACC and the measurements from the DWL show a generally good agreement, some differences, particularly in the African easterly jet (AEJ) intensity, were noted. The observed differences between modeled and measured wind jet speeds are between 5 and 10ms-1. The vertical aerosol distribution within the Saharan dust plume and the marine boundary layer is investigated during the June-July 2013 period based on the MACC aerosol model results and the CALIOP satellite lidar measurements. While the modeled Saharan dust plume extent shows a good agreement with the measurements, a systematic underestimation of the marine boundary layer extinction is observed. Additionally, three selected case studies covering different aspects of the Saharan dust long-range transport along the west African coast, over the North Atlantic Ocean and the Caribbean are presented. For the first time, DWL measurements are used to investigate the Saharan dust long-range transport. Simultaneous wind and backscatter measurements from the DWL are used, in combination with the MACC model, to analyze different features associated with the longrange transport, including an African easterly wave trough, the AEJ and the intertropical convergence zone. [ABSTRACT FROM AUTHOR]

Source apportionment of PM 2.5 was performed using positive matrix factorization (PMF) based on detailed chemical composition data from 24 h filter samples collected over a 3-month period (August–November 2020) at an urban site in Montréal, a Canadian city with a population of approximately 4×106 people. This source apportionment study, which examined the main contributing sources to PM 2.5 using a larger suite of organic molecular markers than other Canadian studies, is the first of its sort in Canada. A focus of this study was on quantifying previously unresolved sources of PM 2.5 through the inclusion in the PMF analysis of additional organic molecular markers beyond those measured typically by the Canadian government's National Air Pollution Surveillance Program (NAPS). The organic species included in the PMF model were comprised of six n -alkanes, two fatty acids, one dicarboxylic acid, two biogenic secondary organic aerosol (SOA) tracers, and hopane. Secondary inorganic aerosols (SIAs) and SOAs were the dominant components and constituted 39 % of the measured PM 2.5 mass, while the local primary anthropogenic sources, namely traffic exhaust, road dust, industrial, and cooking emissions, contributed 23 %. The chemical transport model GEOS-Chem revealed that ammonium sulfate concentrations in Montréal are strongly influenced by both local sources in Quebec and transboundary input from the United States, with the transboundary input exceeding the local emissions for SOA. Co and Cr(VI) presented an elevated cancer risk, highlighting that more attention should be given to these trace metals, which were associated with industrial emissions by the PMF analysis. Furthermore, the results showed that industrial emissions were minor contributors to the total PM 2.5 mass concentration but were the largest contributors to Co and Cr(VI) concentrations. Thus, the health hazards associated with this source cannot be entirely established by the PM 2.5 mass concentration alone. This study highlights that, when evaluating air quality in Montréal and other urban regions, the prioritization of sources for mitigation strategies will diverge if one considers total PM 2.5 mass concentration or the concentration of individual particulate-bound contaminants. Furthermore, the large transboundary contribution from the United States to total PM 2.5 levels suggests that future municipal, provincial, and federal monitoring and regulations would be more effective if they focus on specific high-risk contaminants (e.g., Co and Cr(VI) rather than total PM 2.5). [ABSTRACT FROM AUTHOR]