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

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

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 highlatitude 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 dustemitting sediments from dust hotspots in Iceland (HLD region). Extensive analysis was conducted on samples of top sediments, sediments, and aeolian ripples collected from seven dust sources, with particular emphasis on the Jökulsá basin, encompassing the desert of Dyngjunsandur. Both fully and minimally dispersed PSDs and their respective mass median particle diameters revealed remarkable similarities (56 ± 69 and 55 ± 62 µm, respectively). Mineralogical analyses indicated the prevalence of amorphous phases (68 ± 26 %), feldspars (17 ± 13 %), and pyroxenes (9.3 ± 7.2 %), consistent with thorough analyses of VNIR reflectance spectra. The Fe content reached 9.5 ± 0.40 wt %, predominantly within silicate structures (80 ± 6.3 %), complemented by magnetite (16 ± 5.5 %), hematite/goethite (4.5 ± 2.7 %), and readily exchangeable Fe ions or Fe nano-oxides (1.6 ± 0.63 %). Icelandic top sediments exhibited coarser PSDs compared to the high dust-emitting crusts from mid-latitude arid regions, distinctive mineralogy, and a 3-fold bulk Fe content, with a significant presence of magnetite. The congruence between fully and minimally dispersed PSDs underscores reduced particle aggregation and cohesion of Icelandic top sediments, suggesting that aerodynamic entrainment of dust could also play a role upon emission in this region, alongside saltation bombardment. The extensive analysis in Dyngjusandur enabled the development of a conceptual model to encapsulate Iceland’s rapidly evolving high dust-emitting environments., This research has been supported by the European Research Council, EU H2020 European Research Council (grant no. 773051), the AXA Research Fund (AXA Chair on Sand and Dust Storms), the Agència de Gestió d’Ajuts Universitaris i de Recerca (grant no. 2020_FI B 00678), the Deutsche Forschungsgemeinschaft (grant nos. 264907654 and 416816480), and the Helmholtz Association (grant no. VH-NG-1533)., Peer Reviewed, Postprint (published version)

Understanding the atmospheric processes involving carbonaceous aerosols (CAs) is crucial for assessing air pollution impacts on human health and climate. The sources and formation mechanisms of CAs are not well understood, making it challenging to quantify impacts in models. Studies suggest residential wood combustion (RWC) and traffic significantly contribute to CAs in Europe’s urban and rural areas. Here, we used an atmospheric chemistry model (MONARCH) and three different emission inventories (two versions of the European-scale emission inventory CAMS-REG_v4 and the HERMESv3 detailed national inventory for Spain) to assess the uncertainties in CAs simulation and source allocation (from traffic, RWC, shipping, fires and others) in Northeast Spain. For this, black carbon (BC) and organic aerosol (OA) measurements performed at three supersites representing different environments (urban, regional and remote) were used. Our findings show the importance of model resolution and detailed emission input data in accurately reproducing BC/OA observations. Even though emissions of total particulate matter are rather consistent between inventories in Spain, we found discrepancies between them mainly related to the spatiotemporal disaggregation (particularly relevant for traffic and RWC) and the treatment of the condensable fraction of CAs in RWC (changes in the speciation of elemental/organic carbon). The main source contribution to BC concentrations in the urban site is traffic, accounting for (January/July) in close agreement with the fossil contribution derived from observations (), followed by RWC () and shipping emissions ( ). An over-representation of RWC (winter) and shipping (summer) is obtained with CAMS-REG_v4. Noteworthy uncertainties arise in OA results due to condensables in emissions and a limited secondary aerosol production in the model. These findings offer insights into MONARCH’s effectiveness in simulating CAs concentrations and source contribution in North, Hector Navarro-Barboza acknowledges financial support from the Spanish Ministry for Science and Innovation (FPI PRE2018-084988 financed by MCIN/AEI/10.13039/501100011033 and by ESF Investing in your future). The research leading to these results has received funding from the Ministerio de Ciencia, Innovación y Universidades as H. Navarro-Barboza et al. Environment International 183 (2024) 108252 18 part of the BROWNING project (Grant No. RTI2018-099894-B-I00 funded by MCIN/AEI/10.13039/501100011033 and by ”ERDF A way of making Europe”) and the Ministerio de Asuntos Económicos y Transformaciön Digital, Gobierno de España as part of the CAIAC project (Grant No. PID2019-108990 PB-100). This project has received funding from the Agencia Estatal Consejo Superior de Investigaciones Científicas (CSIC) under the Project 202030E261, and the Generalitat de Catalunya, by AGAUR (2021 SGR 00447) and the Direcció General de Qualitat Ambiental i Canvi Climàtic (DGQACC). This project has also received funding from the European Union’s Horizon Europe research and innovation programme under the RI-URBANs project (grant agreement No 101036245). IDAEA-CSIC is a Centre of Excellence Severo Ochoa (Spanish Ministry of Science and Innovation, Grant No. CEX2018- 000794-S). BSC researchers thankfully acknowledge the computer resources at Marenostrum and the technical support provided by Barcelona Supercomputing Center (RES-AECT-2021–1-0027, RES-AECT-2021–2-0001), Peer Reviewed, Postprint (published version)

The chemical and morphological properties of mineral dust aerosols emitted by wind erosion from arid and semi-arid regions influence climate, ocean, and land ecosystems; air quality; and multiple socio-economic sectors. However, there is an incomplete understanding of the emitted dust particle size distribution (PSD) in terms of its constituent minerals that typically result from the fragmentation of soil aggregates during wind erosion. The emitted dust PSD affects the duration of particle transport and thus each mineral's global distribution, along with its specific effect upon climate. This lack of understanding is largely due to the scarcity of relevant in situ measurements in dust sources. To advance our understanding of the physicochemical properties of the emitted dust PSD, we present insights into the elemental composition and morphology of individual dust particles collected during the FRontiers in dust minerAloGical coMposition and its Effects upoN climaTe (FRAGMENT) field campaign in the Moroccan Sahara in September 2019. We analyzed more than 300 000 freshly emitted individual particles by performing offline analysis in the laboratory using scanning electron microscopy (SEM) coupled with energy-dispersive X-ray spectrometry (EDX). Eight major particle-type classes were identified with clay minerals making up the majority of the analyzed particles both by number and mass, followed by quartz, whereas carbonates and feldspar contributed to a lesser extent. We provide an exhaustive analysis of the PSD and potential mixing state of different particle types, focusing largely on iron-rich (Fe oxide-hydroxides) and feldspar particles, which are key to the effects of dust upon radiation and clouds, respectively. Nearly pure or externally mixed Fe oxide-hydroxides are present mostly in diameters smaller than 2 µm, with the highest fraction below 1 µm at about 3.75 % abundance by mass. Fe oxide-hydroxides tend to be increasingly internally mixed with other minerals, The field campaign and its associated research, including this work, was primarily funded by the European Research Council under the Horizon 2020 research and innovation programme through the ERC Consolidator Grant FRAGMENT (grant agreement no. 773051) and the AXA Research Fund through the AXA Chair on Sand and Dust Storms at BSC. Cristina González-Flórez was supported by a PhD fellowship from the Agència de Gestió d'Ajuts Universitaris i de Recerca (AGAUR) grant 2020_FI B 00678. Konrad Kandler was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) (grant nos. 264907654 and 416816480). Martina Klose received funding through the Helmholtz Association's Initiative and Networking Fund (grant agreement no. VH-NG-1533)., Peer Reviewed, Postprint (published version)

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

Source apportionment (SA) techniques allocate the measured ambient pollutants with their potential source origin; thus, they are a powerful tool for designing air pollution mitigation strategies. Positive Matrix Factorization (PMF) is one of the most widely used SA approaches, and its multi-time resolution (MTR) methodology, which enables mixing different instrument data in their original time resolution, was the focus of this study. One year of co-located measurements in Barcelona, Spain, of non-refractory submicronic particulate matter (NR-PM1), black carbon (BC) and metals were obtained by a Q-ACSM (Aerodyne Research Inc.), an aethalometer (Aerosol d.o.o.) and fine offline quartz-fibre filters, respectively. These data were combined in a MTR PMF analysis preserving the high time resolution (30 min for the NR-PM1 and BC, and 24 h every 4th day for the offline samples). The MTR-PMF outcomes were assessed varying the time resolution of the high-resolution data subset and exploring the error weightings of both subsets. The time resolution assessment revealed that averaging the high-resolution data was disadvantageous in terms of model residuals and environmental interpretability. The MTR-PMF resolved eight PM1 sources: ammonium sulphate + heavy oil combustion (25%), ammonium nitrate + ammonium chloride (17%), aged secondary organic aerosol (SOA) (16%), traffic (14%), biomass burning (9%), fresh SOA (8%), cooking-like organic aerosol (5%), and industry (4%). The MTR-PMF technique identified two more sources relative to the 24 h base case data subset using the same species and four more with respect to the pseudo-conventional approach mimicking offline PMF, indicating that the combination of both high and low TR data is significantly beneficial for SA. Besides the higher number of sources, the MTR-PMF technique has enabled some sources disentanglement compared to the pseudo-conventional and base case PMF as well as the characterisation of their intra-day patterns.

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